$\chi^{(2)}$-induced artifact overwhelming the third-order signal in 2D Raman–THz spectroscopy of non-centrosymmetric materials

Through comprehensive data analysis, we demonstrate that a χ(2)-induced artifact, arising from imperfect balancing in the conventional electro-optic sampling detection scheme, contributes significantly to the measured signal in 2D Raman–THz spectroscopy of non-centrosymmetric materials. The artifact is a product of two 1D responses, overwhelming the desired 2D response. We confirm that by analyzing the 2D Raman–THz response of an x-cut beta barium borate crystal. We furthermore show that this artifact can be effectively suppressed by implementing a special detection scheme. We successfully isolate the desired third-order 2D Raman–THz response, revealing a distinct cross-peak feature, whose frequency position suggests the coupling between two crystal phonons.