Abstract

Borate crystals are traditional nonlinear optical (NLO) materials with superior properties: a wide transparency range, large NLO coefficients, and high resistance to laser damage. More recently, their higher-order nonlinearity, namely cubic nonlinearities ($\chi _{{ijkl}}^{(3)}$), is getting noticed for applications in supercontinuum generation, producing extra-short, few-circle laser pulses, limiting the Gauss pulse to a flat-top shape and directly generating efficient third harmonic generation. The lack of knowledge of the individual tensor element of $\chi _{{ijkl}}^{(3)}$ hinders the optimization of the efficiency of the high-order process, which in principle is a much weaker optic field–matter interaction. Using a recent released CRYSTAL code based on a coupled perturbed Kohn–Sham approximation and a linear combination of atomic orbitals approach, the most important properties of the band gaps, and linear and nonlinear properties of well-known borate and related crystals are calculated. For most of them, the full tensor elements of the calculated cubic nonlinear coefficients $\chi _{{ijkl}}^{(3)}$ are obtained for the first time, to the best of my knowledge. The full knowledge of $\chi _{{ijkl}}^{(3)}$ of each optical crystal may serve as the basis for their use as third harmonic generation (THG) materials and help researchers find promising new THG materials for increasingly important applications in the control of optic field–matter interactions.

© 2021 Optical Society of America

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