Journal
NANO LETTERS
Volume 19, Issue 9, Pages 6104-6108Publisher
AMER CHEMICAL SOC
DOI: 10.1021/acs.nanolett.9b02032
Keywords
electron transfer; Franck-Condon blockade; atomic force microscopy; single-electron tunneling; electron-vibron coupling; single-molecule electronics
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Funding
- Natural Sciences and Engineering Research Council of Canada
- le Fonds Quebecois de le Recherche sur la Nature et les Technologies
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Long-range electron transfer is a ubiquitous process that plays an important role in electrochemistry, biochemistry, organic electronics, and single molecule electronics. Fundamentally, quantum mechanical processes, at their core, manifest through both electron tunneling and the associated transition between quantized nuclear vibronic states (intramolecular vibrational relaxation) mediated by electron-nuclear coupling. Here, we report on measurements of long-range electron transfer at the interface between a single ferrocene molecule and a gold substrate separated by a hexadecanethiol quantum tunneling barrier. These redox measurements exhibit quantized nuclear transitions mediated by electron-nuclear coupling at 4.7 K in vacuum. By detecting the electric force associated with redox events by atomic force microscopy (AFM), with increasing AFM oscillation amplitude, the intensity of the observed cantilever resonance frequency shift peak increases and then exhibits a series of discrete steps that are indicative of quantized nuclear transitions. The observed peak shapes agree well with a single-electron tunneling model with quantized nuclear state transitions associated with the conversion of the molecule between oxidized and reduced electronic states. This technique opens the door to simultaneously investigating quantized electron and nuclear dynamics in a diverse range of systems.
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