期刊
PROCEEDINGS OF THE NATIONAL ACADEMY OF SCIENCES OF THE UNITED STATES OF AMERICA
卷 111, 期 4, 页码 1282-1287出版社
NATL ACAD SCIENCES
DOI: 10.1073/pnas.1320210111
关键词
plasmonics; nanoscale junctions; molecular electronics
资金
- Robert A. Welch Foundation [C-1636]
- US Department of Energy, Office of Basic Energy Sciences, Materials Sciences and Engineering Division [DE-AC02-05CH11231]
- Office of Science, Office of Basic Energy Sciences
- US Department of Energy
- Israel Science Foundation
- Lise Meitner Center for Computational Chemistry
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 C-60 molecules in gold junctions. C-60 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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