最少的开关在表面上跳跃,使用Baek-An合器
Mariana T do Casal1, Josene M Toldo1, Max Pinheiro1
1Aix Marseille University, CNRS, ICR, Marseille, France.
Open research Europe
|August 30, 2023
概括
一个新的时间依赖的Baeck-An (TD-BA) 近似简化了非adiabatic动态计算. 这种方法为化学动力学探索性研究提供了一种具有成本效益的方法.
科学领域:
- 计算化学的计算化学
- 量子动力学 量子动力学是什么?
- 理论化学 理论化学
背景情况:
- 贝克-安 (BA) 近似计算非附加的合向量使用附加的能量差距及其第二导数.
- 准确计算非adiabatic合对于模拟涉及电子转换的分子动力学至关重要.
研究的目的:
- 导出和实现一个时间依赖的版本的Baek-An近似 (TD-BA).
- 为了评估TD-BA合器在最少开关中的性能,对分子系统进行表面跳跃模拟.
主要方法:
- 时间依赖的贝克-安 (TD-BA) 近似的导出.
- 使用能量差距及其二次时间导数计算非adiabatic合的计算.
- 在最少的开关中应用乙烯和的表面跳动动态.
主要成果:
- TD-BA 合器可以通过各种电子结构方法实现非adiabatic 动态.
- 乙烯和烯的模拟显示了质量正确的动态和准确合的半定量一致.
- 该方法在强的合和低速度下扎,并且由于单点不稳定性,TDDFT的表现不佳.
结论:
- TD-BA近似为探索性非adiabatic动态提供了一种计算成本低廉的方法.
- 它适用于小型轨迹组合,但需要仔细考虑其局限性.
- 需要进一步研究其与时间依赖密度函数理论的应用.
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