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Broadband coherent anti-Stokes Raman scattering (BCARS) is an advanced Ramanspectroscopy method that combines the spectral sensitivity of spontaneous Ramanscattering (SR) with the increased signal intensity of single-frequencycoherent Raman techniques. These two features make BCARS particularly suitablefor ultra-fast imaging of heterogeneous samples, as already shown inbiomedicine. Recent studies demonstrated that BCARS also shows exceptionalspectroscopic capabilities when inspecting crystalline materials like lithiumniobate and lithium tantalate, and can be used for fast imaging offerroelectric domain walls. These results strongly suggest the extension ofBCARS towards new imaging applications like mapping defects, strain, or dopantlevels, similar to standard SR imaging. Despite these advantages, BCARS suffersfrom a spurious and chemically unspecific non-resonant background (NRB) thatdistorts and shifts the Raman peaks. Post-processing numerical algorithms arethen used to remove the NRB and to obtain spectra comparable to SR results.Here, we show the reproducibility of BCARS by conducting an internal RoundRobin with two different BCARS experimental setups, comparing the results ondifferent crystalline materials of increasing structural complexity: diamond,6H-SiC, KDP, and KTP. First, we compare the detected and phase-retrievedsignals, the setup-specific NRB-removal steps, and the mode assignment.Subsequently, we demonstrate the versatility of BCARS by showcasing how theselection of pump wavelength, pulse width, and detection geometry can betailored to suit the specific objectives of the experiment. Finally, we compareand optimize measurement parameters for the high-speed, hyperspectral imagingof ferroelectric domain walls in lithium niobate.

Comparing Transmission- and Epi-BCARS: A Transnational Round Robin on Solid State Materials