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- Title
Controlling piezoresistance in single molecules through the isomerisation of bullvalenes.
- Authors
Reimers, Jeffrey R.; Li, Tiexin; Birvé, André P.; Yang, Likun; Aragonès, Albert C.; Fallon, Thomas; Kosov, Daniel S.; Darwish, Nadim
- 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. The quest for miniaturisation of electromechanical nanosystems requires the use of single molecules as active components. Here, the authors develop a piezoresistor based on a single bullvalene molecule that changes its shape by a Cope rearrangement.
- Subjects
SINGLE molecules; ISOMERIZATION; PIEZORESISTANCE; SCANNING tunneling microscopy; GREEN'S functions
- Publication
Nature Communications, 2023, Vol 14, Issue 1, p1
- ISSN
2041-1723
- Publication type
Article
- DOI
10.1038/s41467-023-41674-z