Environmental Control of Single‐Molecule Junction Evolution and Conductance: A Case Study of Expanded Pyridinium Wiring

Environmental control of single‐molecule junction evolution and conductance was demonstrated for expanded pyridinium molecules by scanning tunneling microscopy break junction method and interpreted by quantum transport calculations including solvent molecules explicitly. Fully extended and highly co...

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Bibliographic Details
Published in:Angewandte Chemie 2021-02, Vol.133 (9), p.4782-4789
Main Authors: Nováková Lachmanová, Štěpánka, Kolivoška, Viliam, Šebera, Jakub, Gasior, Jindřich, Mészáros, Gábor, Dupeyre, Grégory, Lainé, Philippe P., Hromadová, Magdaléna
Format: Article
Language:English
Subjects:
Chemistry
Conductance
Electrodes
Electronic devices
Electronic equipment
Environmental control
Evolution
expanded pyridiniums
Mesitylene
molecular electronics
Pyridinium
Quantum transport
Resistance
Scanning tunneling microscopy
single-molecule conductance
solvent gating
Solvents
Substrates
Wiring
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Summary:Environmental control of single‐molecule junction evolution and conductance was demonstrated for expanded pyridinium molecules by scanning tunneling microscopy break junction method and interpreted by quantum transport calculations including solvent molecules explicitly. Fully extended and highly conducting molecular junctions prevail in water environment as opposed to short and less conducting junctions formed in non‐solvating mesitylene. A theoretical approach correctly models single‐molecule conductance values considering the experimental junction length. Most pronounced difference in the molecular junction formation and conductance was identified for a molecule with the highest stabilization energy on the gold substrate confirming the importance of molecule–electrode interactions. Presented concept of tuning conductance through molecule–electrode interactions in the solvent‐driven junctions can be used in the development of new molecular electronic devices. Single‐molecule junction conductance can be efficiently tuned by solvent environment. A series of expanded pyridinium molecular wires gave higher conductance with fully extended junction geometries in solvating water environment as opposed to mesitylene solvent. Environmental control efficiently operates the molecule–electrode interactions.
ISSN:0044-8249
1521-3757
DOI:10.1002/ange.202013882