Superior infrared nonlinear optical (NLO) crystals are in urgent demand in thedevelopment of lasers and optical technologies for communications andcomputing. The critical challenge is to find a crystal with large non-resonantphase-matchable NLO coefficients and high laser damage threshold (LDTs)simultaneously, which however scale inversely. This work reports such amaterial, MgSiP2,that exhibits a large second harmonic generation (SHG)coefficient ofd14≈d36=89±5pmV−1at 1550 nm fundamental wavelength,surpassing the commercial NLO crystals AgGaS2, AgGaSe2, and ZnGeP2.First principles theory reveals the polarizability and geometric arrangement ofthe [SiP4] tetrahedral units as the origin of this large nonlinear response.Remarkably, it also exhibits a high LDT value of 684 GW cm−2, which is sixtimes larger than ZnGeP2and three times larger than CdSiP2. It has a widetransparency window of 0.53–10.35μm, allowing broadband tunability.Further, it is Type I and Type II phase-matchable with large effective SHGcoefficients ofdeff,I≈80.2 pm V−1anddeff,II≈73.4 pm V−1. The outstandingproperties of MgSiP2make it a highly attractive candidate for opticalfrequency conversion in the infrared.
He, J., Guan, Y., Trinquet, V., Brunin, G., Wang, K., Robinson, R., Zu, R., Yoshida, S., Lee, S. H., Wang, Y., Zhu, Y., Rignanese, G.-M., Mao, Z., & Gopalan, V. (2023). MgSiP2: An Infrared Nonlinear Optical Crystal with a Large Non‐Resonant Phase‐Matchable Second Harmonic Coefficient and High Laser Damage Threshold. Advanced Optical Materials, 2301060. https://doi.org/10.1002/adom.202301060 (Original work published 2023)