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Photooxidation driven formation of Fe-Au linked ferrocene-based single-molecule junctions

Woojung Lee, Liang Li, María Camarasa-Gómez, Daniel Hernangómez-Pérez, Xavier Roy, Ferdinand Evers (), Michael S. Inkpen () and Latha Venkataraman ()
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Woojung Lee: Columbia University
Liang Li: Columbia University
María Camarasa-Gómez: University of Regensburg
Daniel Hernangómez-Pérez: University of Regensburg
Xavier Roy: Columbia University
Ferdinand Evers: University of Regensburg
Michael S. Inkpen: University of Southern California
Latha Venkataraman: Columbia University

Nature Communications, 2024, vol. 15, issue 1, 1-9

Abstract: Abstract Metal-metal contacts, though not yet widely realized, may provide exciting opportunities to serve as tunable and functional interfaces in single-molecule devices. One of the simplest components which might facilitate such binding interactions is the ferrocene group. Notably, direct bonds between the ferrocene iron center and metals such as Pd or Co have been demonstrated in molecular complexes comprising coordinating ligands attached to the cyclopentadienyl rings. Here, we demonstrate that ferrocene-based single-molecule devices with Fe-Au interfacial contact geometries form at room temperature in the absence of supporting coordinating ligands. Applying a photoredox reaction, we propose that ferrocene only functions effectively as a contact group when oxidized, binding to gold through a formal Fe3+ center. This observation is further supported by a series of control measurements and density functional theory calculations. Our findings extend the scope of junction contact chemistries beyond those involving main group elements, lay the foundation for light switchable ferrocene-based single-molecule devices, and highlight new potential mechanistic function(s) of unsubstituted ferrocenium groups in synthetic processes.

Date: 2024
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DOI: 10.1038/s41467-024-45707-z

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