Journal
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
Volume 58, Issue 46, Pages 16583-16589Publisher
WILEY-V C H VERLAG GMBH
DOI: 10.1002/anie.201906400
Keywords
density functional calculations; hemilabile ligands; molecular devices; molecular electronics; sulfur ligands
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Funding
- UK EPSRC [EP/M005046/1, EP/M029522/1, EP/M014169/1, EP/P027156/1, EP/N03337X/1, EP/N017188/1]
- ECH2020 FET Open project [767187]
- Leverhulme Trust [ECF-2017-186, ECF-2018-375]
- UKRI [MR/S015329/1]
- EPSRC [EP/N03337X/1, EP/P027156/1, EP/M029522/1, EP/M014169/1, EP/M005046/1, EP/N017188/1] Funding Source: UKRI
- UKRI [MR/S015329/1, MR/S015329/2] Funding Source: UKRI
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Single-molecule junctions that are sensitive to compression or elongation are an emerging class of nanoelectromechanical systems (NEMS). Although the molecule-electrode interface can be engineered to impart such functionality, most studies to date rely on poorly defined interactions. We focused on this issue by synthesizing molecular wires designed to have chemically defined hemilabile contacts based on (methylthio)thiophene moieties. We measured their conductance as a function of junction size and observed conductance changes of up to two orders of magnitude as junctions were compressed and stretched. Localised interactions between weakly coordinating thienyl sulfurs and the electrodes are responsible for the observed effect and allow reversible monodentate reversible arrow bidentate contact transitions as the junction is modulated in size. We observed an up to approximate to 100-fold sensitivity boost of the (methylthio)thiophene-terminated molecular wire compared with its non-hemilabile (methylthio)benzene counterpart and demonstrate a previously unexplored application of hemilabile ligands to molecular electronics.
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