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Centric-to-acentric structure transformation induced by a stereochemically active lone pair: a new insight for design of IR nonlinear optical materials

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Abstract

For second-order nonlinear optical (NLO) responses, such as second-harmonic-generation (SHG), a strict non-centrosymmetric (NCS) structure is the paramount precondition. In this work, a quaternary IR–NLO semiconductor, La2CuSbS5, has been designed by a stereochemically active lone pair induction (SALPI) strategy, with inspiration from the known centrosymmetric (CS) La2CuInS5 and was successfully obtained by a solid-state reaction using CsBr–BaCl2 as the flux. It adopts the orthorhombic Ima2 space group (no. 46), and the remarkable structure features a 3D NCS network built by a unique teeter-totter (SbS4)n chain motif and isolated [CuS4] tetrahedra. The NLO experiments indicated that La2CuSbS5 possesses a phase-matching (PM) behavior with relatively strong SHG (0.5 × commercial AgGaS2) and a large laser-induced damage threshold (LIDT = 6.7 × commercial AgGaS2). In addition, theoretical studies and analyses of the cutoff-energy-dependent dij coefficient were conducted and discussed to further understand the structure–property relationship. Moreover, the [SbS4] tetrahedral building units play a pivotal role in the polarity of the crystal, based on the results of an analysis of the local dipole moment. All these results offer a new route to designing and discovering new IR–NLO materials.

Graphical abstract: Centric-to-acentric structure transformation induced by a stereochemically active lone pair: a new insight for design of IR nonlinear optical materials

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Publication details

The article was received on 02 Feb 2019, accepted on 19 Feb 2019 and first published on 19 Feb 2019


Article type: Communication
DOI: 10.1039/C9TC00647H
Citation: J. Mater. Chem. C, 2019, Advance Article

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    Centric-to-acentric structure transformation induced by a stereochemically active lone pair: a new insight for design of IR nonlinear optical materials

    H. Lin, Y. Li, M. Li, Z. Ma, L. Wu, X. Wu and Q. Zhu, J. Mater. Chem. C, 2019, Advance Article , DOI: 10.1039/C9TC00647H

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