期刊
MATERIALS CHEMISTRY FRONTIERS
卷 5, 期 20, 页码 7580-7586出版社
ROYAL SOC CHEMISTRY
DOI: 10.1039/d1qm01054a
关键词
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资金
- Key Research Program of Frontier Sciences, CAS [ZDBS-LY-SLH035]
- National Natural Science Foundation of China [51922014, 51972336, 61835014]
- West Light Foundation of CAS [2019-YDYLTD-002]
The study found that the fluorooxo-functional units BOxF4-x (x = 2, 3) can enhance birefringence, but as the crystal structure volume decreases, the second harmonic generation (SHG) response tends to decrease. The offset arrangement of BO2F2 and BO3F under pressure is the main reason for the reduced SHG response.
The microscopic anionic groups with specific arrangement are crucial in determining the optical properties of optically functional materials. The responses of linear and nonlinear polarization from external fields change synchronously, while the opposite phenomenon rarely occurs. Here, a dynamic structural fine-tuning strategy is proposed to clarify how the fluorooxo-functional units BOxF4-x (x = 2, 3) affect birefringence and second harmonic generation (SHG) response for typical nonlinear optical (NLO) material fluorooxoborates. Birefringence exhibits an obvious enhancement under external pressure, but a countertrend in the SHG coefficient was observed for Li2B3O4F3. On regulating the structural changes by simulating pressure, the fluorooxo-functional units BO3F and BO2F2 generate strong distortion, and the structural changes are more sensitive than that of BO3. An apparent response electron distribution anisotropy (REDA) in BO2F2 and a large amount of change of BO3F induce the enhancement of birefringence extending from 0.48 to 0.73 at 1064 nm. Here, the fluorooxo-functional units BOxF4-x (x = 2, 3) were proved to be the enhanced factor for birefringence. However, we were surprised to notice that with the decrease in the volume of the crystal structure, the SHG response tends to decrease. The offset arrangement of BO2F2 and BO3F under pressure is the main reason for the reduced SHG response. This study provides a perspective to understand the mechanism of the microstructure on the macroscopic properties of functional materials.
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