Issue 43, 2021

Aliovalent-cation-substitution-induced structure transformation: a new path toward high-performance IR nonlinear optical materials

Abstract

Non-centrosymmetric (NCS) structure is the precondition and foundation for the development of high-performance nonlinear optical (NLO) crystals. In this research, a quaternary NCS thioantimonate, K2Ag3Sb3S7, is designed through an aliovalent-cation-substitution-induced strategy based on the centrosymmetric (CS) parent compound K2Sb4S7 and successfully obtained through a facile surfactant-thermal technology. The unique crystal structure of K2Ag3Sb3S7 belongs to the orthorhombic space group Cmc21 (no. 36) and is made of charge-balanced K+ cations and two-dimensional (2D) anionic layers [Ag3Sb3S7]2− constructed by the vertex-sharing of [Ag3SbS5]4− and [SbS2] chains. Remarkably, K2Ag3Sb3S7 not only possesses a phase-matching (PM) ability in the IR region, but also displays a perfect balance between a high second-harmonic-generation (SHG) coefficient (1.5 × commercial AgGaS2) and a large laser-induced damage threshold (3.2 × commercial AgGaS2). Moreover, theoretical studies uncover that the synergistic effects of three types of asymmetric building motifs (i.e., [SbS3], [Sb2S5] and [Ag3S6]) contribute to the large SHG effect and birefringence (Δn). This study not only demonstrates that aliovalent cation substitution can be a robust means of obtaining the NCS thioantimonates but also provides a deeper insight into the structure–property relationship of IR-NLO chalcogenides.

Graphical abstract: Aliovalent-cation-substitution-induced structure transformation: a new path toward high-performance IR nonlinear optical materials

Supplementary files

Article information

Article type
Communication
Submitted
20 Ndz 2021
Accepted
15 Nhl 2021
First published
15 Nhl 2021

J. Mater. Chem. C, 2021,9, 15407-15414

Aliovalent-cation-substitution-induced structure transformation: a new path toward high-performance IR nonlinear optical materials

C. Liu, S. Zhou, Y. Xiao, C. Zhang, H. Lin and Y. Liu, J. Mater. Chem. C, 2021, 9, 15407 DOI: 10.1039/D1TC04498B

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