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1. Impact of disorder in Nd-based pyrochlore magnets

Author

Léger, Mélanie, Vayer, Florianne, Hatnean, Monica Ciomaga, Damay, Françoise, Decorse, Claudia, Berardan, David, Fåk, Björn, Zanotti, Jean-Marc, Berrod, Quentin, Embs, Jacques Ollivier Jan P., Fennell, Tom, Sheptyakov, Denis, Petit, Sylvain, and Lhotel, Elsa

Subjects
Condensed Matter - Strongly Correlated Electrons, Condensed Matter - Materials Science
Abstract

We study the stability of the antiferromagnetic all-in--all-out state observed in dipolar-octupolar pyrochlores that have neodymium as the magnetic species. Different types of disorder are considered, either affecting the immediate environment of the Nd$^{3+}$ ion, or substituting it with a non-magnetic ion. Starting from the well studied Nd$_2$Zr$_2$O$_7$ compound, Ti substitution on the Zr site and dilution on the Nd magnetic site with La substitution are investigated. The recently discovered entropy stabilized compound NdMox, which exhibits a high degree of disorder on the non magnetic site is also studied. Using a range of experimental techniques, especially very low-temperature magnetization and neutron scattering, we show that the all-in--all-out state is very robust and withstands substitutional disorder up to large rates. From these measurements, we estimate the Hamiltonian parameters and discuss their evolution in the framework of the phase diagram of dipolar-octupolar pyrochlore magnets., Comment: 19 pages, 20 figures (main text: 12 pages, 13 figures)

Published
2024
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2. Dynamics of Water Confined in Mesopores with Variable Surface Interaction

Author

Jani, Aicha, Busch, Mark, Mietner, J Benedikt, Ollivier, Jacques, Appel, Markus, Frick, Bernhard, Zanotti, Jean-Marc, Ghoufi, Aziz, Huber, Patrick, Fröba, Michael, and Morineau, Denis

Subjects
Physics - Chemical Physics
Abstract

We have investigated the dynamics of liquid water confined in mesostructured porous silica (MCM-41) and periodic mesoporous organosilicas (PMOs) by incoherent quasielastic neutron scattering experiments. The effect of tuning the water/surface interaction from hydrophilic to more hydrophobic on the water mobility, while keeping the pore size in the range 3.5-4.1 nm, was assessed from the comparative study of three PMOs comprising different organic bridging units and the purely siliceous MCM-41 case. An extended dynamical range was achieved by combining time-of-flight (IN5B) and backscattering (IN16B) quasielastic neutron spectrometers providing complementary energy resolutions. Liquid water was studied at regularly spaced temperatures ranging from 300 K to 243 K. In all systems, the molecular dynamics could be described consistently by the combination of two independent motions resulting from fast local motion around the average molecule position and the confined translational jump diffusion of its center of mass. All the molecules performed local relaxations, whereas the translational motion of a fraction of molecules was frozen on the experimental timescale. This study provides a comprehensive microscopic view on the dynamics of liquid water confined in mesopores, with distinct surface chemistries, in terms of non-mobile/mobile fraction, self-diffusion coefficient, residence time, confining radius, local relaxation time, and their temperature dependence. Importantly, it demonstrates that the strength of the water/surface interaction determines the long-time tail of the dynamics, which we attributed to the translational diffusion of interfacial molecules, while the water dynamics in the pore center is barely affected by the interface hydrophilicity.

Published
2020
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4. Impact of disorder in Nd-based pyrochlore magnets

Author

Léger, Mélanie, primary, Vayer, Florianne, additional, Hatnean, Monica Ciomaga, additional, Damay, Françoise, additional, Decorse, Claudia, additional, Berardan, David, additional, Fåk, Björn, additional, Zanotti, Jean-Marc, additional, Berrod, Quentin, additional, Ollivier, Jacques, additional, Embs, Jan P., additional, Fennell, Tom, additional, Sheptyakov, Denis, additional, Petit, Sylvain, additional, and Lhotel, Elsa, additional

Published
2024
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6. Ionic liquids confined in 1D CNT membranes:gigantic ionic conductivity

Author

Berrod, Quentin, Judeinstein, Patrick, Fu, Yanbao, Battaglia, Vincent S., Fournier, Adeline, Dijon, Jean, and Zanotti, Jean-Marc

Subjects
Condensed Matter - Soft Condensed Matter
Abstract

Ionic Liquids (ILs) are organic molten salts characterized by the total absence of solvent. They show remarkable properties: low vapor pressure, high ionic conductivity, high chemical, thermal and electrochemical stability. These electrolytes meet therefore key criteria for the development of safe energy storage systems. Due to a competition between electrostatic and van der Walls interactions, ILs show an uncommon property for neat bulk liquids: they self-organize in transient nanometric domains. In ILs-based electrochemical devices, this fluctuating nano-segregation acts as energy barriers to the long range diffusional processes and hence to the ionic conductivity. Here, we show how the ionic conductivity of ILs can be increased by more than one order of magnitude by exploiting one dimensional (1D) confinement effects in macroscopically oriented carbon nanotube (CNT) membranes. We identify 1D CNT membranes as promising separators for high instant power batteries.

Published
2017

9. Influence of Cationic Ordering on the Lattice Dynamics of Monoclinic Cu5Sn2S7and Cubic Cu5Sn2S6.65Cl0.35Sulfides

Author

Candolfi, Christophe, Le Gars, Lucas, Guélou, Gabin, Ventrapati, Pavan Kumar, Prestipino, Carmelo, Guizouarn, Thierry, Pasturel, Mathieu, Levinský, Petr, Lemoine, Pierric, Raveau, Bernard, Shen, Xingchen, Lebedev, Oleg I., Berrod, Quentin, Zanotti, Jean-Marc, and Guilmeau, Emmanuel

Abstract

Cu2SnS3is the parent compound of a series of phases in the Cu2+xSn1–xS3section (0 ≤ x≤ 0.15) of the ternary Cu–Sn–S phase diagram, the crystal structure of which can be controlled by varying the synthesis process and/or through a fine-tuning of the chemical composition. Despite being structurally close to the sphalerite structure, the thermal transport of these compounds is strongly dependent on the exact lattice symmetry and degree of atomic disorder. Here, we investigate the lattice dynamics of the monoclinic ordered Cu5Sn2S7(space group C2) and cubic disordered Cu5Sn2S6.65Cl0.35(space group F4̅3m) compounds by temperature-dependent powder inelastic neutron scattering (INS). In both cases, the INS spectra feature low-energy optical modes mostly weighed by the thermal motion of Cu atoms. The response of the INS spectra of Cu5Sn2S6.65Cl0.35to temperature variations is indicative of quasi-harmonic behavior. Combined with analyses of the low-temperature specific heat, these findings show that the significant lowering of the lattice thermal conductivity in cubic Cu5Sn2S6.65Cl0.35is due to a reduced phonon mean free path tied to the increased level of disorder in the unit cell. These results highlight how the stabilization of highly symmetric, yet strongly disordered crystal structures akin to those observed in high-entropy alloys, can lead to a drastic reduction in the heat transport, offering an effective approach to design high-performance thermoelectric sulfides.

Published
2024
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10. Relation between static short-range order and dynamic heterogeneities in a nanoconfined liquid crystal

Author

Lefort, Ronan, Morineau, Denis, Guégan, Régis, Guendouz, Mohammed, Zanotti, Jean-Marc, and Frick, Bernhard

Subjects
Physics - Chemical Physics, Physics - Optics
Abstract

We analyze the molecular dynamics heterogeneity of the liquid crystal 4-n-octyl-4'-cyanobiphenyl nanoconfined in porous silicon. We show that the temperature dependence of the dynamic correlation length ?wall, which measures the distance over which a memory of the interfacial slowing down of the molecular dynamics persists, is closely related to the growth of the short-range static order arising from quenched random fields. More generally, this result may also shed some light on the connection between static and dynamic heterogeneities in a wide class of condensed and soft matter systems.

Published
2009
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11. Bioprotectant glassforming solutions confined in porous silicon nanocapillaries

Author

Busselez, Rémi, Lefort, Ronan, Ji, Qing, Guégan, Régis, Chahine, Gilbert, Guendouz, Mohammed, Zanotti, Jean-Marc, Frick, Bernhard, and Morineau, Denis

Subjects
Condensed Matter - Soft Condensed Matter
Abstract

Glycerol and trehalose-glycerol binary solutions are glass-forming liquids with remarkable bioprotectant properties. In this paper, we address the effects of confining of these solutions in straight channels of diameter D=8 nm formed by porous silicon. Neutron diffraction and incoherent quasielastic neutron scattering are used to reveal the different effects of nanoconfinement and addition of trehalose on the intermolecular structure and molecular dynamics of the liquid and glassy phases, on a nanosecond timescale., Comment: Accepted for the 2008 MRS Fall Meeting Symposium TT proceedings

Published
2009

12. Collective magnetic state induced by charge disorder in the non-Kramers rare-earth pyrochlore Tb2ScNbO7

Author

Alexanian, Yann, primary, Lhotel, Elsa, additional, Ballou, Rafik, additional, Colin, Claire V., additional, Klein, Holger, additional, Le Priol, Antonin, additional, Museur, Flavien, additional, Robert, Julien, additional, Pachoud, Elise, additional, Lejay, Pascal, additional, Hadj-Azzem, Abdellali, additional, Fåk, Bjorn, additional, Berrod, Quentin, additional, Zanotti, Jean-Marc, additional, Suard, Emmanuelle, additional, Dejoie, Catherine, additional, de Brion, Sophie, additional, and Simonet, Virginie, additional

Published
2023
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13. Incoherent Quasielastic Neutron Scattering Study of Molecular dynamics of 4-n-cyano-4'-octylbiphenyl

Author

Lefort, Ronan, Morineau, Denis, Guégan, Régis, Ecolivet, Claude, Guendouz, Mohammed, Zanotti, Jean-Marc, and Frick, Bernhard

Subjects
Physics - Chemical Physics, Condensed Matter - Soft Condensed Matter
Abstract

We report incoherent quasielastic neutron scattering experiments on the thermotropic liquid crystal 4-n-cyano-4'-octylbiphenyl. The combination of time-of-flight and backscattering data allows analyzing the intermediate scattering function over about three decades of relaxation times. Translational diffusion and uniaxial molecular rotations are clearly identified as the major relaxation processes in respectively the nanosecond and picosecond time scales. The comparison with literature data obtained by other techniques is discussed., Comment: Accepted in Phys. Chem. Chem. Phys

Published
2008
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14. Molecular dynamics of a short range ordered smectic phase nanoconfined into porous silicon

Author

Guégan, Régis, Morineau, Denis, Lefort, Ronan, Moréac, Alain, Béziel, Wilfried, Guendouz, Mohammed, Zanotti, Jean-Marc, and Frick, Bernhard

Subjects
Condensed Matter - Materials Science
Abstract

4-n-octyl-4-cyanobiphenyl (8CB) has been recently shown to display an unusual sequence of phases when confined into porous silicon (PSi). The gradual increase of oriented short-range smectic (SRS) correlations in place of a phase transition has been interpreted as a consequence of the anisotropic quenched disorder induced by confinement in PSi. Combining two quasielastic neutron scattering experiments with complementary energy resolutions, we present the first investigation of the individual molecular dynamics of this system. A large reduction of the molecular dynamics is observed in the confined liquid phase, as a direct consequence of the dynamical boundary conditions imposed by the confinement. Temperature fixed window scans (FWS) reveal a continuous 'glass-like' reduction of the molecular dynamics of the confined liquid and SRS phases on cooling down to 250 K, where a solid-like behavior is finally reached by a two steps crystallization process.

Published
2006
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18. Dynamics of water confined in mesopores with variable surface interaction.

Author

Jani, Aîcha, Busch, Mark, Mietner, J. Benedikt, Ollivier, Jacques, Appel, Markus, Frick, Bernhard, Zanotti, Jean-Marc, Ghoufi, Aziz, Huber, Patrick, Fröba, Michael, and Morineau, Denis

Subjects
SURFACE interactions, MESOPORES, POROUS silica, QUASI-elastic scattering, SURFACE chemistry, NEUTRONS, HYDROPHOBIC interactions
Abstract

We have investigated the dynamics of liquid water confined in mesostructured porous silica (MCM-41) and periodic mesoporous organosilicas (PMOs) by incoherent quasielastic neutron scattering experiments. The effect of tuning the water/surface interaction from hydrophilic to more hydrophobic on the water mobility, while keeping the pore size in the range 3.5 nm–4.1 nm, was assessed from the comparative study of three PMOs comprising different organic bridging units and the purely siliceous MCM-41 case. An extended dynamical range was achieved by combining time-of-flight (IN5B) and backscattering (IN16B) quasielastic neutron spectrometers providing complementary energy resolutions. Liquid water was studied at regularly spaced temperatures ranging from 300 K to 243 K. In all systems, the molecular dynamics could be described consistently by the combination of two independent motions resulting from fast local motion around the average molecule position and the confined translational jump diffusion of its center of mass. All the molecules performed local relaxations, whereas the translational motion of a fraction of molecules was frozen on the experimental timescale. This study provides a comprehensive microscopic view on the dynamics of liquid water confined in mesopores, with distinct surface chemistries, in terms of non-mobile/mobile fraction, self-diffusion coefficient, residence time, confining radius, local relaxation time, and their temperature dependence. Importantly, it demonstrates that the strength of the water/surface interaction determines the long-time tail of the dynamics, which we attributed to the translational diffusion of interfacial molecules, while the water dynamics in the pore center is barely affected by the interface hydrophilicity. [ABSTRACT FROM AUTHOR]

Published
2021
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23. Inelastic and quasi-elastic neutron scattering. Application to soft-matter

Author

Berrod Quentin, Lagrené Karine, Ollivier Jacques, and Zanotti Jean-Marc

Subjects
Physics, QC1-999
Abstract

Microscopic dynamical events control many of the physical processes at play in condensed matter: transport, magnetism, catalysis and even function of biological assemblies. Inelastic (INS) and Quasi-Elastic Neutron Scattering (QENS) are irreplaceable probes of these phenomena. These experimental techniques reveal the displacements of atoms and molecules over distances spanning from angstroms to a few tens of nanometers, on time scales ranging from a fraction of picoseconds to microseconds. In this context, the different INS and QENS machines (Time-of-Flight (ToF), Backscattering (BS) and Neutron spin-echo (NSE)) stand at a central position. After introducing an underlying basic theoretical toolbox for neutron scattering, the principles and key elements of a ToF measurement are described. While, here, we mainly focus on disk choppers spectrometers, all the INS/QENS instruments share a common ground: they directly and simultaneously probe correlation functions in both time and space, so that the scattering vector (Q) dependence of the systems characteristic time(s) can be measured. To illustrate, the potentialities of the technique in the field of soft-matter, we show a multiscale approach of the dynamics of a polymer melt. The system is probed from the molecular to the mesoscopic scale (1 ps to 0.6 μs and 0.1 to 40 nm), in bulk and under nanometric confinement. We address the different dynamical modes of a high mass entangled polymer chain: local monomer dynamics, Rouse modes up to the reptation process. This study exemplifies that, used in conjunction with hydrogen/deuterium isotopic effects, high resolution QENS can be bridged to the Zero Average Contrast (ZAC) method to probe, in a non destructive way, the dynamics of a single polymer chain in bulk but also under severe nanometric confinement. Connection and complementarity of the neutron derived analysis with Pulsed-Field Gradient and Relaxation NMR techniques are discussed.

Published
2018
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24. Dynamic properties of the incommensurately modulated Rb2ZnCl4 phase

Author

de Laitre, Geoffroy, primary, Kotla, Surya Rohith, additional, van Smaalen, Sander, additional, Sidis, Yvan, additional, Berrod, Quentin, additional, Zanotti, Jean-Marc, additional, Ollivier, Jacques, additional, Raymond, Stéphane, additional, Bourdarot, Frédéric, additional, Piovano, Andrea, additional, Opagiste, Christine, additional, Coindeau, Stéphane, additional, and de Boissieu, Marc, additional

Published
2021
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25. Dynamical properties of the incommensurately modulated Rb₂ZnCl₄ phase

Author

Laitre, Geoffroy, Kotla, Surya Rohith, Smaalen, Sander, Sidis, Yvan, Berrod, Quentin, Zanotti, Jean-Marc, Ollivier, Jacques, Raymond, Stéphane, Bourdarot, Frederic, Piovano, Andrea, Opagiste, Christine, Coindeau, Stéphane, Boissieu, Marc, Science et Ingénierie des Matériaux et Procédés (SIMaP), Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS)-Université Grenoble Alpes (UGA)-Institut polytechnique de Grenoble - Grenoble Institute of Technology (Grenoble INP ), Université Grenoble Alpes (UGA), University of Bayreuth, LLB - Nouvelles frontières dans les matériaux quantiques (NFMQ), 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)-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Paris-Saclay-Centre National de la Recherche Scientifique (CNRS), LLB - Matière molle et biophysique (MMB), Institut Laue-Langevin (ILL), Magnétisme et Diffusion Neutronique (MDN ), Modélisation et Exploration des Matériaux (MEM), Institut de Recherche Interdisciplinaire de Grenoble (IRIG), Direction de Recherche Fondamentale (CEA) (DRF (CEA)), Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Direction de Recherche Fondamentale (CEA) (DRF (CEA)), Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Grenoble Alpes (UGA)-Institut de Recherche Interdisciplinaire de Grenoble (IRIG), Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Grenoble Alpes (UGA), Magnétisme et Supraconductivité (NEEL - MagSup), Institut Néel (NEEL), Centre National de la Recherche Scientifique (CNRS)-Université Grenoble Alpes (UGA)-Institut polytechnique de Grenoble - Grenoble Institute of Technology (Grenoble INP ), Université Grenoble Alpes (UGA)-Centre National de la Recherche Scientifique (CNRS)-Université Grenoble Alpes (UGA)-Institut polytechnique de Grenoble - Grenoble Institute of Technology (Grenoble INP ), Consortium des Moyens Technologiques Communs (CMTC), Institut National Polytechnique de Grenoble (INPG), and Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Paris-Saclay-Centre National de la Recherche Scientifique (CNRS)

Subjects
incommensurate modulation, phason modes, aperiodic crystals, lattice dynamics, [PHYS.COND]Physics [physics]/Condensed Matter [cond-mat], inelastic neutron scattering
Abstract

International audience

Published
2021

27. Combining density functional theory and Monte Carlo neutron transport calculations to study the phonon density of states of UO2 up to 1675 K by inelastic neutron scattering

Author

Noguere, Gilles, Scotta, J.P., Xu, Shuqi, Filhol, A., Ollivier, Jacques, FARHI, Emmanuel, calzavarra, yoann, Rols, Stéphane, Fak, Bjorn, Zanotti, Jean-Marc, Berrod, Quentin, Institut de recherche sur les systèmes nucléaires pour la production d'énergie bas carbone (IRESNE), CEA-Direction des Energies (ex-Direction de l'Energie Nucléaire) (CEA-DES (ex-DEN)), Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Commissariat à l'énergie atomique et aux énergies alternatives (CEA), Institut Laue-Langevin (ILL), 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), Synthèse, Structure et Propriétés de Matériaux Fonctionnels (STEP ), SYstèmes Moléculaires et nanoMatériaux pour l’Energie et la Santé (SYMMES), Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS)-Institut de Recherche Interdisciplinaire de Grenoble (IRIG), Direction de Recherche Fondamentale (CEA) (DRF (CEA)), Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Direction de Recherche Fondamentale (CEA) (DRF (CEA)), Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Grenoble Alpes (UGA)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS)-Institut de Recherche Interdisciplinaire de Grenoble (IRIG), Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Grenoble Alpes (UGA), Département Interfaces pour l'énergie, la Santé et l'Environnement (DIESE), ILL, and Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Centre National de la Recherche Scientifique (CNRS)-Université Paris-Saclay

Subjects
[PHYS.COND.CM-SCM]Physics [physics]/Condensed Matter [cond-mat]/Soft Condensed Matter [cond-mat.soft]
Abstract

International audience; Significant advances in the use of atomistic simulation techniques, such as ab initio density functional theory and the molecular dynamics method, made it possible to predictively calculate properties of materials. In parallel, low-energy neutron scattering instruments and data analysis tools available in different institutes become mature for providing high-quality data for experimental validation purposes. Despite such experimental and theoretical improvements, the accurate modeling of experimental neutron-weighted multiphonon spectra for UO 2 over a broad temperature range still remains an issue. Combining prior phonon density of states (PDOS) from density functional theory and Monte Carlo inelastic neutron scattering calculations in a Bayesian fitting procedure is a valuable alternative approach to assess the partial PDOS of uranium and oxygen in UO 2 from 294 to 1675 K for improving the comparison to experiment and exploring the first-principles calculation hypothesis.

Published
2020

29. High temperature molecular motions within a model protomembrane architecture.

Author

Misuraca, Loreto, Matsuo, Tatsuhito, Cisse, Aline, LoRicco, Josephine, Caliò, Antonio, Zanotti, Jean-Marc, Demé, Bruno, Oger, Philippe, and Peters, Judith

Abstract

Modern phospholipid membranes are known to be in a functional, physiological state, corresponding to the liquid crystalline phase, only under very precise external conditions. The phase is characterised by specific lipid motions, which seem mandatory to permit sufficient flexibility and stability for the membrane. It can be assumed that similar principles hold for proto-membranes at the origin of life although they were likely composed of simpler, single chain fatty acids and alcohols. In the present study we investigated molecular motions of four types of model membranes to shed light on the variations of dynamics and structure from low to high temperature as protocells might have existed close to hot vents. We find a clear hierarchy among the flexibilities of the samples, where some structural parameters seem to depend on the lipid type used while others do not. [ABSTRACT FROM AUTHOR]

Published
2022
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32. Water Dynamics in Nanoporous Confinement: A Quasielastic Neutron Scattering Study

Author

Jani, Aicha, Mietner, Benedikt, Busch, Mark, Ollivier, Jacques, Frick, Bernhard, Appel, Markus, Zanotti, Jean-Marc, Huber, Patrick, Fröba, Michael, Morineau, Denis, Institut de Physique de Rennes (IPR), Université de Rennes 1 (UR1), Université de Rennes (UNIV-RENNES)-Université de Rennes (UNIV-RENNES)-Centre National de la Recherche Scientifique (CNRS), Universität Hamburg (UHH), Hamburg University of Technology (TUHH), Institut Laue-Langevin (ILL), ILL, LLB - Matière molle et biophysique (MMB), Laboratoire Léon Brillouin (LLB - UMR 12), Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Centre National de la Recherche Scientifique (CNRS)-Université Paris-Saclay-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Centre National de la Recherche Scientifique (CNRS)-Université Paris-Saclay, ANR-18-CE92-0011,NanoLiquids,Modifications des Propriétés de Fluides Multiphasiques par Confinement Géométrique dans des Matériaux Mésoporeux Avancés(2018), Université de Rennes (UR)-Centre National de la Recherche Scientifique (CNRS), Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Paris-Saclay-Centre National de la Recherche Scientifique (CNRS)-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Paris-Saclay-Centre National de la Recherche Scientifique (CNRS), Morineau, Denis, and APPEL À PROJETS GÉNÉRIQUE 2018 - Modifications des Propriétés de Fluides Multiphasiques par Confinement Géométrique dans des Matériaux Mésoporeux Avancés - - NanoLiquids2018 - ANR-18-CE92-0011 - AAPG2018 - VALID

Subjects
[PHYS.COND.CM-SCM]Physics [physics]/Condensed Matter [cond-mat]/Soft Condensed Matter [cond-mat.soft], ComputingMilieux_MISCELLANEOUS, [PHYS.COND.CM-SCM] Physics [physics]/Condensed Matter [cond-mat]/Soft Condensed Matter [cond-mat.soft]
Abstract

International audience

Published
2020

33. Dynamic heterogeneities in liquid mixtures confined in nanopores

Author

Jani, Aicha, Mhanna, Ramona, MIETNER, Benedikt, Busch, Mark, Zanotti, Jean-Marc, Frick, Bernhard, Ghoufi, Aziz, Huber, Patrick, FRÖBA, Michael, Morineau, Denis, Institut de Physique de Rennes (IPR), Université de Rennes (UR)-Centre National de la Recherche Scientifique (CNRS), Institut Laue-Langevin (ILL), Universität Hamburg (UHH), Hamburg University of Technology (TUHH), LLB - Matière molle et biophysique (MMB), 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)-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Paris-Saclay-Centre National de la Recherche Scientifique (CNRS), Support from Rennes Metropole and Europe (FEDER Fund – CPER PRINT2TAN), ANR-18-CE92-0011,NanoLiquids,Modifications des Propriétés de Fluides Multiphasiques par Confinement Géométrique dans des Matériaux Mésoporeux Avancés(2018), Morineau, Denis, APPEL À PROJETS GÉNÉRIQUE 2018 - Modifications des Propriétés de Fluides Multiphasiques par Confinement Géométrique dans des Matériaux Mésoporeux Avancés - - NanoLiquids2018 - ANR-18-CE92-0011 - AAPG2018 - VALID, Université de Rennes 1 (UR1), Université de Rennes (UNIV-RENNES)-Université de Rennes (UNIV-RENNES)-Centre National de la Recherche Scientifique (CNRS), ILL, and Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Centre National de la Recherche Scientifique (CNRS)-Université Paris-Saclay-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Centre National de la Recherche Scientifique (CNRS)-Université Paris-Saclay

Subjects
[PHYS.COND.CM-SCM]Physics [physics]/Condensed Matter [cond-mat]/Soft Condensed Matter [cond-mat.soft], ComputingMilieux_MISCELLANEOUS, [PHYS.COND.CM-SCM] Physics [physics]/Condensed Matter [cond-mat]/Soft Condensed Matter [cond-mat.soft]
Abstract

International audience

Published
2020

34. PROCEDE DE FABRICATION D’UNE MEMBRANE A ELECTROLYTE

Author

Belime, Agathe, Benwadih, M., Ramos, R., Berrod, Quentin, Zanotti, Jean-Marc, Laboratoire Léon Brillouin (LLB - UMR 12), Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Centre National de la Recherche Scientifique (CNRS)-Université Paris-Saclay, Département des Technologies des NanoMatériaux (DTNM), Laboratoire d'Innovation pour les Technologies des Energies Nouvelles et les nanomatériaux (LITEN), Institut National de L'Energie Solaire (INES), Centre National de la Recherche Scientifique (CNRS)-Université Savoie Mont Blanc (USMB [Université de Savoie] [Université de Chambéry])-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Centre National de la Recherche Scientifique (CNRS)-Université Savoie Mont Blanc (USMB [Université de Savoie] [Université de Chambéry])-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Institut National de L'Energie Solaire (INES), Centre National de la Recherche Scientifique (CNRS)-Université Savoie Mont Blanc (USMB [Université de Savoie] [Université de Chambéry])-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Centre National de la Recherche Scientifique (CNRS)-Université Savoie Mont Blanc (USMB [Université de Savoie] [Université de Chambéry])-Commissariat à l'énergie atomique et aux énergies alternatives (CEA), Synthèse, Structure et Propriétés de Matériaux Fonctionnels (STEP ), SYstèmes Moléculaires et nanoMatériaux pour l’Energie et la Santé (SYMMES), Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS)-Institut de Recherche Interdisciplinaire de Grenoble (IRIG), Direction de Recherche Fondamentale (CEA) (DRF (CEA)), Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Direction de Recherche Fondamentale (CEA) (DRF (CEA)), Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Grenoble Alpes (UGA)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS)-Institut de Recherche Interdisciplinaire de Grenoble (IRIG), Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Grenoble Alpes (UGA), LLB - Matière molle et biophysique (MMB), Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Centre National de la Recherche Scientifique (CNRS)-Université Paris-Saclay-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Centre National de la Recherche Scientifique (CNRS)-Université Paris-Saclay, Berrod, Quentin, Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Paris-Saclay-Centre National de la Recherche Scientifique (CNRS), Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Savoie Mont Blanc (USMB [Université de Savoie] [Université de Chambéry])-Centre National de la Recherche Scientifique (CNRS)-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Savoie Mont Blanc (USMB [Université de Savoie] [Université de Chambéry])-Centre National de la Recherche Scientifique (CNRS)-Institut National de L'Energie Solaire (INES), Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Savoie Mont Blanc (USMB [Université de Savoie] [Université de Chambéry])-Centre National de la Recherche Scientifique (CNRS)-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Savoie Mont Blanc (USMB [Université de Savoie] [Université de Chambéry])-Centre National de la Recherche Scientifique (CNRS), and Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Paris-Saclay-Centre National de la Recherche Scientifique (CNRS)-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Paris-Saclay-Centre National de la Recherche Scientifique (CNRS)

Subjects
[PHYS.COND.CM-SCM]Physics [physics]/Condensed Matter [cond-mat]/Soft Condensed Matter [cond-mat.soft], [PHYS.COND.CM-SCM] Physics [physics]/Condensed Matter [cond-mat]/Soft Condensed Matter [cond-mat.soft]
Published
2020

35. Disorder-driven glasslike thermal conductivity in colusite Cu26V2Sn6S32 investigated by Mössbauer spectroscopy and inelastic neutron scattering

Author

Candolfi, Christophe, Guélou, Gabin, Bourgès, Cédric, Supka, Andrew, Al Rahal Al Orabi, Rabih, Fornari, Marco, Malaman, Bernard, Le Caër, Gérard, Lemoine, Pierric, Hardy, Vincent, Zanotti, Jean-Marc, Chetty, Raju, Ohta, Michihiro, Suekuni, Koichiro, Guilmeau, Emmanuel, Institut Jean Lamour (IJL), Institut de Chimie du CNRS (INC)-Université de Lorraine (UL)-Centre National de la Recherche Scientifique (CNRS), Laboratoire de cristallographie et sciences des matériaux (CRISMAT), Université de Caen Normandie (UNICAEN), Normandie Université (NU)-Normandie Université (NU)-École Nationale Supérieure d'Ingénieurs de Caen (ENSICAEN), Normandie Université (NU)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS)-Institut de Recherche sur les Matériaux Avancés (IRMA), 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)-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université de Rouen Normandie (UNIROUEN), Institut National des Sciences Appliquées (INSA)-Normandie Université (NU)-Institut National des Sciences Appliquées (INSA)-Centre National de la Recherche Scientifique (CNRS), Central Michigan University (CMU), Solvay (France), Institut de Physique de Rennes (IPR), Université de Rennes (UR)-Centre National de la Recherche Scientifique (CNRS), Institut des Sciences Chimiques de Rennes (ISCR), Université de Rennes (UR)-Institut National des Sciences Appliquées - Rennes (INSA Rennes), Institut National des Sciences Appliquées (INSA)-Institut National des Sciences Appliquées (INSA)-Ecole Nationale Supérieure de Chimie de Rennes (ENSCR)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS), LLB - Matière molle et biophysique (MMB), 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)-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Paris-Saclay-Centre National de la Recherche Scientifique (CNRS), Université de Tsukuba = University of Tsukuba, National Institute of Advanced Industrial Science and Technology (AIST), Kyushu University, U.S. Department of Defense, N000141310635, Office of Naval Research, Ministry of Economy, Trade and Industry, ANR-15-CE05-0027,MASSCOTE,Matériaux Sulfures à Structures Complexes: application à la Thermoélectricité(2015), Université de Lorraine (UL)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS), École Nationale Supérieure d'Ingénieurs de Caen (ENSICAEN), Normandie Université (NU)-Normandie Université (NU)-Centre National de la Recherche Scientifique (CNRS)-Université de Caen Normandie (UNICAEN), Normandie Université (NU)-Institut de Chimie du CNRS (INC), Université de Rennes 1 (UR1), Université de Rennes (UNIV-RENNES)-Université de Rennes (UNIV-RENNES)-Centre National de la Recherche Scientifique (CNRS), Centre National de la Recherche Scientifique (CNRS)-Institut de Chimie du CNRS (INC)-Université de Rennes 1 (UR1), Université de Rennes (UNIV-RENNES)-Université de Rennes (UNIV-RENNES)-Ecole Nationale Supérieure de Chimie de Rennes (ENSCR)-Institut National des Sciences Appliquées - Rennes (INSA Rennes), Institut National des Sciences Appliquées (INSA)-Université de Rennes (UNIV-RENNES)-Institut National des Sciences Appliquées (INSA), Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Centre National de la Recherche Scientifique (CNRS)-Université Paris-Saclay-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Centre National de la Recherche Scientifique (CNRS)-Université Paris-Saclay, Kyushu University [Fukuoka], Agence Nationale de la Recherche, Université de Lorraine (UL)-Centre National de la Recherche Scientifique (CNRS), Centre National de la Recherche Scientifique (CNRS)-École Nationale Supérieure d'Ingénieurs de Caen (ENSICAEN), Normandie Université (NU)-Normandie Université (NU)-Université de Caen Normandie (UNICAEN), Normandie Université (NU), Institut National des Sciences Appliquées - Rennes (INSA Rennes), Institut National des Sciences Appliquées (INSA)-Université de Rennes (UNIV-RENNES)-Institut National des Sciences Appliquées (INSA)-Université de Rennes (UNIV-RENNES)-Centre National de la Recherche Scientifique (CNRS)-Ecole Nationale Supérieure de Chimie de Rennes-Université de Rennes 1 (UR1), Université de Rennes (UNIV-RENNES), Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Centre National de la Recherche Scientifique (CNRS)-Université Paris-Saclay, University of Tsukuba, and National Institute for Advanced Industrial Science and Technology - AIST (JAPAN)

Subjects
[PHYS]Physics [physics], Thermal properties, Mössbauer spectroscopy, Time-of-flight neutron spectroscopy, Polycrystalline materials, [PHYS.COND.CM-MS]Physics [physics]/Condensed Matter [cond-mat]/Materials Science [cond-mat.mtrl-sci], [CHIM]Chemical Sciences, [CHIM.MATE]Chemical Sciences/Material chemistry
Abstract

International audience; The influence of structural disorder on the thermal transport in the colusite Cu26V2Sn6S32 has been investigated by means of low-temperature thermal conductivity and specific heat measurements (2–300 K), 119Sn Mössbauer spectroscopy and temperature-dependent powder inelastic neutron scattering (INS). Variations in the high-temperature synthesis conditions act as a key parameter for tuning the degree of disorder in colusite compounds. Intriguingly, we find that all synthesized samples are disordered, the degree of which varies with the synthesis conditions used. Mössbauer data clearly evidence that Sn atoms do not solely occupy the 6c site of the crystal lattice but are present on possibly both the Cu and V sites, leading to a random distribution of these three cations within the unit cell. Increasing the disorder in these materials tends to lead to a smearing out of the main features in the phonon density of states measured by INS. Although the evolution of the inelastic signal upon warming is well described by a quasiharmonic approximation, elastic properties calculations indicate large average Grüneisen parameters, consistent with those determined experimentally from thermodynamic data. Increasing the level of disorder results in a decreased average Grüneisen parameter suggesting that the lowered lattice thermal conductivity is not driven by enhanced anharmonicity. These results provide experimental evidence to support that the remarkable changeover in the lattice thermal conductivity from crystalline to glasslike is solely driven by enhanced disorder accompanied by local lattice distortions.

Published
2020

36. Disentangling water, ion and polymer dynamics in an anion exchange membrane

Author

Foglia, Fabrizia, primary, Berrod, Quentin, additional, Gebel, Gérard, additional, Sakai, V., additional, Appel, Markus, additional, Zanotti, Jean-Marc, additional, Tyagi, Madhu Sudan, additional, Mahmoudi, Najet, additional, Clancy, Adam, additional, Miller, Thomas, additional, Smith, Keenan, additional, Brett, Dan, additional, Shearing, Paul, additional, Lyonnard, Sandrine, additional, and McMillan, Paul, additional

Published
2020
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39. Ionic liquids confined in 1D CNT membranes:gigantic ionic conductivity

Author

Berrod, Quentin, Judeinstein, Patrick, Fu, Yanbao, Battaglia, Vincent S., Fournier, Adeline, Dijon, Jean, Zanotti, Jean-Marc, Lawrence Berkeley National Laboratory [Berkeley] (LBNL), 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), Département des Technologies des NanoMatériaux (DTNM), Laboratoire d'Innovation pour les Technologies des Energies Nouvelles et les nanomatériaux (LITEN), Institut National de L'Energie Solaire (INES), Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Savoie Mont Blanc (USMB [Université de Savoie] [Université de Chambéry])-Centre National de la Recherche Scientifique (CNRS)-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Savoie Mont Blanc (USMB [Université de Savoie] [Université de Chambéry])-Centre National de la Recherche Scientifique (CNRS)-Institut National de L'Energie Solaire (INES), Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Savoie Mont Blanc (USMB [Université de Savoie] [Université de Chambéry])-Centre National de la Recherche Scientifique (CNRS)-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Savoie Mont Blanc (USMB [Université de Savoie] [Université de Chambéry])-Centre National de la Recherche Scientifique (CNRS), Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Centre National de la Recherche Scientifique (CNRS)-Université Paris-Saclay, Centre National de la Recherche Scientifique (CNRS)-Université Savoie Mont Blanc (USMB [Université de Savoie] [Université de Chambéry])-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Centre National de la Recherche Scientifique (CNRS)-Université Savoie Mont Blanc (USMB [Université de Savoie] [Université de Chambéry])-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Institut National de L'Energie Solaire (INES), Centre National de la Recherche Scientifique (CNRS)-Université Savoie Mont Blanc (USMB [Université de Savoie] [Université de Chambéry])-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Centre National de la Recherche Scientifique (CNRS)-Université Savoie Mont Blanc (USMB [Université de Savoie] [Université de Chambéry])-Commissariat à l'énergie atomique et aux énergies alternatives (CEA), and Berrod, Quentin

Subjects
Soft Condensed Matter (cond-mat.soft), FOS: Physical sciences, Condensed Matter - Soft Condensed Matter, [PHYS.COND.CM-SCM]Physics [physics]/Condensed Matter [cond-mat]/Soft Condensed Matter [cond-mat.soft], [PHYS.COND.CM-SCM] Physics [physics]/Condensed Matter [cond-mat]/Soft Condensed Matter [cond-mat.soft]
Abstract

Ionic Liquids (ILs) are organic molten salts characterized by the total absence of solvent. They show remarkable properties: low vapor pressure, high ionic conductivity, high chemical, thermal and electrochemical stability. These electrolytes meet therefore key criteria for the development of safe energy storage systems. Due to a competition between electrostatic and van der Walls interactions, ILs show an uncommon property for neat bulk liquids: they self-organize in transient nanometric domains. In ILs-based electrochemical devices, this fluctuating nano-segregation acts as energy barriers to the long range diffusional processes and hence to the ionic conductivity. Here, we show how the ionic conductivity of ILs can be increased by more than one order of magnitude by exploiting one dimensional (1D) confinement effects in macroscopically oriented carbon nanotube (CNT) membranes. We identify 1D CNT membranes as promising separators for high instant power batteries.

Published
2019

42. Ionic Liquids: evidence of the viscosity scale-dependence

Author

Berrod, Quentin, Ferdeghini, Filippo, Zanotti, Jean-Marc, Judeinstein, Patrick, Lairez, Didier, Sakai, Victoria Garcia, Czakkel, Orsolya, Fouquet, Peter, Constantin, Doru, Lawrence Berkeley National Laboratory [Berkeley] (LBNL), Laboratoire Léon Brillouin (LLB - UMR 12), Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Centre National de la Recherche Scientifique (CNRS)-Université Paris-Saclay, Laboratoire des Interfaces Complexes et de l'Organisation Nanométrique (LICORNE), ECE Ecole d'Ingénieurs, Laboratoire des Solides Irradiés (LSI), Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Centre National de la Recherche Scientifique (CNRS)-École polytechnique (X), ISIS Neutron and Muon Facility, STFC Rutherford Appleton Laboratory (RAL), Science and Technology Facilities Council (STFC)-Science and Technology Facilities Council (STFC), Institut Laue-Langevin (ILL), ILL, Laboratoire de Physique des Solides (LPS), Centre National de la Recherche Scientifique (CNRS)-Université Paris-Sud - Paris 11 (UP11), Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Paris-Saclay-Centre National de la Recherche Scientifique (CNRS), Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-École polytechnique (X)-Centre National de la Recherche Scientifique (CNRS), and Université Paris-Sud - Paris 11 (UP11)-Centre National de la Recherche Scientifique (CNRS)

Subjects
Science, [PHYS.COND.CM-MS]Physics [physics]/Condensed Matter [cond-mat]/Materials Science [cond-mat.mtrl-sci], Medicine, Article
Abstract

International audience; Ionic Liquids (ILs) are a specific class of molecular electrolytes characterized by the total absence of co-solvent. Due to their remarkable chemical and electrochemical stability, they are prime candidates for the development of safe and sustainable energy storage systems. The competition between electrostatic and van der Waals interactions leads to a property original for pure liquids: they self-organize in fluctuating nanometric aggregates. So far, this transient structuration has escaped to direct clear-cut experimental assessment. Here, we focus on a imidazolium based IL and use particle-probe rheology to (i) catch this phenomenon and (ii) highlight an unexpected consequence: the self-diffusion coefficient of the cation shows a one order of magnitude difference depending whether it is inferred at the nanometric or at the microscopic scale. As this quantity partly drives the ionic conductivity, such a peculiar property represents a strong limiting factor to the performances of ILs-based batteries

Published
2017

45. Coupling NMR to SANS: Addressing at once structure and dynamics in soft matter.

Author

de Oliveira-Silva, Rodrigo, Bélime, Agathe, Le Coeur, Clémence, Chennevière, Alexis, Helary, Arnaud, Cousin, Fabrice, Judeinstein, Patrick, Sakellariou, Dimitrios, Zanotti, Jean-Marc, Lelièvre-Berna, E., and Willendrup, P.

Subjects
METHACRYLIC acid, SMALL-angle scattering, NUCLEAR magnetic resonance, POLYMER colloids, NUCLEAR spin, THERMAL neutrons, DIFFUSION coefficients
Abstract

In soft condensed matter, Small Angle Neutron Scattering (SANS) is a central tool to probe structures with characteristic sizes ranging from 1 to 100 nm. However, when used as a standalone technique, the dynamic properties of the sample are not accessible. Nuclear Magnetic Resonance (NMR) is a versatile technique which can easily probe dynamical information. Here, we report on the coupling of a low-field NMR system to a SANS instrument. We show that this original set-up makes it possible to obtain structural information and to simultaneously extract in situ on a same sample, long-range translational diffusion coefficient, T 1 and T 2 nuclear spin relaxation times. Such a feature is of major interest when a sample experiences a transient physical state or evolves rapidly. We illustrate the capabilities of alliancing these experimental methods by following the critical temperature-induced phase separation of a concentrated Poly(Methacrylic Acid) solution at its Lower Critical Solution Temperature. The characteristic size related to the domain growth of the polymer-rich phase of the gel is monitored by the evolution of the SANS spectra, while the dynamics of the sol phase (H2O and polymer) is simultaneously characterized by NMR by measuring T 1 , T 2 and the diffusion coefficient. Great care has been taken to design a cell able to optimize the thermalization of the sample and in particular its equilibration time. Details are given on the sample cell specifically designed and manufactured for these experiments. The acquisition time needed to reach good signal-to-noise ratios, for both NMR and SANS, match: it is of the order of one hour. Altogether, we show that in situ low-field NMR/SANS coupling the NMR is meaningful and is a promising experimental approach. [ABSTRACT FROM AUTHOR]

Published
2019
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47. Competing coexisting phases in 2D water

Author

Zanotti, Jean-Marc, primary, Judeinstein, Patrick, additional, Dalla-Bernardina, Simona, additional, Creff, Gaëlle, additional, Brubach, Jean-Blaise, additional, Roy, Pascale, additional, Bonetti, Marco, additional, Ollivier, Jacques, additional, Sakellariou, Dimitrios, additional, and Bellissent-Funel, Marie-Claire, additional

Published
2016
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49. Nanometric confinement of molecular fluids: from interfacial interactions to one dimensional transport properties

Author

Zanotti, Jean-Marc, Laboratoire Léon Brillouin (LLB - UMR 12), Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Centre National de la Recherche Scientifique (CNRS)-Université Paris-Saclay, Université Pierre et Marie Curie - Paris VI, and Dr. G. Gebel

Subjects
dimensionnalité, polymère, neutron, polymer, confinement, eau, water, transport, dimensionality, [PHYS.COND.CM-SCM]Physics [physics]/Condensed Matter [cond-mat]/Soft Condensed Matter [cond-mat.soft], NMR, RMN
Abstract

Nanometric confinement of molecular fluids is a classical route to stabilize meta-stable states by achieving frustrations of the bulk natural fluctuations and/or phase transitions. In the first chapter of the manuscript, we address the physics of water under confinement and in a second chapter, the specific case of a polymer melt. Confinement of molecular liquids is a route to tune very significant temperature depressions of the melting point. This property has recently been intensively used in the quest for experimental evidences of the existence of a Low Temperature Critical Point (LTCP) in bulk liquid water, at Ts ~ 228 K and Ps ~ 100 MPa. Here, we highlight the surprisingly rich low temperature (from 100 to 300 K) dynamical behavior of interfacial water. Then, we propose a percolation model to account for the dynamical/thermodynamical transitions we observe at 150, 220 and 240 K and reach a global and coherent view of this two dimensional (2D) water. Due to dominant surface interactions, we question the relevance of confined water to prove the reality of the LTCP. Nevertheless, using interfacial water, we show that a liquid-liquid transition (a condition for the existence of the LTCP) involving water is possible. Recently, a corset effect has been proposed: under confinement the reptation tube diameter of a polymer chain, would be only a few Angstroms i.e. one order of magnitude smaller than in bulk. In the second chapter, we describe an inelastic neutron scattering-based multiscale approach to polymer dynamics (bulk and confined) from the atomic scale at short time (ps), up to few tens of nanometers and long times (600 ns). Over this detailed study of the time and spatial dependence of the polymer relaxations we detect no corset effect. When using nanometric confinement to obtain pure volume effects, next to the detrimental so-called surface effects evidenced in the first chapter, the significant physical insight lost by powder average of the spectroscopic observables is another limitation. In the second chapter, we illustrate how to take advantage of a macroscopically oriented confining matrix to lift this severe drawback. The ambition of the third and last chapter is to define a physical system, where macroscopic orientation meets nanometric confinement with no surface effects, to induce strong 1D pure volume effects over macroscopic distances. We discuss how such nano-pipes could enhance macroscopic flow, offering systems of prime interest to both fundamental and applied research.; Le confinement nanométrique permet d'obtenir la frustration des fluctuations et/ou des transitions de phases spontanées qu'un fluide moléculaire présente en volume (i.e. en " bulk "). Le confinement au sein de matrices poreuses est donc une voie usuelle de stabilisation de phases métastables. Nous détaillons ici les propriétés structurales, dynamiques et thermodynamiques de deux systèmes moléculaires confinés : dans un premier chapitre, nous nous intéressons au cas de l'eau puis, dans un deuxième chapitre, nous traitons le cas spécifique d'un polymère semi-cristallin. Le confinement permet d'abaisser considérablement le point de fusion du fluide confiné. Cette propriété a été récemment mise à profit dans la cadre de nombreux travaux visant à tester l'existence d'un hypothétique point critique à basse température dans l'eau volumique à 228 K and 100 MPa. Dans cette contribution, nous mettons en évidence des propriétés dynamiques surprenantes de l'eau interfaciale à basse température (de 100 à 300 K). Nous proposons un modèle de percolation décrivant les transitions dynamiques et thermodynamiques que nous observons à 150, 220 et 240 K. Nous proposons une description cohérente de cette eau à deux dimensions et de ses propriétés. Nous invoquons le rôle dominant des interactions de surface pour remettre en cause la pertinence de l'utilisation de l'eau confinée pour prouver l'existence d'un point critique à basse température dans l'eau volumique. Cette étude met cependant en évidence l'existence d'une transition liquide-liquide (l'une des conditions pour observer un point critique) impliquant des molécules d'eau. Récemment, un " effet corset " a été proposé : le confinement induirait une réduction d'un ordre de grandeur du diamètre du tube de reptation d'un polymère (quelques nanomètres en volume contre quelques angströms sous confinement). Dans le second chapitre, nous utilisons une approche par diffusion de neutrons pour accéder à une description multi-échelles de la dynamique d'un polymère (en volume puis sous confinement) de l'échelle atomique à temps court (picosecondes) jusqu'à une dizaine de nanomètres, à temps long (600 nanosecondes). Cette étude détaillée de la dépendance spatiale de la relaxation temporelle des chaînes de polymère ne permet pas de mettre en évidence d'"effet corset ". De façon générale, lorsque l'on cherche à tirer profit du confinement nanométrique pour obtenir des "effets de volume", en plus d'"effets de surface" parasites décrits dans le premier chapitre, on est également confronté à une perte significative d'information induite par la moyenne spatiale des observables spectroscopiques. Nous décrivons dans le deuxième chapitre comment utiliser des matrices de confinement orientées macroscopiquement pour s'affranchir de ces effets indésirables et/ou limitants. Dans le troisième et dernier chapitre, nous définissons un système de confinement nanométrique qui permet d'associer i) une orientation macroscopique des pores et ii) une absence totale d'interactions de surface. Un tel système permet d'envisager des effets de volume unidimensionnels très significatifs et ayant une portée sur des distances macroscopiques. Nous discutons pourquoi de tels " tuyaux nanométriques" peuvent potentiellement intéresser à la fois la recherche fondamentale et l'industrie.

Published
2011

50. Dynamic and sub-ambient thermal transition relationships in water–sucrose solutions

Author

Champion, Dominique, Loupiac, Camille, Russo, D., Simatos, Denise, Zanotti, Jean-Marc, Eau, Molécules actives, Macromolécules, Activités (EMMA), Université de Bourgogne (UB)-AgroSup Dijon - Institut National Supérieur des Sciences Agronomiques, de l'Alimentation et de l'Environnement, Institut Laue-Langevin (ILL), 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), ILL, and Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Centre National de la Recherche Scientifique (CNRS)-Université Paris-Saclay

Subjects
Sucrose, [SDV.BBM]Life Sciences [q-bio]/Biochemistry, Molecular Biology, Neutron scattering, Glass transition, Physics::Atmospheric and Oceanic Physics, DSC
Abstract

International audience; This work was undertaken to investigate thermal and dynamic transitions observed in the temperature range close to the bulk ice melting temperature in sucrose solutions. Measurements of thermal (differential calorimetry) and dynamic (neutron scattering) properties were compared in order to give a physical interpretation of the thermal transitions observed during the thawing of amorphous sucrose solutions. In fact, the freezing of biological material leads to the distinction between different pools of water: bulk water which becomes ice after freezing, unfrozen water trapped in the glassy matrix or close to the interface of solutes can be considered, and finally freezable confined water with a lower melting point than bulk water and with properties depending on both the ice presence and the microstructure of the material. The transition temperatures such as glass transition or melting are dependent on the freezing protocol used and examples of annealing effects are presented, in order to underline the necessity of a good temperature control during freezing for the study of biological material with freezable water.

Published
2011

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