TY - JOUR
T1 - SnP2S6
T2 - A Promising Infrared Nonlinear Optical Crystal with Strong Nonresonant Second Harmonic Generation and Phase-Matchability
AU - He, Jingyang
AU - Lee, Seng Huat
AU - Naccarato, Francesco
AU - Brunin, Guillaume
AU - Zu, Rui
AU - Wang, Yuanxi
AU - Miao, Leixin
AU - Wang, Huaiyu
AU - Alem, Nasim
AU - Hautier, Geoffroy
AU - Rignanese, Gian Marco
AU - Mao, Zhiqiang
AU - Gopalan, Venkatraman
N1 - Publisher Copyright:
© 2022 American Chemical Society.
PY - 2022/5/18
Y1 - 2022/5/18
N2 - High-power infrared laser systems with broad-band 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 SnP2S6 with a large nonresonant SHG coefficient of d33 = 53 pm V−1 at 1550 nm and a large LIDT of 350 GW cm−2 for femtosecond laser pulses. It also exhibits a broad transparency range from 0.54 to 8.5 μm (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. Two relatively flat conduction bands in the electronic band structure are shown to enhance the nonresonant SHG response through a double resonance enhancement of the nonresonant optical response. Therefore, SnP2S6 is an outstanding candidate for infrared laser applications.
AB - High-power infrared laser systems with broad-band 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 SnP2S6 with a large nonresonant SHG coefficient of d33 = 53 pm V−1 at 1550 nm and a large LIDT of 350 GW cm−2 for femtosecond laser pulses. It also exhibits a broad transparency range from 0.54 to 8.5 μm (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. Two relatively flat conduction bands in the electronic band structure are shown to enhance the nonresonant SHG response through a double resonance enhancement of the nonresonant optical response. Therefore, SnP2S6 is an outstanding candidate for infrared laser applications.
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U2 - 10.1021/acsphotonics.2c00131
DO - 10.1021/acsphotonics.2c00131
M3 - Article
AN - SCOPUS:85130189959
SN - 2330-4022
VL - 9
SP - 1724
EP - 1732
JO - ACS Photonics
JF - ACS Photonics
IS - 5
ER -