Controlling piezoresistance in single molecules through the isomerisation of bullvalenes
Reimers, Jeffrey R., Li, Tiexin, Birvé, André, Yang, Likun, Aragonès, Albert C., Fallon, Thomas, Kosov, Daniel S., and Darwish, Nadim (2023) Controlling piezoresistance in single molecules through the isomerisation of bullvalenes. Nature Communications, 14 (1). 6089.
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Abstract
Nanoscale electro-mechanical systems (NEMS) displaying piezoresistance offer unique measurement opportunities at the sub-cellular level, in detectors and sensors, and in emerging generations of integrated electronic devices. Here, we show a single-molecule NEMS piezoresistor that operates utilising constitutional and conformational isomerisation of individual diaryl-bullvalene molecules and can be switched at 850 Hz. Observations are made using scanning tunnelling microscopy break junction (STMBJ) techniques to characterise piezoresistance, combined with blinking (current-time) experiments that follow single-molecule reactions in real time. A kinetic Monte Carlo methodology (KMC) is developed to simulate isomerisation on the experimental timescale, parameterised using density-functional theory (DFT) combined with non-equilibrium Green’s function (NEGF) calculations. Results indicate that piezoresistance is controlled by both constitutional and conformational isomerisation, occurring at rates that are either fast (equilibrium) or slow (non-equilibrium) compared to the experimental timescale. Two different types of STMBJ traces are observed, one typical of traditional experiments that are interpreted in terms of intramolecular isomerisation occurring on stable tipped-shaped metal-contact junctions, and another attributed to arise from junction‒interface restructuring induced by bullvalene isomerisation.
| Item ID: | 80815 |
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| Item Type: | Article (Research - C1) |
| ISSN: | 2041-1723 |
| Copyright Information: | © The Author(s) 2023. This article is licensed under a Creative Commons Attribution 4.0 International License, which permits use, sharing, adaptation, distribution and reproduction in any medium or format, as long as you give appropriate credit to the original author(s) and the source, provide a link to the Creative Commons license, and indicate if changes were made. The images or other third party material in this article are included in the article’s Creative Commons license, unless indicated otherwise in a credit line to the material. If material is not included in the article’s Creative Commons license and your intended use is not permitted by statutory regulation or exceeds the permitted use, you will need to obtain permission directly from the copyright holder. To view a copy of this license, visit http://creativecommons.org/licenses/by/4.0/. |
| Funders: | Australian Research Council (ARC) |
| Projects and Grants: | ARC grant (DE160101101), ARC grant (DP190100735) |
| Date Deposited: | 30 Oct 2023 23:27 |
| FoR Codes: | 51 PHYSICAL SCIENCES > 5199 Other physical sciences > 519999 Other physical sciences not elsewhere classified @ 100% |
| SEO Codes: | 28 EXPANDING KNOWLEDGE > 2801 Expanding knowledge > 280120 Expanding knowledge in the physical sciences @ 100% |
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