缓和线性响应TDDFT与范围分离的功能和密度适配
Pierpaolo D'Antoni1, Daniele Toffoli1, Mauro Stener1,2
1Dipartimento di Scienze Chimiche e Farmaceutiche, Università di Trieste, Via Giorgieri 1, 34127 Trieste, Italy.
The journal of physical chemistry. A
|September 26, 2025
概括
本研究介绍了一种高效的计算方法,使用时间依赖密度函数理论 (TDDFT) 中的范围分离 (RS) 函数的身份解析 (RI) 来解决. 改进的技术准确地预测光吸收光谱,即使对于大型分子系统.
科学领域:
- 计算化学的计算化学
- 理论化学 理论化学
- 量子化学 是一个量子化学.
背景情况:
- 时间依赖密度函数理论 (TDDFT) 对于模拟分子电子激发状态至关重要.
- 分隔范围 (RS) 交换相关性 (xc-) 函数提供了更好的准确性,但在计算上可能昂贵.
- 需要有效的方法来将高级功能应用于更大的系统.
研究的目的:
- 在TDDFT中提高RS-xc函数的计算效率.
- 实施用于TDDFT计算的身份 (RI) 技术的解决方案.
- 验证RI实施的光吸收光谱预测方法的准确性和效率.
主要方法:
- 采用身份解析 (RI) 技术来近似整数.
- 将RI集成到polTDDFT算法中,这是一个复杂的缓冲极化方法.
- 使用了RS-xc函数的混合诊断近似方法.
- 在AMS/ADF程序套件中实现.
主要成果:
- 与卡西达算法相比,证明了卓越的准确性和计算效率.
- 在一个模型乙烯-四乙烯电荷转移系统上验证.
- 成功复制了大型捐赠者-接受者-接受者三合体的实验光吸收光谱.
结论:
- 基于RI的TDDFT方法为预测光吸收光谱提供了可靠且计算效率高的工具.
- 该方法准确地捕获了电荷转移过渡.
- 适用于大分子系统的应用,大小可达几百个原子.
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