"超零和"区间分离的局部混合功能,具有改进的动态相关性
Artur Wodyński1, Martin Kaupp1
1Technische Universität Berlin, Institut für Chemie, Theoretische Chemie/Quantenchemie, Sekr. C7, Straße des 17. Juni 135, D-10623 Berlin, Germany.
Journal of chemical theory and computation
|July 18, 2025
概括
新的范围分离局部混合 (RSLH) 函数,如 ωLH25tdE,通过解决强相关性和移位错误,显著改善密度函数近似. 这种进步为热化学,动力学和相互作用提供了更高的精度.
科学领域:
- 量子化学 是一个量子化学.
- 计算材料科学科学 计算材料科学
- 理论化学 理论化学
背景情况:
- 范围分离的局部混合 (RSLH) 函数旨在平衡移位和静态关联错误.
- 以前的函数像 ωLH23tdE 这样的函数表现出有希望的结果,但需要进一步的改进.
研究的目的:
- 评估强相关性校正的RSLHs (scRSLHs) 中动态相关性的修改.
- 评估对GMTKN55数据库的性能影响,涵盖热化学,动力学和非共价相互作用.
主要方法:
- 在scRSLHs中用重新优化的B97c动力系列扩展取代B95c相关性.
- 通过DFT-D4分散校正来增强新的 ωLH25tdE 功能.
- 在全面的GMTKN55基准数据库上评估业绩.
主要成果:
- LH25tdE scRSLH实现了GMTKN55 WTMAD-2值为2.64 kcal/mol,这是任何4级功能级别的最低值.
- 在自我一致的计算中表现出色.
- 展示了用于旋转受限键解离和移除旋转污染的保持精度.
结论:
- 开发的 ωLH25tdE scRSLH 代表了密度函数近似的重大进步.
- 它为处理强相关性和外定位错误提供了一个新的范式.
- 为广泛的化学性质提供准确的预测,包括准粒子能量.
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