相对论CASPT2/RASPT2程序以及DIRAC软件。

IF 5.5 1区 化学 Q2 CHEMISTRY, PHYSICAL
Journal of Chemical Theory and Computation Pub Date : 2025-02-11 Epub Date: 2025-01-27 DOI:10.1021/acs.jctc.4c01589
Yasuto Masuda, Kohei Noda, Sumika Iwamuro, Masahiko Hada, Naoki Nakatani, Minori Abe
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引用次数: 0

摘要

探索锕系化合物的电子态是核科学的一个重要方面。然而,在理论计算中考虑相对论效应和电子关联是一个复杂的挑战。为了解决这个问题,我们开发了CASPT2/RASPT2程序和DIRAC程序,使电子相关方法的计算能够使用多构型微扰理论和各种相对论哈密顿量。目前,我们采用一种将改进的虚拟轨道(IVO)方法与CASCI方法相结合作为参考函数的方法,偏离了CASSCF的传统使用。此外,我们实现了RASCI-RASPT2方法来处理更大的活动空间并并行化整个程序。由于在CASPT2和RASPT2中选择轨道空间的复杂过程,我们提供了一个GUI程序来协助输入创建。所有这些程序和教程都可以在GitHub上免费访问,任何人都可以使用。在我们的基准计算中,我们利用1-256个核对UO22+分子进行CASCI-CASPT2计算,证明了并行化的效率。尽管遇到了一些异常,但我们在CASCI和CASPT2计算时间上取得了令人称道的并行化效率。我们还使用RASCI-RASPT2方法计算了UO22+的垂直激发能。通过调整IVO,并将RAS1和RAS3的最大空穴数和电子数设置为3,我们得到的趋势与先前使用替代方法报道的趋势一致。我们计划在未来继续改进该程序,相信它的广泛使用将有助于锕系化学的进一步发展。
本文章由计算机程序翻译,如有差异,请以英文原文为准。
Relativistic CASPT2/RASPT2 Program along with DIRAC Software.

Exploring electronic states in actinide compounds is a critical aspect of nuclear science. However, considering relativistic effects and electron correlation in theoretical calculations poses a complex challenge. To tackle this, we developed the CASPT2/RASPT2 program along with the DIRAC program, enabling calculations of electron correlation methods using multiconfigurational perturbation theory with various relativistic Hamiltonians. Currently, we employ a method that combines the improved virtual orbital (IVO) approach and CASCI methodologies as reference functions, deviating from the traditional use of CASSCF. Additionally, we implemented the RASCI-RASPT2 method to treat larger active spaces and parallelized the entire program. Due to the intricate process of selecting orbital spaces in CASPT2 and RASPT2, we offer a GUI program to assist with input creation. All these programs and tutorials are freely accessible on GitHub for anyone to use. In our benchmark calculations, we demonstrated the efficiency of parallelization by utilizing 1-256 cores for CASCI-CASPT2 calculations on the UO22+ molecule. Despite encountering some anomalies, we achieved commendable parallelization efficiency with CASCI and CASPT2 computational times. We also computed the vertical excitation energies of UO22+ using the RASCI-RASPT2 approach. By adapting the IVO and setting the maximum number of holes and electrons to three for RAS1 and RAS3, we obtained trends consistent with those reported in previous studies using alternative methods. We plan to continue improving the program in the future, believing that its widespread use will contribute to further development in actinide chemistry.

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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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