Issue 36, 2022

Rational design via dual-site aliovalent substitution leads to an outstanding IR nonlinear optical material with well-balanced comprehensive properties

Abstract

The acquisition of a non-centrosymmetric (NCS) structure and achieving a nice trade-off between a large energy gap (Eg > 3.5 eV) and a strong second-harmonic generation (SHG) response (deff > 1.0 × benchmark AgGaS2) are two formidable challenges in the design and development of infrared nonlinear optical (IR-NLO) candidates. In this work, a new quaternary NCS sulfide, SrCdSiS4, has been rationally designed using the centrosymmetric SrGa2S4 as the template via a dual-site aliovalent substitution strategy. SrCdSiS4 crystallizes in the orthorhombic space group Ama2 (no. 40) and features a unique two-dimensional [CdSiS4]2− layer constructed from corner- and edge-sharing [CdS4] and [SiS4] basic building units (BBUs). Remarkably, SrCdSiS4 displays superior IR-NLO comprehensive performances, and this is the first report on an alkaline-earth metal-based IR-NLO material that breaks through the incompatibility between a large Eg (>3.5 eV) and a strong phase-matching deff (>1.0 × AgGaS2). In-depth mechanism explorations strongly demonstrate that the synergistic effect of distorted tetrahedral [CdS4] and [SiS4] BBUs is the main origin of the strong SHG effect and large birefringence. This work not only provides a high-performance IR-NLO candidate, but also offers a feasible chemical design strategy for constructing NCS structures.

Graphical abstract: Rational design via dual-site aliovalent substitution leads to an outstanding IR nonlinear optical material with well-balanced comprehensive properties

Supplementary files

Article information

Article type
Edge Article
Submitted
06 jul 2022
Accepted
23 aug 2022
First published
07 sep 2022
This article is Open Access

All publication charges for this article have been paid for by the Royal Society of Chemistry
Creative Commons BY license

Chem. Sci., 2022,13, 10725-10733

Rational design via dual-site aliovalent substitution leads to an outstanding IR nonlinear optical material with well-balanced comprehensive properties

H. Yang, M. Ran, S. Zhou, X. Wu, H. Lin and Q. Zhu, Chem. Sci., 2022, 13, 10725 DOI: 10.1039/D2SC03760B

This article is licensed under a Creative Commons Attribution 3.0 Unported Licence. You can use material from this article in other publications without requesting further permissions from the RSC, provided that the correct acknowledgement is given.

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