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

IF 8 2区 材料科学 Q1 MATERIALS SCIENCE, MULTIDISCIPLINARY
Jadupati Nag, Saugata Sarker, Safdar Imam, Abishek Iyer, Michael J. Waters, Albert Suceava, James M. Rondinelli, Mercouri G. Kanatzidis, Venkatraman Gopalan
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Abstract

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.

Abstract Image

范德华半导体块状晶体中红外大非谐振二次谐波的产生,SnP2Se6
二维范德华(vdW)材料已成为非线性光学(NLO)应用中非常有前途的候选者。本研究介绍了一种新型二维vdW半导体SnP2Se6的合成、综合线性光学和光学二次谐波产生(SHG)特性。在2µm基波长处,其间接带隙约为1.47 eV,非谐振SHG系数约为d33 ~−222±30 pm V−1,是具有类似带隙的商用AgGaSe2的约7倍。密度泛函理论(DFT)计算的线性和非线性光学性质与实验测量结果基本一致,揭示了增强性质的化学来源。此外,SnP2Se6可以在宽光谱范围内表现出i型和ii型相匹配,满足理想NLO晶体的关键标准之一。这些特殊的性质使SnP2Se6成为NLO应用中非常有前途的候选者。
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来源期刊
Advanced Optical Materials
Advanced Optical Materials MATERIALS SCIENCE, MULTIDISCIPLINARY-OPTICS
CiteScore
13.70
自引率
6.70%
发文量
883
审稿时长
1.5 months
期刊介绍: Advanced Optical Materials, part of the esteemed Advanced portfolio, is a unique materials science journal concentrating on all facets of light-matter interactions. For over a decade, it has been the preferred optical materials journal for significant discoveries in photonics, plasmonics, metamaterials, and more. The Advanced portfolio from Wiley is a collection of globally respected, high-impact journals that disseminate the best science from established and emerging researchers, aiding them in fulfilling their mission and amplifying the reach of their scientific discoveries.
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