We introduced, characterized, and developed instrumentation and spectral processing methods of the two-beam, 3-color broadband coherent Raman approach. The procedure applied for molecular vibrational measurements over the low-frequency spectral domain. We reported the results in our former article [1]. An extended polarization study of the third-order susceptibility revealed an effective non-resonant signal elimination in the vibrational spectra of isotropic and anisotropic samples, such as liquids and crystals [2]. Simultaneous recording of the Stokes and anti-Stokes signals made the spectral processing trustworthy. In the presentation, we will explain the challenges of the technical implementation of the method in ultrafast laser systems and the underlying physics.

[1] Laszlo Ujj, “Contribution to the development of low-frequency terahertz coherent Raman micro-spectroscopy and microscopy”, Spectrochimica Acta Part A: Molecular and Biomolecular Spectroscopy 199, (2018) 448-454.

[2] Laszlo Ujj, Trevor Olsson, Benny Schundelmier, Trevor Bestor, “Effective Polarization Suppression in Two-Beam 3-color Broadband Coherent Raman Micro-Spectroscopy (3CBCRS)”, Vibrational Spectroscopy 108 (2020) 103056.