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Na2Hg3M2S8 (M = Si, Ge, and Sn): New Infrared Nonlinear Optical Materials with Strong Second Harmonic Generation Effects and High Laser-Damage Thresholds

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Key Laboratory of Functional Materials and Devices for Special Environments of CAS; Xinjiang Key Laboratory of Electronic Information Materials and Devices; Xinjiang Technical Institute of Physics & Chemistry of CAS, 40-1 South Beijing Road, Urumqi 830011, China
*E-mail: [email protected]. Phone: (+86)991-3674558. Fax: (+86)991-3838957.
Cite this: Chem. Mater. 2016, 28, 8, 2795–2801
Publication Date (Web):April 5, 2016
https://doi.org/10.1021/acs.chemmater.6b00683
Copyright © 2016 American Chemical Society
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Abstract

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A new family of noncentrosymmetric isostructural compounds, Na2Hg3M2S8 (M = Si, Ge, and Sn), was successfully synthesized. They crystallize in the tetragonal space group P4̅c2 with Z = 2. Their major structures are composed of infinite cross-connected ∞(HgS3)n chains and isolated [MS4] ligands and show the interesting tunnel features. Interestingly, compared with the structures of A2Hg3M2S8 (A = alkali metal, Na–Cs), it can be found that the structural symmetries show a gradually rising tendency from Cs to Na analogues as a result of cation size effect, which rarely exists in quaternary alkali metal chalcogenides. Property measurements show that title compounds exhibit strong second harmonic generation (SHG) effects with a phase-matching behavior at 2.09 μm, wide transparency range in the infrared (IR) region, and large laser-damage thresholds (LDTs). Remarkably, Na2Hg3Si2S8 and Na2Hg3Ge2S8 achieve the suitable balance between large SHG effects (1.3 and 2.2 × benchmark AgGaS2) and high LDTs (4.5 and 3 × AgGaS2), respectively, and can be expected to be potential nonlinear optical (NLO) candidates in the IR region. Moreover, band structures and NLO properties of title compounds are also theoretically studied, and the calculated NLO coefficients are consistent with the experimental observations.

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The Supporting Information is available free of charge on the ACS Publications website at DOI: 10.1021/acs.chemmater.6b00683.

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