New lead-iodide formates with a strong second-harmonic generation response and suitable birefringence obtained by the substitution strategy

Nonlinear optical (NLO) crystals featuring a strong second-harmonic generation (SHG) response and suitable birefringence to achieve phase-matching are in urgent demand in industrial and commercial applications. Based on the substitution strategy, two new NLO lead-iodide formates, K 2 [PbI 2 (HCOO) 2...

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Published in:Chemical science (Cambridge) 2022-12, Vol.14 (1), p.136-142
Main Authors: Zhang, Xiang-Yu, Zhou, Zi-Qi, Bao, Wen-Xiu, Tang, Hong-Xin, Fu, Rui-Biao, Ma, Zu-Ju, Wu, Xin-Tao
Format: Article
Language:English
Subjects:
Birefringence
Chemistry
Dipole moments
Formates
Nonlinear optics
Phase matching
Second harmonic generation
Substitutes
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Summary:Nonlinear optical (NLO) crystals featuring a strong second-harmonic generation (SHG) response and suitable birefringence to achieve phase-matching are in urgent demand in industrial and commercial applications. Based on the substitution strategy, two new NLO lead-iodide formates, K 2 [PbI 2 (HCOO) 2 ] and Rb 2 [PbI 2 (HCOO) 2 ], have been successfully synthesized using a moderate mixed-solvothermal method. K 2 [PbI 2 (HCOO) 2 ] and Rb 2 [PbI 2 (HCOO) 2 ] exhibit strong phase-matching SHG responses of 8 and 6.8 × KDP, respectively, a suitable birefringence and transparent window covering most of the visible light and mid-IR region. Crystal structures and theoretical calculations unveil that the origins of the strong SHG response and suitable birefringence can be credibly attributed to the oriented arrangement of the highly distorted [PbI 2 O 4 ] hexa-coordinated polyhedra, which are consistent in their local dipole moments, as well. This research provides a new strategy to explore high-performance NLO crystals. K 2 [PbI 2 (HCOO) 2 ] and Rb 2 [PbI 2 (HCOO) 2 ] with highly distorted [PbI 2 O 4 ] polyhedra in an oriented arrangement exhibit a very strong phase-matching SHG response, suitable birefringence, wide transparent windows and good thermal stability.
ISSN:2041-6520
2041-6539
DOI:10.1039/d2sc05216d