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1. Synergetic Bottom-Up Synthesis of Graphene Nanoribbons by Matrix-Assisted Direct Transfer

Author

Daniel J. Rizzo, Felix R. Fischer, Peter H. Jacobse, Ryan D. McCurdy, Rafal Zuzak, Zafer Mutlu, Gregory Veber, Ilya Piskun, Jeffrey Bokor, and Michael F. Crommie

Subjects
Chemistry, Graphene, Nanotechnology, General Chemistry, Direct transfer, 010402 general chemistry, 01 natural sciences, Biochemistry, Catalysis, 0104 chemical sciences, law.invention, Matrix (mathematics), Colloid and Surface Chemistry, Polymerization, law, Graphene nanoribbons
Abstract

The scope of graphene nanoribbon (GNR) structures accessible through bottom-up approaches is defined by the intrinsic limitations of either all-on-surface or all-solution-based synthesis. Here, we report a hybrid bottom-up synthesis of GNRs based on a Matrix-Assisted Direct (MAD) transfer technique that successfully leverages technical advantages inherent to both solution-based and on-surface synthesis while sidestepping their drawbacks. Critical structural parameters tightly controlled in solution-based polymerization reactions can seamlessly be translated into the structure of the corresponding GNRs. The transformative potential of the synergetic bottom-up approaches facilitated by the MAD transfer techniques is highlighted by the synthesis of chevron-type GNRs (cGNRs) featuring narrow length distributions and a nitrogen core-doped armchair GNR (N4-7-ANGR) that remains inaccessible using either a solution-based or an on-surface bottom-up approach alone.

Published
2021

2. Microscopic Visualization of Porous Nanographenes Synthesized through a Combination of Solution and On-Surface Chemistry

Author

Iago Pozo, Dolores Pérez, Jose M. Alonso, Rafal Zuzak, Diego Peña, Enrique Guitián, Manuel Vilas-Varela, Szymon Godlewski, and Mads Engelund

Subjects
nanographenes, Nanostructure, Vacuum, Surface Properties, General Chemical Engineering, Nanotechnology, Microscopy, Atomic Force, chemistry, Atomic units, General Biochemistry, Genetics and Molecular Biology, law.invention, Scanning probe microscopy, law, on-surface synthesis, Porosity, Quantum tunnelling, Carbon Monoxide, atomic force microscopy, General Immunology and Microbiology, Spectrum Analysis, General Neuroscience, Nanostructures, Characterization (materials science), Solutions, scanning tunneling microscopy, Graphite, Gold, Hydrogenation, Scanning tunneling microscope, Graphene nanoribbons
Abstract

On-surface synthesis has recently been regarded as a promising approach for the generation of new molecular structures. It has been particularly successful in the synthesis of graphene nanoribbons, nanographenes and intrinsically reactive and instable, yet attractive species. It is based on the combination of solution chemistry aimed at preparation of appropriate molecular precursors for further ultra-high vacuum surface assisted transformations. This approach also owes its success to an incredible development of characterization techniques, such as scanning tunneling/atomic force microscopy and related methods, which allow detailed, local characterization at atomic scale. While the surface-assisted synthesis can provide molecular nanostructures with outstanding precision, down to single atoms, it suffers from basing on metallic surfaces and often limited yield. Therefore, the extension of the approach away from metals and the struggle to increase productivity seem to be significant challenges toward wider applications. Herein, we demonstrate the on-surface synthesis approach for generation of non-planar nanographenes, which are synthesized through a combination of solution chemistry and sequential surface-assisted processes, together with the detailed characterization by scanning probe microscopy methods.

Published
2021
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3. Extended iron phthalocyanine islands self-assembled on a Ge(001):H surface

Author

Rafal Zuzak, Szymon Godlewski, and Marek Szymonski

Subjects
Materials science, Scanning tunneling spectroscopy, General Physics and Astronomy, chemistry.chemical_element, Germanium, 02 engineering and technology, 010402 general chemistry, lcsh:Chemical technology, 01 natural sciences, lcsh:Technology, Full Research Paper, law.invention, chemistry.chemical_compound, Adsorption, law, Monolayer, Nanotechnology, Molecule, General Materials Science, lcsh:TP1-1185, iron phthalocyanine (FePc), Electrical and Electronic Engineering, lcsh:Science, iron phthalocyanine (fepc), lcsh:T, self-assembly, 021001 nanoscience & nanotechnology, lcsh:QC1-999, 0104 chemical sciences, Nanoscience, Crystallography, chemistry, hydrogenated semiconductor, Phthalocyanine, scanning tunneling microscopy, lcsh:Q, Self-assembly, Scanning tunneling microscope, 0210 nano-technology, lcsh:Physics
Abstract

Self-assembly of iron(II) phthalocyanine (FePc) molecules on a Ge(001):H surface results in monolayer islands extending over hundreds of nanometers and comprising upright-oriented entities. Scanning tunneling spectroscopy reveals a transport gap of 2.70 eV in agreement with other reports regarding isolated FePc molecules. Detailed analysis of single FePc molecules trapped at surface defects indicates that the molecules stay intact upon adsorption and can be manipulated away from surface defects onto a perfectly hydrogenated surface. This allows for their isolation from the germanium surface.

Published
2021

4. Bottom-up Assembly of Nanoporous Graphene with Emergent Electronic States

Author

Steven G. Louie, Paul Butler, Michael F. Crommie, Gregory Veber, Jingwei Jiang, Daniel J. Rizzo, Ryan D. McCurdy, Rafal Zuzak, Peter H. Jacobse, and Felix R. Fischer

Subjects
Band gap, Chemistry, Nanoporous, Graphene, band structure, Nanotechnology, Semiconductor device, General Chemistry, electronic structure, 010402 general chemistry, 01 natural sciences, Biochemistry, Catalysis, Semimetal, 0104 chemical sciences, law.invention, interfaces, Nanopore, Colloid and Surface Chemistry, law, Chemical Sciences, scanning tunneling microscopy, Nanoscopic scale, two dimensional materials, Graphene nanoribbons
Abstract

The incorporation of nanoscale pores into a sheet of graphene allows it to switch from an impermeable semimetal to a semiconducting nanosieve. Nanoporous graphenes are desirable for applications ranging from high-performance semiconductor device channels to atomically thin molecular sieve membranes, and their performance is highly dependent on the periodicity and reproducibility of pores at the atomic level. Achieving precise nanopore topologies in graphene using top-down lithographic approaches has proven to be challenging due to poor structural control at the atomic level. Alternatively, atomically precise nanometer-sized pores can be fabricated via lateral fusion of bottom-up synthesized graphene nanoribbons. This technique, however, typically requires an additional high temperature cross-coupling step following the nanoribbon formation that inherently yields poor lateral conjugation, resulting in 2D materials that are weakly connected both mechanically and electronically. Here, we demonstrate a novel bottom-up approach for forming fully conjugated nanoporous graphene through a single, mild annealing step following the initial polymer formation. We find emergent interface-localized electronic states within the bulk band gap of the graphene nanoribbon that hybridize to yield a dispersive two-dimensional low-energy band of states. We show that this low-energy band can be rationalized in terms of edge states of the constituent single-strand nanoribbons. The localization of these 2D states around pores makes this material particularly attractive for applications requiring electronically sensitive molecular sieves.

Published
2020

5. On-surface synthesis of chlorinated narrow graphene nanoribbon organometallic hybrids

Author

Marek Kolmer, Rafal Zuzak, Bartosz Such, André Gourdon, Marios S. Markoulides, Marek Szymonski, Piotr Olszowski, Aran Garcia-Lekue, Daniel Sánchez-Portal, Szymon Godlewski, Pedro Brandimarte, Irena Izydorczyk, National Science Centre (Poland), European Commission, Ministerio de Economía y Competitividad (España), Agencia Estatal de Investigación (España), Ministerio de Ciencia, Innovación y Universidades (España), Universidad del País Vasco, Eusko Jaurlaritza, Groupe NanoSciences (CEMES-GNS), Centre d'élaboration de matériaux et d'études structurales (CEMES), Université Toulouse III - Paul Sabatier (UT3), Université Fédérale Toulouse Midi-Pyrénées-Université Fédérale Toulouse Midi-Pyrénées-Centre National de la Recherche Scientifique (CNRS)-Institut de Chimie de Toulouse (ICT-FR 2599), Institut National Polytechnique (Toulouse) (Toulouse INP), Université Fédérale Toulouse Midi-Pyrénées-Université Fédérale Toulouse Midi-Pyrénées-Centre National de la Recherche Scientifique (CNRS)-Institut de Recherche pour le Développement (IRD)-Université Toulouse III - Paul Sabatier (UT3), Université Fédérale Toulouse Midi-Pyrénées-Institut de Chimie du CNRS (INC)-Institut National Polytechnique (Toulouse) (Toulouse INP), Université Fédérale Toulouse Midi-Pyrénées-Centre National de la Recherche Scientifique (CNRS)-Institut de Recherche pour le Développement (IRD)-Institut de Chimie du CNRS (INC)-Institut National des Sciences Appliquées - Toulouse (INSA Toulouse), Institut National des Sciences Appliquées (INSA)-Institut National des Sciences Appliquées (INSA)-Université Toulouse III - Paul Sabatier (UT3), Institut National des Sciences Appliquées (INSA)-Institut National des Sciences Appliquées (INSA), Institut National des Sciences Appliquées - Toulouse (INSA Toulouse), Institut National des Sciences Appliquées (INSA)-Université de Toulouse (UT)-Institut National des Sciences Appliquées (INSA)-Université de Toulouse (UT)-Institut de Chimie de Toulouse (ICT), Institut de Recherche pour le Développement (IRD)-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)-Institut de Recherche pour le Développement (IRD)-Université Toulouse III - Paul Sabatier (UT3), 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)-Centre National de la Recherche Scientifique (CNRS)-Institut National des Sciences Appliquées - Toulouse (INSA Toulouse), and Université de Toulouse (UT)-Centre National de la Recherche Scientifique (CNRS)

Subjects
chemistry.chemical_classification, Chemical substance, Materials science, Letter, Graphene, Heteroatom, 02 engineering and technology, Hydrogen atom, 010402 general chemistry, 021001 nanoscience & nanotechnology, Photochemistry, 01 natural sciences, 0104 chemical sciences, law.invention, Hydrocarbon, chemistry, Polymerization, law, Molecule, General Materials Science, [CHIM.COOR]Chemical Sciences/Coordination chemistry, [PHYS.PHYS.PHYS-CHEM-PH]Physics [physics]/Physics [physics]/Chemical Physics [physics.chem-ph], Physical and Theoretical Chemistry, 0210 nano-technology, Graphene nanoribbons
Abstract

Graphene nanoribbons (GNRs) and their derivatives attract growing attention due to their excellent electronic and magnetic properties as well as the fine-tuning of such properties that can be obtained by heteroatom substitution and/or edge morphology modification. Here, we introduce graphene nanoribbon derivatives—organometallic hybrids with gold atoms incorporated between the carbon skeleton and side Cl atoms. We show that narrow chlorinated 5-AGNROHs (armchair graphene nanoribbon organometallic hybrids) can be fabricated by on-surface polymerization with omission of the cyclodehydrogenation reaction by a proper choice of tailored molecular precursors. Finally, we describe a route to exchange chlorine atoms connected through gold atoms to the carbon skeleton by hydrogen atom treatment. This is achieved directly on the surface, resulting in perfect unsubstituted hydrogen-terminated GNRs. This will be beneficial in the molecule on-surface processing when the preparation of final unsubstituted hydrocarbon structure is desired., This work was supported by the National Science Center, Poland (2019/35/B/ST5/02666), and the EU Project PAMS (610446). A.G.L., D.S.P., and P.B. acknowledge the Spanish Agencia Estatal de Investigación (Grants MAT2016-78293-C6-4-R, PID2019-107338RB-C66, and FIS2017-83780-P), Dep. Educación of the Basque Government and UPV/EHU (Grant IT-756-13), and the European Union (EU) through Horizon 2020 (FET-Open project SPRING Grant 863098) for support.

Published
2020
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6. The butterfly – a well-defined constant-current topography pattern on Si(001):H and Ge(001):H resulting from current-induced defect fluctuations

Author

Thomas Frederiksen, Szymon Godlewski, Rafal Zuzak, Mads Engelund, Bartosz Such, Marek Szymonski, Marek Kolmer, Daniel Sánchez-Portal, European Commission, Ministerio de Economía y Competitividad (España), Eusko Jaurlaritza, Universidad del País Vasco, Foundation for Polish Science, and CSIC - Unidad de Recursos de Información Científica para la Investigación (URICI)

Subjects
Current (mathematics), Materials science, Bistability, Dangling bond, General Physics and Astronomy, 02 engineering and technology, Rate equation, 021001 nanoscience & nanotechnology, 01 natural sciences, Molecular physics, Characterization (materials science), law.invention, Electronic states, Crystallography, law, 0103 physical sciences, Constant current, Physical and Theoretical Chemistry, Scanning tunneling microscope, 010306 general physics, 0210 nano-technology
Abstract

This article is licensed under a Creative Commons Attribution-NonCommercial 3.0 Unported Licence., Dangling bond (DB) arrays on Si(001):H and Ge(001):H surfaces can be patterned with atomic precision and they exhibit complex and rich physics making them interesting from both technological and fundamental perspectives. But their complex behavior often makes scanning tunneling microscopy (STM) images difficult to interpret and simulate. Recently it was shown that low-temperature imaging of unoccupied states of an unpassivated dimer on Ge(001):H results in a symmetric butterfly-like STM pattern, despite that the equilibrium dimer configuration is expected to be a bistable, buckled geometry. Here, based on a thorough characterization of the low-bias switching events, we propose a new imaging model featuring a dynamical two-state rate equation. This model allows us to reproduce the features of the observed symmetric empty-state images which strongly corroborates the idea that the patterns arise due to fast switching events and provides insight into the relation between the tunneling current and switching rates. Our new imaging model is general and can be applied to other systems that exhibit rapid fluctuations during STM experiments., The work is funded by the European Commission under the FP7 FET-ICT “Planar Atomic and Molecular Scale devices” (PAMS) project (Contract No. 610446) and National Science Centre, Poland (2014/15/D/ST3/02975). ME, TF, and DSP also acknowledge support from the Spanish Ministerio de Economía y Competitividad (MINECO) (Grant No. MAT2013-46593-C6-2-P) and the Basque Dep. de Educación and the UPV/EHU (Grant No. IT-756-13). MK acknowledges financial support received from the Foundation for Polish Science (FNP). RZ acknowledges support received from KNOW (scholarship KNOW/44/SS/RZ/2015)., We acknowledge support by the CSIC Open Access Publication Initiative through its Unit of Information Resources for Research (URICI).

Published
2016
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7. Nonacene generated by on-surface dehydrogenation

Author

Marek Szymonski, Bartosz Such, Rafal Zuzak, Mariusz Krawiec, Antonio M. Echavarren, Ruth Dorel, Szymon Godlewski, and Marek Kolmer

Subjects
Heptacene, 010405 organic chemistry, Chemistry, Scanning tunneling spectroscopy, General Engineering, General Physics and Astronomy, 010402 general chemistry, Photochemistry, 01 natural sciences, 0104 chemical sciences, law.invention, chemistry.chemical_compound, Crystallography, law, Molecule, General Materials Science, Molecular orbital, Dehydrogenation, Density functional theory, Physics::Chemical Physics, Scanning tunneling microscope, Isomerization
Abstract

The on-surface synthesis of nonacene has been accomplished by dehydrogenation of an air-stable partially saturated precursor, which could be aromatized by using a combined scanning tunnelling and atomic force microscope (STM/AFM) tip as well as by on-surface annealing. This transformation allowed the in-detail analysis of the electronic properties of nonacene molecules physisorbed on Au(111) by scanning tunnelling spectroscopy (STS) measurements, which were corroborated by density theory functional (DFT) calculations thus confirming the spatial mapping of its molecular orbitals. Furthermore, the thermally-induced dehydrogenation uncovered the isomerisation of intermediate dihydrononacene species, which allowed for their in-depth structural and electronic characterization.

Published
2017

8. Contacting a Conjugated Molecule with a Surface Dangling Bond Dimer on a Hydrogenated Ge(001) Surface Allows Imaging of the Hidden Ground Electronic State

Author

Marek Kolmer, Bartosz Such, Hiroyo Kawai, Paula de Mendoza, Rafal Zuzak, Antonio M. Echavarren, Mark Saeys, Christian Joachim, Szymon Godlewski, Marek Szymonski, Uniwersytet Jagielloński w Krakowie = Jagiellonian University (UJ), Agency for science, technology and research [Singapore] (A*STAR), Institute of Chemical Research of Catalonia (ICIQ), Groupe NanoSciences (CEMES-GNS), Centre d'élaboration de matériaux et d'études structurales (CEMES), Université Toulouse III - Paul Sabatier (UT3), Université Fédérale Toulouse Midi-Pyrénées-Université Fédérale Toulouse Midi-Pyrénées-Centre National de la Recherche Scientifique (CNRS)-Institut de Chimie de Toulouse (ICT-FR 2599), Institut National Polytechnique (Toulouse) (Toulouse INP), Université Fédérale Toulouse Midi-Pyrénées-Université Fédérale Toulouse Midi-Pyrénées-Centre National de la Recherche Scientifique (CNRS)-Institut de Recherche pour le Développement (IRD)-Université Toulouse III - Paul Sabatier (UT3), Université Fédérale Toulouse Midi-Pyrénées-Institut de Chimie du CNRS (INC)-Institut National Polytechnique (Toulouse) (Toulouse INP), Université Fédérale Toulouse Midi-Pyrénées-Centre National de la Recherche Scientifique (CNRS)-Institut de Recherche pour le Développement (IRD)-Institut de Chimie du CNRS (INC)-Institut National des Sciences Appliquées - Toulouse (INSA Toulouse), Institut National des Sciences Appliquées (INSA)-Institut National des Sciences Appliquées (INSA)-Université Toulouse III - Paul Sabatier (UT3), Institut National des Sciences Appliquées (INSA)-Institut National des Sciences Appliquées (INSA), Institut National des Sciences Appliquées - Toulouse (INSA Toulouse), Institut National des Sciences Appliquées (INSA)-Université de Toulouse (UT)-Institut National des Sciences Appliquées (INSA)-Université de Toulouse (UT)-Institut de Chimie de Toulouse (ICT), Institut de Recherche pour le Développement (IRD)-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)-Institut de Recherche pour le Développement (IRD)-Université Toulouse III - Paul Sabatier (UT3), 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)-Centre National de la Recherche Scientifique (CNRS)-Institut National des Sciences Appliquées - Toulouse (INSA Toulouse), and Université de Toulouse (UT)-Centre National de la Recherche Scientifique (CNRS)

Subjects
Surface (mathematics), Fabrication, Materials science, single-molecule devices, atomic-scale contacts, surface dangling bonds, Dimer, General Physics and Astronomy, Nanotechnology, 02 engineering and technology, Conjugated system, 01 natural sciences, law.invention, Condensed Matter::Materials Science, chemistry.chemical_compound, scanning tunneling microscope, Hardware_GENERAL, law, 0103 physical sciences, [CHIM]Chemical Sciences, General Materials Science, Physics::Chemical Physics, 010306 general physics, Coupling, molecule manipulation, organic molecule, General Engineering, Dangling bond, 021001 nanoscience & nanotechnology, chemistry, hydrogenated semiconductor, Chemical physics, Scanning tunneling microscope, 0210 nano-technology
Abstract

cited By 18; International audience; Fabrication of single-molecule logic devices requires controlled manipulation of molecular states with atomic-scale precision. Tuning molecule–substrate coupling is achieved here by the reversible attachment of a prototypical planar conjugated organic molecule to dangling bonds on the surface of a hydrogenated semiconductor. We show that the ground electronic state resonance of a Y-shaped polyaromatic molecule physisorbed on a defect-free area of a fully hydrogenated surface cannot be observed by scanning tunneling microscopy (STM) measurements because it is decoupled from the Ge bulk states by the hydrogen-passivated surface. The state can be accessed by STM only if the molecule is contacted with the substrate by a dangling bond dimer. The reversibility of the attachment processes will be advantageous in the construction of surface atomic-scale circuits composed of single-molecule devices interconnected by the surface dangling bond wires.

Published
2013
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9. Two-probe STM experiments at the atomic level

Author

Marek Szymonski, Rafal Zuzak, Marek Kolmer, Christian Joachim, Piotr Olszowski, Szymon Godlewski, Centre for Nanometer-Scale Science and Advanced Materials (NANOAM), Uniwersytet Jagielloński w Krakowie = Jagiellonian University (UJ), Groupe NanoSciences (CEMES-GNS), Centre d'élaboration de matériaux et d'études structurales (CEMES), Université Toulouse III - Paul Sabatier (UT3), Université Fédérale Toulouse Midi-Pyrénées-Université Fédérale Toulouse Midi-Pyrénées-Centre National de la Recherche Scientifique (CNRS)-Institut de Chimie de Toulouse (ICT-FR 2599), Institut National Polytechnique (Toulouse) (Toulouse INP), Université Fédérale Toulouse Midi-Pyrénées-Université Fédérale Toulouse Midi-Pyrénées-Centre National de la Recherche Scientifique (CNRS)-Institut de Recherche pour le Développement (IRD)-Université Toulouse III - Paul Sabatier (UT3), Université Fédérale Toulouse Midi-Pyrénées-Institut de Chimie du CNRS (INC)-Institut National Polytechnique (Toulouse) (Toulouse INP), Université Fédérale Toulouse Midi-Pyrénées-Centre National de la Recherche Scientifique (CNRS)-Institut de Recherche pour le Développement (IRD)-Institut de Chimie du CNRS (INC)-Institut National des Sciences Appliquées - Toulouse (INSA Toulouse), Institut National des Sciences Appliquées (INSA)-Institut National des Sciences Appliquées (INSA)-Université Toulouse III - Paul Sabatier (UT3), Institut National des Sciences Appliquées (INSA)-Institut National des Sciences Appliquées (INSA), Institut National des Sciences Appliquées - Toulouse (INSA Toulouse), Institut National des Sciences Appliquées (INSA)-Université de Toulouse (UT)-Institut National des Sciences Appliquées (INSA)-Université de Toulouse (UT)-Institut de Chimie de Toulouse (ICT), Institut de Recherche pour le Développement (IRD)-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)-Institut de Recherche pour le Développement (IRD)-Université Toulouse III - Paul Sabatier (UT3), 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)-Centre National de la Recherche Scientifique (CNRS)-Institut National des Sciences Appliquées - Toulouse (INSA Toulouse), and Université de Toulouse (UT)-Centre National de la Recherche Scientifique (CNRS)

Subjects
hydrogeneted semiconductors, multi-probe techniques, chemistry.chemical_element, Nanotechnology, Germanium, 02 engineering and technology, Scanning capacitance microscopy, 01 natural sciences, law.invention, Scanning probe microscopy, Planar, dangling-bond nanostructures, law, electronic transport, 0103 physical sciences, Atom, General Materials Science, 010306 general physics, atomic wires, [PHYS]Physics [physics], business.industry, Chemistry, Dangling bond, 021001 nanoscience & nanotechnology, Condensed Matter Physics, Characterization (materials science), Optoelectronics, scanning tunneling microscopy, Scanning tunneling microscope, 0210 nano-technology, business
Abstract

cited By 0; International audience; Direct characterization of planar atomic or molecular scale devices and circuits on a supporting surface by multi-probe measurements requires unprecedented stability of single atom contacts and manipulation of scanning probes over large, nanometer scale area with atomic precision. In this work, we describe the full methodology behind atomically defined two-probe scanning tunneling microscopy (STM) experiments performed on a model system: dangling bond dimer wire supported on a hydrogenated germanium (0 0 1) surface. We show that 70 nm long atomic wire can be simultaneously approached by two independent STM scanners with exact probe to probe distance reaching down to 30 nm. This allows direct wire characterization by two-probe I–V characteristics at distances below 50 nm. Our technical results presented in this work open a new area for multi-probe research, which can be now performed with precision so far accessible only by single-probe scanning probe microscopy (SPM) experiments.

Published
2017
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10. Interaction of a conjugated polyaromatic molecule with a single dangling bond quantum dot on a hydrogenated semiconductor

Author

Rafal Zuzak, Hiroyo Kawai, Antonio M. Echavarren, Mark Saeys, Marek Kolmer, Mads Engelund, Daniel Sánchez-Portal, Szymon Godlewski, Aran Garcia-Lekue, Marek Szymonski, Christian Joachim, Centre for Nanometer-Scale Science and Advanced Materials (NANOAM), Uniwersytet Jagielloński w Krakowie = Jagiellonian University (UJ), Departamento de Fisica de Materieles and Centro Mixto CSIC-UPV/EHU, Facultad de Ciencias Quimicas, Institute of Materials Research and Engineering, A*STAR (Agency for Science, Technology and Research), 3 Research Link, Singapore 117602, Singapore., Donostia International Physics Center - DIPC (SPAIN), Donostia International Physics Center (DIPC), University of the Basque Country/Euskal Herriko Unibertsitatea (UPV/EHU)-University of the Basque Country/Euskal Herriko Unibertsitatea (UPV/EHU), Universiteit Gent = Ghent University [Belgium] (UGENT), Institute of Chemical Research of Catalonia (ICIQ), Groupe NanoSciences (CEMES-GNS), Centre d'élaboration de matériaux et d'études structurales (CEMES), Université Toulouse III - Paul Sabatier (UT3), Université Fédérale Toulouse Midi-Pyrénées-Université Fédérale Toulouse Midi-Pyrénées-Centre National de la Recherche Scientifique (CNRS)-Institut de Chimie de Toulouse (ICT-FR 2599), Institut National Polytechnique (Toulouse) (Toulouse INP), Université Fédérale Toulouse Midi-Pyrénées-Université Fédérale Toulouse Midi-Pyrénées-Centre National de la Recherche Scientifique (CNRS)-Institut de Recherche pour le Développement (IRD)-Université Toulouse III - Paul Sabatier (UT3), Université Fédérale Toulouse Midi-Pyrénées-Institut de Chimie du CNRS (INC)-Institut National Polytechnique (Toulouse) (Toulouse INP), Université Fédérale Toulouse Midi-Pyrénées-Centre National de la Recherche Scientifique (CNRS)-Institut de Recherche pour le Développement (IRD)-Institut de Chimie du CNRS (INC)-Institut National des Sciences Appliquées - Toulouse (INSA Toulouse), Institut National des Sciences Appliquées (INSA)-Institut National des Sciences Appliquées (INSA)-Université Toulouse III - Paul Sabatier (UT3), Institut National des Sciences Appliquées (INSA)-Institut National des Sciences Appliquées (INSA), Ministry of Science and Higher Education (Poland), European Commission, Ministerio de Economía y Competitividad (España), Eusko Jaurlaritza, Universidad del País Vasco, Foundation for Polish Science, Agency for Science, Technology and Research A*STAR (Singapore), National Science Centre (Poland), Universiteit Gent = Ghent University (UGENT), Institut National des Sciences Appliquées - Toulouse (INSA Toulouse), Institut National des Sciences Appliquées (INSA)-Université de Toulouse (UT)-Institut National des Sciences Appliquées (INSA)-Université de Toulouse (UT)-Institut de Chimie de Toulouse (ICT), Institut de Recherche pour le Développement (IRD)-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)-Institut de Recherche pour le Développement (IRD)-Université Toulouse III - Paul Sabatier (UT3), 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)-Centre National de la Recherche Scientifique (CNRS)-Institut National des Sciences Appliquées - Toulouse (INSA Toulouse), and Université de Toulouse (UT)-Centre National de la Recherche Scientifique (CNRS)

Subjects
General Physics and Astronomy, 02 engineering and technology, Substrate (electronics), Electronic structure, 01 natural sciences, law.invention, Condensed Matter::Materials Science, law, Computational chemistry, 0103 physical sciences, Molecule, Physical and Theoretical Chemistry, Physics::Chemical Physics, 010306 general physics, HOMO/LUMO, [PHYS]Physics [physics], Quantitative Biology::Biomolecules, business.industry, Chemistry, Dangling bond, 021001 nanoscience & nanotechnology, Semiconductor, Chemical physics, Quantum dot, Scanning tunneling microscope, 0210 nano-technology, business
Abstract

Controlling the strength of the coupling between organic molecules and single atoms provides a powerful tool for tuning electronic properties of single-molecule devices. Here, using scanning tunneling microscopy and spectroscopy (STM/STS) supported by theoretical modeling, we study the interaction of a planar organic molecule (trinaphthylene) with a hydrogen-passivated Ge(001):H substrate and a single dangling bond quantum dot on that surface. The electronic structure of the molecule adsorbed on the hydrogen-passivated surface is similar to the gas phase structure and the measurements show that HOMO and LUMO states contribute to the STM filled and empty state images, respectively. Furthermore, we show that the electronic properties are not significantly affected when the molecule is attached to the single dangling bond, which is in contrast with the strong interaction of the molecule with a dangling bond dimer. Our results show that the dangling bond quantum dots could stabilize organic molecules on a hydrogenated semiconductor without affecting their originally designed gas phase electronic properties. Together with the ability to laterally manipulate the molecules on the surface, this will be advantageous in the construction of single-molecule devices, where the coupling and positioning of the molecules on the substrate could be tuned by a proper design of the surface quantum dot arrays, comprising both single and dimerized dangling bonds., This work was supported by the Polish Ministry for Science and Higher Education, contract no. 0322/IP3/2013/72. The experiment was carried out using equipment purchased with financial support from the European Regional Development Fund within the framework of the Polish Innovation Economy Operational Program (contract no. POIG.02.01.00-12-023/08). ME, AGL and DSP acknowledge funding by the FP7 FET-ICT “Planar Atomic and Molecular Scale devices” (PAMS) project (funded by the European Commission under contract No. 610446), the Spanish Ministerio de Economia y Competitividad (MINECO) (Grant No. MAT2013-46593-C6-2-P) and the Basque Department of Education and the UPV/EHU (Grant No. IT-756-13). MK acknowledges financial support received from the Foundation for Polish Science (FNP). SG acknowledges the support from the National Science Centre, Poland (2014/15/D/ST3/02975). AME acknowledges the MINECO (Grant No. CTQ2013-42106-P). HK acknowledges the A*STAR Computational Resource Centre (A*CRC) for the computational resources and support. RZ acknowledges support received from KNOW (scholarship KNOW/44/SS/RZ/2015).

Published
2016
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11. Single-molecule rotational switch on a dangling bond dimer bearing

Author

Rafal Zuzak, Antonio M. Echavarren, Marek Szymonski, Szymon Godlewski, Mark Saeys, Hiroyo Kawai, Christian Joachim, Marek Kolmer, Centre for Nanometer-Scale Science and Advanced Materials (NANOAM), Uniwersytet Jagielloński w Krakowie = Jagiellonian University (UJ), Institute of Materials Research and Engineering, Singapore, Institute of Materials Research and Engineering, Institute of Chemical Research of Catalonia (ICIQ), Groupe NanoSciences (CEMES-GNS), Centre d'élaboration de matériaux et d'études structurales (CEMES), Université Toulouse III - Paul Sabatier (UT3), Université Fédérale Toulouse Midi-Pyrénées-Université Fédérale Toulouse Midi-Pyrénées-Centre National de la Recherche Scientifique (CNRS)-Institut de Chimie de Toulouse (ICT-FR 2599), Institut National Polytechnique (Toulouse) (Toulouse INP), Université Fédérale Toulouse Midi-Pyrénées-Université Fédérale Toulouse Midi-Pyrénées-Centre National de la Recherche Scientifique (CNRS)-Institut de Recherche pour le Développement (IRD)-Université Toulouse III - Paul Sabatier (UT3), Université Fédérale Toulouse Midi-Pyrénées-Institut de Chimie du CNRS (INC)-Institut National Polytechnique (Toulouse) (Toulouse INP), Université Fédérale Toulouse Midi-Pyrénées-Centre National de la Recherche Scientifique (CNRS)-Institut de Recherche pour le Développement (IRD)-Institut de Chimie du CNRS (INC)-Institut National des Sciences Appliquées - Toulouse (INSA Toulouse), Institut National des Sciences Appliquées (INSA)-Institut National des Sciences Appliquées (INSA)-Université Toulouse III - Paul Sabatier (UT3), Institut National des Sciences Appliquées (INSA)-Institut National des Sciences Appliquées (INSA), Laboratory for Chemical Technology, Universiteit Gent = Ghent University [Belgium] (UGENT), Institut National des Sciences Appliquées - Toulouse (INSA Toulouse), Institut National des Sciences Appliquées (INSA)-Université de Toulouse (UT)-Institut National des Sciences Appliquées (INSA)-Université de Toulouse (UT)-Institut de Chimie de Toulouse (ICT), Institut de Recherche pour le Développement (IRD)-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)-Institut de Recherche pour le Développement (IRD)-Université Toulouse III - Paul Sabatier (UT3), 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)-Centre National de la Recherche Scientifique (CNRS)-Institut National des Sciences Appliquées - Toulouse (INSA Toulouse), Université de Toulouse (UT)-Centre National de la Recherche Scientifique (CNRS), and Universiteit Gent = Ghent University (UGENT)

Subjects
single-molecule devices, surface dangling bonds, Dimer, General Physics and Astronomy, 02 engineering and technology, 010402 general chemistry, 01 natural sciences, Molecular physics, law.invention, symbols.namesake, chemistry.chemical_compound, Condensed Matter::Materials Science, single-molecule manipulation, molecular rotor, law, scanning tunneling microscope, Molecule, hydrogenated semiconductor surface, General Materials Science, Molecular switch, [PHYS]Physics [physics], Chemistry, organic molecule, General Engineering, Dangling bond, 021001 nanoscience & nanotechnology, 0104 chemical sciences, molecular switch, Bond length, Covalent bond, symbols, Scanning tunneling microscope, van der Waals force, Atomic physics, 0210 nano-technology
Abstract

cited By 6; International audience; One of the key challenges in the construction of atomic-scale circuits and molecular machines is to design molecular rotors and switches by controlling the linear or rotational movement of a molecule while preserving its intrinsic electronic properties. Here, we demonstrate both the continuous rotational switching and the controlled step-by-step single switching of a trinaphthylene molecule adsorbed on a dangling bond dimer created on a hydrogen-passivated Ge(001):H surface. The molecular switch is on-surface assembled when the covalent bonds between the molecule and the dangling bond dimer are controllably broken, and the molecule is attached to the dimer by long-range van der Waals interactions. In this configuration, the molecule retains its intrinsic electronic properties, as confirmed by combined scanning tunneling microscopy/spectroscopy (STM/STS) measurements, density functional theory calculations, and advanced STM image calculations. Continuous switching of the molecule is initiated by vibronic excitations when the electrons are tunneling through the lowest unoccupied molecular orbital state of the molecule. The switching path is a combination of a sliding and rotation motion over the dangling bond dimer pivot. By carefully selecting the STM conditions, control over discrete single switching events is also achieved. Combined with the ability to create dangling bond dimers with atomic precision, the controlled rotational molecular switch is expected to be a crucial building block for more complex surface atomic-scale devices.

Published
2016
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12. Diels–Alder attachment of a planar organic molecule to a dangling bond dimer on a hydrogenated semiconductor surface

Author

Mark Saeys, Christian Joachim, Daniel Sánchez-Portal, Mads Engelund, Szymon Godlewski, Hiroyo Kawai, Rafal Zuzak, Antonio M. Echavarren, Marek Kolmer, Gerard Novell-Leruth, Aran Garcia-Lekue, National Science Centre (Poland), European Commission, Ministerio de Economía y Competitividad (España), Eusko Jaurlaritza, Universidad del País Vasco, Foundation for Polish Science, Ministry of Science and Higher Education (Poland), Centre for Nanometer-Scale Science and Advanced Materials (NANOAM), Uniwersytet Jagielloński w Krakowie = Jagiellonian University (UJ), Institute of Materials Research and Engineering, Singapore, Institute of Materials Research and Engineering, CSIC-UPV/EHU, Donostia International Physics Center - DIPC (SPAIN), Donostia International Physics Center (DIPC), University of the Basque Country/Euskal Herriko Unibertsitatea (UPV/EHU)-University of the Basque Country/Euskal Herriko Unibertsitatea (UPV/EHU), Universiteit Gent = Ghent University [Belgium] (UGENT), Institute of Chemical Research of Catalonia (ICIQ), Groupe NanoSciences (CEMES-GNS), Centre d'élaboration de matériaux et d'études structurales (CEMES), Université Toulouse III - Paul Sabatier (UT3), Université Fédérale Toulouse Midi-Pyrénées-Université Fédérale Toulouse Midi-Pyrénées-Centre National de la Recherche Scientifique (CNRS)-Institut de Chimie de Toulouse (ICT-FR 2599), Institut National Polytechnique (Toulouse) (Toulouse INP), Université Fédérale Toulouse Midi-Pyrénées-Université Fédérale Toulouse Midi-Pyrénées-Centre National de la Recherche Scientifique (CNRS)-Institut de Recherche pour le Développement (IRD)-Université Toulouse III - Paul Sabatier (UT3), Université Fédérale Toulouse Midi-Pyrénées-Institut de Chimie du CNRS (INC)-Institut National Polytechnique (Toulouse) (Toulouse INP), Université Fédérale Toulouse Midi-Pyrénées-Centre National de la Recherche Scientifique (CNRS)-Institut de Recherche pour le Développement (IRD)-Institut de Chimie du CNRS (INC)-Institut National des Sciences Appliquées - Toulouse (INSA Toulouse), Institut National des Sciences Appliquées (INSA)-Institut National des Sciences Appliquées (INSA)-Université Toulouse III - Paul Sabatier (UT3), Institut National des Sciences Appliquées (INSA)-Institut National des Sciences Appliquées (INSA), University of the Basque Country/Euskal Herriko Unibertsitatea (UPV/EHU), Universiteit Gent = Ghent University (UGENT), Institut National des Sciences Appliquées - Toulouse (INSA Toulouse), Institut National des Sciences Appliquées (INSA)-Université de Toulouse (UT)-Institut National des Sciences Appliquées (INSA)-Université de Toulouse (UT)-Institut de Chimie de Toulouse (ICT), Institut de Recherche pour le Développement (IRD)-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)-Institut de Recherche pour le Développement (IRD)-Université Toulouse III - Paul Sabatier (UT3), 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)-Centre National de la Recherche Scientifique (CNRS)-Institut National des Sciences Appliquées - Toulouse (INSA Toulouse), and Université de Toulouse (UT)-Centre National de la Recherche Scientifique (CNRS)

Subjects
[PHYS]Physics [physics], Dimer, Dangling bond, General Physics and Astronomy, 02 engineering and technology, Conjugated system, 010402 general chemistry, 021001 nanoscience & nanotechnology, 01 natural sciences, 0104 chemical sciences, law.invention, Crystallography, chemistry.chemical_compound, chemistry, Chemical bond, Computational chemistry, law, Covalent bond, Molecule, Reactivity (chemistry), Physical and Theoretical Chemistry, Scanning tunneling microscope, 0210 nano-technology
Abstract

Construction of single-molecule electronic devices requires the controlled manipulation of organic molecules and their properties. This could be achieved by tuning the interaction between the molecule and individual atoms by local “on-surface” chemistry, i.e., the controlled formation of chemical bonds between the species. We demonstrate here the reversible attachment of a planar conjugated polyaromatic molecule to a pair of unpassivated dangling bonds on a hydrogenated Ge(001):H surface via a Diels–Alder [4+2] addition using the tip of a scanning tunneling microscope (STM). Due to the small stability difference between the covalently bonded and a nearly undistorted structure attached to the dangling bond dimer by long-range dispersive forces, we show that at cryogenic temperatures the molecule can be switched between both configurations. The reversibility of this covalent bond forming reaction may be applied in the construction of complex circuits containing organic molecules with tunable properties., This work was supported by the National Science Centre, Poland (2014/15/D/ST3/02975). The experiment was carried out using equipment purchased with financial support from the European Regional Development Fund within the framework of the Polish Innovation Economy Operational Program (contract no. POIG.02.01.00-12-023/08). ME, AGL and DSP acknowledge funding by the FP7 FET-ICT “Planar Atomic and Molecular Scale devices” (PAMS) project (funded by the European Commission under contract no. 610446), the Spanish Ministerio de Economia y Competitividad (MINECO) (Grant No. MAT2013-46593-C6-2-P) and the Basque Department of Education and the UPV/EHU (Grant No. IT-756-13). MK acknowledges financial support received from the Foundation for Polish Science (FNP). SG acknowledges the support from the Polish Ministry for Science and Higher Education, contract no. 0322/IP3/2013/72. AME acknowledges the MINECO (Grant No. CTQ2013-42106-P). HK acknowledges the A*STAR Computational Resource Centre (A*CRC) for the computational resources and support. CJ acknowledges the MANA NEXT financial support during this work. RZ acknowledges support received from KNOW (scholarship KNOW/44/SS/RZ/2015).

Published
2016
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13. Fermi level pinning at the Ge(001) surface - A case for non-standard explanation

Author

Marek Szymonski, Mateusz Wojtaszek, Jakub Lis, Rafal Zuzak, Bartosz Such, Szymon Godlewski, and Marek Kolmer

Subjects
Materials science, Band gap, General Physics and Astronomy, chemistry.chemical_element, FOS: Physical sciences, Germanium, doping, surface structure, law.invention, symbols.namesake, law, Mesoscale and Nanoscale Physics (cond-mat.mes-hall), surface states, Surface states, Condensed Matter - Materials Science, Valence (chemistry), Condensed matter physics, Dopant, Condensed Matter - Mesoscale and Nanoscale Physics, valence bands, Fermi level, fermi levels, Materials Science (cond-mat.mtrl-sci), Band bending, chemistry, symbols, Scanning tunneling microscope
Abstract

To explore the origin of the Fermi level pinning in germanium we investigate the Ge(001) and Ge(001):H surfaces. The absence of relevant surface states in the case of Ge(001):H should unpin the surface Fermi level. This is not observed. For samples with donors as majority dopants the surface Fermi level appears close to the top of the valence band regardless of the surface structure. Surprisingly, for the passivated surface it is located below the top of the valence band allowing scanning tunneling microscopy imaging within the band gap. We argue that the well known electronic mechanism behind band bending does not apply and a more complicated scenario involving ionic degrees of freedom is therefore necessary. Experimental techniques involve four point probe electric current measurements, scanning tunneling microscopy and spectroscopy., Comment: 5 pages, 4 figures

Published
2015
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14. Tunneling spectroscopy of close-spaced dangling-bond pairs in Si(001):H

Author

Thomas Frederiksen, Aran Garcia-Lekue, Daniel Sánchez-Portal, Rafal Zuzak, Szymon Godlewski, Mads Engelund, Marek Szymonski, Marek Kolmer, Polish Academy of Sciences, Foundation for Polish Science, Universidad del País Vasco, European Commission, Ministerio de Economía y Competitividad (España), and Eusko Jaurlaritza

Subjects
Materials science, health care facilities, manpower, and services, media_common.quotation_subject, education, Scanning tunneling spectroscopy, surface patterning, quantum dots, 02 engineering and technology, computer.software_genre, 01 natural sciences, Molecular physics, Asymmetry, Spectral line, Article, law.invention, law, Condensed Matter::Superconductivity, 0103 physical sciences, 010306 general physics, Spectroscopy, health care economics and organizations, Quantum tunnelling, media_common, Multidisciplinary, Dangling bond, 021001 nanoscience & nanotechnology, electronic devices, Density functional theory, Data mining, Scanning tunneling microscope, 0210 nano-technology, computer
Abstract

This work is licensed under a Creative Commons Attribution 4.0 International License., We present a combined experimental and theoretical study of the electronic properties of close-spaced dangling-bond (DB) pairs in a hydrogen-passivated Si(001):H p-doped surface. Two types of DB pairs are considered, called >cross> and >line> structures. Our scanning tunneling spectroscopy (STS) data show that, although the spectra taken over different DBs in each pair exhibit a remarkable resemblance, they appear shifted by a constant energy that depends on the DB-pair type. This spontaneous asymmetry persists after repeated STS measurements. By comparison with density functional theory (DFT) calculations, we demonstrate that the magnitude of this shift and the relative position of the STS peaks can be explained by distinct charge states for each DB in the pair. We also explain how the charge state is modified by the presence of the scanning tunneling microscopy (STM) tip and the applied bias. Our results indicate that, using the STM tip, it is possible to control the charge state of individual DBs in complex structures, even if they are in close proximity. This observation might have important consequences for the design of electronic circuits and logic gates based on DBs in passivated silicon surfaces., This work is funded by the FP7 FET-ICT “Planar Atomic and Molecular Scale devices” (PAMS) project (funded by the European Commission under contract No. 610446). ME, TF, AGL and DSP also acknowledge support from the Spanish Ministerio de Economía y Competitividad (MINECO) (Grant No. MAT2013-46593-C6-2-P) and the Basque Dep. de Educación and the UPV/EHU (Grant No. IT-756-13). MK acknowledges financial support received from the Polish National Science Centre for preparation of his PhD dissertation (decision number: DEC-2013/08/T/ST3/00047) and from the Foundation for Polish Science (FNP).

Published
2015

15. Dynamical behavior of a dangling bond dimer on a hydrogenated semiconductor : Ge(001):H

Author

Marek Szymonski, Szymon Godlewski, Wojciech Gren, Rafal Zuzak, Marek Kolmer, Lev Kantorovich, Jakub Lis, and Bartosz Such

Subjects
Condensed Matter::Quantum Gases, Materials science, business.industry, Liquid helium, Dimer, Dangling bond, Condensed Matter Physics, Molecular physics, Electronic, Optical and Magnetic Materials, law.invention, chemistry.chemical_compound, Semiconductor, Amplitude, chemistry, law, Atom, Physics::Atomic and Molecular Clusters, Density functional theory, Scanning tunneling microscope, business
Abstract

We show that a dangling bond (DB) dimer on Ge(001):H exhibits a dynamical behavior when the empty states are imaged with scanning tunneling microscopy (STM) at liquid helium temperature. Large amplitude Ge atom vibrations are decisive in facilitating a specific appearance of the structure in the STM images. The underlying mechanism is unraveled using a theoretical model and calculations within the density functional theory framework. Furthermore, we demonstrate the ability to induce controlled switching of the DB dimer with noncontact atomic force microscope and the stabilizing role of the dimer-dimer interaction.

Published
2015

16. On-surface polymerization on a semiconducting oxide : aryl halide coupling controlled by surface hydroxyl groups on rutile $TiO_{2}(011)$

Author

Zbigniew Sojka, Witold Piskorz, Rafal Zuzak, David Bléger, Marek Kolmer, Amir A. Ahmad Zebari, Stefan Hecht, Marek Szymonski, Szymon Godlewski, Jakub S. Prauzner-Bechcicki, and Filip Zasada

Subjects
chemistry.chemical_classification, Aryl halide, Metals and Alloys, Oxide, General Chemistry, Photochemistry, Catalysis, Surfaces, Coatings and Films, Electronic, Optical and Magnetic Materials, law.invention, Hydroxylation, chemistry.chemical_compound, Monomer, chemistry, Polymerization, Rutile, Covalent bond, law, Materials Chemistry, Ceramics and Composites, Scanning tunneling microscope
Abstract

Based on scanning tunneling microscopy experiments, we show that the covalent coupling of aryl halide monomers on the rutile TiO2(011)-(2 \times 1) surface is controlled by the density of surface hydroxyl groups. The efficiency of the polymerization reaction depends on the level of surface hydroxylation, but the presence of hydroxyl groups is also essential for the reaction to occur.

Published
2015

17. Atomic scale fabrication of dangling bond structures on hydrogen passivated Si(0 0 1) wafers processed and nanopackaged in a clean room environment

Author

Rafal Zuzak, Aurélie Thuaire, Mateusz Wojtaszek, Hubert Moriceau, Marek Kolmer, Christian Joachim, Marek Szymonski, Caroline Rauer, Szymon Godlewski, Jean-Michel Hartmann, Centre for Nanometer-Scale Science and Advanced Materials (NANOAM), Uniwersytet Jagielloński w Krakowie = Jagiellonian University (UJ), Commissariat à l'énergie atomique et aux énergies alternatives - Laboratoire d'Electronique et de Technologie de l'Information (CEA-LETI), Direction de Recherche Technologique (CEA) (DRT (CEA)), Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Commissariat à l'énergie atomique et aux énergies alternatives (CEA), Laboratoire Interuniversitaire des Systèmes Atmosphériques (LISA (UMR_7583)), Institut national des sciences de l'Univers (INSU - CNRS)-Université Paris Diderot - Paris 7 (UPD7)-Université Paris-Est Créteil Val-de-Marne - Paris 12 (UPEC UP12)-Centre National de la Recherche Scientifique (CNRS), Groupe NanoSciences (CEMES-GNS), Centre d'élaboration de matériaux et d'études structurales (CEMES), Institut National des Sciences Appliquées - Toulouse (INSA Toulouse), Institut National des Sciences Appliquées (INSA)-Université de Toulouse (UT)-Institut National des Sciences Appliquées (INSA)-Université de Toulouse (UT)-Institut de Chimie de Toulouse (ICT), Institut de Recherche pour le Développement (IRD)-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)-Institut de Recherche pour le Développement (IRD)-Université Toulouse III - Paul Sabatier (UT3), 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)-Centre National de la Recherche Scientifique (CNRS)-Institut National des Sciences Appliquées - Toulouse (INSA Toulouse), Université de Toulouse (UT)-Centre National de la Recherche Scientifique (CNRS), European Project: 270028,EC:FP7:ICT,FP7-ICT-2009-6,ATMOL(2011), Jagiellonian University [Krakow] (UJ), Laboratoire d'Electronique et des Technologies de l'Information (CEA-LETI), Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Grenoble Alpes (UGA), Université Paris-Est Créteil Val-de-Marne - Paris 12 (UPEC UP12)-Institut national des sciences de l'Univers (INSU - CNRS)-Université Paris Diderot - Paris 7 (UPD7)-Centre National de la Recherche Scientifique (CNRS), Institut National des Sciences Appliquées (INSA)-Institut National des Sciences Appliquées (INSA)-Institut de Chimie de Toulouse (ICT-FR 2599), Institut National Polytechnique (Toulouse) (Toulouse INP), Université Fédérale Toulouse Midi-Pyrénées-Université Fédérale Toulouse Midi-Pyrénées-Institut de Recherche pour le Développement (IRD)-Université Toulouse III - Paul Sabatier (UT3), Université Fédérale Toulouse Midi-Pyrénées-Centre National de la Recherche Scientifique (CNRS)-Institut National Polytechnique (Toulouse) (Toulouse INP), Université Fédérale Toulouse Midi-Pyrénées-Centre National de la Recherche Scientifique (CNRS)-Centre National de la Recherche Scientifique (CNRS)-Institut National des Sciences Appliquées - Toulouse (INSA Toulouse), Université Fédérale Toulouse Midi-Pyrénées-Centre National de la Recherche Scientifique (CNRS)-Centre National de la Recherche Scientifique (CNRS), Institut National des Sciences Appliquées (INSA)-Université Fédérale Toulouse Midi-Pyrénées-Institut National des Sciences Appliquées (INSA)-Université Fédérale Toulouse Midi-Pyrénées-Institut de Chimie de Toulouse (ICT-FR 2599), Université Fédérale Toulouse Midi-Pyrénées-Université Fédérale Toulouse Midi-Pyrénées-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS)-Institut National Polytechnique (Toulouse) (Toulouse INP), Université Fédérale Toulouse Midi-Pyrénées-Institut de Recherche pour le Développement (IRD)-Université Toulouse III - Paul Sabatier (UT3), Université Fédérale Toulouse Midi-Pyrénées-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS)-Institut National Polytechnique (Toulouse) (Toulouse INP), Université Fédérale Toulouse Midi-Pyrénées-Centre National de la Recherche Scientifique (CNRS)-Institut National des Sciences Appliquées - Toulouse (INSA Toulouse), Université Fédérale Toulouse Midi-Pyrénées-Centre National de la Recherche Scientifique (CNRS), Université Toulouse III - Paul Sabatier (UT3), Université Fédérale Toulouse Midi-Pyrénées-Université Fédérale Toulouse Midi-Pyrénées-Centre National de la Recherche Scientifique (CNRS)-Institut de Chimie de Toulouse (ICT-FR 2599), Université Fédérale Toulouse Midi-Pyrénées-Université Fédérale Toulouse Midi-Pyrénées-Centre National de la Recherche Scientifique (CNRS)-Institut de Recherche pour le Développement (IRD)-Université Toulouse III - Paul Sabatier (UT3), Université Fédérale Toulouse Midi-Pyrénées-Institut de Chimie du CNRS (INC)-Institut National Polytechnique (Toulouse) (Toulouse INP), Université Fédérale Toulouse Midi-Pyrénées-Centre National de la Recherche Scientifique (CNRS)-Institut de Recherche pour le Développement (IRD)-Institut de Chimie du CNRS (INC)-Institut National des Sciences Appliquées - Toulouse (INSA Toulouse), Institut National des Sciences Appliquées (INSA)-Institut National des Sciences Appliquées (INSA)-Université Toulouse III - Paul Sabatier (UT3), and Institut National des Sciences Appliquées (INSA)-Institut National des Sciences Appliquées (INSA)

Subjects
Fabrication, Materials science, Nanostructure, Hydrogen, nanopackaging, General Physics and Astronomy, chemistry.chemical_element, Nanotechnology, 02 engineering and technology, hydrogen passivated Si (0 0 1) surface, 01 natural sciences, Atomic units, law.invention, law, dangling bond nanostructures, 0103 physical sciences, Wafer, 010306 general physics, [PHYS]Physics [physics], Doping, Dangling bond, low-temperature scanning tunneling microscopy and spectroscopy (LT STM/STS), Surfaces and Interfaces, General Chemistry, 021001 nanoscience & nanotechnology, Condensed Matter Physics, STM-tip-induced desorption, Surfaces, Coatings and Films, chemistry, Scanning tunneling microscope, 0210 nano-technology
Abstract

cited By 21; International audience; Specific surfaces allowing the ultra-high vacuum (UHV) creation of electronic interconnects and atomic nanostructures are required for the successful development of novel nanoscale electronic devices. Atomically flat and reconstructed Si(0 0 1):H surfaces are serious candidates for that role. In this work such Si:H surfaces were prepared in a cleanroom environment on 200 mm silicon wafers with a hydrogen bake and were subsequently bonded together to ensure the surface protection, and allow their transportation and storage for several months in air. Given the nature of the bonding, which was hydrophobic with weak van der Waals forces, we were then able to de-bond them in UHV. We show that the quality of the de-bonded Si:H surface enables the “at will” construction of sophisticated and complex dangling bond (DB) nanostructures by atomically precise scanning tunneling microscope (STM) tip induced desorption of hydrogen atoms. The DB structures created on slightly doped Si:H samples were characterized by scanning tunneling microscopy and spectroscopy (STM/STS) performed at 4 K. Our results demonstrate that DB nanostructures fabricated on UHV de-bonded Si(0 0 1):H wafers could be directly incorporated in future electronics as interconnects and parts of nanoscale logic circuits.

Published
2014
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