A General and Transferable Local Hybrid Functional for Electronic Structure Theory and Many-Fermion Approaches.

IF 5.7 1区 化学 Q2 CHEMISTRY, PHYSICAL Journal of Chemical Theory and Computation Pub Date : 2024-12-20 DOI:10.1021/acs.jctc.4c01309
Christof Holzer, Yannick J Franzke
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Abstract

Density functional theory has become the workhorse of quantum physics, chemistry, and materials science. Within these fields, a broad range of applications needs to be covered. These applications range from solids to molecular systems, from organic to inorganic chemistry, or even from electrons to other Fermions, such as protons or muons. This is emphasized by the plethora of density functional approximations that have been developed for various cases. In this work, two new local hybrid exchange-correlation density functionals are constructed from first-principles, promoting generality and transferability. We show that constraint satisfaction can be achieved even for admixtures with full exact exchange, without sacrificing accuracy. The performance of the new functionals CHYF-PBE and CHYF-B95 is assessed for thermochemical properties, excitation energies, Mössbauer isomer shifts, NMR spin-spin coupling constants, NMR shieldings and shifts, magnetizabilities, and EPR hyperfine coupling constants. Here, the new density functional shows excellent performance throughout all tests and is numerically robust only requiring small grids for converged results. Additionally, both functionals can easily be generalized to arbitrary Fermions as shown for electron-proton correlation energies. Therefore, we outline that density functionals generated in this way are general purpose tools for quantum mechanical studies.

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密度泛函理论已成为量子物理学、化学和材料科学的主力。在这些领域中,需要涵盖广泛的应用。这些应用范围从固体到分子系统,从有机化学到无机化学,甚至从电子到其他费米子,如质子或渺子。针对各种情况开发的大量密度泛函近似方法强调了这一点。在这项工作中,我们从第一原理出发,构建了两个新的局部混合交换相关密度函数,从而提高了通用性和可转移性。我们证明,即使是完全精确交换的混合物,也能在不牺牲精度的情况下满足约束条件。我们评估了新函数 CHYF-PBE 和 CHYF-B95 在热化学性质、激发能、莫斯鲍尔异构体位移、核磁共振自旋-自旋耦合常数、核磁共振屏蔽和位移、磁化率和 EPR 超精细耦合常数方面的性能。在这里,新密度函数在所有测试中都表现出了卓越的性能,而且在数值上非常稳健,只需要较小的网格就能得到收敛结果。此外,正如电子-质子相关能所显示的那样,这两种函数都可以很容易地推广到任意费米子。因此,我们概括说,以这种方式生成的密度函数是量子力学研究的通用工具。
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来源期刊
Journal of Chemical Theory and Computation
Journal of Chemical Theory and Computation 化学-物理:原子、分子和化学物理
CiteScore
9.90
自引率
16.40%
发文量
568
审稿时长
1 months
期刊介绍: The Journal of Chemical Theory and Computation invites new and original contributions with the understanding that, if accepted, they will not be published elsewhere. Papers reporting new theories, methodology, and/or important applications in quantum electronic structure, molecular dynamics, and statistical mechanics are appropriate for submission to this Journal. Specific topics include advances in or applications of ab initio quantum mechanics, density functional theory, design and properties of new materials, surface science, Monte Carlo simulations, solvation models, QM/MM calculations, biomolecular structure prediction, and molecular dynamics in the broadest sense including gas-phase dynamics, ab initio dynamics, biomolecular dynamics, and protein folding. The Journal does not consider papers that are straightforward applications of known methods including DFT and molecular dynamics. The Journal favors submissions that include advances in theory or methodology with applications to compelling problems.
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