期刊
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
卷 135, 期 49, 页码 18560-18566出版社
AMER CHEMICAL SOC
DOI: 10.1021/ja408982d
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资金
- National Natural Science Foundation of China [91222204, 90922035]
- Main Direction Program of Knowledge Innovation of Chinese Academy of Sciences [KJCX2-EW-H03-03]
- Special Project of National Major Scientific Equipment Development of China [2012YQ120060]
The combination of Pb2+ cations with lone-pair electrons and F- anions with the largest electronegativity into the carbonate generates a new nonlinear optical material, CsPbCO3F, with the largest powder second-harmonic generation (SHG) response among carbonates of about 13.4 times that of KDP (KH2PO4), and transparency over the near-UV to middle-IR region. The optical characterization of the compound indicates that it is phase matchable. Its crystal structure exhibits the stacking of [CsF](infinity) and [Pb(CO3)](infinity), layers, and the coplanar alignment of [CO3] triangles which are oriented in the same direction. Yet the Pb2+ cation has an inert or nonstereoactive lone-pair, as indicated by its more spherical shape. Theoretical calculations confirm that the extremely large SHG efficiency indeed originates from enhancement via p-pi interaction between Pb2+. and [CO3](2-) within the [Pb(CO3)] layers.
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