Curing the Divergence in Time-Dependent Density Functional Quadratic Response Theory
Curing the Divergence in Time-Dependent Density Functional Quadratic Response Theory
复制标题
解决瞬态密度泛函二次响应理论中的发散问题
DOI：
10.1021/acs.jpclett.3c00122
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发表时间：
2023
期刊：
影响因子：
--
通讯作者：
Maitra, Neepa T.
中科院分区：
文献类型：
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作者：
Dar, Davood;Roy, Saswata;Maitra, Neepa T.
含时密度泛函理论中的绝热近似在二次响应函数中给出了一个不正确的极点结构，导致激发态到态跃迁概率和超极化率的非物理分歧。我们发现的形式的确切的二次响应内核，并得出一个实用和准确的近似，治愈的分歧。我们展示了我们的结果激发态到状态的跃迁概率的模型系统和LiH分子。
The adiabatic approximation in time-dependent density functional theory is known to give an incorrect pole structure in the quadratic response function, leading to unphysical divergences in excited state-to-state transition probabilities and hyperpolarizabilties. We find the form of the exact quadratic response kernel and derive a practical and accurate approximation that cures the divergence. We demonstrate our results on excited state-to-state transition probabilities of a model system and of the LiH molecule.