Open-Ended Recursive Approach for the Calculation of Multiphoton Absorption Matrix Elements.
Open-Ended Recursive Approach for the Calculation of Multiphoton Absorption Matrix Elements.
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DOI：
10.1021/ct501113y
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发表时间：
2015-03-10
影响因子：
5.5
通讯作者：
Ruud, Kenneth
中科院分区：
文献类型：
--
作者：
Friese, Daniel H.;Beerepoot, Maarten T. P.;Ringholm, Magnus;Ruud, Kenneth
我们提出了一种用递归方法实现任意阶响应函数的单余项。文中还给出了线性、二次、三次和四次响应函数的单个余项的基于密度矩阵的响应理论的显式表达式。这些残基对应于单光子、双光子、三光子和四光子跃迁矩阵元素。新开发的程序被用来计算对硝基苯胺和对硝基氨基二苯乙烯的单、双、三和四光子吸收截面，这是在响应理论框架下的第一个四光子吸收的处理。我们发现，只要使用具有漫射函数的相当大的基组，计算的多光子吸收截面对基组的大小不是很敏感。然而，交换关联泛函的选择显著影响电荷转移跃迁和其他跃迁的计算截面，特别是对于较大的对硝基氨基二苯乙烯分子。因此，我们建议使用距离分离的交换相关泛函与增强的相关一致性双ζ基组AUG-CC-PVDZ相结合来计算多光子吸收性质。
We present an implementation of single residues for response functions to arbitrary order using a recursive approach. Explicit expressions in terms of density-matrix-based response theory for the single residues of the linear, quadratic, cubic, and quartic response functions are also presented. These residues correspond to one-, two-, three- and four-photon transition matrix elements. The newly developed code is used to calculate the one-, two-, three- and four-photon absorption cross sections of para-nitroaniline and para-nitroaminostilbene, making this the first treatment of four-photon absorption in the framework of response theory. We find that the calculated multiphoton absorption cross sections are not very sensitive to the size of the basis set as long as a reasonably large basis set with diffuse functions is used. The choice of exchange–correlation functional, however, significantly affects the calculated cross sections of both charge-transfer transitions and other transitions, in particular, for the larger para-nitroaminostilbene molecule. We therefore recommend the use of a range-separated exchange–correlation functional in combination with the augmented correlation-consistent double-ζ basis set aug-cc-pVDZ for the calculation of multiphoton absorption properties.
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影响因子：
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