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Electron Transport at the Nanoscale - An Electrochemical Approach II

English title Electron Transport at the Nanoscale - An Electrochemical Approach II
Applicant Broekmann Peter
Number 144471
Funding scheme Project funding (Div. I-III)
Research institution Departement für Chemie und Biochemie Universität Bern
Institution of higher education University of Berne - BE
Main discipline Physical Chemistry
Start/End 01.09.2013 - 31.08.2016
Approved amount 520'000.00
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Keywords (6)

Interfacial Electrochemistry; Nanochemistry; Charge Transport; Electrochemical Scanning Tunneling Microscopy; Molecular Electronics; SHINERS

Lay Summary (German)

Lead
Untersuchungen zum Ladungstransport in nanoskaligen Brücken repräsentieren einen wichtigen Schritt zur Entwicklung einer Molekül-basierten Elektronik. Neben molekularen Drähten stehen funktionale molekulare Bausteine, wie Schalter und Speicher, im Fokus. Im Rahmen des Projektes werden experimentelle Methoden entwickelt und molekulare Systeme studiert, welche grundlegende Korrelationen zwischen molekularer Struktur und Ladungstransport ermöglichen. Dazu werden elektrochemische Ansätze gewählt.
Lay summary

Inhalt und Ziel des Forschungsprojektes

Ziel des Forschungsvorhabens sind Studien zum Ladungstransport in Metall (Kohlenstoff)/Molekül/Metall (Kohlenstoff) Konfigurationen. Unter Verwendung des Konzeptes „Electrolyte Gating“ und anderer Stimuli (Photonen, chemisch) werden Transportexperimente mit Einzelmolekülen und molekularen Ensembles durchgeführt und mit struktursensitiven in-situ Experimenten kombiniert. Von besonderer Bedeutung sind dabei die Rastersondenmikroskopie (STM/STS und AFM) und gap-mode Raman-Spektroskopie. Spezifische Arbeitspackete beinhalten (i) die Suche nach alternative Kontaktkonzepten, (ii) Elektronentransportexperimente mit funktionellen molekularer Drähten und Nanoobjekten sowie (iii) spektroskopische und elektromechanische Studien zur molekularen Stimulation und Erkennung. Das Projekt wird neue Ansätze und Erkenntnisse zu fundamentalen Korrelationen zwischen Struktur und Funktionalität/Relativität elektrochemischer Nanoarchitekturen ermöglichen.

Wissenschaftlicher und Gesellschaftlicher Kontext des Forschungsprojektes
Unsere Arbeiten werden neue und wichtige Informationen generieren, die zur Evaluation molekularer Bausteine als Komponenten in einer Molekular-basierten Elektronik dienen. Das interdisziplinäre Vorhaben wird methodische und konzeptionelle Beiträge zur Entwicklung einer elektrochemischen Nanotechnologie ermöglichen, die im Bereich der Sensorik und für das Monitoring von nanoskaligen Prozessen in Elektrolyten von großer Bedeutung sein werden.

Direct link to Lay Summary Last update: 04.10.2013

Responsible applicant and co-applicants

Employees

Publications

Publication
A quantum circuit rule for interference effects in single-molecule electrical junctions.
Manrique David Zsolt, Huang Cancan, Baghernejad Masoud, Zhao Xiaotao, Al-Owaedi Oday A, Sadeghi Hatef, Kaliginedi Veerabhadrarao, Hong Wenjing, Gulcur Murat, Wandlowski Thomas, Bryce Martin R, Lambert Colin J (2015), A quantum circuit rule for interference effects in single-molecule electrical junctions., in Nature communications, 6, 6389-6389.
ATR-SEIRAS study of CO adsorption and oxidation on Rh modified Au (111-25 nm) film electrodes in 0.1 M H2SO4
Xu Qinqin, Berna Antonio, Pobelov Ilya V., Rodes Antonio, Feliu Juan M., Wandlowski Thomas, Kuzume Akiyoshi (2015), ATR-SEIRAS study of CO adsorption and oxidation on Rh modified Au (111-25 nm) film electrodes in 0.1 M H2SO4, in ELECTROCHIMICA ACTA, 176, 1202-1213.
Break junction under electrochemical gating: testbed for single-molecule electronics.
Huang Cancan, Rudnev Alexander V, Hong Wenjing, Wandlowski Thomas (2015), Break junction under electrochemical gating: testbed for single-molecule electronics., in Chemical Society reviews, 44(4), 889-901.
Charge Transport in C-60-Based Dumbbell-type Molecules: Mechanically Induced Switching between Two Distinct Conductance States
Moreno-Garcia Pavel, La Rosa Andrea, Kolivoska Viliam, Bermejo Daniel, Hong Wenjing, Yoshida Koji, Baghernejad Masoud, Filippone Salvatore, Broekmann Peter, Wandlowski Thomas, Martin Nazario (2015), Charge Transport in C-60-Based Dumbbell-type Molecules: Mechanically Induced Switching between Two Distinct Conductance States, in JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 137(6), 2318-2327.
Controlling Electrical Conductance through a π-Conjugated Cruciform Molecule by Selective Anchoring to Gold Electrodes.
Huang Cancan, Chen Songjie, Baruël Ørnsø Kristian, Reber David, Baghernejad Masoud, Fu Yongchun, Wandlowski Thomas, Decurtins Silvio, Hong Wenjing, Thygesen Kristian Sommer, Liu Shi-Xia (2015), Controlling Electrical Conductance through a π-Conjugated Cruciform Molecule by Selective Anchoring to Gold Electrodes., in Angewandte Chemie (International ed. in English), 54(48), 14304-7.
Correlation of breaking forces, conductances and geometries of molecular junctions.
Yoshida Koji, Pobelov Ilya V, Manrique David Zsolt, Pope Thomas, Mészáros Gábor, Gulcur Murat, Bryce Martin R, Lambert Colin J, Wandlowski Thomas (2015), Correlation of breaking forces, conductances and geometries of molecular junctions., in Scientific reports, 5, 9002-9002.
Electrochemical shell-isolated nanoparticle-enhanced Raman spectroscopy: correlating structural information and adsorption processes of pyridine at the Au(hkl) single crystal/solution interface.
Li Jian-Feng, Zhang Yue-Jiao, Rudnev Alexander V, Anema Jason R, Li Song-Bo, Hong Wen-Jing, Rajapandiyan Panneerselvam, Lipkowski Jacek, Wandlowski Thomas, Tian Zhong-Qun (2015), Electrochemical shell-isolated nanoparticle-enhanced Raman spectroscopy: correlating structural information and adsorption processes of pyridine at the Au(hkl) single crystal/solution interface., in Journal of the American Chemical Society, 137(6), 2400-8.
Exploitation of desilylation chemistry in tailor-made functionalization on diverse surfaces.
Fu Yongchun, Chen Songjie, Kuzume Akiyoshi, Rudnev Alexander, Huang Cancan, Kaliginedi Veerabhadrarao, Baghernejad Masoud, Hong Wenjing, Wandlowski Thomas, Decurtins Silvio, Liu Shi-Xia (2015), Exploitation of desilylation chemistry in tailor-made functionalization on diverse surfaces., in Nature communications, 6, 6403-6403.
Magic ratios for connectivity-driven electrical conductance of graphene-like molecules.
Geng Yan, Sangtarash Sara, Huang Cancan, Sadeghi Hatef, Fu Yongchun, Hong Wenjing, Wandlowski Thomas, Decurtins Silvio, Lambert Colin J, Liu Shi-Xia (2015), Magic ratios for connectivity-driven electrical conductance of graphene-like molecules., in Journal of the American Chemical Society, 137(13), 4469-76.
Searching the Hearts of Graphene-like Molecules for Simplicity, Sensitivity, and Logic
Sangtarash Sara, Huang Cancan, Sadeghi Hatef, Sorohhov Gleb, Hauser Juerg, Wandlowski Thomas, Hong Wenjing, Decurtins Silvio, Liu Shi-Xia, Lambert Colin J. (2015), Searching the Hearts of Graphene-like Molecules for Simplicity, Sensitivity, and Logic, in JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 137(35), 11425-11431.
Temperature-Dependent Transport Properties of a Redox-Active Ionic Liquid with a Viologen Group
Bodappa Nataraju, Broekmann Peter, Fu Yong-Chun, Furrer Julien, Furue Yutaro, Sagara Takamasa, Siegenthaler Hans, Tahara Hironobu, Vesztergom Soma, Zick Klaus, Wandlowski Thomas (2015), Temperature-Dependent Transport Properties of a Redox-Active Ionic Liquid with a Viologen Group, in The Journal of Physical Chemistry C, 119(2), 1067-1077.
Three-State Single-Molecule Naphthalenediimide Switch: Integration of a Pendant Redox Unit for Conductance Tuning.
Li Yonghai, Baghernejad Masoud, Qusiy Al-Galiby, Zsolt Manrique David, Zhang Guanxin, Hamill Joseph, Fu Yongchun, Broekmann Peter, Hong Wenjing, Wandlowski Thomas, Zhang Deqing, Lambert Colin (2015), Three-State Single-Molecule Naphthalenediimide Switch: Integration of a Pendant Redox Unit for Conductance Tuning., in Angewandte Chemie (International ed. in English), 54(46), 13586-9.
An in situ surface electrochemistry approach towards whole-cell studies: the structure and reactivity of a Geobacter sulfurreducens submonolayer on electrified metal/electrolyte interfaces
Kuzume Akiyoshi, Zhumaev Ulmas, Li Jianfeng, Fu Yongchun, Füeg Michael, Estévez Marta, Borjas Zulema, Wandlowski Thomas, Esteve-Nuñez Abraham (2014), An in situ surface electrochemistry approach towards whole-cell studies: the structure and reactivity of a Geobacter sulfurreducens submonolayer on electrified metal/electrolyte interfaces, in Phys. Chem. Chem. Phys., 16(40), 22229-22236.
Breaking Force and Conductance of Gold Nanojunctions: Effect of Humidity.
Mohos Miklós, Pobelov Ilya V, Kolivoška Viliam, Mészáros Gábor, Broekmann Peter, Wandlowski Thomas (2014), Breaking Force and Conductance of Gold Nanojunctions: Effect of Humidity., in The journal of physical chemistry letters, 5(20), 3560-4.
Controlled assembly and single electron charging of monolayer protected Au144 clusters: an electrochemistry and scanning tunneling spectroscopy study.
Bodappa Nataraju, Fluch Ulrike, Fu Yongchun, Mayor Marcel, Moreno-García Pavel, Siegenthaler Hans, Wandlowski Thomas (2014), Controlled assembly and single electron charging of monolayer protected Au144 clusters: an electrochemistry and scanning tunneling spectroscopy study., in Nanoscale, 6(24), 15117-26.
Decoupling surface reconstruction and perchlorate adsorption on Au(111)
Zhumaev U. E., Pobelov I. V., Rudnev A. V., Kuzume A., Wandlowski Th. (2014), Decoupling surface reconstruction and perchlorate adsorption on Au(111), in ELECTROCHEMISTRY COMMUNICATIONS, 44, 31-33.
Electrochemical control of a non-covalent binding between ferrocene and beta-cyclodextrin.
Kolivoška V, Mohos M, Pobelov I V, Rohrbach S, Yoshida K, Hong W J, Fu Y C, Moreno-García P, Mészáros G, Broekmann P, Hromadová M, Sokolová R, Valášek M, Wandlowski Th (2014), Electrochemical control of a non-covalent binding between ferrocene and beta-cyclodextrin., in Chemical communications (Cambridge, England), 50(79), 11757-9.
Electrochemical control of single-molecule conductance by Fermi-level tuning and conjugation switching.
Baghernejad Masoud, Zhao Xiaotao, Baruël Ørnsø Kristian, Füeg Michael, Moreno-García Pavel, Rudnev Alexander V, Kaliginedi Veerabhadrarao, Vesztergom Soma, Huang Cancan, Hong Wenjing, Broekmann Peter, Wandlowski Thomas, Thygesen Kristian S, Bryce Martin R (2014), Electrochemical control of single-molecule conductance by Fermi-level tuning and conjugation switching., in Journal of the American Chemical Society, 136(52), 17922-5.
Highly-effective gating of single-molecule junctions: an electrochemical approach.
Baghernejad Masoud, Manrique David Zsolt, Li Chen, Pope Thomas, Zhumaev Ulmas, Pobelov Ilya, Moreno-García Pavel, Kaliginedi Veerabhadrarao, Huang Cancan, Hong Wenjing, Lambert Colin, Wandlowski Thomas (2014), Highly-effective gating of single-molecule junctions: an electrochemical approach., in Chemical communications (Cambridge, England), 50(100), 15975-8.
Promising anchoring groups for single-molecule conductance measurements.
Kaliginedi Veerabhadrarao, Rudnev Alexander V, Moreno-García Pavel, Baghernejad Masoud, Huang Cancan, Hong Wenjing, Wandlowski Thomas (2014), Promising anchoring groups for single-molecule conductance measurements., in Physical chemistry chemical physics : PCCP, 16(43), 23529-39.
Quantifying perchlorate adsorption on Au(111) electrodes
Zhumaev U. E., Lai A. S., Pobelov I. V., Kuzume A., Rudnev A. V., Wandlowski Th. (2014), Quantifying perchlorate adsorption on Au(111) electrodes, in ELECTROCHIMICA ACTA, 146, 112-118.
Reconstruction and electrochemical oxidation of Au(110) surface in 0.1 M H2SO4
Yoshida Koji, Kuzume Akiyoshi, Broekmann Peter, Pobelov Ilya V., Wandlowski Thomas (2014), Reconstruction and electrochemical oxidation of Au(110) surface in 0.1 M H2SO4, in ELECTROCHIMICA ACTA, 139, 281-288.
Redox control of thermopower and figure of merit in phase-coherent molecular wires.
García-Suárez Víctor M, Lambert Colin J, Manrique David Zs, Wandlowski Thomas (2014), Redox control of thermopower and figure of merit in phase-coherent molecular wires., in Nanotechnology, 25(20), 205402-205402.
The synthesis of functionalised diaryltetraynes and their transport properties in single-molecule junctions.
Gulcur Murat, Moreno-García Pavel, Zhao Xiaotao, Baghernejad Masoud, Batsanov Andrei S, Hong Wenjing, Bryce Martin R, Wandlowski Thomas (2014), The synthesis of functionalised diaryltetraynes and their transport properties in single-molecule junctions., in Chemistry (Weinheim an der Bergstrasse, Germany), 20(16), 4653-60.
Electrochemical current-sensing atomic force microscopy in conductive solutions.
Pobelov Ilya V, Mohos Miklós, Yoshida Koji, Kolivoska Viliam, Avdic Amra, Lugstein Alois, Bertagnolli Emmerich, Leonhardt Kelly, Denuault Guy, Gollas Bernhard, Wandlowski Thomas (2013), Electrochemical current-sensing atomic force microscopy in conductive solutions., in Nanotechnology, 24(11), 115501-115501.
Oligo(aryleneethynylene)s with Terminal Pyridyl Groups: Synthesis and Length Dependence of the Tunneling-to-Hopping Transition of Single-Molecule Conductances
Zhao Xiaotao, Huang Cancan, Gulcur Murat, Batsanov Andrei S., Baghernejad Masoud, Hong Wenjing, Bryce Martin R., Wandlowski Thomas (2013), Oligo(aryleneethynylene)s with Terminal Pyridyl Groups: Synthesis and Length Dependence of the Tunneling-to-Hopping Transition of Single-Molecule Conductances, in CHEMISTRY OF MATERIALS, 25(21), 4340-4347.

Collaboration

Group / person Country
Types of collaboration
Prof. Dr. S. Decurtins, Departement für Chemie und Biochemie, University of Bern Switzerland (Europe)
- in-depth/constructive exchanges on approaches, methods or results
- Publication
- Research Infrastructure
- Exchange of personnel
Prof. Dr. C. Lambert, Physik Department, Universität Lancaster Great Britain and Northern Ireland (Europe)
- in-depth/constructive exchanges on approaches, methods or results
Dr. S. Gausch Switzerland (Europe)
- in-depth/constructive exchanges on approaches, methods or results
- Publication
Prof. Dr. M. Mayor,Departement für Chemie, Universität Basel Switzerland (Europe)
- in-depth/constructive exchanges on approaches, methods or results
- Publication
- Research Infrastructure
Prof. Dr. R. Fasel, EMPA Dübendorf Switzerland (Europe)
- in-depth/constructive exchanges on approaches, methods or results
Prof. Dr. M. Bryce, Chemie Department, Durham Universität Great Britain and Northern Ireland (Europe)
- in-depth/constructive exchanges on approaches, methods or results
- Exchange of personnel
Prof. Dr. K. Müllen, MPI für Polymerforschung, Mainz Germany (Europe)
- in-depth/constructive exchanges on approaches, methods or results
Prof. Dr. Z. Q. Tian, State Key Institute of Phys. Chem. Sol. Surfaces, Xiamen University China (Asia)
- in-depth/constructive exchanges on approaches, methods or results
- Publication
- Exchange of personnel
Dr. F. Pauly, Physik Department, KIT Karlsruhe Germany (Europe)
- in-depth/constructive exchanges on approaches, methods or results
Prof. Dr. G. Royal, Dr. C. Bucher, Department of Chemistry, University of Grenoble France (Europe)
- in-depth/constructive exchanges on approaches, methods or results
Prof. Dr. N. Martin, Chemie Department, Universität Complutense Madrid Spain (Europe)
- in-depth/constructive exchanges on approaches, methods or results
- Publication
- Exchange of personnel

Scientific events

Active participation

Title Type of contribution Title of article or contribution Date Place Persons involved
66th Annual Meeting of the International Society of Electrochemistry Talk given at a conference Break junctions under electrochemical gating 04.10.2015 Taipei, Taiwan Wandlowski Thomas; Broekmann Peter; Kaliginedi Veera Bhadra Rao; Huang Blaser Cancan; Baghernejad Masoud;
66th Annual Meeting of the International Society of Electrochemistry Poster Tuning of charge transport in single molecule with chemical and electrochemical methods 04.10.2015 Taipei, Taiwan Huang Blaser Cancan; Broekmann Peter; Baghernejad Masoud; Wandlowski Thomas;
13th International Fischer Symposium Talk given at a conference Molecular break junctions 07.07.2015 Lübeck, Germany Baghernejad Masoud; Huang Blaser Cancan; Broekmann Peter; Kaliginedi Veera Bhadra Rao; Wandlowski Thomas;
65th Annual Meeting of the International Society of Electrochemistry (ISE) Talk given at a conference Towards in situ Raman spectroscopy on electrochemical gated single-molecule junctions 31.08.2014 Lausanne, Switzerland Wandlowski Thomas; Baghernejad Masoud; Huang Blaser Cancan; Broekmann Peter;
65th Annual Meeting of the International Society of Electrochemistry (ISE) Poster Single-molecule charge transport study using electrochemical and mechanical controllable break junction 31.08.2014 Lausanne, Switzerland Huang Blaser Cancan; Wandlowski Thomas;


Awards

Title Year
2015 National Award for Outstanding Self-financed Chinese Students Study Abroad 2015

Associated projects

Number Title Start Funding scheme
126969 Electromechanical Systems 01.10.2009 Sinergia
124643 Electron Transport at the Nanoscale - An Electrochemical Approach 01.09.2009 Project funding (Div. I-III)
124643 Electron Transport at the Nanoscale - An Electrochemical Approach 01.09.2009 Project funding (Div. I-III)

Abstract

The proposal aims at exploring charge transport in metal (carbon)/molecule/metal (carbon) junctions employing a nanoscale electrochemical approach. Based on the concept of “electrolyte gating” single molecule and ensemble measurements on electron transport in active nanometer-scale junctions will be combined with structure-sensitive in-situ techniques (STM/STS, current-probe AFM (CP-AFM), infrared (SEIRAS) and gap-mode Raman spectroscopy (SHINERS)). We attempt to establish an electrochemical surface-science-based approach at the nanoscale with a particular focus on contact, molecular backbone and functionality. We will apply the following topology: A central functional unit F is attached via spacer units S and anchoring groups A, either symmetrically (A-S-F-S-A) or asymmetrically (A-S-F-S) to contacting leads. The latter are represented either by the tip of an STM or CP-AFM and an adsorbate-modified single crystal metal substrate or a pair of nanoelectrodes in a fixed or variable (mechanically-controlled break junction, MCBJ) geometry. Functional moieties will be placed either within the molecular backbone or as pendent substituents. We aim at evaluating how charge transport through single molecules and hybrid assemblies is modulated by external stimuli. We will explore switching phenomena via electric field control, redox control and with light-responsive molecules. We aim at establishing fundamental aspects of electron transport as well as relationships between structural functionality of nanoscale molecular junctions and their electronic response upon electrochemical and/or light stimulation at the single molecule level. The development and implementation of CP-AFM and gap-mode Raman spectroscopy (in combination with our MCBJ set-up) for applications in a nanoscale electrochemical environment will enable (1) unprecedented load control and (2) direct access for monitoring structure changes upon stimulations. Application studies towards molecular recognition are anticipated.We identify the following specific working packages:WP 1:Search for alternative contact conceptsWP 2:Electron transport in “inactive” molecular wires.WP 3:Stimulus-responsive electron transport in “active” nanojunctionsWP 4:Electrochemical MCBJ combined with gap-mode Raman spectroscopyWP 5:Load control and recognition in electrochemical CP-AFMThe project will provide unique new insights into fundamental structure-property relationships in electrochemical nanojunctions and their response upon stimulation. New grafting concepts will be developed. Exciting new results on nanoscale structure and reactivity are expected from the development and application of in-situ single molecule Raman spectroscopy and CP-AFM. The proposed research represents an interdisciplinary approach, which will benefit substantially from several active collaborations with complementary teams representing expertise in molecular and supramolecular chemistry (M. Bryce, Durham; S. Decurtins, Bern; N. Martin, Madrid; M. Mayor, Basel; K. Müllen, Mainz; R. Royal/Ch. Bucher, Grenoble), surface science (R. Fasel, EMPA), interfacial spectroscopy (Z. Q. Tian, Xiamen), theoretical physics (C. Lambert, Lancaster; F. Pauly, Karlsruhe), and engineering (Samlab, EPFL).
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