Shooting short-wavelength nonlinear optical materials with targeted balance performances in hydroxyborates through first-principles high-throughput screening†

Aiming to discover short-wavelength ultraviolet (UV) excellent nonlinear optical (NLO) materials, we used the first-principles high-throughput screening pipeline for hydroxyborate NLO materials. We systematically assessed over 222 non-centrosymmetric (NCS) compounds from 718 hydroxyborates in the Inorganic Crystal Structure Database (ICSD), employing screening criteria based on band gaps, the shortest phase-matching (PM) wavelengths, and second harmonic generation (SHG) coefficients. Three crystals are identified as promising short-wavelength UV NLO materials, with their PM SHG capacity extending to the solar blind region (200–280 nm). Additionally, an investigation on the relationship among the birefringence, the dimensionality of the B–O/OH anionic framework, and the (A + OH)/B (where A represents metal cations) ratio was conducted on screened hydroxyborates to illuminate the exploration of hydroxyborates with desirable short PM wavelengths for NLO properties.