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

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• 作者：Philip D. Simmons Jr. ; Hubert K. Turley ; Daniel W. Silverstein ; Lasse Jensen ; Jon P. Camden
• 刊名：The Journal of Physical Chemistry Letters
• 出版年：2015
• 出版时间：December 17, 2015
• 年：2015
• 卷：6
• 期：24
• 页码：5067-5071
• 全文大小：343K
• ISSN：1948-7185

文摘

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 10p>5p> 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.