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Redox-Addressable Single-Molecule Junctions Incorporating a Persistent Organic Radical.


ABSTRACT: 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.

SUBMITTER: Naghibi S 

PROVIDER: S-EPMC9322687 | biostudies-literature | 2022 Jun

REPOSITORIES: biostudies-literature

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Redox-Addressable Single-Molecule Junctions Incorporating a Persistent Organic Radical.

Naghibi Saman S   Sangtarash Sara S   Kumar Varshini J VJ   Wu Jian-Zhong JZ   Judd Martyna M MM   Qiao Xiaohang X   Gorenskaia Elena E   Higgins Simon J SJ   Cox Nicholas N   Nichols Richard J RJ   Sadeghi Hatef H   Low Paul J PJ   Vezzoli Andrea A  

Angewandte Chemie (International ed. in English) 20220405 23


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 r  ...[more]

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