SnP2S6: A Promising Infrared Nonlinear Optical Crystal with Strong Nonresonant Second Harmonic Generation and Phase-Matchability

He, Jingyang;Lee, Seng Huat;Naccarato, Francesco;Brunin, Guillaume;Gopalan, Venkatraman;et.al.
(2022) ACS Photonics — Vol. 9, n° 5, p. 1724-1732 (2022)

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Authors
  • He, Jingyangorcid-logoDepartment of Materials Science and Engineering, Pennsylvania State University, University Park, Pennsylvania 16802, United States
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  • Lee, Seng Huat2D Crystal Consortium, Materials Research Institute, Pennsylvania State University, University Park, Pennsylvania 16802, United States; Department of Physics, Pennsylvania State University, University Park, Pennsylvania 16802, United States
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  • Naccarato, FrancescoUCLouvain
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  • Brunin, GuillaumeUCLouvain
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  • Hautier, Geoffroyorcid-logoUCLouvain
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  • Rignanese, Gian-Marcoorcid-logoUCLouvain
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  • Gopalan, VenkatramanDepartment of Materials Science and Engineering, Department of Physics, and Department of Engineering Science and Mechanics, Pennsylvania State University, University Park, Pennsylvania 16802, United States
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Abstract
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, largelaser-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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He, J., Lee, S. H., Naccarato, F., Brunin, G., Zu, R., Wang, Y., Miao, L., Wang, H., Alem, N., Hautier, G., Rignanese, G.-M., Mao, Z., & Gopalan, V. (2022). SnP2S6: A Promising Infrared Nonlinear Optical Crystal with Strong Nonresonant Second Harmonic Generation and Phase-Matchability. ACS Photonics, 9(5), 1724-1732. https://doi.org/10.1021/acsphotonics.2c00131 (Original work published 2022)