Multimodal nonlinear Raman microspectroscopy with ultrashort chirped laser pulses

We demonstrate the physical principles of multimodal nonlinear optical microspectroscopy, integrating methods of coherent and stimulated Raman scattering of ultrashort chirped laser pulses in a single optical scheme. Nonlinear phase distortions of ultrashort laser pulses are accurately compensated within a broad spectral range in this scheme to enable a high-spectral-resolution laser microspectroscopy that can reliably resolve groups of fingerprint molecular vibrations with close frequencies, thus facilitating an analysis of complex multicomponent systems.