Francisco H, Cancio A C, Trickey S B
Quantum Theory Project, Department of Physics, University of Florida, Gainesville, Florida 32611, United States.
Department of Physics and Astronomy, Ball State University, Muncie, Indiana 47306, United States.
J Phys Chem A. 2024 Jul 25;128(29):6010-6018. doi: 10.1021/acs.jpca.4c02635. Epub 2024 Jul 12.
We present a deorbitalization of the recent simplified, regularized Tao-Mo exchange functional ( 2023, 159, 214102) that is faithful to the parent functional. That is a major gain relative to our earlier deorbitalization which did poorly on molecular heats of formation ( 2023, 159, 214103). The improvement arises from augmentation of the Mejía-Rodríguez and Trickey deorbitalization strategy ( 2017, 96, 052512) to use a smoothed replacement for the reduced density Laplacian (conventionally denoted ) obtained from that Laplacian itself. The augmentation also rationalizes the improvement obtained from the cutoff of < 0 that was poorly understood at the time of the previous paper. The new scheme yields deorbitalized chemical region indicators that are much closer to those from the parent, orbital-dependent functional than were obtainable from the previous deorbitalization. It also replicates the good 3d elemental magnetization of the parent functional reasonably well.
我们展示了对近期简化、正则化的陶-莫交换泛函（2023, 159, 214102）的去轨道化处理，该处理忠实于母泛函。相对于我们早期在分子生成热方面表现不佳的去轨道化处理（2023, 159, 214103），这是一个重大进步。这种改进源于对梅希亚 - 罗德里格斯和特里克伊去轨道化策略（2017, 96, 052512）的扩充，即使用一个平滑的替代量来取代从拉普拉斯算子本身得到的约化密度拉普拉斯算子（通常记为 ）。这种扩充还解释了通过截断 < 0 所获得的改进，而上一篇论文发表时对这一点理解得并不充分。新方案产生的去轨道化化学区域指标比之前的去轨道化处理得到的指标更接近母泛函（依赖轨道的泛函）的指标。它还能较好地复制母泛函良好的三维元素磁化强度。
