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

doi:10.1021/acs.jpclett.5b02342

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 journal › Article › peer-review

19 Scopus citations

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 language	English (US)
Pages (from-to)	5067-5071
Number of pages	5
Journal	Journal of Physical Chemistry Letters
Volume	6
Issue number	24
DOIs	https://doi.org/10.1021/acs.jpclett.5b02342
State	Published - Dec 1 2015

All Science Journal Classification (ASJC) codes

Materials Science(all)
Physical and Theoretical Chemistry

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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.",

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AU - Jensen, Lasse

AU - Camden, Jon P.

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AB - 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.

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

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