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

Saman Naghibi, Sara Sangtarash, Varshini J. Kumar, Jian Zhong Wu, Martyna M. Judd, Xiaohang Qiao, Elena Gorenskaia, Simon J. Higgins, Nicholas Cox, Richard J. Nichols, Hatef Sadeghi, Paul J. Low, Andrea Vezzoli

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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.

Original languageEnglish
Article numbere202116985
JournalAngewandte Chemie - International Edition
Volume61
Issue number23
DOIs
Publication statusPublished - 7 Jun 2022

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