TY - JOUR
T1 - Surface-Enhanced Spectroscopy for Higher-Order Light Scattering
T2 - A Combined Experimental and Theoretical Study of Second Hyper-Raman Scattering
AU - Simmons, Philip D.
AU - Turley, Hubert K.
AU - Silverstein, Daniel W.
AU - Jensen, Lasse
AU - Camden, Jon P.
N1 - Publisher Copyright:
© 2015 American Chemical Society.
PY - 2015/12/1
Y1 - 2015/12/1
N2 - 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.
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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U2 - 10.1021/acs.jpclett.5b02342
DO - 10.1021/acs.jpclett.5b02342
M3 - Article
AN - SCOPUS:84951859078
SN - 1948-7185
VL - 6
SP - 5067
EP - 5071
JO - Journal of Physical Chemistry Letters
JF - Journal of Physical Chemistry Letters
IS - 24
ER -