Journal
ACS PHOTONICS
Volume 9, Issue 5, Pages 1724-1732Publisher
AMER CHEMICAL SOC
DOI: 10.1021/acsphotonics.2c00131
Keywords
second harmonic generation; nonlinear optics; infrared nonlinear optical crystals; metal chalcogenides
Categories
Funding
- Air Force Office of Scientific Research Grant [FA9550-18-S-0003]
- National Science Foundation through the Penn State 2D Crystal Consortium-Materials Innovation Platform (2DCC-MIP) under NSF [DMR-1539916, DMR-2039351]
- NSF Materials Research Science and Engineering Center for Nanoscale Science [DMR2011839]
- Air Force Office of Scientific Research (AFOSR) [FA9550-18-1-0277]
- GAME MURI [10059059-PENN]
- F.R.S.-FNRS
- University of North Texas
- U.S. Department of Energy, Office of Science, Basic Energy Sciences [DE-SC0020145, DESC0012375]
- Walloon Region [1117545]
- Fond de la Recherche Scientifique de Belgique (F.R. S.-FNRS) [2.5020.11]
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This study reports the bulk single crystals of SnP2S6 with a large nonlinear optical susceptibility, a large laser-induced damage threshold, and a wide transparency range, making it an outstanding candidate for infrared laser applications.
High-power infrared laser systems with broad-band tunability are of greatimportance due to their wide range of applications in spectroscopy and free-spacecommunications. These systems require nonlinear optical (NLO) crystals for wavelengthup/down conversion using sum/difference frequency generation, respectively. NLO crystalsneed 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 SnP2S6with a large nonresonant SHG coefficient ofd33=53pmV-1at 1550 nm and a large LIDT of 350 GW cm-2for femtosecond laser pulses. Italso exhibits a broad transparency range from 0.54 to 8.5 mu m (bandgap of similar to 2.3 eV) and canbe both Type I and Type II phase-matched. The complete linear and SHG tensors aremeasured as well as predicted byfirst-principles calculations, and they are in excellentagreement. Two relativelyflat conduction bands in the electronic band structure are shown toenhance the nonresonant SHG response through a double resonance enhancement of thenonresonant optical response. Therefore, SnP2S6is an outstanding candidate for infrared laserapplications
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