Three-pulse multiplex coherent anti-Stokes/Stokes Raman scattering (CARS/CSRS) microspectroscopy using a white-light laser source

We have developed a three-pulse non-degenerate multiplex coherent Raman microspectroscopic system using a white-light laser source. The fundamental output (1064 nm) of a Nd:YAG laser is used for the pump radiation with the white-light laser output (1100–1700 nm) for the Stokes radiation to achieve broadband multiplex excitations of vibrational coherences. The second harmonic (532 nm) of the same Nd:YAG laser is used for the probe radiation. Thanks to the large wavelength difference between the pump and probe radiations, coherent anti-Stokes Raman scattering (CARS) and coherent Stokes Raman scattering (CSRS) can be detected simultaneously. Simultaneous detection of CARS and CSRS enables us to obtain information on the electronic resonance effect that affects differently the CARS and CSRS signals. Simultaneous analysis of the CARS and CSRS signals provides us the imaginary part of χ(3) without introducing any arbitrary parameter in the maximum entropy method (MEM)