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SnP$_2$S$_6$: A Promising Infrared Nonlinear Optical Crystal with Strong Non-Resonant Second Harmonic Generation and Phase-matchability

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Version 2 2023-06-08, 12:54
Version 1 2023-01-12, 15:27
posted on 2023-06-08, 12:54 authored by Jingyang He, Seng Huat Lee, Francesco Naccarato, Guillaume Brunin, Rui Zu, Yuanxi Wang, Leixin Miao, Huaiyu Wang, Nasim Alem, Geoffroy Hautier, Gian-Marco Rignanese, Zhiqiang Mao, Venkatraman Gopalan
High-power infrared laser systems with broadband tunability are of great importance due to their wide range of applications in spectroscopy and free-space communications. These systems require nonlinear optical (NLO) crystals for wavelength up/down conversion using sum/difference frequency generation, respectively. NLO crystals need to satisfy many competing criteria, including large nonlinear optical susceptibility, large laser induced damage threshold (LIDT), wide transparency range and phase-matchability. Here, we report bulk single crystals of SnP_2S_6 with a large non-resonant SHG coefficient of d33= 53 pm/V at 1550nm and a large LIDT of 350 GW/cm^2 for femtosecond laser pulses. It also exhibits a broad transparency range from 0.54 {\mu}m to 8.5{\mu}m (bandgap of ~2.3 eV) and can be both Type I and Type II phase-matched. The complete linear and SHG tensors are measured as well as predicted by first principles calculations, and they are in excellent agreement. A proximate double-resonance condition in the electronic band structure for both the fundamental and the SHG light is shown to enhance the non-resonant SHG response. Therefore, SnP2S6 is an outstanding candidate for infrared laser applications.



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