Hemilabile Ligands as Mechanosensitive Electrode Contacts for Molecular Electronics

Ferri, Nicolò and Algethami, Norah and Vezzoli, Andrea and Sangtarash, Sara and McLaughlin, Maeve and Sadeghi, Hatef and Lambert, Colin J. and Nichols, Richard J. and Higgins, Simon J. (2019) Hemilabile Ligands as Mechanosensitive Electrode Contacts for Molecular Electronics. Angewandte Chemie International Edition, 58 (46). pp. 16583-16589. ISSN 1433-7851

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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⇄bidentate contact transitions as the junction is modulated in size. We observed an up 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.

Item Type:
Journal Article
Journal or Publication Title:
Angewandte Chemie International Edition
Uncontrolled Keywords:
?? general chemistrycatalysischemistry(all)catalysis ??
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Deposited On:
17 Feb 2022 15:55
Last Modified:
16 Feb 2024 00:54