Controlling piezoresistance in single molecules through the isomerisation of bullvalenes
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...
| Main Authors: | , , , , , , , |
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| Format: | Journal Article |
| Language: | English |
| Published: |
2023
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| Online Access: | http://purl.org/au-research/grants/arc/DE160101101 http://hdl.handle.net/20.500.11937/94705 |
| _version_ | 1848765900680855552 |
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| author | Reimers, J.R. Li, T. Birvé, A.P. Yang, L. Aragonès, A.C. Fallon, T. Kosov, D.S. Darwish, Nadim |
| author_facet | Reimers, J.R. Li, T. Birvé, A.P. Yang, L. Aragonès, A.C. Fallon, T. Kosov, D.S. Darwish, Nadim |
| author_sort | Reimers, J.R. |
| building | Curtin Institutional Repository |
| collection | Online Access |
| 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. |
| first_indexed | 2025-11-14T11:42:36Z |
| format | Journal Article |
| id | curtin-20.500.11937-94705 |
| institution | Curtin University Malaysia |
| institution_category | Local University |
| language | eng |
| last_indexed | 2025-11-14T11:42:36Z |
| publishDate | 2023 |
| recordtype | eprints |
| repository_type | Digital Repository |
| spelling | curtin-20.500.11937-947052024-05-07T06:27:38Z Controlling piezoresistance in single molecules through the isomerisation of bullvalenes Reimers, J.R. Li, T. Birvé, A.P. Yang, L. Aragonès, A.C. Fallon, T. Kosov, D.S. Darwish, Nadim 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. 2023 Journal Article http://hdl.handle.net/20.500.11937/94705 10.1038/s41467-023-41674-z eng http://purl.org/au-research/grants/arc/DE160101101 http://purl.org/au-research/grants/arc/DP190100735 http://creativecommons.org/licenses/by/4.0/ fulltext |
| spellingShingle | Reimers, J.R. Li, T. Birvé, A.P. Yang, L. Aragonès, A.C. Fallon, T. Kosov, D.S. Darwish, Nadim Controlling piezoresistance in single molecules through the isomerisation of bullvalenes |
| title | Controlling piezoresistance in single molecules through the isomerisation of bullvalenes |
| title_full | Controlling piezoresistance in single molecules through the isomerisation of bullvalenes |
| title_fullStr | Controlling piezoresistance in single molecules through the isomerisation of bullvalenes |
| title_full_unstemmed | Controlling piezoresistance in single molecules through the isomerisation of bullvalenes |
| title_short | Controlling piezoresistance in single molecules through the isomerisation of bullvalenes |
| title_sort | controlling piezoresistance in single molecules through the isomerisation of bullvalenes |
| url | http://purl.org/au-research/grants/arc/DE160101101 http://purl.org/au-research/grants/arc/DE160101101 http://hdl.handle.net/20.500.11937/94705 |