时间依赖的元概括梯度近似 Kohn-Sham理论:当前密度校正的重要性
Rian Richter1, Thilo Aschebrock1, Ingo Schelter1
1Theoretical Physics IV, University of Bayreuth, 95440 Bayreuth, Germany.
The Journal of chemical physics
|December 21, 2023
概括
我们在时间依赖密度函数理论中探索了Meta-Generalized Gradient Approximations (mGGAs). 电流密度校正对某些系统的激发能产生显著影响,提高了准确性.
科学领域:
- 计算化学计算化学
- 量子力学就是量子力学.
- 材料科学 材料科学 材料科学
背景情况:
- 超一般化梯度近似 (mGGAs) 是密度函数理论中的高级函数.
- 时间依赖密度函数理论 (TD-DFT) 对于研究电子刺激至关重要.
- 测量器不变性是物理理论中的一个基本原理.
研究的目的:
- 调查基于电流密度的测量器不变性校正对TD-DFT内的mGGAs的影响.
- 为了评估TASK和r2SCANmGGAs的性能,有和没有纠正.
- 分析这些校正对计算激发能量的影响.
主要方法:
- 一般化科恩-沙姆方程的实时传播.
- 实施和测试TASK和r2SCAN的mGGAs.
- 在实时空间和基础集合方法中使用伪潜在的结果的比较.
- 对电流密度计不变度校正的评估.
主要成果:
- 电流密度调整对一些系统的效果可以忽略不计.
- 对于其他系统,校正将激发能变化高达40% (>0.8 eV).
- 校正通常会改善对研究系统的参考数据的一致性.
结论:
- 电流密度计不变性校正对于使用某些mGGAs进行准确的TD-DFT计算至关重要.
- 选择的mGGA和系统属性影响了这一纠正的重要性.
- 对这些纠正进行进一步的调查是有必要的,以获得可靠的电子结构预测.
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