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Experimental and theoretical studies on the NLO properties of two quaternary non-centrosymmetric chalcogenides: BaAg 2 GeS 4 and BaAg 2 SnS 4 .
- Source :
-
Dalton transactions (Cambridge, England : 2003) [Dalton Trans] 2018 Jan 02; Vol. 47 (2), pp. 429-437. - Publication Year :
- 2018
-
Abstract
- New middle and far-infrared (MFIR) nonlinear optical (NLO) chalcogenides have been receiving increasing attention for their great importance in military and civil fields. In addition, the current challenge in the efforts for identifying a promising MFIR NLO material lies in achieving simultaneously large second-harmonic generation (SHG) intensity and high laser-induced damage threshold (LIDT) in the same material. In this study, two quaternary non-centrosymmetric (NCS) sulfides, BaAg <subscript>2</subscript> GeS <subscript>4</subscript> (1) and BaAg <subscript>2</subscript> SnS <subscript>4</subscript> (2), were synthesized from a high-temperature solid-state reaction using BaCl <subscript>2</subscript> flux in evacuated closed silica tubes. Although 1 and 2 show identical stoichiometry, they crystallize in different NCS space groups, tetragonal I4[combining macron]2m (no. 121) and orthorhombic I222 (no. 23), respectively, based on the results of crystal structure solution. In their structures, highly distorted AgS <subscript>4</subscript> tetrahedra interconnect together via corner-sharing to form two-dimensional (2D) layers, which are further bridged with isolated GeS <subscript>4</subscript> or SnS <subscript>4</subscript> units to produce a three-dimensional (3D) framework structure with Ba cations lying in the tunnels. Remarkably, they not only possess phase-matchable (PM) abilities but also exhibit a good balance between strong SHG responses (1.7× and 0.4× AgGaS <subscript>2</subscript> ) and high LIDTs (3.2× and 1.5× AgGaS <subscript>2</subscript> ). Moreover, theoretical calculations based on density functional theory (DFT) methods have aided the understanding of energy bands, electronic structures, and linear and NLO properties.
Details
- Language :
- English
- ISSN :
- 1477-9234
- Volume :
- 47
- Issue :
- 2
- Database :
- MEDLINE
- Journal :
- Dalton transactions (Cambridge, England : 2003)
- Publication Type :
- Academic Journal
- Accession number :
- 29220054
- Full Text :
- https://doi.org/10.1039/c7dt04178k