Quantitative multiplex CARS spectroscopy in congested spectral regions

A novel procedure is developed to describe and reproduce experimental coherent anti-Stokes Raman scattering (CARS) data, with particular emphasis on highly congested spectral regions. The approach - exemplified here with high-quality multiplex CARS data - makes use the maximum entropy method for phase retrieval. The retrieved imaginary part of the nonlinear susceptibility is shown to be equal to the spontaneous Raman spectrum. The phase retrieval procedure does not influence the noise contained in the spectra. The conversion of CARS to Raman data permits a quantitative interpretation of CARS spectra. This novel approach is demonstrated for highly congested multiplex CARS spectra of sucrose, fructose and glucose. This novel procedures enables extraction of vibrational information from multiplex CARS data without the use of a priori information of the sample.