Surface-Enhanced Femtosecond Stimulated Raman Spectroscopy at 1 MHz Repetition Rates

Lauren E. Buchanan, Natalie L. Gruenke, Michael O. McAnally, Bogdan Negru, Hannah E. Mayhew, Vartkess A. Apkarian, George C. Schatz, Richard P. Van Duyne*

*Corresponding author for this work

Research output: Contribution to journalArticlepeer-review

22 Scopus citations


Surface-enhanced femtosecond stimulated Raman spectroscopy (SE-FSRS) is an ultrafast Raman technique that combines the sensitivity of surface-enhanced Raman scattering with the temporal resolution of femtosecond stimulated Raman spectroscopy (FSRS). Here, we present the first successful implementation of SE-FSRS using a 1 MHz amplified femtosecond laser system. We compare SE-FSRS and FSRS spectra measured at 1 MHz and 100 kHz using both equal pump average powers and equal pump energies to demonstrate that higher repetition rates allow spectra with higher signal-to-noise ratios to be obtained at lower pulse energies, a significant advance in the implementation of SE-FSRS. The ability to use lower pulse energies significantly mitigates sample damage that results from plasmonic enhancement of high-energy ultrafast pulses. As a result of the improvements to SE-FSRS developed in this Letter, we believe that SE-FSRS is now poised to become a powerful tool for studying the dynamics of plasmonic materials and adsorbates thereon.

Original languageEnglish (US)
Pages (from-to)4629-4634
Number of pages6
JournalJournal of Physical Chemistry Letters
Issue number22
StatePublished - Nov 17 2016

ASJC Scopus subject areas

  • General Materials Science
  • Physical and Theoretical Chemistry


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