Origin of negative and dispersive features in anti-Stokes and resonance femtosecond stimulated Raman spectroscopy

The Journal of Chemical Physics
Renee R FrontieraRichard A Mathies

Abstract

Femtosecond stimulated Raman spectroscopy is extended to probe ground state anti-Stokes vibrational features. Off resonance, negative anti-Stokes features are seen that are the mirror image of the positive Stokes side spectra. On resonance, the observed dispersive lineshapes are dramatically dependent on the frequencies of the picosecond pump and femtosecond probe pulses used to generate the stimulated Raman spectra. These observations are explained by the contributions of the inverse Raman and hot luminescence four-wave mixing processes discussed by Sun et al. [J. Chem. Phys. 128, 144114 (2008)], which contribute to the overall femtosecond stimulated Raman signal.

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Citations

Feb 27, 2010·Proceedings of the National Academy of Sciences of the United States of America·Saar Rahav, Shaul Mukamel
Feb 6, 2014·Physical Chemistry Chemical Physics : PCCP·Hyung Min KimYung Doug Suh
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Nov 30, 2019·The Journal of Chemical Physics·Chong FangCheng Chen
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