Chemical imaging and microspectroscopy with spectral focusing coherent anti-Stokes Raman scattering.

We demonstrate two different coherent anti-Stokes Raman scattering (CARS) microscopy and microspectroscopy methods based on the spectral focusing mechanism. The first method uses strongly chirped broadband pulses from a single Ti:sapphire laser and generates CARS signals at the fingerprint region. Fast modulation of the time delay between the pump and Stokes laser pulses coupled with lock-in signal detection significantly reduces the nonresonant background and produces Raman-like CARS signals with a spectral resolution of 20 cm(-1). The second method generates CARS signals in the CH (carbon-hydrogen) stretching region with IR supercontinuum pulses from a photonic crystal fiber. The spectral resolution of 30 cm(-1) is achieved. Maximum entropy method is used to retrieve a Raman-equivalent CARS spectrum from lipid membranes. Chemical imaging and microspectroscopy are demonstrated with various samples.