Avoidance of Cross-Phase Modulation in Femtosecond Stimulated Raman Scattering

Raman scattering has become a powerful method in analytic spectroscopy and label-free imaging to study the chemical composition of a sample. Especially coherent Raman scattering (CRS) techniques such as stimulated Raman scattering (SRS) and coherent anti-Stokes Raman scattering (CARS) are developed further and show a great potential, due to their amplified signal in comparison to spontaneous Raman scattering. In CRS the interaction of light pulses with molecular vibrations are investigated, typically resulting in a characteristic molecular spectrum. However, especially CARS spectra are effected by the non-resonant contribution to the Raman scattering signal, resulting in a non-specific background and a distortion of the lineshape. SRS is free of a non-resonant background but is affected by two-photon absorption, cross-phase modulation (XPM) [1], and thermal scattering (temperature-induced refractive index change) [2]. The resulting artefacts in SRS become relevant for high pulses energies and ultra-short pulses. One example, where high pulse energies and ultra-short pulses are needed, is the field of spatial resolution enhancement in CRS. All techniques to overcome the diffraction limit by Abbe are based on depleting one of the scattering resources, as for example the pump or probe photons [3]. High pulse energies in the order of up to 200-300 nJ are needed, leading to also unwanted spectral distortions through XPM [4].