ArticleProceedings of the National Academy of Sciences of the United States of America2014
Voltage tuning of vibrational mode energies in single-molecule junctions.
Article in Proceedings of the National Academy of Sciences of the United States of America, 2014. The graph could read no effect estimate from its abstract, so it casts no vote on the map. Cited by 6 papers.
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Who cites it
6 citing papers in PubMed.
- Two-Dimensional Spectroscopy of Open Quantum Systems: Nonequilibrium Green's Function Formulation.The journal of physical chemistry letters · 2025Article
- Large negative differential conductance and its transformation in a single radical molecule.Chemical science · 2024Article
- Single-Molecule Surface-Enhanced Raman Spectroscopy.Sensors (Basel, Switzerland) · 2022Review
- High spatial resolution nanoslit SERS for single-molecule nucleobase sensing.Nature communications · 2018Article
- Surface-Enhanced Raman Scattering in Molecular Junctions.Sensors (Basel, Switzerland) · 2017Review
- Unconventional molecule-resolved current rectification in diamondoid-fullerene hybrids.Nature communications · 2014Article
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5 authors.
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Abstract
Vibrational modes of molecules are fundamental properties determined by intramolecular bonding, atomic masses, and molecular geometry, and often serve as important channels for dissipation in nanoscale processes. Although single-molecule junctions have been used to manipulate electronic structure and related functional properties of molecules, electrical control of vibrational mode energies has remained elusive. Here we use simultaneous transport and surface-enhanced Raman spectroscopy measurements to demonstrate large, reversible, voltage-driven shifts of vibrational mode energies of C60 molecules in gold junctions. C60 mode energies are found to vary approximately quadratically with bias, but in a manner inconsistent with a simple vibrational Stark effect. Our theoretical model instead suggests that the mode shifts are a signature of bias-driven addition of electronic charge to the molecule. These results imply that voltage-controlled tuning of vibrational modes is a general phenomenon at metal-molecule interfaces and is a means of achieving significant shifts in vibrational energies relative to a pure Stark effect.
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