Time-Resolved Exciton Wave Functions from Time-Dependent Density-Functional Theory
Time-Resolved Exciton Wave Functions from Time-Dependent Density-Functional Theory
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来自瞬态密度泛函理论的时间分辨激子波函数
DOI：
10.1021/acs.jctc.0c01334
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发表时间：
2021
影响因子：
5.5
通讯作者：
Ullrich, Carsten A.
中科院分区：
文献类型：
--
作者：
Williams, Jared R.;Tancogne-Dejean, Nicolas;Ullrich, Carsten A.
含时密度泛函理论（英语：Time-dependent density-functional theory，TDDFT）是一种计算效率高的第一性原理方法，用于计算包括激子效应在内的绝缘体和半导体的光谱。我们展示了如何激子波函数可以通过Kohn-Sham跃迁密度矩阵从TDDFT获得，无论是在依赖于频率的线性响应制度和实时传播。使用一维模型固体的方法进行说明。特别是，我们表明，我们的方法提供了洞察激子的形成和解离在真实的时间。这为通过实时TDDFT对材料中激子动力学进行时间分辨研究打开了大门。
Time-dependent density-functional theory (TDDFT) is a computationally efficient first-principles approach for calculating optical spectra in insulators and semiconductors including excitonic effects. We show how exciton wave functions can be obtained from TDDFT via the Kohn–Sham transition density matrix, both in the frequency-dependent linear-response regime and in real-time propagation. The method is illustrated using one-dimensional model solids. In particular, we show that our approach provides insight into the formation and dissociation of excitons in real time. This opens the door to time-resolved studies of exciton dynamics in materials by means of real-time TDDFT.