Oxychalcogenides as Promising Ultraviolet Nonlinear Optical Candidates: Experimental and Theoretical Studies of AEGeOS2 (AE = Sr and Ba)

He-Di Yang; Sheng-Hua Zhou; Mao-Yin Ran; Xin-Tao Wu; Hua Lin; Qi-Long Zhu

doi:10.1021/acs.inorgchem.2c02798

Oxychalcogenides as Promising Ultraviolet Nonlinear Optical Candidates: Experimental and Theoretical Studies of AEGeOS₂ (AE = Sr and Ba)

Inorg Chem. 2022 Oct 3;61(39):15711-15720. doi: 10.1021/acs.inorgchem.2c02798. Epub 2022 Sep 21.

Authors

He-Di Yang^{1

2}, Sheng-Hua Zhou^{2

3}, Mao-Yin Ran^{2

3}, Xin-Tao Wu^{2

4}, Hua Lin^{1

4}, Qi-Long Zhu^{2

4}

Affiliations

¹ College of Chemistry, Fuzhou University, Fuzhou, Fujian 350002, China.
² State Key Laboratory of Structural Chemistry, Fujian Institute of Research on the Structure of Matter, Chinese Academy of Sciences, Fuzhou, Fujian 350002, China.
³ University of Chinese Academy of Sciences, Beijing 100049, China.
⁴ Fujian Science & Technology Innovation Laboratory for Optoelectronic Information of China, Fuzhou, Fujian 350108, China.

PMID: 36130922
DOI: 10.1021/acs.inorgchem.2c02798

Abstract

Oxychalcogenides have gained widespread attention as promising infrared nonlinear optical (IR-NLO) candidates. However, high-performance oxychalcogenides have rarely been reported in the ultraviolet (UV) region owing to the low energy gaps (E_g < 4.0 eV). Herein, two non-centrosymmetric (NCS) oxychalcogenides with one-dimensional (1D) chain structures and wide E_g (>4.3 eV), namely, AEGeOS₂ (AE = Sr and Ba), have been discovered by combined experiments and theory calculations as a new source of UV-NLO materials. Significantly, they exhibit excellent comprehensive performance comparable to the commercial UV-NLO material KH₂PO₄ (KDP), including large phase-matching ranges (>380 nm), sufficient second harmonic generation intensities (0.7-1.1 × KDP), high laser-induced damage thresholds (1.2 × KDP), wide transparent regions (0.26-12.2 μm), and good thermal stability (up to 1100 K). Moreover, systematic structure-activity relationship analysis illustrates that the 1D homochiral helical [GeOS₂]^2- chains composed of heteroanionic [GeS₂O₂] units make major contribution to the desirable UV-NLO performance. This work makes the two compounds shine out as new energy in the UV-NLO field and offers a new perspective for the exploration of structure-driven functional oxychalcogenides.