Journal
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
Volume 141, Issue 2, Pages 748-752Publisher
AMER CHEMICAL SOC
DOI: 10.1021/jacs.8b11485
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Funding
- National Natural Science Foundation of China [91622118, 91622124, 51702330, 51802321, 11611530680, 11474292]
- Fujian Institute of Innovation, Chinese Academy of Sciences
- Youth Innovation Promotion Association at CAS
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Wide bandgap and strong second-order generation (SHG) effect are two crucial but contradictory conditions for practical nonlinear optical (NLO) materials. Herein, a new NLO crystal Pb2GaF2(SeO3)(2)Cl (I) containing novel functional (GaO3F3)(6-) octahedra is designed and synthesized by a rational band engineering strategy with aliovalent substitution. Benefiting from the removal of transition metal cations and the introduction of bridged F anions, I exhibits the widest bandgap among all reported phase-matchable NLO selenites. Meanwhile, a strong SHG response more than 4.5 times of KH2PO4 (KDP) is maintained. The dominate role of the (GaO3F3)(6-) groups to the enlarged bandgap in I are elucidated by first-principles studies.
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