Hemilabile ligands as mechanosensitive electrode contacts for molecular electronics

Ferri, N, Algethami, Norah, Vezzoli, A ORCID: 0000-0002-8059-0113, Sangtarash, Sara, McLaughlin, Maeve, Sadeghi, Hatef, Lambert, Colin, Nichols, Richard ORCID: 0000-0002-1446-8275 and Higgins, Simon ORCID: 0000-0003-3518-9061
(2019) Hemilabile ligands as mechanosensitive electrode contacts for molecular electronics. Angewandte Chemie (International Edition), 58 (46). 16583 - 16589.

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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 we observed conductance changes of up to two orders of magnitude as junctions were compressed and stretched. Localized interactions between weakly‐coordinating thienyl sulfurs and the electrodes are responsible for the observed effect, which 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: Article
Uncontrolled Keywords: density functional calculations, hemilabile ligands, molecular devices, molecular electronics, sulfur ligands
Depositing User: Symplectic Admin
Date Deposited: 13 Aug 2019 09:38
Last Modified: 24 Jun 2022 18:10
DOI: 10.1002/anie.201906400
Open Access URL: https://dx.doi.org/10.1002/anie.201906400
Related URLs:
URI: https://livrepository.liverpool.ac.uk/id/eprint/3051608