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首页> 外文期刊>The journal of physical chemistry, A. Molecules, spectroscopy, kinetics, environment, & general theory >Perspective on Simplified Quantum Chemistry Methods for Excited States and Response Properties
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Perspective on Simplified Quantum Chemistry Methods for Excited States and Response Properties

机译：关于兴奋状态的简化量子化学方法和响应性能的透视图

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摘要

We review recent developments in the framework of simplified quantum chemistry for excited state and optical response properties (sTD-DFT) and present future challenges for new method developments to improve accuracy and extend the range of application. In recent years, the scope of sTD-DFT was extended to molecular response calculations of the polarizability, optical rotation, first hyperpolarizability, two-photon absorption (2PA), and excited-state absorption for large systems with hundreds to thousands of atoms. The recently introduced spin-flip simplified time-dependent density functional theory (SF-sTD-DFT) variant enables an ultrafast treatment for diradicals and related strongly correlated systems. A few drawbacks were also identified, specifically for the computation of 2PA cross sections. We propose solutions to this problem and how to generally improve the accuracy of simplified schemes. New possible simplified schemes are also introduced for strongly correlated systems, e.g., with a second-order perturbative correlation correction. Interpretation tools that can extract chemical structure-property relationships from excited state or response calculations are also discussed. In particular, the recently introduced method-agnostic RespA approach based on natural response orbitals (NROs) as the key concept is employed.
机译：我们回顾了激发态和光学响应性质简化量子化学（sTD DFT）框架的最新进展，并提出了新方法开发的未来挑战，以提高精度并扩大应用范围。近年来，sTD-DFT的应用范围扩展到了具有数百到数千个原子的大系统的极化率、旋光率、第一超极化率、双光子吸收（2PA）和激发态吸收的分子响应计算。最近引入的自旋翻转简化含时密度泛函理论（SF-sTD-DFT）变体使我们能够对双自由基和相关的强关联系统进行超快处理。还发现了一些缺点，特别是在计算2PA横截面时。我们提出了这个问题的解决方案，以及如何提高简化方案的精度。对于强相关系统，也引入了新的可能的简化方案，例如，具有二阶微扰相关校正的系统。还讨论了可以从激发态或响应计算中提取化学结构-性质关系的解释工具。特别是，最近引入的方法不可知响应方法以自然响应轨道（NRO）为关键概念。

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