Metal-Single-Molecule-Semiconductor Junctions Formed by a Radical Reaction Bridging Gold and Silicon Electrodes.
Here we report molecular films terminated with diazonium salts moieties at both ends which enables single-molecule contacts between gold and silicon electrodes at open circuit via a radical reaction. We show that the kinetics of film grafting is crystal-facet dependent, being more favorable on ⟨111⟩...
| Main Authors: | , , , , , , , |
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| Format: | Journal Article |
| Language: | English |
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AMER CHEMICAL SOC
2019
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| Online Access: | https://openresearch-repository.anu.edu.au/handle/1885/205914 http://hdl.handle.net/20.500.11937/90486 |
| _version_ | 1848765387344183296 |
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| author | Peiris, Chandramalika R Vogel, Yan B Le Brun, Anton P Aragonès, Albert C Coote, Michelle L Díez-Pérez, Ismael Ciampi, Simone Darwish, Nadim |
| author_facet | Peiris, Chandramalika R Vogel, Yan B Le Brun, Anton P Aragonès, Albert C Coote, Michelle L Díez-Pérez, Ismael Ciampi, Simone Darwish, Nadim |
| author_sort | Peiris, Chandramalika R |
| building | Curtin Institutional Repository |
| collection | Online Access |
| description | Here we report molecular films terminated with diazonium salts moieties at both ends which enables single-molecule contacts between gold and silicon electrodes at open circuit via a radical reaction. We show that the kinetics of film grafting is crystal-facet dependent, being more favorable on ⟨111⟩ than on ⟨100⟩, a finding that adds control over surface chemistry during the device fabrication. The impact of this spontaneous chemistry in single-molecule electronics is demonstrated using STM-break junction approaches by forming metal-single-molecule-semiconductor junctions between silicon and gold source and drain, electrodes. Au-C and Si-C molecule-electrode contacts result in single-molecule wires that are mechanically stable, with an average lifetime at room temperature of 1.1 s, which is 30-400% higher than that reported for conventional molecular junctions formed between gold electrodes using thiol and amine contact groups. The high stability enabled measuring current-voltage properties during the lifetime of the molecular junction. We show that current rectification, which is intrinsic to metal-semiconductor junctions, can be controlled when a single-molecule bridges the gap in the junction. The system changes from being a current rectifier in the absence of a molecular bridge to an ohmic contact when a single molecule is covalently bonded to both silicon and gold electrodes. This study paves the way for the merging of the fields of single-molecule and silicon electronics. |
| first_indexed | 2025-11-14T11:34:26Z |
| format | Journal Article |
| id | curtin-20.500.11937-90486 |
| institution | Curtin University Malaysia |
| institution_category | Local University |
| language | eng |
| last_indexed | 2025-11-14T11:34:26Z |
| publishDate | 2019 |
| publisher | AMER CHEMICAL SOC |
| recordtype | eprints |
| repository_type | Digital Repository |
| spelling | curtin-20.500.11937-904862023-03-20T06:27:34Z Metal-Single-Molecule-Semiconductor Junctions Formed by a Radical Reaction Bridging Gold and Silicon Electrodes. Peiris, Chandramalika R Vogel, Yan B Le Brun, Anton P Aragonès, Albert C Coote, Michelle L Díez-Pérez, Ismael Ciampi, Simone Darwish, Nadim Science & Technology Physical Sciences Chemistry, Multidisciplinary Chemistry DIAZONIUM SALTS GLASSY-CARBON ELECTROCHEMICAL REDUCTION SURFACES MONOLAYERS TRANSPORT PLATINUM CONTACTS BEHAVIOR Here we report molecular films terminated with diazonium salts moieties at both ends which enables single-molecule contacts between gold and silicon electrodes at open circuit via a radical reaction. We show that the kinetics of film grafting is crystal-facet dependent, being more favorable on ⟨111⟩ than on ⟨100⟩, a finding that adds control over surface chemistry during the device fabrication. The impact of this spontaneous chemistry in single-molecule electronics is demonstrated using STM-break junction approaches by forming metal-single-molecule-semiconductor junctions between silicon and gold source and drain, electrodes. Au-C and Si-C molecule-electrode contacts result in single-molecule wires that are mechanically stable, with an average lifetime at room temperature of 1.1 s, which is 30-400% higher than that reported for conventional molecular junctions formed between gold electrodes using thiol and amine contact groups. The high stability enabled measuring current-voltage properties during the lifetime of the molecular junction. We show that current rectification, which is intrinsic to metal-semiconductor junctions, can be controlled when a single-molecule bridges the gap in the junction. The system changes from being a current rectifier in the absence of a molecular bridge to an ohmic contact when a single molecule is covalently bonded to both silicon and gold electrodes. This study paves the way for the merging of the fields of single-molecule and silicon electronics. 2019 Journal Article http://hdl.handle.net/20.500.11937/90486 10.1021/jacs.9b07125 eng https://openresearch-repository.anu.edu.au/handle/1885/205914 http://purl.org/au-research/grants/arc/DE160100732 http://purl.org/au-research/grants/arc/DP190100735 http://purl.org/au-research/grants/arc/DE160101101 AMER CHEMICAL SOC fulltext |
| spellingShingle | Science & Technology Physical Sciences Chemistry, Multidisciplinary Chemistry DIAZONIUM SALTS GLASSY-CARBON ELECTROCHEMICAL REDUCTION SURFACES MONOLAYERS TRANSPORT PLATINUM CONTACTS BEHAVIOR Peiris, Chandramalika R Vogel, Yan B Le Brun, Anton P Aragonès, Albert C Coote, Michelle L Díez-Pérez, Ismael Ciampi, Simone Darwish, Nadim Metal-Single-Molecule-Semiconductor Junctions Formed by a Radical Reaction Bridging Gold and Silicon Electrodes. |
| title | Metal-Single-Molecule-Semiconductor Junctions Formed by a Radical Reaction Bridging Gold and Silicon Electrodes. |
| title_full | Metal-Single-Molecule-Semiconductor Junctions Formed by a Radical Reaction Bridging Gold and Silicon Electrodes. |
| title_fullStr | Metal-Single-Molecule-Semiconductor Junctions Formed by a Radical Reaction Bridging Gold and Silicon Electrodes. |
| title_full_unstemmed | Metal-Single-Molecule-Semiconductor Junctions Formed by a Radical Reaction Bridging Gold and Silicon Electrodes. |
| title_short | Metal-Single-Molecule-Semiconductor Junctions Formed by a Radical Reaction Bridging Gold and Silicon Electrodes. |
| title_sort | metal-single-molecule-semiconductor junctions formed by a radical reaction bridging gold and silicon electrodes. |
| topic | Science & Technology Physical Sciences Chemistry, Multidisciplinary Chemistry DIAZONIUM SALTS GLASSY-CARBON ELECTROCHEMICAL REDUCTION SURFACES MONOLAYERS TRANSPORT PLATINUM CONTACTS BEHAVIOR |
| url | https://openresearch-repository.anu.edu.au/handle/1885/205914 https://openresearch-repository.anu.edu.au/handle/1885/205914 https://openresearch-repository.anu.edu.au/handle/1885/205914 https://openresearch-repository.anu.edu.au/handle/1885/205914 http://hdl.handle.net/20.500.11937/90486 |