A transition-amplitude based representation of heterodyne detected coherent anti-Stokes Raman signals is used to separate them into a parametric component that involves no change in the material and dissipative processes associated with various transitions between states. Qualitatively different contributions from the two processes are predicted for the signal generated by an overlapping narrow (picosecond) and broad-band (femtosecond) pulse.

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http://www.ncbi.nlm.nih.gov/pmc/articles/PMC2792328PMC
http://dx.doi.org/10.1063/1.3259653DOI Listing

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