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

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

Research output: Contribution to journalArticlepeer-review

11 Scopus citations

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, 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.

Original languageEnglish (US)
Pages (from-to)1724-1732
Number of pages9
JournalACS Photonics
Volume9
Issue number5
DOIs
StatePublished - May 18 2022

All Science Journal Classification (ASJC) codes

  • Electronic, Optical and Magnetic Materials
  • Biotechnology
  • Atomic and Molecular Physics, and Optics
  • Electrical and Electronic Engineering

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