- Title
- Controlling piezoresistance in single molecules through the isomerisation of bullvalenes
- Creator
- Reimers, Jeffrey R.; Li, Tiexin; Birvé, André P.; Yang, Likun; Aragonès, Albert C.; Fallon, Thomas; Kosov, Daniel S.; Darwish, Nadim
- Relation
- Nature Communications Vol. 14, no. 6089
- Publisher Link
- http://dx.doi.org/10.1038/s41467-023-41674-z
- Publisher
- Nature Publishing Group
- Resource Type
- journal article
- Date
- 2023
- Description
- 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.
- Subject
- nanoscale electro-mechanical systems (NEMS); electronic devices; molecules; density-functional theory (DFT)
- Identifier
- http://hdl.handle.net/1959.13/1493211
- Identifier
- uon:53500
- Identifier
- ISSN:2041-1723
- Rights
- x
- Language
- eng
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