Coherent Raman scattering (CRS) is a popular technique for ultrafast spectroscopy and microscopy studies. CRS is based on a third-order nonlinear light-matter interaction, characterized by a nonlinear susceptibility with nonzero elements for bulk samples. It is challenging to perform CRS measurements at interfaces, as bulk contributions can often overwhelm. We have developed a surface-sensitive approach for CRS spectroscopy and microscopy, which enhances the sensitivity to interfacial processes by at least tenfold.

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Eric O. Potma and John Kenison, "Coherent Raman scattering at interfaces (Conference Presentation)," Proc. SPIE 10753, Ultrafast Nonlinear Imaging and Spectroscopy VI, 1075305 (Presented at SPIE Optical Engineering + Applications: August 19, 2018; Published: 17 September 2018); https://doi.org/10.1117/12.2322636.5836064704001.