Details
| Original language | English |
|---|---|
| Pages (from-to) | 6207-6212 |
| Number of pages | 6 |
| Journal | Angewandte Chemie - International Edition |
| Volume | 59 |
| Issue number | 15 |
| Early online date | 22 Jan 2020 |
| Publication status | Published - 1 Apr 2020 |
| Externally published | Yes |
Abstract
Among the prerequisites for the progress of single-molecule-based electronic devices are a better understanding of the electronic properties at the individual molecular level and the development of methods to tune the charge transport through molecular junctions. Scanning tunneling microscopy (STM) is an ideal tool not only for the characterization, but also for the manipulation of single atoms and molecules on surfaces. The conductance through a single molecule can be measured by contacting the molecule with atomic precision and forming a molecular bridge between the metallic STM tip electrode and the metallic surface electrode. The parameters affecting the conductance are mainly related to their electronic structure and to the coupling to the metallic electrodes. Here, the experimental and theoretical analyses are focused on single tetracenothiophene molecules and demonstrate that an in situ-induced direct desulfurization reaction of the thiophene moiety strongly improves the molecular anchoring by forming covalent bonds between molecular carbon and copper surface atoms. This bond formation leads to an increase of the conductance by about 50 % compared to the initial state.
Keywords
- covalent-bond formation, DFT, single-molecule conductance, STM/AFM, strong anchoring
ASJC Scopus subject areas
- Chemical Engineering(all)
- Catalysis
- Chemistry(all)
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In: Angewandte Chemie - International Edition, Vol. 59, No. 15, 01.04.2020, p. 6207-6212.
Research output: Contribution to journal › Article › Research › peer review
}
TY - JOUR
T1 - Controlling Single Molecule Conductance by a Locally Induced Chemical Reaction on Individual Thiophene Units
AU - Michnowicz, Tomasz
AU - Borca, Bogdana
AU - Pétuya, Rémi
AU - Schendel, Verena
AU - Pristl, Marcel
AU - Pentegov, Ivan
AU - Kraft, Ulrike
AU - Klauk, Hagen
AU - Wahl, Peter
AU - Mutombo, Pingo
AU - Jelínek, Pavel
AU - Arnau, Andrés
AU - Schlickum, Uta
AU - Kern, Klaus
N1 - Funding information: The authors acknowledge the Emmy-Noether-Program of the Deutsche Forschungsgemeinschaft, the SFB 767, Core Program PN19-03 (contract number 21 N/08.02.2019) founded by the Romanian Ministry of Research and Innovation, Basque Departamento de Universidades e Investigación (grant no. IT-756-13), the Spanish Ministerio de Economía y Competitividad (grant no. FIS2013-48286-C2-8752-P and FIS2016-75862-P) and the Operational Programme Research, Development and Education financed by European Structural and Investment Funds and the Czech Ministry of Education, Youth and Sports (Project No. SOLID21 CZ.02.1.01/0.0/0.0/16_019/0000760). P.M. and P.J. acknowledge access to computing and storage facilities owned by parties and projects contributing to the Czech National Grid Infrastructure MetaCentrum provided under the programme “Projects of Large Research, Development, and Innovations Infrastructures” (CESNET LM2015042). P.J. acknowledges support from Praemium Academie of the Academy of Science of the Czech Republic and MEYS LM2015087.
PY - 2020/4/1
Y1 - 2020/4/1
N2 - Among the prerequisites for the progress of single-molecule-based electronic devices are a better understanding of the electronic properties at the individual molecular level and the development of methods to tune the charge transport through molecular junctions. Scanning tunneling microscopy (STM) is an ideal tool not only for the characterization, but also for the manipulation of single atoms and molecules on surfaces. The conductance through a single molecule can be measured by contacting the molecule with atomic precision and forming a molecular bridge between the metallic STM tip electrode and the metallic surface electrode. The parameters affecting the conductance are mainly related to their electronic structure and to the coupling to the metallic electrodes. Here, the experimental and theoretical analyses are focused on single tetracenothiophene molecules and demonstrate that an in situ-induced direct desulfurization reaction of the thiophene moiety strongly improves the molecular anchoring by forming covalent bonds between molecular carbon and copper surface atoms. This bond formation leads to an increase of the conductance by about 50 % compared to the initial state.
AB - Among the prerequisites for the progress of single-molecule-based electronic devices are a better understanding of the electronic properties at the individual molecular level and the development of methods to tune the charge transport through molecular junctions. Scanning tunneling microscopy (STM) is an ideal tool not only for the characterization, but also for the manipulation of single atoms and molecules on surfaces. The conductance through a single molecule can be measured by contacting the molecule with atomic precision and forming a molecular bridge between the metallic STM tip electrode and the metallic surface electrode. The parameters affecting the conductance are mainly related to their electronic structure and to the coupling to the metallic electrodes. Here, the experimental and theoretical analyses are focused on single tetracenothiophene molecules and demonstrate that an in situ-induced direct desulfurization reaction of the thiophene moiety strongly improves the molecular anchoring by forming covalent bonds between molecular carbon and copper surface atoms. This bond formation leads to an increase of the conductance by about 50 % compared to the initial state.
KW - covalent-bond formation
KW - DFT
KW - single-molecule conductance
KW - STM/AFM
KW - strong anchoring
UR - http://www.scopus.com/inward/record.url?scp=85079713656&partnerID=8YFLogxK
U2 - 10.1002/anie.201915200
DO - 10.1002/anie.201915200
M3 - Article
C2 - 31965698
AN - SCOPUS:85079713656
VL - 59
SP - 6207
EP - 6212
JO - Angewandte Chemie - International Edition
JF - Angewandte Chemie - International Edition
SN - 1433-7851
IS - 15
ER -