电子亲和度与GPU加速密度合适的EOM-CCSD,近似的EOM-CCSD方法和EOM-CCSD与结的自然轨道
Yanmei Hu1, Zhifan Wang2, Fan Wang1
1Institute of Atomic and Molecular Physics, Key Laboratory of High Energy Density Physics and Technology, Ministry of Education, Sichuan University, Chengdu 610065, People's Republic of China. wangf44@gmail.com.
Physical chemistry chemical physics : PCCP
|December 5, 2025
概括
这项研究优化了使用高效的运动方程合集群方法对有机光伏的电子亲和度计算. 密度匹配,GPU加速和结自然轨道等技术显著降低了具有高精度的计算成本.
科学领域:
- 计算化学的计算化学
- 量子化学 是一个量子化学.
- 材料科学 材料科学 材料科学
背景情况:
- 计算电子亲和度 (EA) 对于理解和设计有机光伏材料至关重要.
- 传统的运动方程合集群单双 (EOMEA-CCSD) 方法在计算上昂贵.
- 在更大的分子系统中,开发高效的计算策略对于准确的EA预测至关重要.
研究的目的:
- 开发和实施战略,以降低电子亲和关系的EOMEA-CCSD计算计算的计算成本.
- 评估这些优化方法对有机光伏相关的中型有机分子的准确性.
- 调查基准集和近似方法对EA计算的影响.
主要方法:
- 开发了一个EOMEA-CCSD程序,包括密度调整和GPU加速,以减少存储和计算时间.
- 用 aug-cc-pVXZ (X = D,T,Q) 基数组计算了24个有机分子的EAs.
- 采用了像corr-CIS(D∞) 和用结自然轨道 (FNO) 的EOMEA-CCSD等近似方法.
主要成果:
- 基本集不完整性显著影响EA与DZ集;TZ和QZ集显示良好协议.
- 通过corr-CIS(D∞) 方法,使用QZ基础实现了EAs,平均绝对偏差 (MAD) 为~0.18 eV.
- 来自电子附着状态波函数 (eaNOs) 的FNO将MAD降低到0.03 eV,保留了约30%的虚拟轨道.
结论:
- 优化的EOMEA-CCSD方法,包括密度匹配,GPU加速和FNO,提供高效和准确的EA计算.
- 在FNO中使用eaNOs可以显著降低计算成本,使EA的准确性降低至最低.
- 像corr-CIS ((D∞) 和FNO这样的近似方法是有机光伏材料高通量选的可行替代方案.
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