期刊
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
卷 136, 期 24, 页码 8560-8563出版社
AMER CHEMICAL SOC
DOI: 10.1021/ja504319x
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资金
- National Natural Science Foundation of China [21222102, 21373220, 51102231, 21171166, 11174297, 91022036]
- National Basic Research Project of China [2010CB630701, 2010CB933501, 2011CB922204, 2011CB935904]
It is challenging to explore deep-ultraviolet (deep-UV) nonlinear optical (NLO) materials that can achieve a subtle balance between deep-UV transparency and high NLO activity. Known deep-UV NLO materials are almost exclusively limited to borates, except few newly discovered phosphates despite their small NLO activities. Here we report two asymmetric phosphates, RbBa2(PO3)(5) (I) and Rb2Ba3(P2O7)(2) (II), which feature [PO3](infinity) chains and [P2O7](4-) dimers formed by condensation of [PO4](3-) units, respectively. Remarkably, I achieves the desired balance, with the shortest deep-UV absorption edge at 163 nm and the largest NLO activity of 1.4 x KDP (KH2PO4) in deep-UV NLO phosphates. According to first-principles calculations, the enhanced macroscopic SHG response of I can be attributed to the [PO3](infinity) chains which exhibit significantly larger microscopic SHG coefficients as compared with the [P2O7](4-) dimers.
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