A2SnS5: A Structural Incommensurate Modulation Exhibiting Strong Second‐Harmonic Generation and a High Laser‐Induced Damage Threshold (A=Ba, Sr)

Structural modulations have been recently found to cause some unusual physical properties, such as superconductivity or charge density waves; however, thus‐induced nonlinear optical properties are rare. We report herein two unprecedented incommensurately modulated nonlinear optical sulfides exhibiti...

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Published in:Angewandte Chemie International Edition 2020-07, Vol.59 (29), p.11861-11865
Main Authors: Li, Rui‐An, Zhou, Zhengyang, Lian, Yu‐Kun, Jia, Fei, Jiang, Xingxing, Tang, Ming‐Cong, Wu, Li‐Ming, Sun, Junliang, Chen, Ling
Format: Article
Language:English
Subjects:
Barium
Charge density waves
incommensurate modulation
Laser damage
Modulation
nonlinear optics
Optical properties
Phase matching
Physical properties
polychalcogenides
Second harmonic generation
Silver gallium sulfide
Strontium
sulfides
Superconductivity
Thermal expansion
Yield point
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Summary:Structural modulations have been recently found to cause some unusual physical properties, such as superconductivity or charge density waves; however, thus‐induced nonlinear optical properties are rare. We report herein two unprecedented incommensurately modulated nonlinear optical sulfides exhibiting phase matching behavior, A2SnS5 (A=Ba, Sr), with the (3+1)D superspace groups P21212(00γ)00s or P21(α0γ)0, featuring different modulations of the [Sn2S7]∞ belts. Remarkably, Ba2SnS5 exhibits an excellent second harmonic generation (SHG) of 1.1 times that of the benchmark compound AgGaS2 at 1570 nm and a very large laser‐induced damage threshold (LIDT) of 8×AgGaS2. Theoretical studies revealed that the structural modulations increase the distortions of the Sn/S building units by about 44 or 25 % in A2SnS5 (A=Ba, Sr), respectively, and enhance significantly the SHG compared with α‐Ba2SnSe5 without modulation. Besides, despite the smaller Eg, the A2SnS5 samples exhibit higher LIDTs owing to their smaller thermal expansion anisotropies (Ba2SnS5 (1.51)
ISSN:1433-7851
1521-3773
DOI:10.1002/anie.202004059