Single molecule SERS spectral blinking and vibronic coupling

John R. Lombardi, Ronald L. Birke, Gilad Haran

Research output: Contribution to journalArticlepeer-review

Abstract

We examine the time evolution of spectral blinking behavior of single molecule surface-enhanced Raman spectra (SERS). For the molecules examined, it is found that the on-off behavior of the spectral lines is not always in tandem and that the spectral lines can be divided into subsets with separate tandem blinking behavior. One group, despite fluctuating somewhat, is relatively steady in intensity, until they either abruptly or sometimes more gradually disappear. A second group, blinks more sharply, on briefly or off for a longer period. They appear more erratically and often are more intense while on. The former set of lines are found to obtain most of their intensity through Franck-Condon terms in the polarizability expression, while lines for which the Raman intensity is correlated with vibronic coupling tend to blink with sharper on-off differences. We interpret these observations in terms of the theory of vibronic coupling as applied to SERS.

Original languageEnglish
Pages (from-to)4540-4545
Number of pages6
JournalJournal of Physical chemistry c
Volume115
Issue number11
DOIs
StatePublished - 24 Mar 2011

All Science Journal Classification (ASJC) codes

  • Electronic, Optical and Magnetic Materials
  • General Energy
  • Surfaces, Coatings and Films
  • Physical and Theoretical Chemistry

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