Real‐time time‐dependent electronic structure theory is one of the most promising methods for investigating time‐dependent molecular responses and electronic dynamics. Since its first modern use in the 1990s, it has been used to study a wide variety of spectroscopic properties and electronic responses to intense external electromagnetic fields, complex environments, and open quantum systems. It has also been used to study molecular conductance, excited state dynamics, ionization, and nonlinear optical effects. Real‐time techniques describe non‐perturbative responses of molecules, allowing for studies that go above and beyond the more traditional energy‐ or frequency‐domain‐based response theories. Recent progress in signal analysis, accurate treatment of environmental responses, relativistic Hamiltonians, and even quantized electromagnetic fields have opened up new avenues of research in time‐dependent molecular response. After discussing the history of real‐time methods, we explore some of the necessary mathematical theory behind the methods, and then survey a wide (yet incomplete) variety of applications for real‐time methods. We then present some brief remarks on the future of real‐time time‐dependent electronic structure theory. WIREs Comput Mol Sci 2018, 8:e1341. doi: 10.1002/wcms.1341

中文翻译：

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实时时变电子结构理论

实时时间依赖性电子结构理论是研究时间依赖性分子响应和电子动力学的最有前途的方法之一。自从1990年代首次在现代中使用以来，它已被用于研究各种光谱特性以及对强外部电磁场，复杂环境和开放量子系统的电子响应。它也已用于研究分子电导，激发态动力学，电离和非线性光学效应。实时技术描述了分子的非扰动响应，从而使研究超出了传统的基于能量或频域的响应理论的范围。信号分析的最新进展，对环境响应的精确处理，相对论的哈密顿量，甚至量化的电磁场都为依赖时间的分子响应开辟了新的研究途径。在讨论了实时方法的历史之后，我们探索了这些方法背后的一些必要的数学理论，然后对实时方法的广泛（但不完整）应用进行了调查。然后，我们简要介绍一下实时时变电子结构理论的未来。电线计算科学2018，8：e1341。doi：10.1002 / wcms.1341