Journal
CHEMISTRY OF MATERIALS
Volume 28, Issue 19, Pages 7110-7116Publisher
AMER CHEMICAL SOC
DOI: 10.1021/acs.chemmater.6b03333
Keywords
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Funding
- Strategic Priority Research Program of Chinese Academy of Sciences [XDB20000000]
- NSFC [11174297, 21525104, 21571178, 21601188, 51277091, 51402296, 51502288, 51502290, 91422301]
- NSF of Fujian Province [2015J01219, 2015J05040]
- 863 Program of China [2015AA034203]
- Middle-aged and Young Teachers' Rroject of Fujian Province [JAT160380]
- Youth Innovation Promotion of CAS [2015240, 2016274]
- NSF for Distinguished Young Scholars of Fujian Province [2016J06012]
- Chunmiao Projects of Haixi Institute of Chinese Academy of Sciences [CMZX-2014-003]
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Developing superior deep-ultraviolet (deep-UV) nonlinear optical (NLO) materials is a great challenge because of the contradiction between deep-UV transparency and enhanced second harmonic generation (SHG), especially for deep-UV NLO phosphates in which the constituent P-O groups have relatively small microscopic SHG coefficients. Here we report a new noncentrosymmetric phosphate Cs2LiPO4 (I), whose crystal structure consists of [LiPO4](infinity) layered structural units with a novel honeycomb-like topology. As compared with the benchmark deep-UV NLO material KBe2BO3F2 I is beryllium-free, and it is relatively easy to grow its large single crystals because of its congruent melting. Furthermore, it not only is deep-UV transparent but also exhibits an unexpectedly enhanced SHG response of 1.8 X KH2PO4 that hits a new high in deep-UV NLO phosphates. These results demonstrate that I satisfies the key requirements of being a promising deep-UV NLO candidate. Theory calculations and structural analysis reveal that the enhanced SHG response can be attributed to the honeycomb-like topological structure, which endows the constituent [PO4](3-) monomers of I with an aligned arrangement and as a result a favorable superposition of their microscopic SHG coefficients. These findings may provide useful insights into the development of both deep-UV NLO materials and honeycomb-like topological structures.
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