Large Non‐Resonant Infrared Optical Second Harmonic Generation in Bulk Crystals of Van der Waals Semiconductor, SnP2Se6

Nag, Jadupati; Sarker, Saugata; Imam, Safdar; Iyer, Abishek; Waters, Michael J.; Suceava, Albert; Rondinelli, James M.; Kanatzidis, Mercouri G.; Gopalan, Venkatraman

doi:10.1002/adom.202402649

Large Non‐Resonant Infrared Optical Second Harmonic Generation in Bulk Crystals of Van der Waals Semiconductor, SnP₂Se₆

Journal Article · Fri Mar 07 00:00:00 EST 2025 · Advanced Optical Materials

DOI:https://doi.org/10.1002/adom.202402649· OSTI ID:2997501

^[1]; ^[2]; Imam, Safdar ^[3]; ^[3]; ^[3]; Suceava, Albert ^[1]; ^[3]; ^[3]; ^[1]

Pennsylvania State University, University Park, PA (United States)
Department of Materials Science and Engineering Materials Research Institute Pennsylvania State University Millennium Science Complex Building University Park PA 16802 USA
Northwestern University, Evanston, IL (United States)

2D van der Waals (vdW) materials have emerged as a highly promising candidates for nonlinear optical (NLO) applications. This study presents the synthesis, comprehensive linear optical, and optical second harmonic generation (SHG) characterization of a novel 2D vdW semiconductor SnP2Se6 in its bulk single crystal form. It exhibits an indirect bandgap of ≈1.47 eV and an exceptional non-resonant SHG coefficient of d₃₃ ∼ −222 ± 30 pm V⁻¹ at a fundamental wavelength of 2 µm, which is ≈7 times larger than that of the commercial AgGaSe₂ with a comparable bandgap. Density functional theory (DFT) calculations of the linear and nonlinear optical properties exhibit reasonable agreement with the experimental measurements, revealing the chemical origin of the enhanced properties. Moreover, SnP₂Se₆ can exhibit both type-I and type-II phase matching over a wide spectral range, fulfilling one of the key criteria for an ideal NLO crystal. These exceptional properties position SnP₂Se₆ as a highly promising candidate for NLO applications.

View Accepted Manuscript (DOE)

Research Organization:: Pennsylvania State University, University Park, PA (United States)

Sponsoring Organization:: Air Force Office of Scientific Research (AFOSR); National Energy Research Scientific Computing Center (NERSC); National Science Foundation (NSF); USDOE Office of Science (SC), Basic Energy Sciences (BES). Scientific User Facilities (SUF)

Grant/Contract Number:: AC02-05CH11231; SC0021118

OSTI ID:: 2997501

Journal Information:: Advanced Optical Materials, Journal Name: Advanced Optical Materials Journal Issue: 9 Vol. 13; ISSN 2195-1071

Publisher:: WileyCopyright Statement

Country of Publication:: United States

Language:: English

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Large Non‐Resonant Infrared Optical Second Harmonic Generation in Bulk Crystals of Van der Waals Semiconductor, SnP2Se6

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