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1. Highly Efficient Wideband Microwave Absorbers Based on Zero-Valent Fe@γ-Fe2O3 and Fe/Co/Ni Carbon-Protected Alloy Nanoparticles Supported on Reduced Graphene Oxide

Author

Francisco Mederos-Henry, Julien Mahin, Benoit P. Pichon, Marinela M. Dîrtu, Yann Garcia, Arnaud Delcorte, Christian Bailly, Isabelle Huynen, and Sophie Hermans

Subjects
magnetic nanoparticles, reduced graphene oxide, nanocomposites, microwave absorbing materials, electromagnetic interference shielding, Chemistry, QD1-999
Abstract

Electronic systems and telecommunication devices based on low-power microwaves, ranging from 2 to 40 GHz, have massively developed in the last decades. Their extensive use has contributed to the emergence of diverse electromagnetic interference (EMI) phenomena. Consequently, EMI shielding has become a ubiquitous necessity and, in certain countries, a legal requirement. Broadband absorption is considered the only convincing EMI shielding solution when the complete disappearance of the unwanted microwave is required. In this study, a new type of microwave absorber materials (MAMs) based on reduced graphene oxide (rGO) decorated with zero-valent Fe@γ-Fe2O3 and Fe/Co/Ni carbon-protected alloy nanoparticles (NPs) were synthesized using the Pechini sol-gel method. Synthetic parameters were varied to determine their influence on the deposited NPs size and spatial distribution. The deposited superparamagnetic nanoparticles were found to induce a ferromagnetic resonance (FMR) absorption process in all cases. Furthermore, a direct relationship between the nanocomposites’ natural FMR frequency and their composition-dependent saturation magnetization (Ms) was established. Finally, the microwave absorption efficiency (0.4 MHz to 20 GHz) of these new materials was found to range from 60% to 100%, depending on the nature of the metallic particles grafted onto rGO.

Published
2019
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2. Landscape structure and dispersal rate drive large scale catastrophic shifts in spatially explicit metapopulations

Author

Sonia Kéfi, Camille Saade, Emanuel A. Fronhofer, Benoit P. Pichon, Institut des Sciences de l'Evolution de Montpellier (UMR ISEM), Centre de Coopération Internationale en Recherche Agronomique pour le Développement (Cirad)-École Pratique des Hautes Études (EPHE), and Université Paris sciences et lettres (PSL)-Université Paris sciences et lettres (PSL)-Institut de recherche pour le développement [IRD] : UR226-Centre National de la Recherche Scientifique (CNRS)-Université de Montpellier (UM)

Subjects
bistability, Landscape structure, Spatial structure, Ecology, metapopulation, Metapopulation, space, Stability (probability), Hysteresis (economics), hysteresis, Environmental science, Biological dispersal, Ecosystem, [SDE.BE]Environmental Sciences/Biodiversity and Ecology, Scale (map), catastrophic shifts
Abstract

Even when environments deteriorate gradually, ecosystems may shift abruptly from one state to another. Such catastrophic shifts are difficult to predict and reverse (hysteresis). While well studied in simplified contexts, we lack a general understanding of how catastrophic shifts spread in realistic spatial contexts. For different types of landscape structure, including typical terrestrial modular and riverine dendritic networks, we here investigate landscape-scale stability in metapopulations made of bistable patches. We find that such metapopulations usually exhibit large scale catastrophic shifts and hysteresis, and that the properties of these shifts depend strongly on metapopulation spatial structure and dispersal rate: intermediate dispersal rates and a riverine spatial structure can largely reduce hysteresis size. Interestingly, our study suggests that large-scale restoration is easier with spatially clustered restoration efforts and in populations characterized by an intermediate dispersal rate.

Published
2023

4. Crossover from individual to collective magnetism in dense nanoparticle systems : local anisotropy versus dipolar interactions

Author

Elena H. Sánchez, Marianna Vasilakaki, Su Seong Lee, Peter S. Normile, Mikael S. Andersson, Roland Mathieu, Alberto López‐Ortega, Benoit P. Pichon, Davide Peddis, Chris Binns, Per Nordblad, Kalliopi Trohidou, Josep Nogués, José A. De Toro, Universidad Pública de Navarra. Departamento de Universidad Pública de Navarra. Departamento de Ciencias, Universidad Pública de Navarra / Nafarroako Unibertsitate Publikoa. INAMAT2 - Institute for Advanced Materials and Mathematics, Nafarroako Unibertsitate Publikoa. Nafarroako Unibertsitate Publikoa. Zientziak Saila Saila, Universidad Pública de Navarra / Nafarroako Unibertsitate Publikoa, Ministerio de Economía y Competitividad (España), European Commission, Ministerio de Ciencia, Innovación y Universidades (España), Agencia Estatal de Investigación (España), Swedish Research Council, Generalitat de Catalunya, and Universidad Pública de Navarra

Subjects
Dipolar interactions, General Chemistry, Cobalt, Condensed Matter Physics, Phase Transition, Biomaterials, Magnetics, Superspin glass, Magnetic nanoparticles, Anisotropy, Nanoparticles, General Materials Science, Den kondenserade materiens fysik, Magnetic anisotropy, Biotechnology
Abstract

Dense systems of magnetic nanoparticles may exhibit dipolar collective behavior. However, two fundamental questions remain unsolved: i) whether the transition temperature may be affected by the particle anisotropy or it is essentially determined by the intensity of the interparticle dipolar interactions, and ii) what is the minimum ratio of dipole–dipole interaction (Edd) to nanoparticle anisotropy (KefV, anisotropy⋅volume) energies necessary to crossover from individual to collective behavior. A series of particle assemblies with similarly intense dipolar interactions but widely varying anisotropy is studied. The Kef is tuned through different degrees of cobalt-doping in maghemite nanoparticles, resulting in a variation of nearly an order of magnitude. All the bare particle compacts display collective behavior, except the one made with the highest anisotropy particles, which presents “marginal” features. Thus, a threshold of KefV/Edd ≈ 130 to suppress collective behavior is derived, in good agreement with Monte Carlo simulations. This translates into a crossover value of ≈1.7 for the easily accessible parameter TMAX(interacting)/TMAX(non-interacting) (ratio of the peak temperatures of the zero-field-cooled magnetization curves of interacting and dilute particle systems), which is successfully tested against the literature to predict the individual-like/collective behavior of any given interacting particle assembly comprising relatively uniform particles., The authors acknowledge financial support from grant No. MAT2015-65295-R funded by MCIN/AEI/10.13039/501100011033 and by “ERDF A way of making Europe”, grant No. PID2019-106229RB-I00 funded by MCIN/AEI/10.13039/501100011033 and the Spanish MEC (through the contract No. BEAGAL18/00095). The authors also acknowledge funding from UCLM's Plan Propio, the Swedish Research Council (VR), the Universidad Pública de Navarra (grant No. PJUPNA2020) and the Generalitat de Catalunya (grant No. 2017-SGR-292). ICN2 is funded by the CERCA program/Generalitat de Catalunya and supported by SEV-2017-0706 grant funded by MCIN/AEI/10.13039/501100011033. K.T., D.P., and M.V. acknowledge support from the European Union's Horizon 2020 Programme: under gran agreement No. 731976 (MAGENTA) and partially the Horizon Europe EIC Pathfinder Programme: under grant agreement No. 101046909 (REMAP).

Published
2022

5. A detailed investigation of the core@shell structure of exchanged coupled magnetic nanoparticles after performing solvent annealing

Author

Kevin Sartori, Dris Ihiawakrim, Christophe Lefèvre, Solenn Reguer, Cristian Mocuta, Sylvie Bégin-Colin, Fadi Choueikani, Benoit P. Pichon, Lefevre, Christophe, Institut de Physique et Chimie des Matériaux de Strasbourg (IPCMS), Université de Strasbourg (UNISTRA)-Centre National de la Recherche Scientifique (CNRS)-Matériaux et Nanosciences Grand-Est (MNGE), Université de Strasbourg (UNISTRA)-Université de Haute-Alsace (UHA) Mulhouse - Colmar (Université de Haute-Alsace (UHA))-Institut National de la Santé et de la Recherche Médicale (INSERM)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS)-Université de Strasbourg (UNISTRA)-Université de Haute-Alsace (UHA) Mulhouse - Colmar (Université de Haute-Alsace (UHA))-Institut National de la Santé et de la Recherche Médicale (INSERM)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS)-Réseau nanophotonique et optique, Université de Strasbourg (UNISTRA)-Université de Haute-Alsace (UHA) Mulhouse - Colmar (Université de Haute-Alsace (UHA))-Centre National de la Recherche Scientifique (CNRS)-Université de Strasbourg (UNISTRA)-Centre National de la Recherche Scientifique (CNRS), Synchrotron SOLEIL (SSOLEIL), Centre National de la Recherche Scientifique (CNRS), Institut Universitaire de France (IUF), and Ministère de l'Education nationale, de l’Enseignement supérieur et de la Recherche (M.E.N.E.S.R.)

Subjects
[CHIM.MATE] Chemical Sciences/Material chemistry, Chemistry (miscellaneous), General Materials Science, [CHIM.MATE]Chemical Sciences/Material chemistry
Abstract

International audience; Thanks to important advances in synthesis techniques, a wide collection of bimagnetic core-shell nanoparticles with tunable properties was reported in the literature. Such nanoparticles may combine two phases with different intrinsic magnetic properties (magnetization, anisotropy, coercive field, etc.). Core-shell structures with large interfaces usually favor efficient exchange coupling between both phases that may result in the enhancement of the effective magnetic anisotropy energy and of the coercive field. In this context, the chemical composition and the crystal structure of the core/shell interface in nanoparticles are crucial parameters to modulate efficiently their magnetic properties. Here, we report on the solvent mediated thermal annealing of Fe 3Àd O 4 @CoO nanoparticles in a high boiling point solvent. The structure of nanoparticles was investigated before and after thermal annealing by advanced characterization techniques such as high resolution transmission electron microscopy (HR-TEM), X-ray absorption spectroscopy (XAS), X-ray magnetic circular dichroism (XMCD) and diffraction anomalous near edge structure (DANES). The combination of DANES and XAS/XMCD allowed studying the cationic distribution in spinel and wu ¨stite crystal structures as a function of site occupancy and oxidation state. To the best of our knowledge, it is the first time that DANES is performed to quantitatively investigate the chemical composition of biphasic metal oxide nanoparticles. Hence, we have investigated precisely the chemical composition of the spinel phase and that of the wu ¨stite phase. Besides the partial solubilisation of the CoO shell observed by HR-TEM, thermal annealing favors the formation of a thicker intermediate Co-doped ferrite layer at the spinel/wu ¨stite interface. Such significant modifications of the core@shell structure markedly influence interfacial coupling phenomena between the core and the shell, hence offering wide perspectives towards nanoparticles with tunable magnetic properties for a variety of applications.

Published
2022

6. A Detailed Investigation of the Onion Structure of Exchanged Coupled Magnetic Fe(3-delta)O4@CoFe2O4@Fe(3-delta)O4 Nanoparticles

Author

Anamaria Musat, Kevin Sartori, Simon Hettler, Fadi Choueikani, Sylvie Begin-Colin, Jean-Marc Greneche, Raul Arenal, Peter Bencok, Benoit P. Pichon, Paul Steadman, Agence Nationale de la Recherche (France), German Research Foundation, Ministerio de Economía y Competitividad (España), Agencia Estatal de Investigación (España), Ministerio de Ciencia, Innovación y Universidades (España), European Commission, Institut de Physique et Chimie des Matériaux de Strasbourg (IPCMS), Université de Strasbourg (UNISTRA)-Centre National de la Recherche Scientifique (CNRS)-Matériaux et Nanosciences Grand-Est (MNGE), Université de Strasbourg (UNISTRA)-Université de Haute-Alsace (UHA) Mulhouse - Colmar (Université de Haute-Alsace (UHA))-Institut National de la Santé et de la Recherche Médicale (INSERM)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS)-Université de Strasbourg (UNISTRA)-Université de Haute-Alsace (UHA) Mulhouse - Colmar (Université de Haute-Alsace (UHA))-Institut National de la Santé et de la Recherche Médicale (INSERM)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS)-Réseau nanophotonique et optique, Université de Strasbourg (UNISTRA)-Université de Haute-Alsace (UHA) Mulhouse - Colmar (Université de Haute-Alsace (UHA))-Centre National de la Recherche Scientifique (CNRS)-Université de Strasbourg (UNISTRA)-Centre National de la Recherche Scientifique (CNRS), Synchrotron SOLEIL (SSOLEIL), Centre National de la Recherche Scientifique (CNRS), Laboratoire Léon Brillouin (LLB - UMR 12), Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Paris-Saclay-Centre National de la Recherche Scientifique (CNRS), Institut des Molécules et Matériaux du Mans (IMMM), Le Mans Université (UM)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS), Instituto de Nanociencia y Materiales de Aragón (INMA), Consejo Superior de Investigaciones Científicas [Madrid] (CSIC)-Universidad de Zaragossa, Laboratorio de microscopias avanzadas (LMA), University of Zaragoza - Universidad de Zaragoza [Zaragoza], Fundación Agencia Aragonesa para la Investigación y el Desarrollo (ARAID), Institut Universitaire de France (IUF), and Ministère de l'Education nationale, de l’Enseignement supérieur et de la Recherche (M.E.N.E.S.R.)

Subjects
EELS, Materials science, Magnetism, Iron oxide, Nanoparticle, FOS: Physical sciences, 02 engineering and technology, 010402 general chemistry, 01 natural sciences, exchanged-coupling, chemistry.chemical_compound, onion-type, General Materials Science, X-ray absorption spectroscopy, Condensed Matter - Materials Science, XMCD, Magnetic circular dichroism, Electron energy loss spectroscopy, Materials Science (cond-mat.mtrl-sci), [CHIM.MATE]Chemical Sciences/Material chemistry, 021001 nanoscience & nanotechnology, 0104 chemical sciences, Condensed Matter - Other Condensed Matter, chemistry, Chemical engineering, magnetism, Mössbauer, nanoparticles, 0210 nano-technology, Iron oxide nanoparticles, Superparamagnetism, Other Condensed Matter (cond-mat.other)
Abstract

Nanoparticles that combine several magnetic phases offer wide perspectives for cutting edge applications because of the high modularity of their magnetic properties. Besides the addition of the magnetic characteristics intrinsic to each phase, the interface that results from core–shell and, further, from onion structures leads to synergistic properties such as magnetic exchange coupling. Such a phenomenon is of high interest to overcome the superparamagnetic limit of iron oxide nanoparticles which hampers potential applications such as data storage or sensors. In this manuscript, we report on the design of nanoparticles with an onion-like structure which has been scarcely reported yet. These nanoparticles consist of a Fe3−δO4 core covered by a first shell of CoFe2O4 and a second shell of Fe3−δO4, e.g., a Fe3−δO4@CoFe2O4@Fe3−δO4 onion-like structure. They were synthesized through a multistep seed-mediated growth approach which consists consists in performing three successive thermal decomposition of metal complexes in a high-boiling-point solvent (about 300 °C). Although TEM micrographs clearly show the growth of each shell from the iron oxide core, core sizes and shell thicknesses markedly differ from what is suggested by the size increasing. We investigated very precisely the structure of nanoparticles in performing high resolution (scanning) TEM imaging and geometrical phase analysis (GPA). The chemical composition and spatial distribution of atoms were studied by electron energy loss spectroscopy (EELS) mapping and spectroscopy. The chemical environment and oxidation state of cations were investigated by 57Fe Mössbauer spectrometry, soft X-ray absorption spectroscopy (XAS) and X-ray magnetic circular dichroism (XMCD). The combination of these techniques allowed us to estimate the increase of Fe2+ content in the iron oxide core of the core@shell structure and the increase of the cobalt ferrite shell thickness in the core@shell@shell one, whereas the iron oxide shell appears to be much thinner than expected. Thus, the modification of the chemical composition as well as the size of the Fe3−δO4 core and the thickness of the cobalt ferrite shell have a high impact on the magnetic properties. Furthermore, the growth of the iron oxide shell also markedly modifies the magnetic properties of the core–shell nanoparticles, thus demonstrating the high potential of onion-like nanoparticles to accurately tune the magnetic properties of nanoparticles according to the desired applications., K.S. was supported by a PhD grant from the French Agence Nationale de la Recherche (ANR) under the reference ANR11-LABX-0058-NIE within the Investissement d’Avenir program ANR-10-IDEX-0002-02 and SOLEIL synchrotron/Laboratoire Léon Brillouin fellowship. The authors are grateful to SOLEIL synchrotron light source for providing the access to DEIMOS beamline and to DIAMOND synchrotron light source for providing access to BLADE beamline. HRSTEM and STEM-EELS studies were conducted at the Laboratorio de Microscopias Avanzadas, Universidad de Zaragoza, Spain. S.H. is grateful to DFG (HE 7675/1-1). R.A. gratefully acknowledges the support from the Spanish Ministry of Economy and Competitiveness (MINECO) and the MICINN through project grants MAT2016-79776-P (AEI/FEDER, UE) and PID2019-104739GB-100/AEI/10.13039/501100011033 as well as from the European Union H2020 program “ESTEEM3” (823717).

Published
2022
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7. Phosphate glasses containing monodisperse Fe3−δO4@SiO2 stellate nanoparticles obtained by melt-quenching process

Author

Marcelo Nalin, Juliane Resges Orives, Damien Mertz, Benoit P. Pichon, Wesley Renato Viali, Sidney José Lima Ribeiro, Kevin Sartori, Sylvie Begin-Colin, Universidade Estadual Paulista (Unesp), UMR 7504, Institut de Physique et Chimie des Matériaux de Strasbourg (IPCMS), Université de Strasbourg (UNISTRA)-Matériaux et nanosciences d'Alsace (FMNGE), Institut de Chimie du CNRS (INC)-Université de Strasbourg (UNISTRA)-Université de Haute-Alsace (UHA) Mulhouse - Colmar (Université de Haute-Alsace (UHA))-Institut National de la Santé et de la Recherche Médicale (INSERM)-Centre National de la Recherche Scientifique (CNRS)-Institut de Chimie du CNRS (INC)-Université de Strasbourg (UNISTRA)-Université de Haute-Alsace (UHA) Mulhouse - Colmar (Université de Haute-Alsace (UHA))-Institut National de la Santé et de la Recherche Médicale (INSERM)-Centre National de la Recherche Scientifique (CNRS)-Centre National de la Recherche Scientifique (CNRS)-Réseau nanophotonique et optique, and Centre National de la Recherche Scientifique (CNRS)-Université de Strasbourg (UNISTRA)-Université de Haute-Alsace (UHA) Mulhouse - Colmar (Université de Haute-Alsace (UHA))-Centre National de la Recherche Scientifique (CNRS)-Université de Strasbourg (UNISTRA)

Subjects
Materials science, Dispersity, Physics::Optics, Nanoparticle, [CHIM.THER]Chemical Sciences/Medicinal Chemistry, 02 engineering and technology, 01 natural sciences, Iron oxide nanoparticles, chemistry.chemical_compound, Coacervate, 0103 physical sciences, Materials Chemistry, Magnetic materials, Bimetallic strip, ComputingMilieux_MISCELLANEOUS, 010302 applied physics, Nanocomposite, Process Chemistry and Technology, Thermal decomposition, [CHIM.MATE]Chemical Sciences/Material chemistry, Mesoporous silica, 021001 nanoscience & nanotechnology, Surfaces, Coatings and Films, Electronic, Optical and Magnetic Materials, Condensed Matter::Soft Condensed Matter, chemistry, Chemical engineering, Ceramics and Composites, Magnetic nanoparticles, Glass, 0210 nano-technology
Abstract

Made available in DSpace on 2020-12-12T01:15:00Z (GMT). No. of bitstreams: 0 Previous issue date: 2020-06-01 Conselho Nacional de Desenvolvimento Científico e Tecnológico (CNPq) Fundação de Amparo à Pesquisa do Estado de São Paulo (FAPESP) Coordenação de Aperfeiçoamento de Pessoal de Nível Superior (CAPES) The challenge to obtain stable glasses containing monodisperse magnetic nanoparticles with controlled size and shape is an exciting and almost unexplored field of research. Such new materials can be used in magneto-photonics or ultra-sensitive magnetic sensors. In this work, for the first time, colorless and transparent bulk glasses containing monodisperse 20 nm Fe3−δO4 nanoparticles were prepared by a melt-quenching route. Magnetic nanoparticles were synthesized by thermal decomposition and covered with a stellate mesoporous silica shell in order to protect them against dissolution during the glass melting process. The incorporation of nanoparticles into glasses and the ideal parameters obtained for this system are discussed. The new nanocomposite materials were characterized in order to investigate the structure, thermal, and magnetic properties. Such an original approach is a very promising way to incorporate a wide panel of nanoparticles, including metallic, bimetallic and metal oxide nanoparticles, into a variety of glasses providing new properties to these materials. São Paulo State University - UNESP Institute of Chemistry, P. O. Box 355 Université de Strasbourg CNRS Institut de Physique et Chimie des Matériaux de Strasbourg UMR 7504 São Paulo State University - UNESP Institute of Chemistry, P. O. Box 355 CNPq: 153762/2018-7 FAPESP: 2013/07793-6 FAPESP: 2018/07727-7 FAPESP: 2019/19609-1 CAPES: 88881.134870/2016-01

Published
2020

8. Increasing the size of Fe3-δO4 Nanoparticles by Performing a Multistep Seed-Mediated Growth Approach

Author

Jean-Marc Greneche, Paula Duenas-Ramirez, Corinne Bouillet, Diane Gailly, Benoit P. Pichon, Kevin Sartori, Sylvie Begin-Colin, Fadi Choueikani, Institut des Molécules et Matériaux du Mans (IMMM), Le Mans Université (UM)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS), Institut de Physique et Chimie des Matériaux de Strasbourg (IPCMS), Université de Strasbourg (UNISTRA)-Centre National de la Recherche Scientifique (CNRS)-Matériaux et Nanosciences Grand-Est (MNGE), Université de Strasbourg (UNISTRA)-Université de Haute-Alsace (UHA) Mulhouse - Colmar (Université de Haute-Alsace (UHA))-Institut National de la Santé et de la Recherche Médicale (INSERM)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS)-Université de Strasbourg (UNISTRA)-Université de Haute-Alsace (UHA) Mulhouse - Colmar (Université de Haute-Alsace (UHA))-Institut National de la Santé et de la Recherche Médicale (INSERM)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS)-Réseau nanophotonique et optique, Université de Strasbourg (UNISTRA)-Université de Haute-Alsace (UHA) Mulhouse - Colmar (Université de Haute-Alsace (UHA))-Centre National de la Recherche Scientifique (CNRS)-Université de Strasbourg (UNISTRA)-Centre National de la Recherche Scientifique (CNRS), Synchrotron SOLEIL (SSOLEIL), Centre National de la Recherche Scientifique (CNRS), Laboratoire Léon Brillouin (LLB - UMR 12), Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Paris-Saclay-Centre National de la Recherche Scientifique (CNRS), Institut Universitaire de France (IUF), and Ministère de l'Education nationale, de l’Enseignement supérieur et de la Recherche (M.E.N.E.S.R.)

Subjects
[PHYS]Physics [physics], Materials science, 010405 organic chemistry, Thermal decomposition, Nanoparticle, General Chemistry, 010402 general chemistry, Condensed Matter Physics, 01 natural sciences, 0104 chemical sciences, Magnetite, chemistry.chemical_compound, chemistry, Chemical engineering, Metal oxide nanoparticles, Stearate, Magnetic properties, Nanoparticles, General Materials Science, Seed mediated, [PHYS.COND]Physics [physics]/Condensed Matter [cond-mat], Transmission electron microscopy, ComputingMilieux_MISCELLANEOUS, Iron oxide nanoparticles
Abstract

International audience; Iron oxide nanoparticles were synthesized by an original multistep seed-mediated growth approach. The thermal decomposition of an iron stearate precursor was performed successively up to 5 times to produce nanoparticles with a narrow size distribution from 6.4 to 15.0 nm. The chemical composition and crystal structure of each set of nanoparticles was characterized by TEM, FT-IR, XRD, and Mössbauer spectrometry. Each layer was successively grown at the surface of a pristine Fe3-δO4 nanoparticle by epitaxial relationship and resulted in a single crystal structure. An intermediate wash after each thermal decomposition step resulted in the surface oxidation of each layer. Therefore, the maghemite phase increased relative to the magnetite phase as the nanoparticle expanded. Finally, the study of the magnetic properties by SQUID magnetometry showed the trend of the magnetic anisotropy energy to increase as a function of the nanoparticle size. In contrast, the coercive field and the magnetization saturation display nonmonotonic variations that may result from the interplay of intrinsic and collective properties.

Published
2020

9. Effect of Dipolar Interactions on the Assembly Process of Iron Oxide Nanoparticles Promoted by the CuAAC 'Click' Chemistry Reaction

Author

Yu-ting Lei, Céline Kiefer, Benoit P. Pichon, Mathias Dolci, Lise-Marie Lacroix, Sylvie Begin-Colin, Cédric Leuvrey, Institut de Physique et Chimie des Matériaux de Strasbourg (IPCMS), Université de Strasbourg (UNISTRA)-Matériaux et nanosciences d'Alsace (FMNGE), Institut de Chimie du CNRS (INC)-Université de Strasbourg (UNISTRA)-Université de Haute-Alsace (UHA) Mulhouse - Colmar (Université de Haute-Alsace (UHA))-Institut National de la Santé et de la Recherche Médicale (INSERM)-Centre National de la Recherche Scientifique (CNRS)-Institut de Chimie du CNRS (INC)-Université de Strasbourg (UNISTRA)-Université de Haute-Alsace (UHA) Mulhouse - Colmar (Université de Haute-Alsace (UHA))-Institut National de la Santé et de la Recherche Médicale (INSERM)-Centre National de la Recherche Scientifique (CNRS)-Centre National de la Recherche Scientifique (CNRS)-Réseau nanophotonique et optique, Centre National de la Recherche Scientifique (CNRS)-Université de Strasbourg (UNISTRA)-Université de Haute-Alsace (UHA) Mulhouse - Colmar (Université de Haute-Alsace (UHA))-Centre National de la Recherche Scientifique (CNRS)-Université de Strasbourg (UNISTRA), and Université Louis Pasteur - Strasbourg I-Centre National de la Recherche Scientifique (CNRS)

Subjects
Materials science, Kinetics, Iron oxide, Nanoparticle, Nanotechnology, 02 engineering and technology, 010402 general chemistry, 021001 nanoscience & nanotechnology, 01 natural sciences, Cycloaddition, 0104 chemical sciences, Surfaces, Coatings and Films, Electronic, Optical and Magnetic Materials, Nanomaterials, chemistry.chemical_compound, General Energy, chemistry, Click chemistry, Magnetic nanoparticles, [SPI.NANO]Engineering Sciences [physics]/Micro and nanotechnologies/Microelectronics, Physical and Theoretical Chemistry, 0210 nano-technology, Iron oxide nanoparticles
Abstract

Nanoparticle assemblies are very attractive because they allow the fine-tuning of magnetic properties by taking advantage of collective behavior ruled by interparticle interactions. Nevertheless, great efforts to control the spatial arrangement of nanoparticles still have to be developed in order to integrate such nanomaterials in devices for applications in fields such as sensors and recording media. Herein, we report on the assembly of iron oxide magnetic nanoparticles promoted by copper-catalyzed alkyne-azide cycloaddition (CuAAC) “click” reaction. Azido-terminated nanoparticles were assembled onto alkyne-terminated gold substrates. The assembly mechanism was investigated by monitoring the density of nanoparticles as a function of their size and concentration. The kinetics of the assembly process is exponential and is favored by the increase of the nanoparticle size and of the concentration. We show that the assembly of nanoparticles is controlled by the random sequential adsorption (RSA) mechanism below a critical size. In contrast, large nanoparticles allow strong dipolar interactions which participate actively in the assembly process, thus they avoid the RSA pathway. These two different mechanism pathways have a significant influence on the spatial arrangement of nanoparticles. The RSA results in rather isolated small nanoparticles at the earliest reaction times which become gradually a discontinuous monolayer. In contrast, the dipolar interaction assisted RSA mechanism (DIA-RSA) favors linear or 2D small assemblies which quickly grow in tight-packed monolayers of nanoparticles. Finally, the magnetic collective properties of these assemblies are markedly favored by the increase of the nanoparticle size.

Published
2019

10. A Detailed Investigation of the Onion Structure of Exchanged Coupled Magnetic Fe

Author

Kevin, Sartori, Anamaria, Musat, Fadi, Choueikani, Jean-Marc, Grenèche, Simon, Hettler, Peter, Bencok, Sylvie, Begin-Colin, Paul, Steadman, Raul, Arenal, and Benoit P, Pichon

Abstract

Nanoparticles that combine several magnetic phases offer wide perspectives for cutting edge applications because of the high modularity of their magnetic properties. Besides the addition of the magnetic characteristics intrinsic to each phase, the interface that results from core-shell and, further, from onion structures leads to synergistic properties such as magnetic exchange coupling. Such a phenomenon is of high interest to overcome the superparamagnetic limit of iron oxide nanoparticles which hampers potential applications such as data storage or sensors. In this manuscript, we report on the design of nanoparticles with an onion-like structure which has been scarcely reported yet. These nanoparticles consist of a Fe

Published
2021

11. Iron Stearate Structures: An Original Tool for Nanoparticles Design

Author

Jean-Marc Strub, Nathalie Parizel, Benoît Heinrich, Damien Mertz, Céline Kiefer, Benoit P. Pichon, Sarah Cianférani, Sylvie Begin-Colin, Geoffrey Cotin, Francis Perton, Jean-Marc Greneche, Institut de Physique et Chimie des Matériaux de Strasbourg (IPCMS), Université de Strasbourg (UNISTRA)-Matériaux et nanosciences d'Alsace (FMNGE), Institut de Chimie du CNRS (INC)-Université de Strasbourg (UNISTRA)-Université de Haute-Alsace (UHA) Mulhouse - Colmar (Université de Haute-Alsace (UHA))-Institut National de la Santé et de la Recherche Médicale (INSERM)-Centre National de la Recherche Scientifique (CNRS)-Institut de Chimie du CNRS (INC)-Université de Strasbourg (UNISTRA)-Université de Haute-Alsace (UHA) Mulhouse - Colmar (Université de Haute-Alsace (UHA))-Institut National de la Santé et de la Recherche Médicale (INSERM)-Centre National de la Recherche Scientifique (CNRS)-Centre National de la Recherche Scientifique (CNRS)-Réseau nanophotonique et optique, Centre National de la Recherche Scientifique (CNRS)-Université de Strasbourg (UNISTRA)-Université de Haute-Alsace (UHA) Mulhouse - Colmar (Université de Haute-Alsace (UHA))-Centre National de la Recherche Scientifique (CNRS)-Université de Strasbourg (UNISTRA), Département Sciences Analytiques et Interactions Ioniques et Biomoléculaires (DSA-IPHC), Institut Pluridisciplinaire Hubert Curien (IPHC), Institut National de Physique Nucléaire et de Physique des Particules du CNRS (IN2P3)-Université de Strasbourg (UNISTRA)-Centre National de la Recherche Scientifique (CNRS)-Institut National de Physique Nucléaire et de Physique des Particules du CNRS (IN2P3)-Université de Strasbourg (UNISTRA)-Centre National de la Recherche Scientifique (CNRS), Institut des Molécules et Matériaux du Mans (IMMM), Le Mans Université (UM)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS), Institut de Chimie de Strasbourg, Université de Strasbourg (UNISTRA)-Centre National de la Recherche Scientifique (CNRS)-Institut de Chimie du CNRS (INC), RENARD (TGE Réseau National de RPE interdisciplinaire - 3443 ), Aix Marseille Université (AMU)-Université de Strasbourg (UNISTRA)-Ecole Nationale Supérieure de Chimie de Paris - Chimie ParisTech-PSL (ENSCP), Université Paris sciences et lettres (PSL)-Université Paris sciences et lettres (PSL)-Institut de Chimie du CNRS (INC)-Université de Lille-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS)-Université de Paris (UP)-Laboratoire de Chimie et de Biochimie Pharmacologiques et Toxicologiques (LCBPT - UMR 8601), Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS)-Université de Paris (UP)-Centre National de la Recherche Scientifique (CNRS)-Université de Paris (UP)-Université Grenoble Alpes (UGA), Université de Strasbourg (UNISTRA)-Centre National de la Recherche Scientifique (CNRS)-Matériaux et Nanosciences Grand-Est (MNGE), Université de Strasbourg (UNISTRA)-Université de Haute-Alsace (UHA) Mulhouse - Colmar (Université de Haute-Alsace (UHA))-Institut National de la Santé et de la Recherche Médicale (INSERM)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS)-Université de Strasbourg (UNISTRA)-Université de Haute-Alsace (UHA) Mulhouse - Colmar (Université de Haute-Alsace (UHA))-Institut National de la Santé et de la Recherche Médicale (INSERM)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS)-Réseau nanophotonique et optique, Université de Strasbourg (UNISTRA)-Université de Haute-Alsace (UHA) Mulhouse - Colmar (Université de Haute-Alsace (UHA))-Centre National de la Recherche Scientifique (CNRS)-Université de Strasbourg (UNISTRA)-Centre National de la Recherche Scientifique (CNRS), Université de Strasbourg (UNISTRA)-Université de Haute-Alsace (UHA) Mulhouse - Colmar (Université de Haute-Alsace (UHA))-Institut National de Physique Nucléaire et de Physique des Particules du CNRS (IN2P3)-Centre National de la Recherche Scientifique (CNRS)-Université de Strasbourg (UNISTRA)-Université de Haute-Alsace (UHA) Mulhouse - Colmar (Université de Haute-Alsace (UHA))-Institut National de Physique Nucléaire et de Physique des Particules du CNRS (IN2P3)-Centre National de la Recherche Scientifique (CNRS), Université de Strasbourg (UNISTRA)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS), Université Paris sciences et lettres (PSL)-Université Paris sciences et lettres (PSL)-Institut de Chimie du CNRS (INC)-Université de Lille-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS)-Université Paris Cité (UPCité)-Laboratoire de Chimie et de Biochimie Pharmacologiques et Toxicologiques (LCBPT - UMR 8601), Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS)-Université Paris Cité (UPCité)-Centre National de la Recherche Scientifique (CNRS)-Université Paris Cité (UPCité)-Université Grenoble Alpes (UGA), Université de Strasbourg (UNISTRA)-Institut National de Physique Nucléaire et de Physique des Particules du CNRS (IN2P3)-Centre National de la Recherche Scientifique (CNRS)-Université de Strasbourg (UNISTRA)-Institut National de Physique Nucléaire et de Physique des Particules du CNRS (IN2P3)-Centre National de la Recherche Scientifique (CNRS), and Gaillard, Brigitte

Subjects
[CHIM.INOR] Chemical Sciences/Inorganic chemistry, 02 engineering and technology, [CHIM.INOR]Chemical Sciences/Inorganic chemistry, 010402 general chemistry, 01 natural sciences, Chloride, Catalysis, Inorganic Chemistry, chemistry.chemical_compound, Stearate, Polymer chemistry, medicine, Lamellar structure, Carboxylate, Physical and Theoretical Chemistry, iron stearate synthesis mechanisms, Thermal decomposition, nucleation mechanism, iron oxide nanoparticles, 021001 nanoscience & nanotechnology, 0104 chemical sciences, iron stearate, chemistry, Chimie/Chimie inorganique, iron stearate composition and structure, Stearic acid, 0210 nano-technology, Iron oxide nanoparticles, medicine.drug
Abstract

International audience; Iron carboxylates are widely used as iron precursors in the thermal decomposition process or considered as in situ formed intermediate precursors. Their molecular and three-dimensional (3D)-structural nature has been shown to affect the shape, size, and composition of the resulting iron oxide nanoparticles (NPs). Among carboxylate precursors, stearates are particularly attractive because of their higher stability to aging and hydration and they are used as additives in many applications. Despite the huge interest of iron stearates, very few studies aimed up to now at deciphering their full metal-ligand structures and the mechanisms allowing us to achieve in a controlled manner the bottom-up NP formation. In this work, we have thus investigated the molecular structure and composition of two iron stearate precursors, synthesized by introducing either two (FeSt2) or three (FeSt3) stearate (St) chains. Interestingly, both iron stearates consist of lamellar structures with planes of iron polynuclear complexes (polycations) separated with stearate chains in all-trans conformation. The iron content in polycations was found very different between both iron stearates. Their detailed characterizations indicate that FeSt2 is mainly composed of [Fe3-(μ3-O)St6·xH2O]Cl, with no (or few) free stearate, whereas FeSt3 is a mixture of mainly [Fe7(μ3-O(H))6(μ2-OH)xSt12–2x]St with some [Fe3(μ3-O)St6·xH2O]St and free stearic acid. The formation of bigger polynuclear complexes with FeSt3 was related to higher hydrolysis and condensation rates within the iron(III) chloride solution compared to the iron(II) chloride solution. These data suggested a nucleation mechanism based on the condensation of polycation radicals generated by the catalytic departure of two stearate chains from an iron polycation-based molecule.

Published
2021

12. Harnessing Composition of Iron Oxide Nanoparticle: Impact of Solvent-Mediated Ligand–Ligand Interaction and Competition between Oxidation and Growth Kinetics

Author

Valentin Begin, Damien Mertz, Corinne Petit, Christophe Lefevre, Geoffrey Cotin, Jean-Marc Greneche, Sylvie Begin-Colin, Francis Perton, Sécou Sall, Céline Kiefer, Benoit P. Pichon, Institut de Physique et Chimie des Matériaux de Strasbourg (IPCMS), Université de Strasbourg (UNISTRA)-Matériaux et nanosciences d'Alsace (FMNGE), Institut de Chimie du CNRS (INC)-Université de Strasbourg (UNISTRA)-Université de Haute-Alsace (UHA) Mulhouse - Colmar (Université de Haute-Alsace (UHA))-Institut National de la Santé et de la Recherche Médicale (INSERM)-Centre National de la Recherche Scientifique (CNRS)-Institut de Chimie du CNRS (INC)-Université de Strasbourg (UNISTRA)-Université de Haute-Alsace (UHA) Mulhouse - Colmar (Université de Haute-Alsace (UHA))-Institut National de la Santé et de la Recherche Médicale (INSERM)-Centre National de la Recherche Scientifique (CNRS)-Centre National de la Recherche Scientifique (CNRS)-Réseau nanophotonique et optique, Centre National de la Recherche Scientifique (CNRS)-Université de Strasbourg (UNISTRA)-Université de Haute-Alsace (UHA) Mulhouse - Colmar (Université de Haute-Alsace (UHA))-Centre National de la Recherche Scientifique (CNRS)-Université de Strasbourg (UNISTRA), Institut des Molécules et Matériaux du Mans (IMMM), and Le Mans Université (UM)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS)

Subjects
Chemistry, Growth kinetics, Ligand, General Chemical Engineering, media_common.quotation_subject, Iron oxide, Nanoparticle, 02 engineering and technology, General Chemistry, 010402 general chemistry, 021001 nanoscience & nanotechnology, 01 natural sciences, Competition (biology), 0104 chemical sciences, Solvent, chemistry.chemical_compound, Chemical engineering, Materials Chemistry, [CHIM]Chemical Sciences, Composition (visual arts), 0210 nano-technology, Stoichiometry, media_common
Abstract

International audience; The composition of metal oxide nanoparticles is of great importance for their applications because defects and/or deviation from stoechiometry strongly affect their physical properties. We report here on the crucial role of synthesis parameters such as solvent, ligand and iron precursors on the composition of spinel iron oxide nanoparticles synthesized by the thermal decomposition method. At first, the investigation of the thermal decomposition of iron stearates bearing either two or three stearate chains by thermogravimetric analysis, IR spectroscopy and Mössbauer spectrometry as a function of temperature and syntheses with only oleic acid and iron stearate confirmed that the composition of the first nuclei is wüstite Fe 1-x O. The synthesis of nanoparticles with high sizes requires the use of very high boiling point solvents to ensure an effective growth step. We observed that, when the grain growth and oxidation kinetics are similar, nanoparticles with a spinel composition and quite no defects are produced. An oxidation rate slower than the nuclei growth rate favours the formation of core-shell Fe 1-x O@Fe 3-x O 4 NPs. The oxidation kinetics is shown to be influenced by surfactant and solvent natures. Indeed, surfactants such as oleic acid form a dense monolayer at the nuclei surface which oxidation kinetics will depend on this monolayer permeability. Temperature, solvents with high surfactant affinity, deprotonated surfactants or decomposition products of solvents affect the monolayer stability and thus the nanoparticle composition. The solvents' nature and solvent mediated ligand-ligand interactions are thus evidenced to be important parameters to control the formation of defectsfree and stoechiometric oxide nanoparticles.

Published
2020

13. Investigation of the structure of iron oxide nanoparticle assemblies in order to optimize the sensitivity of surface plasmon resonance-based sensors

Author

Grégory Barbillon, Mathias Dolci, Benoit P. Pichon, Cédric Leuvrey, Julien Moreau, Sylvie Begin-Colin, Jean-François Bryche, Institut de Physique et Chimie des Matériaux de Strasbourg (IPCMS), Université de Strasbourg (UNISTRA)-Matériaux et nanosciences d'Alsace (FMNGE), Institut de Chimie du CNRS (INC)-Université de Strasbourg (UNISTRA)-Université de Haute-Alsace (UHA) Mulhouse - Colmar (Université de Haute-Alsace (UHA))-Institut National de la Santé et de la Recherche Médicale (INSERM)-Centre National de la Recherche Scientifique (CNRS)-Institut de Chimie du CNRS (INC)-Université de Strasbourg (UNISTRA)-Université de Haute-Alsace (UHA) Mulhouse - Colmar (Université de Haute-Alsace (UHA))-Institut National de la Santé et de la Recherche Médicale (INSERM)-Centre National de la Recherche Scientifique (CNRS)-Centre National de la Recherche Scientifique (CNRS)-Réseau nanophotonique et optique, Centre National de la Recherche Scientifique (CNRS)-Université de Strasbourg (UNISTRA)-Université de Haute-Alsace (UHA) Mulhouse - Colmar (Université de Haute-Alsace (UHA))-Centre National de la Recherche Scientifique (CNRS)-Université de Strasbourg (UNISTRA), Laboratoire Charles Fabry / Biophotonique, Laboratoire Charles Fabry (LCF), Institut d'Optique Graduate School (IOGS)-Université Paris-Saclay-Centre National de la Recherche Scientifique (CNRS)-Institut d'Optique Graduate School (IOGS)-Université Paris-Saclay-Centre National de la Recherche Scientifique (CNRS), Centre de Nanosciences et de Nanotechnologies (C2N), Université Paris-Saclay-Centre National de la Recherche Scientifique (CNRS), Ecole Polytechnique Féminine-Sceaux 92330 (EPF), Institut Universitaire de France (IUF), and Ministère de l'Education nationale, de l’Enseignement supérieur et de la Recherche (M.E.N.E.S.R.)

Subjects
Streptavidin, Materials science, Iron oxide, General Physics and Astronomy, Nanoparticle, Nanotechnology, 02 engineering and technology, 010402 general chemistry, 01 natural sciences, chemistry.chemical_compound, Thin film, Surface plasmon resonance, ComputingMilieux_MISCELLANEOUS, chemistry.chemical_classification, [PHYS.PHYS.PHYS-OPTICS]Physics [physics]/Physics [physics]/Optics [physics.optics], Biomolecule, Surface plasmon, Surfaces and Interfaces, General Chemistry, 021001 nanoscience & nanotechnology, Condensed Matter Physics, 0104 chemical sciences, Surfaces, Coatings and Films, chemistry, 0210 nano-technology, Biosensor
Abstract

Surface plasmon resonance (SPR) biosensors based on metal thin films are very attractive for detection of biomolecules. Nanoparticle assemblies were recently demonstrated to significantly enhance sensitivity. Here, we show that the fine control of the structure of nanoparticle assemblies is critical to optimize the sensitivity. Iron oxide (Fe3-δO4) nanoparticles were assembled onto a gold thin film by performing the Copper Catalyzed Alkyne-Azide cycloaddition (CuAAC) “click” reaction. A biotin derivative was grafted by CuAAC at the surface of nanoparticle assemblies in order to detect streptavidin (SA). The fine control of the size and of the density of nanoparticles allowed tuning the surface plasmon waves at the surface of the gold thin film in order to optimize the response of the sensors. The accessibility of biotin at the nanoparticle surface to SA was also investigated as a function of the interparticle distance. We show that the interplay between the volume fraction of iron oxide and the accessibility of biotin at the nanoparticle surface is critical to enhance the sensitivity of SPR sensors.

Published
2020

14. Investigation of the Collective Properties in Monolayers of Exchange-Biased Fe3−δO4@CoO Core–Shell Nanoparticles

Author

Xiaojie Liu, Yu Liu, Sylvie Begin-Colin, Mathias Dolci, Dominique Begin, Elodie Pardieu, Alain Derory, Benoit P. Pichon, Cédric Leuvrey, Institut de Physique et Chimie des Matériaux de Strasbourg (IPCMS), Université de Strasbourg (UNISTRA)-Matériaux et nanosciences d'Alsace (FMNGE), Institut de Chimie du CNRS (INC)-Université de Strasbourg (UNISTRA)-Université de Haute-Alsace (UHA) Mulhouse - Colmar (Université de Haute-Alsace (UHA))-Institut National de la Santé et de la Recherche Médicale (INSERM)-Centre National de la Recherche Scientifique (CNRS)-Institut de Chimie du CNRS (INC)-Université de Strasbourg (UNISTRA)-Université de Haute-Alsace (UHA) Mulhouse - Colmar (Université de Haute-Alsace (UHA))-Institut National de la Santé et de la Recherche Médicale (INSERM)-Centre National de la Recherche Scientifique (CNRS)-Centre National de la Recherche Scientifique (CNRS)-Réseau nanophotonique et optique, Centre National de la Recherche Scientifique (CNRS)-Université de Strasbourg (UNISTRA)-Université de Haute-Alsace (UHA) Mulhouse - Colmar (Université de Haute-Alsace (UHA))-Centre National de la Recherche Scientifique (CNRS)-Université de Strasbourg (UNISTRA), Université Louis Pasteur - Strasbourg I-Centre National de la Recherche Scientifique (CNRS), Institut de chimie et procédés pour l'énergie, l'environnement et la santé (ICPEES), and Institut de Chimie du CNRS (INC)-Université de Strasbourg (UNISTRA)-Université de Haute-Alsace (UHA) Mulhouse - Colmar (Université de Haute-Alsace (UHA))-Institut National de la Santé et de la Recherche Médicale (INSERM)-Centre National de la Recherche Scientifique (CNRS)-Institut de Chimie du CNRS (INC)-Université de Strasbourg (UNISTRA)-Université de Haute-Alsace (UHA) Mulhouse - Colmar (Université de Haute-Alsace (UHA))-Institut National de la Santé et de la Recherche Médicale (INSERM)-Centre National de la Recherche Scientifique (CNRS)-Centre National de la Recherche Scientifique (CNRS)

Subjects
Materials science, [PHYS.PHYS]Physics [physics]/Physics [physics], Nanoparticle, Context (language use), 02 engineering and technology, 021001 nanoscience & nanotechnology, 01 natural sciences, Surfaces, Coatings and Films, Electronic, Optical and Magnetic Materials, Magnetic anisotropy, General Energy, Exchange bias, Chemical physics, Ferrimagnetism, 0103 physical sciences, Monolayer, Antiferromagnetism, Physical and Theoretical Chemistry, 010306 general physics, 0210 nano-technology, Anisotropy
Abstract

Owing to its potential to enhance the effective magnetic anisotropy energy of nanoparticles, exchange bias has been extensively studied during the last few years. Although most of studies have been conducted in the powder state, the effect of the dimensionality of nanoparticle assemblies has been scarcely investigated. In this context, we report on the study of the collective properties of monolayers of exchange-biased nanoparticles with different core–shell structures. Nanoparticles consist in a ferrimagnetic Fe3−δO4 core coated with an antiferromagnetic CoO shell. They were assembled in monolayers with local order by using the Langmuir–Blodgett technique. Exchange bias is significantly altered in 2D assemblies in comparison to powder samples which can be assimilated to 3D random assemblies. We show that exchange bias in Fe3−δO4@CoO nanoparticles is directly influenced by dipolar interactions between Fe3−δO4 cores, which are enhanced by shape anisotropy of 2D assemblies. Besides the dramatic influence of...

Published
2018

15. Effect of reaction environment andin situformation of the precursor on the composition and shape of iron oxide nanoparticles synthesized by the thermal decomposition method

Author

Benoit P. Pichon, Jean-Marc Greneche, Walid Baaziz, Sylvie Begin-Colin, Institut de chimie et procédés pour l'énergie, l'environnement et la santé (ICPEES), Université de Strasbourg (UNISTRA)-Matériaux et nanosciences d'Alsace (FMNGE), Institut de Chimie du CNRS (INC)-Université de Strasbourg (UNISTRA)-Université de Haute-Alsace (UHA) Mulhouse - Colmar (Université de Haute-Alsace (UHA))-Institut National de la Santé et de la Recherche Médicale (INSERM)-Centre National de la Recherche Scientifique (CNRS)-Institut de Chimie du CNRS (INC)-Université de Strasbourg (UNISTRA)-Université de Haute-Alsace (UHA) Mulhouse - Colmar (Université de Haute-Alsace (UHA))-Institut National de la Santé et de la Recherche Médicale (INSERM)-Centre National de la Recherche Scientifique (CNRS)-Centre National de la Recherche Scientifique (CNRS), Institut de Physique et Chimie des Matériaux de Strasbourg (IPCMS), Institut de Chimie du CNRS (INC)-Université de Strasbourg (UNISTRA)-Université de Haute-Alsace (UHA) Mulhouse - Colmar (Université de Haute-Alsace (UHA))-Institut National de la Santé et de la Recherche Médicale (INSERM)-Centre National de la Recherche Scientifique (CNRS)-Institut de Chimie du CNRS (INC)-Université de Strasbourg (UNISTRA)-Université de Haute-Alsace (UHA) Mulhouse - Colmar (Université de Haute-Alsace (UHA))-Institut National de la Santé et de la Recherche Médicale (INSERM)-Centre National de la Recherche Scientifique (CNRS)-Centre National de la Recherche Scientifique (CNRS)-Réseau nanophotonique et optique, Centre National de la Recherche Scientifique (CNRS)-Université de Strasbourg (UNISTRA)-Université de Haute-Alsace (UHA) Mulhouse - Colmar (Université de Haute-Alsace (UHA))-Centre National de la Recherche Scientifique (CNRS)-Université de Strasbourg (UNISTRA), and Université Louis Pasteur - Strasbourg I-Centre National de la Recherche Scientifique (CNRS)

Subjects
Materials science, Thermal decomposition, Spinel, 02 engineering and technology, General Chemistry, engineering.material, 010402 general chemistry, 021001 nanoscience & nanotechnology, Condensed Matter Physics, 01 natural sciences, 0104 chemical sciences, chemistry.chemical_compound, chemistry, Chemical engineering, Stearate, Ferrimagnetism, Transmission electron microscopy, [CHIM.CRIS]Chemical Sciences/Cristallography, engineering, General Materials Science, 0210 nano-technology, Saturation (magnetic), Iron oxide nanoparticles, Mossbauer spectrometry
Abstract

In this work, we investigate the effect of the reaction environment and the in situ formation of an iron precursor on the synthesis of iron oxide nanoparticles (IONPs) through thermal decomposition. Spherical IONPs with a spinel Fe3-xO4 structure were synthesized reproducibly through the thermal decomposition of iron stearate (Fe(stearate)(2)) assisted by oleic acid in octyl ether or eicosene solvents under air. Under similar conditions and by adjusting only the reaction environment, namely under argon, core-shell FeO@Fe3-xO4 NPs with the same sizes were obtained. On the other hand, the thermal decomposition of iron oleate (Fe(oleate)(3)) in the presence of a mixture of oleic acid and sodium oleate, under air and argon, leads to the formation of cubic-shaped NPs with a similar FeO@Fe3-xO4 structure. Cubic NPs with a homogenous Fe3-xO4 composition were synthesized from the iron oleate formed in situ from FeCl(3)6H(2)O and sodium oleate reactants, which was immediately decomposed. The composition and shape dependence on the experimental conditions, i.e. atmosphere and iron complex, is discussed. The synthesized NPs were characterized by combining several techniques including transmission electron microscopy (TEM), scanning-TEM, X-ray diffraction (XRD) and Fe-57 Mossbauer spectrometry. The correlation between the crystalline composition and the magnetic properties was investigated by carrying out magnetization measurements as a function of the applied field and temperature. The spherical and cubic-shaped NPs with a core-shell structure display exchange bias coupling due to the interaction between the antiferromagnetic (AFM) core and the ferrimagnetic (FiM) layer at the surface, while the Fe3-xO4 NPs exhibit a saturation magnetisation lower than that for the bulk counterpart due to the oxidation effects and the presence of a spin canted layer at their surface.

Published
2018

16. Synergistic photo optical and magnetic properties of a hybrid nanocomposite consisting of a zinc oxide nanorod array decorated with iron oxide nanoparticles

Author

Spyridon Zafairatos, Brandon Azeredo, Cédric Leuvrey, Pierre Gilliot, Mathieu Gallart, Anne Carton, Céline Kiefer, Benoit P. Pichon, Dris Ihawakrim, Centre Régional de Ressources du Développement rural (CRDR), Centre Régional de Ressources du Développement rural, Institut de Physique et Chimie des Matériaux de Strasbourg (IPCMS), Université Louis Pasteur - Strasbourg I-Centre National de la Recherche Scientifique (CNRS), Université de Strasbourg (UNISTRA)-Matériaux et nanosciences d'Alsace (FMNGE), Institut de Chimie du CNRS (INC)-Université de Strasbourg (UNISTRA)-Université de Haute-Alsace (UHA) Mulhouse - Colmar (Université de Haute-Alsace (UHA))-Institut National de la Santé et de la Recherche Médicale (INSERM)-Centre National de la Recherche Scientifique (CNRS)-Institut de Chimie du CNRS (INC)-Université de Strasbourg (UNISTRA)-Université de Haute-Alsace (UHA) Mulhouse - Colmar (Université de Haute-Alsace (UHA))-Institut National de la Santé et de la Recherche Médicale (INSERM)-Centre National de la Recherche Scientifique (CNRS)-Centre National de la Recherche Scientifique (CNRS)-Réseau nanophotonique et optique, and Centre National de la Recherche Scientifique (CNRS)-Université de Strasbourg (UNISTRA)-Université de Haute-Alsace (UHA) Mulhouse - Colmar (Université de Haute-Alsace (UHA))-Centre National de la Recherche Scientifique (CNRS)-Université de Strasbourg (UNISTRA)

Subjects
Materials science, Iron oxide, Nanoparticle, 02 engineering and technology, 010402 general chemistry, 7. Clean energy, 01 natural sciences, chemistry.chemical_compound, X-ray photoelectron spectroscopy, Materials Chemistry, [CHIM]Chemical Sciences, ComputingMilieux_MISCELLANEOUS, [PHYS]Physics [physics], Nanocomposite, [CHIM.ORGA]Chemical Sciences/Organic chemistry, General Chemistry, Coercivity, 021001 nanoscience & nanotechnology, 0104 chemical sciences, Chemical engineering, chemistry, [PHYS.COND.CM-MS]Physics [physics]/Condensed Matter [cond-mat]/Materials Science [cond-mat.mtrl-sci], Magnetic nanoparticles, Nanorod, 0210 nano-technology, Iron oxide nanoparticles
Abstract

Multifunctional nanocomposite materials recently emerged as a powerful concept because they offer to combine physical properties of different inorganic materials. Besides the simple combination of physical properties, the real challenge is to provide high control of the structure of nanocomposites (i.e. the spatial arrangement of the two entities, interface or separating distance, etc.). In this case, synergy between the two entities may be favoured in order to dramatically enhance the physical properties. Herein, we report on a multifunctional hybrid nanocomposite material consisting of a zinc oxide (ZnO) nanorod array decorated with iron oxide (Fe3−δO4) nanoparticles through a 1,4-phenylenebis(phosphonic acid) (PBA) linkage. We report on an original, easy to process, and versatile preparation method based on self-assembly mediated by specific interactions between metal oxides and phosphonic acid groups. This strategy allows grafting irreversibly Fe3−δO4 nanoparticles to ZnO nanorod arrays while preserving the pristine crystal structure of both inorganic entities. The structure and physical properties of such hybrid nanocomposites were investigated by means of a large panel of characterisation techniques: SEM, TEM, FTIR, XPS, SQUID and PL. The assembly mechanism was studied by varying several experimental parameters, such as the concentration of the ligand solution and nanoparticle suspension as well as the reaction time of ZnO arrays in the aforementioned suspensions. Finally, we show for the first time that the ZnO/PBA/Fe3−δO4 nanocomposite displays enhanced magnetic and optical properties as a result of dual synergy. We show unambiguously that a ZnO nanorod array acts as a very efficient anisotropic scaffold which favours unidirectional dipolar interactions and enhances the in-axis collective magnetic properties of Fe3−δO4 nanoparticles (a 10-fold increase of the coercive field in comparison to the same magnetic nanoparticles in the powder state). ZnO nanorods also benefit from Fe3−δO4 nanoparticles by enhancement of their optical properties in the visible range (a 2-fold increase of PL intensity with respect to bare ZnO nanorods) which we propose to result from photon energy transfer.

Published
2018

17. Defect‐Driven Magnetization Configuration of Isolated Linear Assemblies of Iron Oxide Nanoparticles

Author

Riccardo Hertel, Attila Kákay, Sylvie Begin-Colin, Ebenezer Tetsi, Mircea V. Rastei, V. Pierron-Bohnes, Benoit P. Pichon, Delphine Toulemon, Corinne Bouillet, Institut de Physique et Chimie des Matériaux de Strasbourg (IPCMS), Université de Strasbourg (UNISTRA)-Matériaux et nanosciences d'Alsace (FMNGE), Institut de Chimie du CNRS (INC)-Université de Strasbourg (UNISTRA)-Université de Haute-Alsace (UHA) Mulhouse - Colmar (Université de Haute-Alsace (UHA))-Institut National de la Santé et de la Recherche Médicale (INSERM)-Centre National de la Recherche Scientifique (CNRS)-Institut de Chimie du CNRS (INC)-Université de Strasbourg (UNISTRA)-Université de Haute-Alsace (UHA) Mulhouse - Colmar (Université de Haute-Alsace (UHA))-Institut National de la Santé et de la Recherche Médicale (INSERM)-Centre National de la Recherche Scientifique (CNRS)-Centre National de la Recherche Scientifique (CNRS)-Réseau nanophotonique et optique, and Centre National de la Recherche Scientifique (CNRS)-Université de Strasbourg (UNISTRA)-Université de Haute-Alsace (UHA) Mulhouse - Colmar (Université de Haute-Alsace (UHA))-Centre National de la Recherche Scientifique (CNRS)-Université de Strasbourg (UNISTRA)

Subjects
Materials science, Magnetic domain, AFM / MFM, magnetization states, Nanoparticle, 02 engineering and technology, 010402 general chemistry, 01 natural sciences, e-holography, HR-TEM, Biomaterials, Magnetization, chemistry.chemical_compound, micromagnetic simulations, Electrochemistry, [PHYS.COND]Physics [physics]/Condensed Matter [cond-mat], One-NP-wide chains, Magnetic structure, Condensed matter physics, [CHIM.MATE]Chemical Sciences/Material chemistry, 021001 nanoscience & nanotechnology, Condensed Matter Physics, 3. Good health, 0104 chemical sciences, Electronic, Optical and Magnetic Materials, Magnetic anisotropy, chemistry, Particle, Magnetic force microscope, 0210 nano-technology, Iron oxide nanoparticles
Abstract

International audience; The magnetization state of one-dimensional magnetic nanoparticle chains plays a key role for a wide range of applications ranging from diagnosis and therapy in medicine to actuators, sensors and quantum recording media. The interplay between the exact particle orientation and the magnetic anisotropy is in turn crucial for controlling the overall magnetization state with high precision. Here, we report on a three-dimensional description of the magnetic structure of one-NP-wide chains. In this aim, we combined two complementary experimental techniques, magnetic force microscopy (MFM) and electronic holography (EH) which are sensitive to out-of-plane and in-plane magnetization components, respectively. We extended our approach to micromagnetic simulations which provided results in good agreement with MFM and EH. The findings are at variance with the known results on unidirectional nanoparticle assemblies, and show that magnetization is rarely strictly collinear to the chain axis. The magnetic structure of one-NP-wide chains can be interpreted as head-to-head magnetic domain structures with off-axis magnetization components, which is very sensitive to morphological defects in the chain structure such as minute size variation of NPs, tiny misalignment of NPs and/or crystal orientation with respect to easy magnetization axis.

Published
2019

18. Strong interfacial coupling through exchange interactions in soft/hard core-shell nanoparticles as a function of cationic distribution

Author

Fadi Choueikani, Benoit P. Pichon, Corinne Bouillet, Kevin Sartori, Sylvie Begin-Colin, V. Halté, and Geoffrey Cotin

Subjects
X-ray absorption spectroscopy, Materials science, Spintronics, Nanoparticle, 02 engineering and technology, Coercivity, 010402 general chemistry, 021001 nanoscience & nanotechnology, 01 natural sciences, Inductive coupling, 0104 chemical sciences, Magnetic anisotropy, Chemical engineering, Ferrimagnetism, Antiferromagnetism, General Materials Science, 0210 nano-technology
Abstract

Exchange coupled core–shell nanoparticles present high potential to tune adequately the magnetic properties for specific applications such as nanomedicine or spintronics. Here, we report on the design of core–shell nanoparticles by performing the successive thermal decomposition of Fe and Co complexes. Depending on the thermal stability and the concentration of the Co precursor, we were able to control the formation of a hard ferrimagnetic (FiM) Co-ferrite shell or an antiferromagnetic (AFM) CoO shell at the surface of a soft FiM Fe3−δO4 core. The formation of the Co-ferrite shell was also found to occur through two different mechanisms: the diffusion of Co or the growth at the iron oxide surface. The structural properties of core–shell nanoparticles were investigated by a wide panel of techniques such as HAADF, STEM and XRD. The distribution of Fe and Co elements in the crystal structure was described accurately by XAS and XMCD. The operating conditions influenced significantly the oxidation rate of Fe2+ in the core as well as the occupancy of Oh sites by Fe2+ and Co2+ cations. The structural properties of nanoparticles were correlated with their magnetic properties which were investigated by SQUID magnetometry. Each core–shell nanoparticle displayed enhanced effective magnetic anisotropy energy (Eeff) in comparison with pristine Fe3−δO4 nanoparticles because of magnetic coupling at the core–shell interface. The Co-ferrite FiM shells resulted in better enhancement of Eeff than a CoO AFM shell. In addition, the magnetic properties were also influenced by the core size. The coercive field (HC) was increased by core reduction while the blocking temperature (TB) was increased by a larger core. Element-specific XMCD measurements showed the fine coupling of Fe and Co cations which agree with Co-ferrite in each sample, e.g. the formation of a Co-doped interfacial layer in the Fe3−δO4@CoO nanoparticles.

Published
2019

19. Room Temperature Blocked Magnetic Nanoparticles Based on Ferrite Promoted by a Three-Step Thermal Decomposition Process

Author

Sylvie Begin-Colin, Dario Taverna, Benoit P. Pichon, Fadi Choueikani, Kevin Sartori, Alexandre Gloter, Institut de Physique et Chimie des Matériaux de Strasbourg (IPCMS), Université de Strasbourg (UNISTRA)-Centre National de la Recherche Scientifique (CNRS)-Matériaux et Nanosciences Grand-Est (MNGE), Université de Strasbourg (UNISTRA)-Université de Haute-Alsace (UHA) Mulhouse - Colmar (Université de Haute-Alsace (UHA))-Institut National de la Santé et de la Recherche Médicale (INSERM)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS)-Université de Strasbourg (UNISTRA)-Université de Haute-Alsace (UHA) Mulhouse - Colmar (Université de Haute-Alsace (UHA))-Institut National de la Santé et de la Recherche Médicale (INSERM)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS)-Réseau nanophotonique et optique, Université de Strasbourg (UNISTRA)-Université de Haute-Alsace (UHA) Mulhouse - Colmar (Université de Haute-Alsace (UHA))-Centre National de la Recherche Scientifique (CNRS)-Université de Strasbourg (UNISTRA)-Centre National de la Recherche Scientifique (CNRS), Synchrotron SOLEIL (SSOLEIL), Centre National de la Recherche Scientifique (CNRS), Laboratoire de Physique des Solides (LPS), Université Paris-Sud - Paris 11 (UP11)-Centre National de la Recherche Scientifique (CNRS), Institut de minéralogie, de physique des matériaux et de cosmochimie (IMPMC), Muséum national d'Histoire naturelle (MNHN)-Institut de recherche pour le développement [IRD] : UR206-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS), Gloter, Alexandre, Université de Strasbourg (UNISTRA)-Centre National de la Recherche Scientifique (CNRS)-Matériaux et nanosciences d'Alsace (FMNGE), Institut de Chimie du CNRS (INC)-Université de Strasbourg (UNISTRA)-Université de Haute-Alsace (UHA) Mulhouse - Colmar (Université de Haute-Alsace (UHA))-Institut National de la Santé et de la Recherche Médicale (INSERM)-Centre National de la Recherche Scientifique (CNRS)-Institut de Chimie du CNRS (INC)-Université de Strasbourg (UNISTRA)-Université de Haute-Alsace (UHA) Mulhouse - Colmar (Université de Haute-Alsace (UHA))-Institut National de la Santé et de la Recherche Médicale (INSERM)-Centre National de la Recherche Scientifique (CNRS)-Réseau nanophotonique et optique, Centre National de la Recherche Scientifique (CNRS)-Université de Strasbourg (UNISTRA)-Université de Haute-Alsace (UHA) Mulhouse - Colmar (Université de Haute-Alsace (UHA))-Centre National de la Recherche Scientifique (CNRS)-Université de Strasbourg (UNISTRA), and Centre National de la Recherche Scientifique (CNRS)-Université Paris-Sud - Paris 11 (UP11)

Subjects
[PHYS]Physics [physics], Chemistry, Thermal decomposition, Nanoparticle, General Chemistry, 010402 general chemistry, 01 natural sciences, Biochemistry, Catalysis, 0104 chemical sciences, [PHYS] Physics [physics], Magnetic anisotropy, Colloid and Surface Chemistry, Chemical engineering, [CHIM] Chemical Sciences, Ferrite (magnet), Magnetic nanoparticles, [CHIM]Chemical Sciences
Abstract

International audience; Exchange coupled nanoparticles that combine hard and soft magnetic phases are very promising to enhance the effective magnetic anisotropy while preserving sizes below 20 nm. However, the core−shell structure is usually insufficient to produce rare earth-free ferro(i)-magnetic blocked nanoparticles at room temperature. We report on onion-type magnetic nanoparticles prepared by a three-step seed mediated growth based on the thermal decomposition method. The core@shell@shell structure consists of a core and an external shell of Fe 3−δ O 4 separated by an intermediate Co-doped ferrite shell. The double exchange coupling at both core@shell and shell@ shell interfaces results in such an increased of the magnetic anisotropy energy, that onion-type nanoparticles of 16 nm mainly based on iron oxide are blocked at room temperature. We envision that these results are very appealing for potential applications based on permanent magnets. H ard−soft coupled magnetic nanoparticles have gained a tremendous amount of interest during the past decade for short-term development of advanced applications related to spintronics (magnetoresistive sensors, magnetic recording, etc.). 1 Indeed, they are a potential alternative to produce permanent magnets 2 in order to circumvent supply storage caused by the critical need for rare earth elements in communications and mobility applications. With this purpose, the main goal is to overcome superparamagnetism, which results from size reduction to the nanoscale. 3 A very attractive approach is the design of core−shell nanoparticles that combine hard and soft magnetic phases in direct contact. 4

Published
2019

20. Nanoparticle Assembling through Click Chemistry Directed by Mixed SAMs for Magnetic Applications

Author

Monica Calatayud, Delphine Toulemon, Mathias Dolci, J. L. Bubendorff, Zaineb Chaffar, Frederik Tielens, Sylvie Begin-Colin, Spyridon Zafeiratos, Benoit P. Pichon, Institut de Physique et Chimie des Matériaux de Strasbourg (IPCMS), Université de Strasbourg (UNISTRA)-Centre National de la Recherche Scientifique (CNRS)-Matériaux et Nanosciences Grand-Est (MNGE), Université de Strasbourg (UNISTRA)-Université de Haute-Alsace (UHA) Mulhouse - Colmar (Université de Haute-Alsace (UHA))-Institut National de la Santé et de la Recherche Médicale (INSERM)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS)-Université de Strasbourg (UNISTRA)-Université de Haute-Alsace (UHA) Mulhouse - Colmar (Université de Haute-Alsace (UHA))-Institut National de la Santé et de la Recherche Médicale (INSERM)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS)-Réseau nanophotonique et optique, Université de Strasbourg (UNISTRA)-Université de Haute-Alsace (UHA) Mulhouse - Colmar (Université de Haute-Alsace (UHA))-Centre National de la Recherche Scientifique (CNRS)-Université de Strasbourg (UNISTRA)-Centre National de la Recherche Scientifique (CNRS), Institut de Science des Matériaux de Mulhouse (IS2M), Université de Haute-Alsace (UHA) Mulhouse - Colmar (Université de Haute-Alsace (UHA))-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS)-Matériaux et Nanosciences Grand-Est (MNGE), Université de Strasbourg (UNISTRA)-Université de Haute-Alsace (UHA) Mulhouse - Colmar (Université de Haute-Alsace (UHA))-Institut National de la Santé et de la Recherche Médicale (INSERM)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS)-Université de Strasbourg (UNISTRA)-Institut National de la Santé et de la Recherche Médicale (INSERM)-Centre National de la Recherche Scientifique (CNRS)-Réseau nanophotonique et optique, Spectroscopie, Modélisation, Interfaces pour L'Environnement et la Santé (LCMCP-SMiLES), Laboratoire de Chimie de la Matière Condensée de Paris (LCMCP), Institut de Chimie du CNRS (INC)-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS)-Institut de Chimie du CNRS (INC)-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS), Departement of General Chemistry (ALGC) (ALG), Université libre de Bruxelles (ULB), Laboratoire de chimie théorique (LCT), Institut de Chimie du CNRS (INC)-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS), Institut de chimie et procédés pour l'énergie, l'environnement et la santé (ICPEES), Université de Strasbourg (UNISTRA)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS)-Matériaux et Nanosciences Grand-Est (MNGE), Université de Strasbourg (UNISTRA)-Université de Haute-Alsace (UHA) Mulhouse - Colmar (Université de Haute-Alsace (UHA))-Institut National de la Santé et de la Recherche Médicale (INSERM)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS)-Université de Strasbourg (UNISTRA)-Université de Haute-Alsace (UHA) Mulhouse - Colmar (Université de Haute-Alsace (UHA))-Institut National de la Santé et de la Recherche Médicale (INSERM)-Centre National de la Recherche Scientifique (CNRS), Institut Universitaire de France (IUF), Ministère de l'Education nationale, de l’Enseignement supérieur et de la Recherche (M.E.N.E.S.R.), GENCI-[CCRT/CINES/IDRIS] (Grants 2016-[x2016082022] and 2017- x2017082131), CCRE of Université Pierre et Marie Curie, Direction générale de l’armement (DGA), Région Alsace, ANR-10-IDEX-0002,UNISTRA,Par-delà les frontières, l'Université de Strasbourg(2010), Laurent, Guillaume, Initiative d'excellence - Par-delà les frontières, l'Université de Strasbourg - - UNISTRA2010 - ANR-10-IDEX-0002 - IDEX - VALID, Chemistry, Université de Strasbourg (UNISTRA)-Matériaux et nanosciences d'Alsace (FMNGE), Institut de Chimie du CNRS (INC)-Université de Strasbourg (UNISTRA)-Université de Haute-Alsace (UHA) Mulhouse - Colmar (Université de Haute-Alsace (UHA))-Institut National de la Santé et de la Recherche Médicale (INSERM)-Centre National de la Recherche Scientifique (CNRS)-Institut de Chimie du CNRS (INC)-Université de Strasbourg (UNISTRA)-Université de Haute-Alsace (UHA) Mulhouse - Colmar (Université de Haute-Alsace (UHA))-Institut National de la Santé et de la Recherche Médicale (INSERM)-Centre National de la Recherche Scientifique (CNRS)-Centre National de la Recherche Scientifique (CNRS)-Réseau nanophotonique et optique, Centre National de la Recherche Scientifique (CNRS)-Université de Strasbourg (UNISTRA)-Université de Haute-Alsace (UHA) Mulhouse - Colmar (Université de Haute-Alsace (UHA))-Centre National de la Recherche Scientifique (CNRS)-Université de Strasbourg (UNISTRA), Centre National de la Recherche Scientifique (CNRS)-Matériaux et nanosciences d'Alsace (FMNGE), Institut de Chimie du CNRS (INC)-Université de Strasbourg (UNISTRA)-Université de Haute-Alsace (UHA) Mulhouse - Colmar (Université de Haute-Alsace (UHA))-Institut National de la Santé et de la Recherche Médicale (INSERM)-Centre National de la Recherche Scientifique (CNRS)-Institut de Chimie du CNRS (INC)-Université de Strasbourg (UNISTRA)-Université de Haute-Alsace (UHA) Mulhouse - Colmar (Université de Haute-Alsace (UHA))-Institut National de la Santé et de la Recherche Médicale (INSERM)-Centre National de la Recherche Scientifique (CNRS)-Réseau nanophotonique et optique, and Institut de Chimie du CNRS (INC)-Université de Strasbourg (UNISTRA)-Université de Haute-Alsace (UHA) Mulhouse - Colmar (Université de Haute-Alsace (UHA))-Institut National de la Santé et de la Recherche Médicale (INSERM)-Centre National de la Recherche Scientifique (CNRS)-Institut de Chimie du CNRS (INC)-Université de Strasbourg (UNISTRA)-Université de Haute-Alsace (UHA) Mulhouse - Colmar (Université de Haute-Alsace (UHA))-Institut National de la Santé et de la Recherche Médicale (INSERM)-Centre National de la Recherche Scientifique (CNRS)-Centre National de la Recherche Scientifique (CNRS)

Subjects
[CHIM.MATE] Chemical Sciences/Material chemistry, Materials science, thiol molecule, theoretical modeling, Nanoparticle, Nanotechnology, collective properties, 02 engineering and technology, [CHIM.MATE]Chemical Sciences/Material chemistry, 010402 general chemistry, 021001 nanoscience & nanotechnology, 01 natural sciences, 0104 chemical sciences, defect mediated replacement, click chemistry, Click chemistry, General Materials Science, structure, 0210 nano-technology, phase segregation
Abstract

International audience; "Click" chemistry, used to promote nanoparticle assemblies, is a powerful strategy which has emerged very recently to control the spatial arrangement of nanoparticles onto surfaces. Such a strategy may be of high interest for applications such as magnetic recording media or magnetic sensors which are based on the fine control of the collective properties of nanoparticles. Nevertheless, self-assembly driven by clickable functional groups still remains to be understood. Mixed self-assembled monolayers (SAMs) of alkane−thiol molecules were used to control the spatial arrangement of nanoparticles onto gold substrates. This approach was combined with click chemistry in order to control the immobilization of nanoparticles on selective areas through specific copper catalyzed alkyne−azide cycloaddition (CuAAC) reaction. Mixed SAMs consist of co-adsorbed 11-(undec-1-ynyl)thiol (S-CC) and 12-(dodecane)thiol (S-CH 3) molecules. The variation of the molar ratio between both molecules resulted in significant modulation of the structure of nanoparticle assemblies. The spatial arrangement of nanoparticles revealed the very complex structure of alkyne/methylene terminated mixed SAMs. Alkyne terminal groups could not be only studied by the usual characterization surface techniques such as PM-IRRAS and XPS. Therefore, azido-terminated nanoparticles acted as probing agents to determine the spatial distribution of alkyne groups at the surface of mixed SAMs. This approach was combined with scanning tunneling microscopy (STM) and DFT calculations to get a deeper insight into the structure of mixed SAMs of S-CC and S-CH 3 molecules. Gold substrate topography, chemical affinity of molecules, intermolecular interactions and length of alkyl chains were found to be critical parameters that rule the SAM structure.

Published
2019

21. Design of Anisotropic Iron-Oxide-Based Nanoparticles for Magnetic Hyperthermia

Author

Benoit P. Pichon, Geoffrey Cotin, Sylvie Begin-Colin, Cristina Blanco-Andujar, Damien Mertz, Francis Perton, Institut de Physique et Chimie des Matériaux de Strasbourg (IPCMS), Université de Strasbourg (UNISTRA)-Matériaux et nanosciences d'Alsace (FMNGE), Institut de Chimie du CNRS (INC)-Université de Strasbourg (UNISTRA)-Université de Haute-Alsace (UHA) Mulhouse - Colmar (Université de Haute-Alsace (UHA))-Institut National de la Santé et de la Recherche Médicale (INSERM)-Centre National de la Recherche Scientifique (CNRS)-Institut de Chimie du CNRS (INC)-Université de Strasbourg (UNISTRA)-Université de Haute-Alsace (UHA) Mulhouse - Colmar (Université de Haute-Alsace (UHA))-Institut National de la Santé et de la Recherche Médicale (INSERM)-Centre National de la Recherche Scientifique (CNRS)-Centre National de la Recherche Scientifique (CNRS)-Réseau nanophotonique et optique, and Centre National de la Recherche Scientifique (CNRS)-Université de Strasbourg (UNISTRA)-Université de Haute-Alsace (UHA) Mulhouse - Colmar (Université de Haute-Alsace (UHA))-Centre National de la Recherche Scientifique (CNRS)-Université de Strasbourg (UNISTRA)

Subjects
Heating power, Materials science, Anisotropy energy, Thermal ablation, Iron oxide, Nanoparticle, Nanotechnology, 02 engineering and technology, [CHIM.MATE]Chemical Sciences/Material chemistry, [CHIM.THER]Chemical Sciences/Medicinal Chemistry, 010402 general chemistry, 021001 nanoscience & nanotechnology, 01 natural sciences, 0104 chemical sciences, 3. Good health, chemistry.chemical_compound, Magnetic hyperthermia, chemistry, Surface modification, 0210 nano-technology, Anisotropy, ComputingMilieux_MISCELLANEOUS
Abstract

In the field of the synthesis and functionalization of iron-oxide nanoparticles (IONPs) for biomedical applications, most researches aimed at first at optimizing IONPs to be used as contrast agent for MRI. Then functionalized iron-oxide NPs have been also shown promising for therapy by magnetic hyperthermia (MH). The use of MH as a stand-alone or an adjacent therapy for cancer is closer to be a reality in every hospital to the positive results achieved by the clinical trials carried out by Magforce (Germany). Nonetheless, one of MH limitations is the low-power heating of usual magnetic NPs, requiring a local injection of large quantities of NPs. There is thus currently a challenge for optimizing the heating power of magnetic NPs. The amount of heat generated by magnetic NPs strongly depends on the NPs magnetic properties, which have to display high saturation magnetization and in particular high anisotropy energy, which depends strongly on their size, composition, and shape. The particle size distribution is also important as size distribution or energy barriers can cause overheating and undesired magnetic thermal ablation. Current developments for the synthesis of NPs optimized for MH rely on quality by design. Indeed first studies have shown that spherical IONPs with a mean size around 20 nm are suitable for clinical MH and progress in the NPs synthesis allowed synthesizing NPs with different shapes and core-shell structures which improved the NPs magnetic properties. Some intrinsic parameters of the NPs have thus been underlined as boosters for MH. Yet, the synthesis development/strategy remains empirical. In this chapter, we briefly list the features that can help increasing the heating values of NPs and we present an overview of the ways to control those NPs characteristics with the thermal decomposition synthesis method.

Published
2019

22. Unravelling the Thermal Decomposition Parameters for The Synthesis of Anisotropic Iron Oxide Nanoparticles

Author

Christophe Lefevre, Simona Moldovan, Céline Kiefer, Sylvie Begin-Colin, Cristina Blanco-Andujar, Dris Ihiawakrim, Ovidiu Ersen, Benoit P. Pichon, Damien Mertz, Geoffrey Cotin, Francis Perton, Moldovan, Simona, Institut de Physique et Chimie des Matériaux de Strasbourg (IPCMS), Université de Strasbourg (UNISTRA)-Centre National de la Recherche Scientifique (CNRS)-Matériaux et Nanosciences Grand-Est (MNGE), Université de Strasbourg (UNISTRA)-Université de Haute-Alsace (UHA) Mulhouse - Colmar (Université de Haute-Alsace (UHA))-Institut National de la Santé et de la Recherche Médicale (INSERM)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS)-Université de Strasbourg (UNISTRA)-Université de Haute-Alsace (UHA) Mulhouse - Colmar (Université de Haute-Alsace (UHA))-Institut National de la Santé et de la Recherche Médicale (INSERM)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS)-Réseau nanophotonique et optique, Université de Strasbourg (UNISTRA)-Université de Haute-Alsace (UHA) Mulhouse - Colmar (Université de Haute-Alsace (UHA))-Centre National de la Recherche Scientifique (CNRS)-Université de Strasbourg (UNISTRA)-Centre National de la Recherche Scientifique (CNRS), Groupe de physique des matériaux (GPM), Université de Rouen Normandie (UNIROUEN), Normandie Université (NU)-Normandie Université (NU)-Institut national des sciences appliquées Rouen Normandie (INSA Rouen Normandie), Institut National des Sciences Appliquées (INSA)-Normandie Université (NU)-Institut National des Sciences Appliquées (INSA)-Centre National de la Recherche Scientifique (CNRS)-Institut de Recherche sur les Matériaux Avancés (IRMA), Université de Caen Normandie (UNICAEN), Normandie Université (NU)-Normandie Université (NU)-École Nationale Supérieure d'Ingénieurs de Caen (ENSICAEN), Normandie Université (NU)-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université de Rouen Normandie (UNIROUEN), Normandie Université (NU)-Institut national des sciences appliquées Rouen Normandie (INSA Rouen Normandie), Institut National des Sciences Appliquées (INSA)-Normandie Université (NU)-Institut National des Sciences Appliquées (INSA)-Centre National de la Recherche Scientifique (CNRS)-Université de Caen Normandie (UNICAEN), Normandie Université (NU)-École Nationale Supérieure d'Ingénieurs de Caen (ENSICAEN), Normandie Université (NU)-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Centre National de la Recherche Scientifique (CNRS), Université de Strasbourg (UNISTRA)-Matériaux et nanosciences d'Alsace (FMNGE), Institut de Chimie du CNRS (INC)-Université de Strasbourg (UNISTRA)-Université de Haute-Alsace (UHA) Mulhouse - Colmar (Université de Haute-Alsace (UHA))-Institut National de la Santé et de la Recherche Médicale (INSERM)-Centre National de la Recherche Scientifique (CNRS)-Institut de Chimie du CNRS (INC)-Université de Strasbourg (UNISTRA)-Université de Haute-Alsace (UHA) Mulhouse - Colmar (Université de Haute-Alsace (UHA))-Institut National de la Santé et de la Recherche Médicale (INSERM)-Centre National de la Recherche Scientifique (CNRS)-Centre National de la Recherche Scientifique (CNRS)-Réseau nanophotonique et optique, Centre National de la Recherche Scientifique (CNRS)-Université de Strasbourg (UNISTRA)-Université de Haute-Alsace (UHA) Mulhouse - Colmar (Université de Haute-Alsace (UHA))-Centre National de la Recherche Scientifique (CNRS)-Université de Strasbourg (UNISTRA), Centre National de la Recherche Scientifique (CNRS)-Institut national des sciences appliquées Rouen Normandie (INSA Rouen Normandie), Institut National des Sciences Appliquées (INSA)-Normandie Université (NU)-Institut National des Sciences Appliquées (INSA)-Normandie Université (NU)-Université de Rouen Normandie (UNIROUEN), and Normandie Université (NU)

Subjects
Materials science, synthesis, General Chemical Engineering, precursor, Iron oxide, Nucleation, Nanoparticle, 02 engineering and technology, 010402 general chemistry, 01 natural sciences, Article, lcsh:Chemistry, 03 medical and health sciences, chemistry.chemical_compound, Stearate, [CHIM] Chemical Sciences, [CHIM]Chemical Sciences, General Materials Science, shape control, thermal decomposition, 030304 developmental biology, 0303 health sciences, nanotechnology, 030302 biochemistry & molecular biology, Thermal decomposition, iron oxide nanoparticles, 021001 nanoscience & nanotechnology, 0104 chemical sciences, Oleic acid, Magnetic hyperthermia, chemistry, Chemical engineering, lcsh:QD1-999, 0210 nano-technology, Iron oxide nanoparticles
Abstract

Iron oxide nanoparticles are widely used as a contrast agent in magnetic resonance imaging (MRI), and may be used as therapeutic agent for magnetic hyperthermia if they display in particular high magnetic anisotropy. Considering the effect of nanoparticles shape on anisotropy, a reproducible shape control of nanoparticles is a current synthesis challenge. By investigating reaction parameters, such as the iron precursor structure, its water content, but also the amount of the surfactant (sodium oleate) reported to control the shape, iron oxide nanoparticles with different shape and composition were obtained, in particular, iron oxide nanoplates. The effect of the surfactant coming from precursor was taking into account by using in house iron stearates bearing either two or three stearate chains and the negative effect of water on shape was confirmed by considering these precursors after their dehydration. Iron stearates with three chains in presence of a ratio sodium oleate/oleic acid 1:1 led mainly to nanocubes presenting a core-shell Fe1&minus, xO@Fe3&minus, xO4 composition. Nanocubes with straight faces were only obtained with dehydrated precursors. Meanwhile, iron stearates with two chains led preferentially to the formation of nanoplates with a ratio sodium oleate/oleic acid 4:1. The rarely reported flat shape of the plates was confirmed with 3D transmission electronic microscopy (TEM) tomography. The investigation of the synthesis mechanisms confirmed the major role of chelating ligand and of the heating rate to drive the cubic shape of nanoparticles and showed that the nanoplate formation would depend mainly on the nucleation step and possibly on the presence of a given ratio of oleic acid and chelating ligand (oleate and/or stearate).

Published
2018

23. Stability of M13 Phage in Organic Solvents

Author

Vesna Srot, Pouya Moghimian, Peter A. van Aken, Benoit P. Pichon, and Sandra J. Facey

Subjects
Scanning electron microscope, viruses, Organic solvent, Structural integrity, 02 engineering and technology, 010402 general chemistry, 021001 nanoscience & nanotechnology, 01 natural sciences, 0104 chemical sciences, law.invention, Hexane, chemistry.chemical_compound, chemistry, Chemical engineering, law, Organic chemistry, Self-assembly, Electron microscope, 0210 nano-technology, Inorganic nanoparticles, Macromolecule
Abstract

The effect of different types of organic solvents on the structural integrity of M13 phages has been directly visualized by transmission and scanning electron microscopy. The exposure of M13 phages to apolar hexane had no effect on the structure of the phages for up to 8 h. In contrast, phages showed ~10-fold contraction into rod-like I-forms and to flattened spheroids with ~12 nm diameter upon exposure to polar organic solvents. We show that this finding can be beneficial for the macromolecular self-assembly and in broader aspects, to enhance the spatial arrangement of desired inorganic nanoparticles in the rapidly developing field of virotronics.

Published
2016

24. Stretchable magneto-dielectric composites based on raspberry-shaped iron oxide nanostructures

Author

Leo C. Kempel, Elodie Barraud, Benoit P. Pichon, Mert Vural, Olivier Gerber, Sylvie Begin-Colin, Peter Kofinas, and Sébastien Lemonnier

Subjects
Materials science, Iron oxide, Maghemite, 02 engineering and technology, General Chemistry, Dielectric, engineering.material, Coercivity, 010402 general chemistry, 021001 nanoscience & nanotechnology, Elastomer, 01 natural sciences, Ferromagnetic resonance, 0104 chemical sciences, chemistry.chemical_compound, Magnetization, chemistry, Materials Chemistry, engineering, Composite material, 0210 nano-technology, Magnetite
Abstract

Stretchable magneto-dielectric composites were prepared using collectively assembled iron oxide nanostructures as fillers in an elastomer (polydimethylsiloxane) matrix. These raspberry-shaped nanostructures (RSNs), synthesized by a one-pot polyol solvothermal method, consist of oriented aggregates of iron oxide nanocrystals. The oriented aggregation of nanocrystals generates a large interface between nanograins significantly reducing their surface oxidation, improving crystal quality and preventing the formation of surface and volume spin canting. Therefore these iron oxide RSNs display low coercivity with enhanced saturation magnetization (MS). The use of such citrated RSN as filler material with improved magnetization and low coercivity allowed the fabrication of magneto-dielectric composites that can attain permeability values reaching 2.3 with magnetic loss values limited to 0.11. The resulting composites can also be stretched up to 155% strain before failure due to good adhesion between the elastomer and citrate capped RSNs. In addition, the composition of these fillers was altered to adjust the resonance frequency of the resulting composite material. Stretchable magneto-dielectric composites consisting of maghemite-rich RSNs and magnetite-rich RSNs demonstrated resonance frequencies similar to the spherical ferromagnetic resonance of maghemite and magnetite, respectively.

Published
2016

25. Preparation of magnetically recoverable carbon nanotube-supported Pd(II) catalyst

Author

Antonin Desmecht, Anaëlle L’hoost, Sophie Hermans, Irina Nircha, Florence Pennetreau, Olivier Riant, Benoit P. Pichon, Institut de Physique et Chimie des Matériaux de Strasbourg (IPCMS), Université de Strasbourg (UNISTRA)-Matériaux et nanosciences d'Alsace (FMNGE), Institut de Chimie du CNRS (INC)-Université de Strasbourg (UNISTRA)-Université de Haute-Alsace (UHA) Mulhouse - Colmar (Université de Haute-Alsace (UHA))-Institut National de la Santé et de la Recherche Médicale (INSERM)-Centre National de la Recherche Scientifique (CNRS)-Institut de Chimie du CNRS (INC)-Université de Strasbourg (UNISTRA)-Université de Haute-Alsace (UHA) Mulhouse - Colmar (Université de Haute-Alsace (UHA))-Institut National de la Santé et de la Recherche Médicale (INSERM)-Centre National de la Recherche Scientifique (CNRS)-Centre National de la Recherche Scientifique (CNRS)-Réseau nanophotonique et optique, Centre National de la Recherche Scientifique (CNRS)-Université de Strasbourg (UNISTRA)-Université de Haute-Alsace (UHA) Mulhouse - Colmar (Université de Haute-Alsace (UHA))-Centre National de la Recherche Scientifique (CNRS)-Université de Strasbourg (UNISTRA), Université Louis Pasteur - Strasbourg I-Centre National de la Recherche Scientifique (CNRS), and UCL - SST/IMCN - Institute of Condensed Matter and Nanosciences

Subjects
Materials science, 010405 organic chemistry, chemistry.chemical_element, Nanoparticle, Carbon nanotube, General Chemistry, 010402 general chemistry, 01 natural sciences, Catalysis, 0104 chemical sciences, law.invention, chemistry.chemical_compound, [SPI.ELEC]Engineering Sciences [physics]/Electromagnetism, chemistry, X-ray photoelectron spectroscopy, Chemical engineering, law, Surface modification, Xanthate, Carbon, Palladium
Abstract

Multi-walled carbon nanotubes were filled or externally decorated with iron oxide nanoparticles to make them magnetically-recoverable. In the first case, the external surface was treated to be free of defects and oxygenated groups to favor internalization. A thermal decomposition route was followed in the second case. The formed nanoparticles were characterized and shown to consist in magnetite and/or maghemite. Moreover, when placed on the external surface of carbon nanotubes, they remained small and well-dispersed, leaving high proportion of free carbon surface for further functionalization. The intact sp2 carbon atoms were subsequently attacked by means of xanthate radical chemistry, followed by post-functionalization to graft a dipyridylamine ligand on the surface of both solids and pristine carbon nanotubes for comparison. Solids at each step of the syntheses were characterized by X-ray photoelectron spectroscopy (XPS). Palladium coordination onto the surface ligand was studied and the precursor [Pd(COD)Cl2] complex gave the best results to afford CNT-supported molecular Pd(II) catalysts. XPS confirmed the +2 oxidation state of palladium on the carbon surface. The so-prepared magnetically-recoverable catalysts were successfully used in Suzuki-Miyaura cross-coupling catalytic application.

Published
2018

26. Robust clicked assembly based on iron oxide nanoparticles for a new type of SPR biosensor

Author

Mathias Dolci, Spyridon Zafeiratos, Jean-François Bryche, Simon Gree, Benoit P. Pichon, Cédric Leuvrey, Sylvie Begin-Colin, Grégory Barbillon, Institut de Physique et Chimie des Matériaux de Strasbourg (IPCMS), Université de Strasbourg (UNISTRA)-Matériaux et nanosciences d'Alsace (FMNGE), Institut de Chimie du CNRS (INC)-Université de Strasbourg (UNISTRA)-Université de Haute-Alsace (UHA) Mulhouse - Colmar (Université de Haute-Alsace (UHA))-Institut National de la Santé et de la Recherche Médicale (INSERM)-Centre National de la Recherche Scientifique (CNRS)-Institut de Chimie du CNRS (INC)-Université de Strasbourg (UNISTRA)-Université de Haute-Alsace (UHA) Mulhouse - Colmar (Université de Haute-Alsace (UHA))-Institut National de la Santé et de la Recherche Médicale (INSERM)-Centre National de la Recherche Scientifique (CNRS)-Centre National de la Recherche Scientifique (CNRS)-Réseau nanophotonique et optique, Centre National de la Recherche Scientifique (CNRS)-Université de Strasbourg (UNISTRA)-Université de Haute-Alsace (UHA) Mulhouse - Colmar (Université de Haute-Alsace (UHA))-Centre National de la Recherche Scientifique (CNRS)-Université de Strasbourg (UNISTRA), Institut d'électronique fondamentale (IEF), Université Paris-Sud - Paris 11 (UP11)-Centre National de la Recherche Scientifique (CNRS), Institut de chimie et procédés pour l'énergie, l'environnement et la santé (ICPEES), Institut de Chimie du CNRS (INC)-Université de Strasbourg (UNISTRA)-Université de Haute-Alsace (UHA) Mulhouse - Colmar (Université de Haute-Alsace (UHA))-Institut National de la Santé et de la Recherche Médicale (INSERM)-Centre National de la Recherche Scientifique (CNRS)-Institut de Chimie du CNRS (INC)-Université de Strasbourg (UNISTRA)-Université de Haute-Alsace (UHA) Mulhouse - Colmar (Université de Haute-Alsace (UHA))-Institut National de la Santé et de la Recherche Médicale (INSERM)-Centre National de la Recherche Scientifique (CNRS)-Centre National de la Recherche Scientifique (CNRS), Institut de Science des Matériaux de Mulhouse (IS2M), Centre National de la Recherche Scientifique (CNRS)-Matériaux et nanosciences d'Alsace (FMNGE), and Institut de Chimie du CNRS (INC)-Université de Strasbourg (UNISTRA)-Université de Haute-Alsace (UHA) Mulhouse - Colmar (Université de Haute-Alsace (UHA))-Institut National de la Santé et de la Recherche Médicale (INSERM)-Centre National de la Recherche Scientifique (CNRS)-Institut de Chimie du CNRS (INC)-Université de Strasbourg (UNISTRA)-Université de Haute-Alsace (UHA) Mulhouse - Colmar (Université de Haute-Alsace (UHA))-Institut National de la Santé et de la Recherche Médicale (INSERM)-Centre National de la Recherche Scientifique (CNRS)-Réseau nanophotonique et optique

Subjects
chemistry.chemical_classification, Streptavidin, Materials science, High-refractive-index polymer, Biomolecule, Nanoparticle, Nanotechnology, 02 engineering and technology, General Chemistry, Dielectric, 010402 general chemistry, 021001 nanoscience & nanotechnology, 01 natural sciences, 0104 chemical sciences, chemistry.chemical_compound, chemistry, Materials Chemistry, [CHIM]Chemical Sciences, Thin film, 0210 nano-technology, Biosensor, Iron oxide nanoparticles, ComputingMilieux_MISCELLANEOUS
Abstract

We present a novel strategy to create an original nanostructured SPR biosensor with enhanced sensitivity. Our approach consists of using high refractive index dielectric materials to increase the sensitivity factor of a gold thin film despite its large evanescent electromagnetic field decay lengths. Iron oxide nanoparticles were grafted onto a gold thin film and were easily functionalized by biomolecular receptors through a two step copper catalyzed alkyne–azide cycloaddition (CuAAC) “click” reaction. This strategy allowed us to prepare a highly stable and robust nanostructured biosensor. We selected the very-well known biotin–streptavidin couple to demonstrate the efficiency of our strategy toward the enhancement of the detection of biomolecules without using any labelling of the target molecules. High refractive index nanoparticles were demonstrated to enhance markedly the sensitivity to the detection of streptavidin by increasing the sensitivity factor of the gold thin film and the accessibility of biotin groups (reduction of steric hindrance).

Published
2018

27. Exploring Exchange Bias Coupling in Fe3-O4@CoO Core-Shell Nanoparticle 2D Assemblies

Author

Xiaojie Liu, Mathias Dolci, Yu Liu, Dominique Begin, Alain Derory, Cédric Leuvrey, Sylvie Begin-Colin, Benoit P. Pichon, Institut de Physique et Chimie des Matériaux de Strasbourg (IPCMS), Université de Strasbourg (UNISTRA)-Matériaux et nanosciences d'Alsace (FMNGE), Institut de Chimie du CNRS (INC)-Université de Strasbourg (UNISTRA)-Université de Haute-Alsace (UHA) Mulhouse - Colmar (Université de Haute-Alsace (UHA))-Institut National de la Santé et de la Recherche Médicale (INSERM)-Centre National de la Recherche Scientifique (CNRS)-Institut de Chimie du CNRS (INC)-Université de Strasbourg (UNISTRA)-Université de Haute-Alsace (UHA) Mulhouse - Colmar (Université de Haute-Alsace (UHA))-Institut National de la Santé et de la Recherche Médicale (INSERM)-Centre National de la Recherche Scientifique (CNRS)-Centre National de la Recherche Scientifique (CNRS)-Réseau nanophotonique et optique, Centre National de la Recherche Scientifique (CNRS)-Université de Strasbourg (UNISTRA)-Université de Haute-Alsace (UHA) Mulhouse - Colmar (Université de Haute-Alsace (UHA))-Centre National de la Recherche Scientifique (CNRS)-Université de Strasbourg (UNISTRA), Université Louis Pasteur - Strasbourg I-Centre National de la Recherche Scientifique (CNRS), Institut de chimie et procédés pour l'énergie, l'environnement et la santé (ICPEES), and Institut de Chimie du CNRS (INC)-Université de Strasbourg (UNISTRA)-Université de Haute-Alsace (UHA) Mulhouse - Colmar (Université de Haute-Alsace (UHA))-Institut National de la Santé et de la Recherche Médicale (INSERM)-Centre National de la Recherche Scientifique (CNRS)-Institut de Chimie du CNRS (INC)-Université de Strasbourg (UNISTRA)-Université de Haute-Alsace (UHA) Mulhouse - Colmar (Université de Haute-Alsace (UHA))-Institut National de la Santé et de la Recherche Médicale (INSERM)-Centre National de la Recherche Scientifique (CNRS)-Centre National de la Recherche Scientifique (CNRS)

Subjects
Materials science, Nanoparticle, 02 engineering and technology, 010402 general chemistry, 021001 nanoscience & nanotechnology, Condensed Matter Physics, 01 natural sciences, 0104 chemical sciences, Electronic, Optical and Magnetic Materials, [SPI.MAT]Engineering Sciences [physics]/Materials, Biomaterials, Coupling (electronics), Core shell, Magnetic anisotropy, Exchange bias, Chemical physics, Monolayer, Electrochemistry, Click chemistry, 0210 nano-technology
Abstract

Core-shell ferro(i)magnetic@antiferromagnetic (F(i)M@AFM) nanoparticles exhibiting exchange bias coupling are very promising to push back the superparamagnetic limits. However, their intrinsic magnetic properties can be strongly affected by interparticle interactions. This work reports on the collective properties of Fe3-dO4@CoO core-shell nanoparticles as function of the structure of their assembly. The structure of nanoparticle assembly is controlled by a copper (I) catalyzed alkyne-azide cycloaddition (CuAAC) click reaction between complementary functional groups located at the surface of both substrates and nanoparticles. 2D arrays of nanoparticles with tunable sizes ranging from clusters of few nanoparticles to a dense and homogenous monolayer were prepared. The spatial arrangement of nanoparticles strongly influences the exchange bias coupling which is significantly enhanced for large 2D nanoparticle assemblies and, even more in 3D assemblies such as powder, which favour weak and random dipolar interactions.

Published
2018

28. Synthesis engineering of iron oxide raspberry-shaped nanostructures

Author

Simona Moldovan, D. Begin, Ovidiu Ersen, Sylvie Begin-Colin, Sébastien Lemonnier, Elodie Barraud, Dris Ihiawakrim, Olivier Gerber, Benoit P. Pichon, Ileana Florea, Jean-Marc Greneche, Institut de biologie et chimie des protéines [Lyon] (IBCP), Université Claude Bernard Lyon 1 (UCBL), Université de Lyon-Université de Lyon-Centre National de la Recherche Scientifique (CNRS), Institut de Physique et Chimie des Matériaux de Strasbourg (IPCMS), Université de Strasbourg (UNISTRA)-Centre National de la Recherche Scientifique (CNRS)-Matériaux et nanosciences d'Alsace (FMNGE), Institut de Chimie du CNRS (INC)-Université de Strasbourg (UNISTRA)-Université de Haute-Alsace (UHA) Mulhouse - Colmar (Université de Haute-Alsace (UHA))-Institut National de la Santé et de la Recherche Médicale (INSERM)-Centre National de la Recherche Scientifique (CNRS)-Institut de Chimie du CNRS (INC)-Université de Strasbourg (UNISTRA)-Université de Haute-Alsace (UHA) Mulhouse - Colmar (Université de Haute-Alsace (UHA))-Institut National de la Santé et de la Recherche Médicale (INSERM)-Centre National de la Recherche Scientifique (CNRS)-Réseau nanophotonique et optique, Centre National de la Recherche Scientifique (CNRS)-Université de Strasbourg (UNISTRA)-Université de Haute-Alsace (UHA) Mulhouse - Colmar (Université de Haute-Alsace (UHA))-Centre National de la Recherche Scientifique (CNRS)-Université de Strasbourg (UNISTRA), Laboratoire de physique des interfaces et des couches minces [Palaiseau] (LPICM), École polytechnique (X)-Centre National de la Recherche Scientifique (CNRS), Institut de chimie et procédés pour l'énergie, l'environnement et la santé (ICPEES), Université de Strasbourg (UNISTRA)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS)-Matériaux et nanosciences d'Alsace (FMNGE), Institut de Chimie du CNRS (INC)-Université de Strasbourg (UNISTRA)-Université de Haute-Alsace (UHA) Mulhouse - Colmar (Université de Haute-Alsace (UHA))-Institut National de la Santé et de la Recherche Médicale (INSERM)-Centre National de la Recherche Scientifique (CNRS)-Université de Strasbourg (UNISTRA)-Université de Haute-Alsace (UHA) Mulhouse - Colmar (Université de Haute-Alsace (UHA))-Institut National de la Santé et de la Recherche Médicale (INSERM)-Centre National de la Recherche Scientifique (CNRS), Institut des Molécules et Matériaux du Mans (IMMM), Le Mans Université (UM)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS), Institut franco-allemand de recherches de Saint-Louis (ISL), DGA-Matériaux et nanosciences d'Alsace (FMNGE), Institut de Chimie du CNRS (INC)-Université de Strasbourg (UNISTRA)-Université de Haute-Alsace (UHA) Mulhouse - Colmar (Université de Haute-Alsace (UHA))-Institut National de la Santé et de la Recherche Médicale (INSERM)-Centre National de la Recherche Scientifique (CNRS)-Institut de Chimie du CNRS (INC)-Université de Strasbourg (UNISTRA)-Université de Haute-Alsace (UHA) Mulhouse - Colmar (Université de Haute-Alsace (UHA))-Institut National de la Santé et de la Recherche Médicale (INSERM)-Centre National de la Recherche Scientifique (CNRS), Université Louis Pasteur - Strasbourg I-Centre National de la Recherche Scientifique (CNRS), Université de Strasbourg (UNISTRA)-Matériaux et nanosciences d'Alsace (FMNGE), Institut de Chimie du CNRS (INC)-Université de Strasbourg (UNISTRA)-Université de Haute-Alsace (UHA) Mulhouse - Colmar (Université de Haute-Alsace (UHA))-Institut National de la Santé et de la Recherche Médicale (INSERM)-Centre National de la Recherche Scientifique (CNRS)-Institut de Chimie du CNRS (INC)-Université de Strasbourg (UNISTRA)-Université de Haute-Alsace (UHA) Mulhouse - Colmar (Université de Haute-Alsace (UHA))-Institut National de la Santé et de la Recherche Médicale (INSERM)-Centre National de la Recherche Scientifique (CNRS)-Centre National de la Recherche Scientifique (CNRS)-Réseau nanophotonique et optique, and Institut de Chimie du CNRS (INC)-Université de Strasbourg (UNISTRA)-Université de Haute-Alsace (UHA) Mulhouse - Colmar (Université de Haute-Alsace (UHA))-Institut National de la Santé et de la Recherche Médicale (INSERM)-Centre National de la Recherche Scientifique (CNRS)-Institut de Chimie du CNRS (INC)-Université de Strasbourg (UNISTRA)-Université de Haute-Alsace (UHA) Mulhouse - Colmar (Université de Haute-Alsace (UHA))-Institut National de la Santé et de la Recherche Médicale (INSERM)-Centre National de la Recherche Scientifique (CNRS)-Centre National de la Recherche Scientifique (CNRS)

Subjects
[PHYS]Physics [physics], Materials science, Nanostructure, Iron oxide, Nanoparticle, Nanotechnology, 02 engineering and technology, 010402 general chemistry, 021001 nanoscience & nanotechnology, 01 natural sciences, 0104 chemical sciences, chemistry.chemical_compound, chemistry, Nanocrystal, Phase (matter), Alkoxide, General Materials Science, Lamellar structure, [PHYS.COND]Physics [physics]/Condensed Matter [cond-mat], 0210 nano-technology, ComputingMilieux_MISCELLANEOUS, Magnetite
Abstract

Magnetic porous nanostructures consisting of oriented aggregates of iron oxide nanocrystals display very interesting properties such as a lower oxidation state of magnetite, and enhanced saturation magnetization in comparison with individual nanoparticles of similar sizes and porosity. However, the formation mechanism of these promising nanostructures is not well understood, which hampers the fine tuning of their magnetic properties, for instance by doping them with other elements. Therefore the formation mechanism of porous raspberry shaped nanostructures (RSNs) synthesized by a one-pot polyol solvothermal method has been investigated in detail from the early stages by using a wide panel of characterization techniques, and especially by performing original in situ HR-TEM studies in temperature. A time-resolved study showed the intermediate formation of an amorphous iron alkoxide phase with a plate-like lamellar structure (PLS). Then, the fine investigation of PLS transformation upon heating up to 500 °C confirmed that the synthesis of RSNs involves two iron precursors: the starting one (hydrated iron chlorides) and the in situ formed iron alkoxide precursor which decomposes with time and heating and contributes to the growth step of nanostructures. Such an understanding of the formation mechanism of RSNs is necessary to envision efficient and rational enhancement of their magnetic properties.

Published
2017

29. Chapter 4. Iron-oxide Nanoparticle-based Contrast Agents

Author

Sophie Laurent, Vlad Socoliuc, Jean-Marc Greneche, Rodica Turcu, Ladislau Vekas, Luce Vander Elst, Benoit P. Pichon, Dimitri Stanicki, Audrey Parat, Delphine Felder-Flesch, Robert Bartha, Damien Mertz, Geoffrey Cotin, Sylvie Begin-Colin, Victor Kuncser, Paula Foster, Ovidiu Ersen, and Robert N. Muller

Subjects
chemistry.chemical_compound, Materials science, chemistry, Iron oxide, Surface modification, Nanoparticle, Nanometre, Nanotechnology, Iron oxide nanoparticles, Superparamagnetism, Characterization (materials science), Nanomaterials
Abstract

This chapter discusses the synthesis, functionalization, characterization, and imaging applications of iron-oxide-nanoparticle-based contrast agents. By reducing the size from bulk to the nanometer scale (

Published
2017

30. Fast Assembling of Magnetic Iron Oxide Nanoparticles by Microwave-Assisted Copper(I) Catalyzed Alkyne–Azide Cycloaddition (CuAAC)

Author

Sylvie Begin-Colin, Spyridon Zafeiratos, Vasiliki Papaefthimiou, Cédric Leuvrey, Delphine Toulemon, Xavier Cattoën, Benoit P. Pichon, Institut de Physique et Chimie des Matériaux de Strasbourg (IPCMS), Université de Strasbourg (UNISTRA)-Matériaux et nanosciences d'Alsace (FMNGE), Institut de Chimie du CNRS (INC)-Université de Strasbourg (UNISTRA)-Université de Haute-Alsace (UHA) Mulhouse - Colmar (Université de Haute-Alsace (UHA))-Institut National de la Santé et de la Recherche Médicale (INSERM)-Centre National de la Recherche Scientifique (CNRS)-Institut de Chimie du CNRS (INC)-Université de Strasbourg (UNISTRA)-Université de Haute-Alsace (UHA) Mulhouse - Colmar (Université de Haute-Alsace (UHA))-Institut National de la Santé et de la Recherche Médicale (INSERM)-Centre National de la Recherche Scientifique (CNRS)-Centre National de la Recherche Scientifique (CNRS)-Réseau nanophotonique et optique, Centre National de la Recherche Scientifique (CNRS)-Université de Strasbourg (UNISTRA)-Université de Haute-Alsace (UHA) Mulhouse - Colmar (Université de Haute-Alsace (UHA))-Centre National de la Recherche Scientifique (CNRS)-Université de Strasbourg (UNISTRA), Institut de chimie et procédés pour l'énergie, l'environnement et la santé (ICPEES), Institut de Chimie du CNRS (INC)-Université de Strasbourg (UNISTRA)-Université de Haute-Alsace (UHA) Mulhouse - Colmar (Université de Haute-Alsace (UHA))-Institut National de la Santé et de la Recherche Médicale (INSERM)-Centre National de la Recherche Scientifique (CNRS)-Institut de Chimie du CNRS (INC)-Université de Strasbourg (UNISTRA)-Université de Haute-Alsace (UHA) Mulhouse - Colmar (Université de Haute-Alsace (UHA))-Institut National de la Santé et de la Recherche Médicale (INSERM)-Centre National de la Recherche Scientifique (CNRS)-Centre National de la Recherche Scientifique (CNRS), Institut Charles Gerhardt Montpellier - Institut de Chimie Moléculaire et des Matériaux de Montpellier (ICGM ICMMM), and Université Montpellier 1 (UM1)-Université Montpellier 2 - Sciences et Techniques (UM2)-Ecole Nationale Supérieure de Chimie de Montpellier (ENSCM)-Institut de Chimie du CNRS (INC)-Université de Montpellier (UM)-Centre National de la Recherche Scientifique (CNRS)

Subjects
chemistry.chemical_classification, Materials science, Nanostructure, General Chemical Engineering, Alkyne, Nanoparticle, Nanotechnology, [CHIM.MATE]Chemical Sciences/Material chemistry, 02 engineering and technology, General Chemistry, 010402 general chemistry, 021001 nanoscience & nanotechnology, 01 natural sciences, Cycloaddition, 0104 chemical sciences, Catalysis, chemistry.chemical_compound, chemistry, Materials Chemistry, Click chemistry, Azide, 0210 nano-technology, ComputingMilieux_MISCELLANEOUS, Iron oxide nanoparticles
Abstract

Two dimensional (2D) nanoparticles (NP) assemblies have become very attractive due to their original collective properties, which can be modulated as a function of the nanostructure. Beyond precise control on nanostructure and easy way to perform, fast assembling processes are highly desirable to develop efficient and popular strategies to prepare systems with tunable collective properties. In this article, we report on the highly efficient and fast 2D assembling of iron oxide nanoparticles on a self-assembled monolayer (SAM) of organic molecules by the microwave (MW)-assisted copper(I) catalyzed alkyne–azide cycloaddition (CuAAC) click reaction. Microwave irradiation favors a dramatic enhancement of the assembling reaction, which was completed with maximum density in NPs within one hour, much faster than the conventional CuAAC click reactions that require up to 48 h. Moreover, the MW-assisted click reaction presents the great advantage to preserve specific reactions between alkyne and azide groups at SAM...

Published
2013

31. Genotoxic and mutagenic effects of lipid-coated CdSe/ZnS quantum dots

Author

Michel De Méo, Carole Di Giorgio, Isabelle Berque-Bestel, Ahissan Aimé, Philippe Barthélémy, Mélanie Aye, Yves Jammes, and Benoit P. Pichon

Subjects
DNA damage, Health, Toxicology and Mutagenesis, Sulfides, Cadmium chloride, medicine.disease_cause, chemistry.chemical_compound, Clastogen, Cadmium Chloride, Quantum Dots, Cadmium Compounds, Genetics, medicine, Selenium Compounds, Uridine, Mutagenicity Tests, Chemistry, Molecular biology, Comet assay, Zinc Compounds, Micronucleus test, Phosphatidylcholines, Microsome, Micronucleus, Genotoxicity, DNA Damage, Mutagens
Abstract

We proposed to evaluate the genotoxicity and mutagenicity of a new quantum dots (QDs) nanoplatform (QDsN), consisting of CdSe/ZnS core-shell QDs encapsulated by a natural fusogenic lipid (1,2-di-oleoyl-sn-glycero-3-phosphocholine (DOPC)) and functionalized by a nucleolipid N-[5'-(2',3'-di-oleoyl) uridine]-N',N',N'-trimethylammoniumtosylate (DOTAU). This QDs nanoplatform may represent a new therapeutic tool for the diagnosis and treatment of human cancers. The genotoxic, mutagenic and clastogenic effects of QDsN were compared to those of cadmium chloride (CdCl(2)). Three assays were used: (1) the Salmonella/microsome assay with four tester strains, (2) the comet assay and (3) the micronucleus test on CHO cells. The contribution of simulated sunlight was studied in the three assays while oxidative events were only explored in the comet assay in aliquots pretreated with the antioxidant l-ergothioneine. We found that QDsN could enter CHO-K1 cells and accumulate in cytoplasmic vesicles. It was not mutagenic in the Salmonella/mutagenicity test whereas CdCl(2) was weakly positive. In the dark, both the QDsN and CdCl(2) similarly induced dose-dependent increases in single-strand breaks and micronuclei. Exposure to simulated sunlight significantly potentiated the genotoxic activities of both QDsN and CdCl(2), but did not significantly increase micronucleus frequencies. l-Ergothioneine significantly reduced but did not completely suppress the DNA-damaging activity of QDsN and CdCl(2). The present results clearly point to the genotoxic properties and the risk of long-term adverse effects of such a nanoplatform if used for human anticancer therapy and diagnosis in the future.

Published
2013

32. Effect of Disorder and Dipolar Interactions in Two-Dimensional Assemblies of Iron-Oxide Magnetic Nanoparticles

Author

Paul-Antoine Hervieux, Benoit P. Pichon, Guillaume Klughertz, Giovanni Manfredi, and Sylvie Begin-Colin

Subjects
Zeeman effect, Condensed matter physics, Magnetic structure, Chemistry, Monte Carlo method, Aucun, Nanoparticle, 02 engineering and technology, 010402 general chemistry, 021001 nanoscience & nanotechnology, 01 natural sciences, 0104 chemical sciences, Surfaces, Coatings and Films, Electronic, Optical and Magnetic Materials, symbols.namesake, Dipole, General Energy, symbols, Magnetic nanoparticles, Hexagonal lattice, Physical and Theoretical Chemistry, 0210 nano-technology, Magnetic dipole
Abstract

We examine the magnetic properties of two-dimensional monolayers of iron-oxide magnetic nanoparticles arranged on a hexagonal lattice and interacting through magnetic dipole forces. Monte Carlo simulations are used to reconstruct the zero-field cooled magnetization curve, as well as other relevant quantities (Zeeman and dipolar energies). The blocking temperature is found to increase with shorter interparticle distance. The effect of structural disorder is studied by randomly removing some nanoparticles from their lattice sites. Surprisingly, it is found that disorder has little impact on the global magnetic structure of the sample. The numerical results are compared to existing experimental measurements.

Published
2016

33. Enhanced Collective Magnetic Properties Induced by the Controlled Assembly of Iron Oxide Nanoparticles in Chains

Author

Delphine Toulemon, Xavier Cattoën, Jose Javier Saiz Garitaonandia, Luis Lezama, Mircea V. Rastei, David S. Schmool, Benoit P. Pichon, Sylvie Begin-Colin, Institut de Physique et Chimie des Matériaux de Strasbourg (IPCMS), Université de Strasbourg (UNISTRA)-Matériaux et nanosciences d'Alsace (FMNGE), Institut de Chimie du CNRS (INC)-Université de Strasbourg (UNISTRA)-Université de Haute-Alsace (UHA) Mulhouse - Colmar (Université de Haute-Alsace (UHA))-Institut National de la Santé et de la Recherche Médicale (INSERM)-Centre National de la Recherche Scientifique (CNRS)-Institut de Chimie du CNRS (INC)-Université de Strasbourg (UNISTRA)-Université de Haute-Alsace (UHA) Mulhouse - Colmar (Université de Haute-Alsace (UHA))-Institut National de la Santé et de la Recherche Médicale (INSERM)-Centre National de la Recherche Scientifique (CNRS)-Centre National de la Recherche Scientifique (CNRS)-Réseau nanophotonique et optique, Centre National de la Recherche Scientifique (CNRS)-Université de Strasbourg (UNISTRA)-Université de Haute-Alsace (UHA) Mulhouse - Colmar (Université de Haute-Alsace (UHA))-Centre National de la Recherche Scientifique (CNRS)-Université de Strasbourg (UNISTRA), Departamento de Química Inorgánica, Facultad de Ciencia y Tecnologia, Universidad del Pais Vasco / Euskal Herriko Unibertsitatea [Espagne] (UPV/EHU), Optique et Matériaux (OPTIMA ), Institut Néel (NEEL), Institut polytechnique de Grenoble - Grenoble Institute of Technology (Grenoble INP )-Centre National de la Recherche Scientifique (CNRS)-Université Grenoble Alpes [2016-2019] (UGA [2016-2019])-Institut polytechnique de Grenoble - Grenoble Institute of Technology (Grenoble INP )-Centre National de la Recherche Scientifique (CNRS)-Université Grenoble Alpes [2016-2019] (UGA [2016-2019]), and Université Louis Pasteur - Strasbourg I-Centre National de la Recherche Scientifique (CNRS)

Subjects
Materials science, Magnetism, Magnetometer, Nanoparticle, Nanotechnology, 02 engineering and technology, 010402 general chemistry, 01 natural sciences, law.invention, Biomaterials, chemistry.chemical_compound, law, Electrochemistry, ComputingMilieux_MISCELLANEOUS, [PHYS]Physics [physics], 021001 nanoscience & nanotechnology, Condensed Matter Physics, Ferromagnetic resonance, 0104 chemical sciences, Electronic, Optical and Magnetic Materials, Magnetic field, chemistry, Magnetic nanoparticles, Magnetic force microscope, 0210 nano-technology, Iron oxide nanoparticles
Abstract

1D assemblies of magnetic nanoparticles are of great potential for designing novel nanostructured materials with enhanced collective magnetic properties. In that challenging context, a new assembly strategy is presented to prepare chains of magnetic nanoparticles that are well-defined in structure and in spatial arrangement. The 1D assembly of iron oxide nanoparticles onto a substrate is controlled using “click” chemistry under an external magnetic field. Co-aligned single nanoparticle chains separated by regular distances can be obtained by this strategy. The intrinsic high uniaxial anisotropy results in a strong enhancement of magnetic collective properties in comparison to 2D monolayers or isolated nanoparticles. In contrast to the intensively studied bundle chains of nanoparticles, the finely tuned chain structure reported here allows evidencing a first order intrachain dipolar interaction and a second order interchain magnetic coupling. This study offers new insights into the collective magnetic properties of highly anisotropic particulate assemblies which have been investigated by combining superconducting quantum interference device magnetometry, magnetic force microscopy, and ferromagnetic resonance.

Published
2016

34. Design of Fe3–xO4 raspberry decorated graphene nanocomposites with high performances in lithium-ion battery

Author

Olivier Gerber, Elodie Barraud, Cuong Pham-Huu, Patrice Simon, Barbara Daffos, Benoit P. Pichon, Sébastien Lemonnier, Dominique Begin, Jeremy Come, Sylvie Begin-Colin, Centre National de la Recherche Scientifique - CNRS (FRANCE), Institut National Polytechnique de Toulouse - INPT (FRANCE), Université de Strasbourg - UNISTRA (FRANCE), Université Toulouse III - Paul Sabatier - UPS (FRANCE), Institut franco-allemand de recherches de Saint-Louis - ISL (FRANCE), Institut de Physique et Chimie des Matériaux de Strasbourg - IPCMS (Strasbourg, France), Institut de Chimie et Procédés pour l’ Energie, l’ Environnement et la Santé - ICPEES (Strasbourg, France), Centre Interuniversitaire de Recherche et d'Ingénierie des Matériaux - CIRIMAT (Toulouse, France), Réseau sur le Stockage Electrochimique de l'Energie - RS2E (Amiens, France), Université Toulouse III - Paul Sabatier - UT3 (FRANCE), Institut National Polytechnique de Toulouse - Toulouse INP (FRANCE), Institut de Physique et Chimie des Matériaux de Strasbourg (IPCMS), Université Louis Pasteur - Strasbourg I-Centre National de la Recherche Scientifique (CNRS), French-German Research Institute of Saint Louis, Institut de chimie et procédés pour l'énergie, l'environnement et la santé (ICPEES), Université de Strasbourg (UNISTRA)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS)-Matériaux et nanosciences d'Alsace (FMNGE), Institut de Chimie du CNRS (INC)-Université de Strasbourg (UNISTRA)-Université de Haute-Alsace (UHA) Mulhouse - Colmar (Université de Haute-Alsace (UHA))-Institut National de la Santé et de la Recherche Médicale (INSERM)-Centre National de la Recherche Scientifique (CNRS)-Université de Strasbourg (UNISTRA)-Université de Haute-Alsace (UHA) Mulhouse - Colmar (Université de Haute-Alsace (UHA))-Institut National de la Santé et de la Recherche Médicale (INSERM)-Centre National de la Recherche Scientifique (CNRS), Centre interuniversitaire de recherche et d'ingenierie des matériaux (CIRIMAT), Centre National de la Recherche Scientifique (CNRS)-Université Toulouse III - Paul Sabatier (UT3), Université Fédérale Toulouse Midi-Pyrénées-Université Fédérale Toulouse Midi-Pyrénées-Institut National Polytechnique (Toulouse) (Toulouse INP), Université Fédérale Toulouse Midi-Pyrénées-Institut de Chimie du CNRS (INC), Réseau sur le stockage électrochimique de l'énergie (RS2E), Université de Picardie Jules Verne (UPJV)-Institut de Chimie du CNRS (INC)-Aix Marseille Université (AMU)-Université de Pau et des Pays de l'Adour (UPPA)-Université de Nantes (UN)-Université de Montpellier (UM)-Centre National de la Recherche Scientifique (CNRS)-Sorbonne Université (SU)-Ecole Nationale Supérieure de Chimie de Paris - Chimie ParisTech-PSL (ENSCP), Université Paris sciences et lettres (PSL)-Université Paris sciences et lettres (PSL)-Université de Haute-Alsace (UHA) Mulhouse - Colmar (Université de Haute-Alsace (UHA))-Collège de France (CdF (institution))-Institut polytechnique de Grenoble - Grenoble Institute of Technology (Grenoble INP ), Université Grenoble Alpes (UGA)-Université Grenoble Alpes (UGA)-Institut National Polytechnique (Toulouse) (Toulouse INP), Université Fédérale Toulouse Midi-Pyrénées-Université Fédérale Toulouse Midi-Pyrénées-Ecole Nationale Supérieure de Chimie de Montpellier (ENSCM), Université de Strasbourg (UNISTRA)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS)-Matériaux et Nanosciences Grand-Est (MNGE), Université de Strasbourg (UNISTRA)-Université de Haute-Alsace (UHA) Mulhouse - Colmar (Université de Haute-Alsace (UHA))-Institut National de la Santé et de la Recherche Médicale (INSERM)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS)-Université de Strasbourg (UNISTRA)-Université de Haute-Alsace (UHA) Mulhouse - Colmar (Université de Haute-Alsace (UHA))-Institut National de la Santé et de la Recherche Médicale (INSERM)-Centre National de la Recherche Scientifique (CNRS), Université Toulouse III - Paul Sabatier (UT3), Université de Toulouse (UT)-Université de Toulouse (UT)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS)-Institut National Polytechnique (Toulouse) (Toulouse INP), Université de Toulouse (UT), Université de Nantes (UN)-Aix Marseille Université (AMU)-Université de Haute-Alsace (UHA) Mulhouse - Colmar (Université de Haute-Alsace (UHA))-Collège de France (CdF (institution))-Université de Picardie Jules Verne (UPJV)-Ecole Nationale Supérieure de Chimie de Montpellier (ENSCM)-Ecole Nationale Supérieure de Chimie de Paris - Chimie ParisTech-PSL (ENSCP), Université Paris sciences et lettres (PSL)-Université Paris sciences et lettres (PSL)-Université de Pau et des Pays de l'Adour (UPPA)-Institut de Chimie du CNRS (INC)-Université de Montpellier (UM)-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS)-Institut National Polytechnique (Toulouse) (Toulouse INP), Université de Toulouse (UT)-Université de Toulouse (UT)-Institut polytechnique de Grenoble - Grenoble Institute of Technology (Grenoble INP ), and Université Grenoble Alpes (UGA)-Université Grenoble Alpes (UGA)

Subjects
Battery (electricity), Materials science, Nanostructure, Matériaux, Energy Engineering and Power Technology, Nanotechnology, 02 engineering and technology, 010402 general chemistry, 01 natural sciences, 7. Clean energy, Lithium-ion battery, law.invention, [SPI.MAT]Engineering Sciences [physics]/Materials, chemistry.chemical_compound, Fe3–xO4/graphene nanocomposites, law, Reversible capacity, Electrochemistry, Magnetite, Nanocomposite, Graphene, [CHIM.MATE]Chemical Sciences/Material chemistry, 021001 nanoscience & nanotechnology, 0104 chemical sciences, Anode, Fuel Technology, chemistry, Nanocrystal, Fe3–xO4 raspberry shaped nanostructures, 0210 nano-technology, Energy (miscellaneous)
Abstract

International audience; Fe3–xO4 raspberry shaped nanostructures/graphene nanocomposites were synthesized by a one-step polyol-solvothermal method to be tested as electrode materials for Li-ion battery (LIB). Indeed, Fe3–xO4 raspberry shaped nanostructures consist of original oriented aggregates of Fe3–xO4 magnetite nanocrystals, ensuring a low oxidation state of magnetite and a hollow and porous structure, which has been easily combined with graphene sheets. The resulting nanocomposite powder displays a very homogeneous spatial distribution of Fe3–xO4 nanostructures at the surface of the graphene sheets. These original nanostructures and their strong interaction with the graphene sheets resulted in very small capacity fading upon Li+ ion intercalation. Reversible capacity, as high as 660 mAh/g, makes this material promising for anode in Li-ion batteries application.

Published
2016

35. Enhanced Collective Magnetic Properties in 2D Monolayers of Iron Oxide Nanoparticles Favored by Local Order and Local 1D Shape Anisotropy

Author

Sylvie Begin-Colin, Delphine Toulemon, Xavier Cattoën, Yu Liu, Benoit P. Pichon, Cédric Leuvrey, Institut de Physique et Chimie des Matériaux de Strasbourg (IPCMS), Université de Strasbourg (UNISTRA)-Matériaux et nanosciences d'Alsace (FMNGE), Institut de Chimie du CNRS (INC)-Université de Strasbourg (UNISTRA)-Université de Haute-Alsace (UHA) Mulhouse - Colmar (Université de Haute-Alsace (UHA))-Institut National de la Santé et de la Recherche Médicale (INSERM)-Centre National de la Recherche Scientifique (CNRS)-Institut de Chimie du CNRS (INC)-Université de Strasbourg (UNISTRA)-Université de Haute-Alsace (UHA) Mulhouse - Colmar (Université de Haute-Alsace (UHA))-Institut National de la Santé et de la Recherche Médicale (INSERM)-Centre National de la Recherche Scientifique (CNRS)-Centre National de la Recherche Scientifique (CNRS)-Réseau nanophotonique et optique, Centre National de la Recherche Scientifique (CNRS)-Université de Strasbourg (UNISTRA)-Université de Haute-Alsace (UHA) Mulhouse - Colmar (Université de Haute-Alsace (UHA))-Centre National de la Recherche Scientifique (CNRS)-Université de Strasbourg (UNISTRA), Optique et Matériaux (OPTIMA ), Institut Néel (NEEL), Institut polytechnique de Grenoble - Grenoble Institute of Technology (Grenoble INP )-Centre National de la Recherche Scientifique (CNRS)-Université Grenoble Alpes [2016-2019] (UGA [2016-2019])-Institut polytechnique de Grenoble - Grenoble Institute of Technology (Grenoble INP )-Centre National de la Recherche Scientifique (CNRS)-Université Grenoble Alpes [2016-2019] (UGA [2016-2019]), and Université Louis Pasteur - Strasbourg I-Centre National de la Recherche Scientifique (CNRS)

Subjects
[PHYS]Physics [physics], Materials science, Kinetics, Nanoparticle, Nanotechnology, 02 engineering and technology, Surfaces and Interfaces, 010402 general chemistry, 021001 nanoscience & nanotechnology, Condensed Matter Physics, 01 natural sciences, 0104 chemical sciences, chemistry.chemical_compound, Dipole, Order (biology), chemistry, Monolayer, Electrochemistry, General Materials Science, 0210 nano-technology, Anisotropy, Spectroscopy, Iron oxide nanoparticles, ComputingMilieux_MISCELLANEOUS
Abstract

Magnetic nanoparticle arrays represent a very attractive research field because their collective properties can be efficiently modulated as a function of the structure of the assembly. Nevertheless, understanding the way dipolar interactions influence the intrinsic magnetic properties of nanoparticles still remains a great challenge. In this study, we report on the preparation of 2D assemblies of iron oxide nanoparticles as monolayers deposited onto substrates. Assemblies have been prepared by using the Langmuir-Blodgett technique and the SAM assisted assembling technique combined to CuAAC "click" reaction. These techniques afford to control the formation of well-defined monolayers of nanoparticles on large areas. The LB technique controls local ordering of nanoparticles, while adjusting the kinetics of CuAAC "click" reaction strongly affects the spatial arrangement of nanoparticles in monolayers. Fast kinetics favor disordered assemblies while slow kinetics favor the formation of chain-like structures. Such anisotropic assemblies are induced by dipolar interactions between nanoparticles as no magnetic field is applied and no solvent evaporation is performed. The collective magnetic properties of monolayers are studied as a function of average interparticle distance, local order and local shape anisotropy. We demonstrate that local control on spatial arrangement of nanoparticles in monolayers significantly strengthens dipolar interactions which enhances collective properties and results in possible super ferromagnetic order.

Published
2016

36. Decoration of nanocarbon solids with magnetite nanoparticles: towards microwave metamaterial absorbers

Author

Yzaora Tchuitio Yagang, Francisco Mederos-Henry, Benoit P. Pichon, Christian Bailly, Arnaud Delcorte, Sophie Hermans, Isabelle Huynen, UCL - SST/IMCN/MOST - Molecules, Solids and Reactivity, UCL - SST/IMCN/BSMA - Bio and soft matter, and UCL - SST/ICTM/ELEN - Pôle en ingénierie électrique

Subjects
Materials science, Nanocomposite, Solvothermal synthesis, Metamaterial, Nanotechnology, 02 engineering and technology, General Chemistry, 010402 general chemistry, 021001 nanoscience & nanotechnology, 01 natural sciences, Ferromagnetic resonance, 0104 chemical sciences, Chemical engineering, Oxidation state, Materials Chemistry, 0210 nano-technology, Absorption (electromagnetic radiation), NANO [ICTEAM], Microwave, Superparamagnetism
Abstract

Three methods for decoration of nanocarbon solids (NcSs) with magnetite nanoparticles (MaNPs) were compared, namely covalent linkage, direct co-precipitation and solvothermal synthesis. The influence of each method on the obtained nanocomposites' most relevant characteristics was studied, such as chemical identity, size, loading rate and spatial distribution of the MaNPs over the NcS. The impact of the variables controlling the solvothermal decoration of a wide variety of NcSs was investigated in more detail, such as the nature of the iron precursor and the NcS (type and oxidation state), the reaction temperature, time and water content. Finally, the obtained nanocomposites' superparamagnetic MaNPs were found to induce a ferromagnetic resonance (FMR) phenomenon, imparting a natural or zero-field resonance around 4 GHz. It was also demonstrated that the amount of loaded MaNPs had an effect on the FMR absorption intensity as well as on the nanocomposites' electrical properties. The latter were also shown to be governed by the chosen NcS type. These features could easily be exploited as control mechanisms to construct highly effective microwave metamaterial absorbers possessing low incident microwave reflection and maximal absorption rates.

Published
2016

37. Assembling of Magnetic Iron Oxide Nanoparticles Controlled by Self- Assembled Monolayers of Functional Coordinating or Chelating Trialkoxysilanes

Author

Benoit P. Pichon

Subjects
Magnetism, technology, industry, and agriculture, Nanotechnology, Self-assembled monolayer, equipment and supplies, Silanol, chemistry.chemical_compound, chemistry, Chemical engineering, Monolayer, Magnetic nanoparticles, Amine gas treating, Chelation, Iron oxide nanoparticles
Abstract

Magnetic nanoparticles (NPs) have been assembled in films by using self-assembled monolayers (SAMs) of organic molecules. SAMs were prepared by the reaction of organotrialkoxysilanes with surface silanol groups of silicon wafers. SAMs were prepared and their surface was decorated either by amine or thymine groups which have the ability to immobilize iron oxide nanoparticles as monolayers. These groups have different coordinating and chelating abilities and influence the kinetic of the assembling reaction. Finally, the magnetic properties of the assemblies of NPs were studied.

Published
2012

38. Low Oxidation State and Enhanced Magnetic Properties Induced by Raspberry Shaped Nanostructures of Iron Oxide

Author

Ovidiu Ersen, Elodie Barraud, Corinne Ulhaq, Jean-Marc Greneche, Ileana Florea, Sébastien Lemonnier, Benoit P. Pichon, Olivier Gerber, Dominique Begin, Sylvie Begin-Colin, Christophe Lefevre, Institut de Physique et Chimie des Matériaux de Strasbourg (IPCMS), Université Louis Pasteur - Strasbourg I-Centre National de la Recherche Scientifique (CNRS), Université de Strasbourg (UNISTRA)-Centre National de la Recherche Scientifique (CNRS)-Matériaux et nanosciences d'Alsace (FMNGE), Institut de Chimie du CNRS (INC)-Université de Strasbourg (UNISTRA)-Université de Haute-Alsace (UHA) Mulhouse - Colmar (Université de Haute-Alsace (UHA))-Institut National de la Santé et de la Recherche Médicale (INSERM)-Centre National de la Recherche Scientifique (CNRS)-Institut de Chimie du CNRS (INC)-Université de Strasbourg (UNISTRA)-Université de Haute-Alsace (UHA) Mulhouse - Colmar (Université de Haute-Alsace (UHA))-Institut National de la Santé et de la Recherche Médicale (INSERM)-Centre National de la Recherche Scientifique (CNRS)-Réseau nanophotonique et optique, Centre National de la Recherche Scientifique (CNRS)-Université de Strasbourg (UNISTRA)-Université de Haute-Alsace (UHA) Mulhouse - Colmar (Université de Haute-Alsace (UHA))-Centre National de la Recherche Scientifique (CNRS)-Université de Strasbourg (UNISTRA), Institut des Molécules et Matériaux du Mans (IMMM), Le Mans Université (UM)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS), Laboratoire de physique des interfaces et des couches minces [Palaiseau] (LPICM), École polytechnique (X)-Centre National de la Recherche Scientifique (CNRS), Institut de chimie et procédés pour l'énergie, l'environnement et la santé (ICPEES), Université de Strasbourg (UNISTRA)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS)-Matériaux et nanosciences d'Alsace (FMNGE), Institut de Chimie du CNRS (INC)-Université de Strasbourg (UNISTRA)-Université de Haute-Alsace (UHA) Mulhouse - Colmar (Université de Haute-Alsace (UHA))-Institut National de la Santé et de la Recherche Médicale (INSERM)-Centre National de la Recherche Scientifique (CNRS)-Université de Strasbourg (UNISTRA)-Université de Haute-Alsace (UHA) Mulhouse - Colmar (Université de Haute-Alsace (UHA))-Institut National de la Santé et de la Recherche Médicale (INSERM)-Centre National de la Recherche Scientifique (CNRS), French-German Research Institute of Saint Louis, and Institut National Polytechnique de Lorraine (INPL)

Subjects
Materials science, Nanostructure, Iron oxide, Aucun, Nanotechnology, 02 engineering and technology, 010402 general chemistry, 01 natural sciences, Nanomaterials, chemistry.chemical_compound, Oxidation state, Specific surface area, [PHYS.COND]Physics [physics]/Condensed Matter [cond-mat], Physical and Theoretical Chemistry, Porosity, ComputingMilieux_MISCELLANEOUS, [PHYS]Physics [physics], 021001 nanoscience & nanotechnology, 0104 chemical sciences, Surfaces, Coatings and Films, Electronic, Optical and Magnetic Materials, General Energy, chemistry, Nanocrystal, Ferrite (magnet), 0210 nano-technology
Abstract

Nanostructures with controlled size, morphology, and composition represent a main challenge in materials science because controlling these parameters is fundamental to optimizing the subsequent functional properties. Aggregated nanostructures, combining both individual and collective properties of nanocrystals, offer interesting perspectives to design new magnetic nanomaterials. In that context, original porous raspberry shaped nanostructures consisting of oriented aggregates of ferrite nanocrystals have been synthesized by an one-pot polyol solvothermal method. Synthesis conditions have been optimized to obtain nanostructures featured by similar sizes of about 250 nm and nanocrystal sizes modulated from 5 to 60 nm, leading to porous structures with tunable specific surface area. Structural and magnetic studies of nanostructures as a function of the nanocrystal size evidenced their low oxidation state and enhanced magnetic properties. Indeed, the oriented aggregation of nanocrystals leads to high interface between nanograins reducing significantly their surface oxidation and enhancing their saturation magnetization in comparison to individual nanoparticles of similar sizes. Magnetic moments of each grain are also consequently strongly coupled by dipolar interactions which led to superspin glass effects.

Published
2015

39. Co-tunneling Enhancement of the Electrical Response of Nanoparticle Networks

Author

Jean-Francois Dayen, Dimitry Golubev, Bernard Doudin, Sylvie Begin-Colin, Benoit P. Pichon, Jean-Baptiste Beaufrand, and Matthias Pauly

Subjects
Materials science, Magnetoresistance, Spintronics, business.industry, Aucun, Conductance, Nanoparticle, Biasing, Nanotechnology, General Chemistry, Condensed Matter::Mesoscopic Systems and Quantum Hall Effect, Biomaterials, Electrode, Optoelectronics, General Materials Science, Wafer, business, Quantum tunnelling, Biotechnology
Abstract

A co-tunneling charge-transfer process dominates the electrical properties of a nanometer-sized "slice" in a nanoparticle network, which results in universal scaling of the conductance with temperature and bias voltage, as well as enhanced spintronics properties. By designing two large (10 μm) electrodes with short (60 nm) separation, access is obtained to transport dominated by charge transfer involving "nanoslices" made of three nanoparticles only. Magnetic iron oxide nanoparticle networks exhibit a magnetoresistance ratio that is not reachable by tunneling or hopping processes, thereby illustrating how such a size-matched planar device with dominant co-tunneling charge-transfer process is optimal for realizing multifunctional devices with enhanced change of conductance under external stimulus.

Published
2011

40. Magnetotunable Hybrid Films of Stratified Iron Oxide Nanoparticles Assembled by the Layer-by-Layer Technique

Author

Benoit P. Pichon, Olivier Felix, Marc Drillon, Gero Decher, Pierric Louet, and Sylvie Begin-Colin

Subjects
Materials science, Nanostructure, General Chemical Engineering, Physics::Medical Physics, Layer by layer, Stacking, Iron oxide, Physics::Optics, Nanoparticle, Nanotechnology, General Chemistry, Polyelectrolyte, Condensed Matter::Materials Science, chemistry.chemical_compound, chemistry, Chemical engineering, Materials Chemistry, Magnetic nanoparticles, Iron oxide nanoparticles
Abstract

Multilayer assemblies of iron oxide nanoparticles with tunable magnetic properties have been prepared by the layer-by-layer technique. The magnetic properties of multilayer assemblies depend closely on the stacking of nonagglomerated nanoparticles and, in particular, on the interlayer distance between nanoparticles, which is defined by the thickness of the polyelectrolyte multilayers. Therefore, the dipolar interactions between nanoparticles were demonstrated to occur preferentially in the plane of the nanoparticle layers and to result in the antiparallel magnetic coupling of adjacent nanoparticle layers, which is modulated as a function of the interlayer distance.

Published
2011

41. Microstructural and Magnetic Investigations of Wüstite-Spinel Core-Shell Cubic-Shaped Nanoparticles

Author

Matthias Pauly, Pierre Panissod, Veronique Pierron-Bohnes, Ovidiu Ersen, Corinne Ulhaq, Olivier Gerber, Benoit P. Pichon, Walid Baaziz, Maxime Ohlmann, Ileana Florea, Solenne Fleutot, Marc Drillon, Sylvie Begin-Colin, and Christophe Lefevre

Subjects
Materials science, General Chemical Engineering, Spinel, Aucun, Nanoparticle, Nanotechnology, General Chemistry, engineering.material, Core shell nanoparticles, equipment and supplies, Electron holography, Core shell, Condensed Matter::Materials Science, chemistry.chemical_compound, chemistry, Electron tomography, Materials Chemistry, engineering, Wüstite, human activities, Iron oxide nanoparticles
Abstract

Most studies on the synthesis of nanoparticles are currently focused on the controlled synthesis of new morphologies, including core-shell structures, which are expected to exhibit new magnetic properties for uses in spintronics and recording media applications. In this study, the structure, morphology, and composition of cubic-shaped nanoparticles are carefully investigated and compared to those of spherically shaped nanoparticles through the use of a combination of techniques: X-ray diffraction (XRD) and transmission electronic microscopy (TEM) combined with more sensitive techniques such as scanning transmission electron microscopy-high-angle annular dark field (STEM-HAADF) imaging, electron tomography, and holography. While spherically shaped nanoparticles (NPs) crystallize with the spinel structure, cubic-shaped NPs can be described as a cubic core of w€ustite surrounded by a spinel shell. Stresses are observed at the core-shell interface and within the spinel shell due to the epitaxial growth and oxidation mechanisms of the wüstite phase. Furthermore, magnetic measurements displayed an exchange bias coupling between the antiferromagnetic (AFM) core and the ferrimagnetic (FIM) shell structure of cubic-shaped nanoparticles. It is shown that the magnetic properties are influenced by stresses generated by the oxidation of w€ustite and, also exhibit variations depending upon the evolution of this core-shell structure as a function of the oxidation time.

Published
2011

42. Size-dependent properties of magnetic iron oxidenanocrystals

Author

Arnaud Demortière, Pierre Panissod, Benoit P. Pichon, Geneviève Pourroy, Bertrand Donnio, Sylvie Begin-Colin, and Daniel Guillon

Subjects
Materials science, Thermal decomposition, Aucun, Iron oxide, Metal Nanoparticles, Nanoparticle, Maghemite, engineering.material, Ferrosoferric Oxide, Magnetics, chemistry.chemical_compound, Nuclear magnetic resonance, X-Ray Diffraction, Nanocrystal, chemistry, Chemical physics, engineering, General Materials Science, Nanometre, Particle Size, Anisotropy, Magnetite
Abstract

The fine control of iron oxide nanocrystal sizes within the nanometre scale (diameters range from 2.5 to 14 nm) allows us to investigate accurately the size-dependence of their structural and magnetic properties. A study of the growth conditions of these nanocrystals obtained by thermal decomposition of an iron oleate precursor in high-boiling point solvents has been carried out. Both the type of solvent used and the ligand/precursor ratio have been systematically varied, and were found to be the key parameters to control the growth process. The lattice parameters of all the nanocrystals deduced from X-ray diffraction measurements are consistent with a structure of the type Fe(3-x)O(4), i.e. intermediate between magnetite and maghemite, which evolves toward the maghemite structure for the smallest sizes (x = 1/3). The evolution of the magnetic behavior with nanoparticle sizes emphasizes clearly the influence of the surface, especially on the saturation magnetization M(s) and the magneto-crystalline anisotropy K. Dipolar interactions and thermal dependence have been also taken into account in the study on the nanoscale size-effect of magnetic properties.

Published
2011

43. Nematic-like Organization of Magnetic Mesogen-Hybridized Nanoparticles

Author

Benoit P. Pichon, Daniel Guillon, Arnaud Demortière, Pierre Panissod, Sylvie Begin-Colin, Saïwan Buathong, and Bertrand Donnio

Subjects
Materials science, Mesogen, Supramolecular chemistry, Nanoparticle, Nanotechnology, General Chemistry, Biomaterials, chemistry.chemical_compound, Magnetic anisotropy, chemistry, Chemical engineering, Liquid crystal, Magnetic nanoparticles, General Materials Science, Hybrid material, Iron oxide nanoparticles, Biotechnology
Abstract

A fluid nematic-like phase is induced in monodisperse iron oxide nanoparticles with a diameter of 3.3 nm. This supramolecular arrangement is governed by the covalent functionalization of the nanoparticle surface with cyanobiphenyl-based ligands as mesogenic promoters. The design and synthesis of these hybrid materials and the study of their mesogenic properties are reported. In addition, the modifications of the magnetic properties of the hybridized nanoparticles are investigated as a function of the different grafted ligands. Owing to the rather large interparticular distances (about 7 nm), the dipolar interaction between nanoparticles is shown to play only a minor role. Conversely, the surface magnetic anisotropy of the particles is significantly affected by the surface derivatization.

Published
2010

44. 2D Assembling of Magnetic Iron Oxide Nanoparticles Promoted by SAMs Used as Well-Addressed Surfaces

Author

Matthias Pauly, Arnaud Demortière, Benoit P. Pichon, Alain Derory, Karin Mougin, and Sylvie Begin-Colin

Subjects
chemistry.chemical_compound, General Energy, Materials science, Chemical engineering, chemistry, Monolayer, Physical and Theoretical Chemistry, Iron oxide nanoparticles, Surfaces, Coatings and Films, Electronic, Optical and Magnetic Materials, Organic molecules
Abstract

Well-addressed surfaces which consist of self-assembled monolayers (SAMs) of organic molecules have been used to control the assembling of magnetic iron oxide nanoparticles (NPs) coated with oleic ...

Published
2010

45. Large 2D monolayer assemblies of iron oxide nanocrystals by the Langmuir–Blodgett technique

Author

Matthias Pauly, Benoit P. Pichon, Cédric Leuvrey, Sylvie Begin-Colin, Julie Delahaye, Arnaud Demortière, and Geneviève Pourroy

Subjects
Materials science, Magnetism, Iron oxide, Nanoparticle, Nanotechnology, Condensed Matter Physics, Langmuir–Blodgett film, chemistry.chemical_compound, chemistry, Nanocrystal, Monolayer, General Materials Science, Electrical and Electronic Engineering, Thin film, Iron oxide nanoparticles
Abstract

Dense monolayer assemblies of iron oxide nanoparticles have been obtained on large areas using the Langmuir–Blodgett technique. The density and ordering of the film were found to depend on the quality of the nanoparticle suspensions, which should display monodisperse nanoparticles and no free molecules. A modification of nanocrystals magnetic properties was noticed between the random configuration (powder sample) and the assembly in monolayer (Langmuir–Blodgett). The organisation in film is suggested to induce an enhancement of magnetic interactions.

Published
2009

46. Preparation and Microstructure of Titanate Nanotube Thin Films by Spray Layer-by-Layer Assembly Method

Author

Valérie Keller-Spitzer, Mathieu Grandcolas, Yoshikazu Suzuki, Susumu Yoshikawa, Nicolas Keller, and Benoit P. Pichon

Subjects
Nanotube, Materials science, Layer by layer, Nanowire, Hydrothermal synthesis, Nanoparticle, Thin film, Composite material, Microstructure, Titanate
Abstract

Hydrogen titanate nanowires were prepared by hydrothermal method in 10 M NaOH followed by ion-exchanging process. Titanate nanowire thin films were successfully obtained by spray Layer-by-Layer (spray LbL) method within a short time. Due to the good dispersion state of the nanowires in an aqueous suspension and their linear morphology, titanate nanowires effectively adsorbed on the glass substrate. As a reference, TiO2-anatase nanoparticle thin films were also prepared by spray LbL method

Published
2009

47. Structural adaptability in an organic template for CaCO3 mineralization

Author

Nico A. J. M. Sommerdijk, Elaine DiMasi, Benoit P. Pichon, Seo-Young Kwak, Materials and Interface Chemistry, and Chemical Engineering and Chemistry

Subjects
Calcite, Langmuir, Materials science, Nucleation, Context (language use), General Chemistry, Condensed Matter Physics, Mineralization (biology), Crystallography, chemistry.chemical_compound, Pulmonary surfactant, chemistry, Chemical engineering, Monolayer, General Materials Science, Biomineralization
Abstract

Biomimetic strategies to control mineral nucleation include the development of self-assembled monolayers with appropriate structural properties. We present a bis-urea based surfactant with variable structural adaptability, which induces habit modification in calcite crystals under optimal conditions. In situ surface-sensitive synchrotron X-ray scattering measurements are reported, which yield surprising conclusions for the film structure. In particular, it is found that nucleation of modified calcite is correlated with the release of two-dimensional ordering in the surfactant layer. The model system is discussed in the context of the history of Langmuir films as models for biomineralization.

Published
2007

48. Design, synthesis, characterization and properties of magnetic nanoparticle-nanocarbon hybrids

Author

Isabella Anna Vacchi, Cécilia Ménard-Moyon, Benoit P. Pichon, Eijiro Miyako, Alberto Bianco, Sylvie Begin-Colin, Christophe Lefevre, Immunopathologie et chimie thérapeutique (ICT), Institut de biologie moléculaire et cellulaire (IBMC), Université de Strasbourg (UNISTRA)-Centre National de la Recherche Scientifique (CNRS)-Université de Strasbourg (UNISTRA)-Centre National de la Recherche Scientifique (CNRS)-Centre National de la Recherche Scientifique (CNRS), Institut de Physique et Chimie des Matériaux de Strasbourg (IPCMS), Université de Strasbourg (UNISTRA)-Matériaux et nanosciences d'Alsace (FMNGE), Institut de Chimie du CNRS (INC)-Université de Strasbourg (UNISTRA)-Université de Haute-Alsace (UHA) Mulhouse - Colmar (Université de Haute-Alsace (UHA))-Institut National de la Santé et de la Recherche Médicale (INSERM)-Centre National de la Recherche Scientifique (CNRS)-Institut de Chimie du CNRS (INC)-Université de Strasbourg (UNISTRA)-Université de Haute-Alsace (UHA) Mulhouse - Colmar (Université de Haute-Alsace (UHA))-Institut National de la Santé et de la Recherche Médicale (INSERM)-Centre National de la Recherche Scientifique (CNRS)-Centre National de la Recherche Scientifique (CNRS)-Réseau nanophotonique et optique, Centre National de la Recherche Scientifique (CNRS)-Université de Strasbourg (UNISTRA)-Université de Haute-Alsace (UHA) Mulhouse - Colmar (Université de Haute-Alsace (UHA))-Centre National de la Recherche Scientifique (CNRS)-Université de Strasbourg (UNISTRA), and Université Louis Pasteur - Strasbourg I-Centre National de la Recherche Scientifique (CNRS)

Subjects
Materials science, Oxide, Iron oxide, Nanoparticle, Nanotechnology, 02 engineering and technology, Carbon nanotube, [CHIM.THER]Chemical Sciences/Medicinal Chemistry, engineering.material, 010402 general chemistry, 01 natural sciences, law.invention, chemistry.chemical_compound, Coating, law, General Materials Science, chemistry.chemical_classification, Nanocomposite, Graphene, Biomolecule, General Chemistry, 021001 nanoscience & nanotechnology, 6. Clean water, 0104 chemical sciences, chemistry, engineering, Chimie/Chimie thérapeutique, 0210 nano-technology
Abstract

International audience; Carbon nanostructured materials such as carbon nanotubes and graphene oxide are attracting much attention due to their outstanding chemical and physical properties. Metal nanoparticle-decoration can provide additional functionalities to these nanocarbons. Many chemical methods are being used for the synthesis of these metal nanoparticle-functionalized nanocarbon hybrids. On the other hand, the outstanding properties of spinelle iron oxide magnetic (MAG) nanoparticles have been efficiently used for a variety of applications such as manipulation of biomolecules and cells, cancer hyperthermia, and medical devices. Therefore, MAG nanoparticle decoration of carbon nanotubes and graphene oxide can provide promising nanohybrid materials for nanobiotechnological applications. In this work, we present a straightforward chemical route for MAG nanopartide decoration of nanocarbon supports including carbon nanotubes and graphene oxide using in situ high-temperature decomposition method. This chemical methodology allows precisely controlling the MAG nanoparticle content, the MAG nanopartide size leading to a uniform coating on the different carbon supports. The properties of these new hybrids have been thoroughly evaluated. Our results show that the MAG nanoparticle decoration process strongly affects the structural and magnetic characteristics of the hybrids. The combination of MAG nanopartide and nanocarbon materials will open the door to their use in different domains including nanocomposites, wastewater treatment, sensors, biomaterials, and cancer therapy. (C) 2015 Elsevier Ltd. All rights reserved.

Published
2015
Full Text
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49. Selective Nanotrench Filling by One-Pot Electroclick Self-Constructed Nanoparticle Films

Author

Benoit P. Pichon, Cédric Leuvrey, Pierre Schaaf, Delphine Toulemon, Loïc Jierry, Antonio Garofalo, Fouzia Boulmedais, Gaulthier Rydzek, Sylvie Begin-Colin, Delphine Felder-Flesch, Jean-Francois Dayen, Boulmedais, Fouzia, National Institute for Materials Science (NIMS), Institut de Physique et Chimie des Matériaux de Strasbourg (IPCMS), Université de Strasbourg (UNISTRA)-Centre National de la Recherche Scientifique (CNRS)-Matériaux et Nanosciences Grand-Est (MNGE), Université de Strasbourg (UNISTRA)-Université de Haute-Alsace (UHA) Mulhouse - Colmar (Université de Haute-Alsace (UHA))-Institut National de la Santé et de la Recherche Médicale (INSERM)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS)-Université de Strasbourg (UNISTRA)-Université de Haute-Alsace (UHA) Mulhouse - Colmar (Université de Haute-Alsace (UHA))-Institut National de la Santé et de la Recherche Médicale (INSERM)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS)-Réseau nanophotonique et optique, Université de Strasbourg (UNISTRA)-Université de Haute-Alsace (UHA) Mulhouse - Colmar (Université de Haute-Alsace (UHA))-Centre National de la Recherche Scientifique (CNRS)-Université de Strasbourg (UNISTRA)-Centre National de la Recherche Scientifique (CNRS), Institut de Chimie Pharmaceutique Albert Lespagnol (ICPAL), Université de Lille, Droit et Santé, Institut Charles Sadron (ICS), Université de Strasbourg (UNISTRA)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS)-Matériaux et Nanosciences Grand-Est (MNGE), Université de Strasbourg (UNISTRA)-Université de Haute-Alsace (UHA) Mulhouse - Colmar (Université de Haute-Alsace (UHA))-Institut National de la Santé et de la Recherche Médicale (INSERM)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS)-Université de Strasbourg (UNISTRA)-Université de Haute-Alsace (UHA) Mulhouse - Colmar (Université de Haute-Alsace (UHA))-Institut National de la Santé et de la Recherche Médicale (INSERM)-Centre National de la Recherche Scientifique (CNRS)-Réseau nanophotonique et optique, Université de Strasbourg (UNISTRA)-Centre National de la Recherche Scientifique (CNRS)-Matériaux et nanosciences d'Alsace (FMNGE), Institut de Chimie du CNRS (INC)-Université de Strasbourg (UNISTRA)-Université de Haute-Alsace (UHA) Mulhouse - Colmar (Université de Haute-Alsace (UHA))-Institut National de la Santé et de la Recherche Médicale (INSERM)-Centre National de la Recherche Scientifique (CNRS)-Institut de Chimie du CNRS (INC)-Université de Strasbourg (UNISTRA)-Université de Haute-Alsace (UHA) Mulhouse - Colmar (Université de Haute-Alsace (UHA))-Institut National de la Santé et de la Recherche Médicale (INSERM)-Centre National de la Recherche Scientifique (CNRS)-Réseau nanophotonique et optique, Centre National de la Recherche Scientifique (CNRS)-Université de Strasbourg (UNISTRA)-Université de Haute-Alsace (UHA) Mulhouse - Colmar (Université de Haute-Alsace (UHA))-Centre National de la Recherche Scientifique (CNRS)-Université de Strasbourg (UNISTRA), Université de Strasbourg (UNISTRA)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS)-Réseau nanophotonique et optique, Centre National de la Recherche Scientifique (CNRS)-Université de Strasbourg (UNISTRA)-Université de Haute-Alsace (UHA) Mulhouse - Colmar (Université de Haute-Alsace (UHA))-Centre National de la Recherche Scientifique (CNRS)-Université de Strasbourg (UNISTRA)-Université de Haute-Alsace (UHA) Mulhouse - Colmar (Université de Haute-Alsace (UHA))-Matériaux et nanosciences d'Alsace (FMNGE), and Institut de Chimie du CNRS (INC)-Université de Strasbourg (UNISTRA)-Université de Haute-Alsace (UHA) Mulhouse - Colmar (Université de Haute-Alsace (UHA))-Institut National de la Santé et de la Recherche Médicale (INSERM)-Centre National de la Recherche Scientifique (CNRS)-Université de Strasbourg (UNISTRA)-Institut National de la Santé et de la Recherche Médicale (INSERM)-Centre National de la Recherche Scientifique (CNRS)

Subjects
Materials science, electrical conductivity, Aucun, Nanoparticle, electroclick chemistry, Nanotechnology, General Chemistry, nanogaps, self-assembly, Electrical connection, Biomaterials, Covalent bond, Electrode, [CHIM] Chemical Sciences, magnetite iron oxide nanoparticles, [CHIM]Chemical Sciences, General Materials Science, Self-assembly, Electrical conductor, Biotechnology
Abstract

Integration of nanoparticles (NPs) into nanodevices is a challenge for enhanced sensor development. Using NPs as building blocks, a bottom-up approach based on one-pot morphogen-driven electroclick chemistry is reported to self-construct dense and robust conductive Fe3O4 NP films. Deposited covalent NP assemblies establish an electrical connection between two gold electrodes separated by a 100 nm-wide nanotrench. journal article research support, non-u.s. gov't 2015 Sep 2015 06 19 imported

Published
2015

50. Systematic Study of Exchange Coupling in Core Shell Fe3-delta O4@CoO Nanoparticles

Author

Benoit P. Pichon, Jean-Marc Greneche, Sylvie Begin-Colin, Dominique Begin, Christophe Lefevre, Xiaojie Liu, Corinne Ulhaq, Chemistry Department, Shaanxi Key Laboratory of Physico-Inorganic Chemistry, Northwest University (Xi'an), Institut de Physique et Chimie des Matériaux de Strasbourg (IPCMS), Université de Strasbourg (UNISTRA)-Centre National de la Recherche Scientifique (CNRS)-Matériaux et nanosciences d'Alsace (FMNGE), Institut de Chimie du CNRS (INC)-Université de Strasbourg (UNISTRA)-Université de Haute-Alsace (UHA) Mulhouse - Colmar (Université de Haute-Alsace (UHA))-Institut National de la Santé et de la Recherche Médicale (INSERM)-Centre National de la Recherche Scientifique (CNRS)-Institut de Chimie du CNRS (INC)-Université de Strasbourg (UNISTRA)-Université de Haute-Alsace (UHA) Mulhouse - Colmar (Université de Haute-Alsace (UHA))-Institut National de la Santé et de la Recherche Médicale (INSERM)-Centre National de la Recherche Scientifique (CNRS)-Réseau nanophotonique et optique, Centre National de la Recherche Scientifique (CNRS)-Université de Strasbourg (UNISTRA)-Université de Haute-Alsace (UHA) Mulhouse - Colmar (Université de Haute-Alsace (UHA))-Centre National de la Recherche Scientifique (CNRS)-Université de Strasbourg (UNISTRA), Institut des Molécules et Matériaux du Mans (IMMM), Le Mans Université (UM)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS), Institut de chimie et procédés pour l'énergie, l'environnement et la santé (ICPEES), Université de Strasbourg (UNISTRA)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS)-Matériaux et nanosciences d'Alsace (FMNGE), and Institut de Chimie du CNRS (INC)-Université de Strasbourg (UNISTRA)-Université de Haute-Alsace (UHA) Mulhouse - Colmar (Université de Haute-Alsace (UHA))-Institut National de la Santé et de la Recherche Médicale (INSERM)-Centre National de la Recherche Scientifique (CNRS)-Université de Strasbourg (UNISTRA)-Université de Haute-Alsace (UHA) Mulhouse - Colmar (Université de Haute-Alsace (UHA))-Institut National de la Santé et de la Recherche Médicale (INSERM)-Centre National de la Recherche Scientifique (CNRS)

Subjects
[PHYS]Physics [physics], Materials science, Magnetic domain, General Chemical Engineering, Thermal decomposition, Aucun, Nanoparticle, Nanotechnology, 02 engineering and technology, General Chemistry, 010402 general chemistry, 021001 nanoscience & nanotechnology, 01 natural sciences, 0104 chemical sciences, Crystallinity, Magnetic anisotropy, Condensed Matter::Materials Science, Exchange bias, Chemical physics, Materials Chemistry, Antiferromagnetism, [PHYS.COND]Physics [physics]/Condensed Matter [cond-mat], 0210 nano-technology, ComputingMilieux_MISCELLANEOUS, Superparamagnetism
Abstract

Although single magnetic domain nanoparticles are very promising for many applications, size reduction usually results in low magnetic anisotropy and unblocked domain at room temperature, e.g., superparamagnetism. An alternative approach is core-shell nanoparticles featured by exchange bias coupling between ferro(i)magnetic [F(i)M] and antiferromagnetic (AFM) phases. Although exchange bias coupling has been reported for very diverse coreshell nanoparticles, it is difficult to compare these studies to rationalize the effect of many structural parameters on the magnetic properties. Herein, we report on a systematic study which consists of the modulation of the shell structure and its influence on the exchange bias coupling. A series of Fe-3-O-delta(4)@CoO core-shell nanoparticles has been synthesized by seed-mediated growth based on the thermal decomposition technique. The variation of Co reactant concentration resulted in the modulation of the shell structure for which thickness, crystallinity, and interface with the iron oxide core strongly affect the magnetic properties. The thickest CoO shell and the largest F(i)M/AFM interface led to the largest exchange bias coupling. Very high values of coercive field (19?000 Oe) and M-R/M-S ratio (0.86) were obtained. The most stricking results consist of the increase of the coercive field while exchange field vanishes when the CoO thickness decreases: it is ascribed to the diffusion of Co species in the surface layer of iron oxide which generates to some extent cobalt ferrite and induces hard/soft exchange coupling between ferrimagnetic phases.

Published
2015

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