Tip-enhanced Raman spectroscopy with picosecond pulses

Jordan M. Klingsporn, Matthew D. Sonntag, Tamar Seideman, Richard P. Van Duyne*

*Corresponding author for this work

Research output: Contribution to journalArticlepeer-review

36 Scopus citations

Abstract

Tip-enhanced Raman spectroscopy (TERS) can probe chemistry occurring at surfaces with both nanometer spectroscopic and submolecular spatial resolution. Combining ultrafast spectroscopy with TERS allows for picosecond and, in principle, femtosecond temporal resolution. Here we couple an optical parametric oscillator (OPO) with a scanning tunneling microscopy (STM)-TERS microscope to excite the tip plasmon with a picosecond excitation source. The plasmonic tip was not damaged with OPO excitation, and TER spectra were observed for two resonant adsorbates. The TERS signal under ultrafast pulsed excitation decays on the time scale of 10 s of seconds; whereas with continuous-wave excitation no decay occurs. An analysis of possible decay mechanisms and their temporal characteristics is given.

Original languageEnglish (US)
Pages (from-to)106-110
Number of pages5
JournalJournal of Physical Chemistry Letters
Volume5
Issue number1
DOIs
StatePublished - Jan 2 2014

Keywords

  • kinetics
  • picosecond excitation
  • plasmonics
  • tip-enhanced raman spectroscopy
  • ultrafast raman spectroscopy

ASJC Scopus subject areas

  • Materials Science(all)
  • Physical and Theoretical Chemistry

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