Journal
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
Volume 61, Issue 23, Pages -Publisher
WILEY-V C H VERLAG GMBH
DOI: 10.1002/anie.202116985
Keywords
Molecular Devices; Molecular Electronics; Radicals
Categories
Funding
- Royal Society [RGS\R2\202119, URF\R1\191241]
- EPSRC [EP/V037765/1, EP/M005046/1, EP/M029522/1]
- Australian Research Council [DP190100073, DP190100074]
- UKRI [MR/S015329/2]
- Leverhulme Trust [ECF-2018-375]
- Schlumberger Faculty for the Future scholarship program
- Scholarship for International Research Fees from the University of Western Australia.
- Leverhulme Foundation [RPG-2019-308]
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Integrating radical species into non-cryogenic nanodevices is crucial for molecular electronics. This study successfully fabricates single-molecule devices incorporating a persistent radical and demonstrates the retention of open-shell character at room temperature. Electrochemical gating enables reduction to a closed-shell state, and bias-dependent alignment of open-shell resonances leads to electronically driven rectification.
Integrating radical (open-shell) species into non-cryogenic nanodevices is key to unlocking the potential of molecular electronics. While many efforts have been devoted to this issue, in the absence of a chemical/electrochemical potential the open-shell character is generally lost in contact with the metallic electrodes. Herein, single-molecule devices incorporating a 6-oxo-verdazyl persistent radical have been fabricated using break-junction techniques. The open-shell character is retained at room temperature, and electrochemical gating permits in situ reduction to a closed-shell anionic state in a single-molecule transistor configuration. Furthermore, electronically driven rectification arises from bias-dependent alignment of the open-shell resonances. The integration of radical character, transistor-like switching, and rectification in a single molecular component paves the way to further studies of the electronic, magnetic, and thermoelectric properties of open-shell species.
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