Coherent Raman scattering techniques as coherent anti-Stokes Raman scattering (CARS), offer significant advantages in terms of pixel dwell times and speed as compared to spontaneous Raman scattering for investigations of crystalline materials. However, the spectral information in CARS is often hampered by the presence of a nonresonant contribution to the scattering process that shifts and distorts the Raman peaks. In this work, we apply a method to obtain nonresonant background-free spectra based on time-delayed, broadband CARS (TD-BCARS) using an intrapulse excitation scheme. In particular, this method can measure the phononic dephasing times across the full phonon spectrum at once. We test the methodology on amorphous ${\mathrm{SiO}}_2$ (glass), which is used to characterize the setup-specific and material-independent response times, and then apply TD-BCARS to the analysis of single crystals of diamond and ferroelectrics of potassium titanyl phosphate (KTP) and potassium titanyl arsenate (KTA). For diamond, we determine a dephasing time of $\tau =7.81$ ps for the single ${sp}^3$ peak.

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• Nonlinear optical susceptibility
• Nonlinear optics
• Phonons
• Raman spectroscopy
• Spectroscopy