Surface-Enhanced Spectroscopy for Higher-Order Light Scattering: A Combined Experimental and Theoretical Study of Second Hyper-Raman Scattering

Philip D. Simmons, Hubert K. Turley, Daniel W. Silverstein, Lasse Jensen, Jon P. Camden

Research output: Contribution to journalArticle

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Abstract

Motivated to explore the ultimate limits of surface-enhanced nonlinear spectroscopies, we report on the first observation of molecular second hyper-Raman scattering with the aid of surface enhancement and provide a new theoretical framework for first-principles calculations of the second hyper-Raman effect. Second hyper-Raman enhancement factors, determined to be a minimum of 105 times stronger than those in Raman scattering, demonstrate a clear trend toward larger enhancements for nonlinear phenomena, and the nearly quantitative agreement between simulation and experiment provides a unique spectroscopic window into higher-order molecular responses.

Original languageEnglish (US)
Pages (from-to)5067-5071
Number of pages5
JournalJournal of Physical Chemistry Letters
Volume6
Issue number24
DOIs
StatePublished - Dec 1 2015

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All Science Journal Classification (ASJC) codes

  • Materials Science(all)

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