Traditional infrared (IR) nonlinear optical (NLO) materials such as AgGaS 2 are crucial to key devices for solid-state lasers, however, low laser damage thresholds intrinsically hinder their practical application. Here, a robust strategy is proposed for unbiased highthroughput screening of more than 140 000 materials to explore novel IR NLO materials with high thermal conductivity and wide band gap which are crucial to intrinsic laser damage threshold. Via our strategy, 106 compounds with desired band gaps, NLO coefficients and thermal conductivity are screened out, including 8 nitrides, 68 chalcogenides, in which Sr 2 SnS 4 is synthesized to verify the reliability of our process. Remarkably, thermal conductivity of nitrides is much higher than that of chalcogenides, e.g., 5 × AgGaS 2 (5.13 W/m K) for ZrZnN 2 , indicating that nitrides could be a longneglected system for IR NLO materials. This strategy provides a powerful tool for searching NLO compounds with high thermal conductivity.
Fluorine-containing compounds have stimulated the exploration
of
ultraviolet/deep-ultraviolet nonlinear optical (NLO) materials. Alkali/alkaline-earth
metal phosphates are one of the important potential systems as NLO
materials, while the common small birefringence limits the phase-matching
(PM) ability in the ultraviolet/deep-ultraviolet region. Herein, by
applying a “fluorination synergy-induced enhancement of optical
property” strategy, novel structures of phosphate fluoride/fluorophosphate
in BePO3F with good thermodynamic/dynamic stability and
promising NLO-related properties are discovered via performing crystal
structure prediction combined with first-principles calculations.
BePO3F-I–VI exhibit relatively large birefringence
of 0.025, 0.048, 0.049, 0.049, 0.059, and 0.063 at 1064 nm, respectively.
Simultaneously, BePO3F-I (Pc) is a new
thermodynamically stable phosphate fluoride which possesses a wide
band gap (E
g = 8.03 eV), large second-harmonic
generation (SHG) coefficient (d
11 = 0.67
pm/V, 1.7 × KDP), and the shortest PM wavelength of 292 nm. Other
five thermodynamically metastable noncentrosymmetric (NCS) BePO3F structures (II–VI) belong to fluorophosphates and
exhibit deep-ultraviolet PM wavelengths of 187, 183, 186, 188, and
196 nm. It reveals that the aligned nonbonding O 2p orbitals of [BeO2F2] and [PO4] units lead to a large
SHG coefficient in the phosphate fluoride BePO3F-I. For
fluorophosphates (BePO3F-II–VI), the synergy of
[BeO3] planar units and [PO3F] units induces
relatively large birefringence. Our research results provide an idea
for exploring novel high-performance NLO materials.
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