Premium
The Large Second‐Harmonic Generation of LiCs 2 PO 4 is caused by the Metal‐Cation‐Centered Groups
Author(s) -
Cheng Xiyue,
Whangbo MyungHwan,
Guo GuoCong,
Hong Maochun,
Deng Shuiquan
Publication year - 2018
Publication title -
angewandte chemie
Language(s) - English
Resource type - Journals
eISSN - 1521-3757
pISSN - 0044-8249
DOI - 10.1002/ange.201711465
Subject(s) - polarizability , atomic orbital , second harmonic generation , atom (system on chip) , chemistry , nonmetal , metal , atomic physics , basis set , density functional theory , computational chemistry , physics , molecule , quantum mechanics , electron , laser , organic chemistry , computer science , embedded system
We evaluated the individual atom contributions to the second harmonic generation (SHG) coefficients of LiCs 2 PO 4 (LCPO) by introducing the partial response functionals on the basis of first principles calculations. The SHG response of LCPO is dominated by the metal‐cation‐centered groups CsO 6 and LiO 4 , not by the nonmetal‐cation‐centered groups PO 4 expected from the existing models and theories. The SHG coefficients of LCPO are determined mainly by the occupied orbitals O 2p and Cs 5p as well as by the unoccupied orbitals Cs 5d and Li 2p. For the SHG response of a material, the polarizable atomic orbitals of the occupied and the unoccupied states are both important.