Nonlinear optical property calculations by the long-range-corrected coupled-perturbed Kohn-Sham method
Nonlinear optical property calculations by the long-range-corrected coupled-perturbed Kohn-Sham method
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DOI：
10.1063/1.1935514
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发表时间：
2005-06-15
影响因子：
4.4
通讯作者：
Hirao, K
中科院分区：
文献类型：
--
作者：
Kamiya, M;Sekino, H;Hirao, K
将密度泛函理论（DFT）中交换泛函的长程修正（LC）方法与耦合微扰Kohn-Sham（CPKS）方法相结合，计算了该体系的非线性光学响应特性.利用LC-CPKS方法，我们计算了典型分子的超极化率和推拉π共轭体系的偶极矩、极化率和超极化率：对硝基苯胺、4-氨基-4（'）-硝基二苯乙烯和α，ω-硝基氨基多烯。结果发现，LC方案明显改善了所有这些系统的这些光学性质的计算，这已被显着高估了传统的DFT。因此，我们得出结论，长程交换相互作用在使用DFT形式主义计算光学性质中起着重要的作用。(C)2005年美国物理学会。
The long-range correction (LC) scheme for the exchange functional of density-functional theory (DFT) was combined with the coupled-perturbed Kohn-Sham (CPKS) method to calculate nonlinear optical response properties. By using this LC-CPKS method, we calculated the hyperpolarizabilities of typical molecules and the dipole moments, polarizabilities, and hyperpolarizabilities of push-pull pi-conjugated systems: p-nitroaniline, 4-amino-4(')-nitrostilbene, and alpha,omega-nitroaminopolyenes. It was found that the LC scheme clearly improved the calculation of these optical properties for all of these systems, which have been significantly overestimated by conventional DFTs. We therefore concluded that the long-range exchange interaction played an important role in calculating the optical properties using the DFT formalism. (C) 2005 American Institute of Physics.