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开壳层体系在大耦合强度下的莫勒-普莱塞绝热连接

Møller-Plesset Adiabatic Connection at Large Coupling Strengths for Open-Shell Systems.

作者信息

Daas Kimberly J, Klute Eveline, Seidl Michael, Gori-Giorgi Paola

机构信息

Department of Chemistry & Pharmaceutical Sciences and Amsterdam Institute of Molecular and Life Sciences (AIMMS), Faculty of Science, Vrije Universiteit, De Boelelaan 1083, Amsterdam 1081 HV, The Netherlands.

Microsoft Research AI for Science, Evert van de Beekstraat 354, Schiphol 1118 CZ, The Netherlands.

出版信息

J Phys Chem A. 2024 May 23;128(20):4138-4149. doi: 10.1021/acs.jpca.4c00788. Epub 2024 May 8.

DOI:10.1021/acs.jpca.4c00788
PMID:38717868
原文链接:https://pmc.ncbi.nlm.nih.gov/articles/PMC11129316/
Abstract

We study the adiabatic connection that has as weak-coupling expansion the Møller-Plesset perturbation series, generalizing to the open-shell case previous closed-shell results for the large-coupling limit. We first focus on the hydrogen atom with fractional spins, providing results along the adiabatic connection from small to large coupling strengths. We reveal an intriguing phase diagram and an equation for the large-coupling leading order that has closed-form solutions for specific choices of its relevant quantum numbers. We then show that the hydrogen atom results provide variational estimates for the large-coupling leading terms for the general many-electron open-shell case in terms of functionals of the Hartree-Fock α-spin and β-spin densities.

摘要

我们研究了绝热连接，其弱耦合展开为莫勒-普列塞特微扰级数，将之前闭壳层情形下大耦合极限的结果推广到了开壳层情形。我们首先关注具有分数自旋的氢原子，给出了从小耦合强度到 大耦合强度沿绝热连接的结果。我们揭示了一个有趣的相图以及一个大耦合主导阶的方程，该方程对于其相关量子数的特定选择具有闭式解。然后我们表明，氢原子的结果为一般多电子开壳层情形下大耦合主导项提供了基于哈特里-福克α自旋和β自旋密度泛函的变分估计。

https://cdn.ncbi.nlm.nih.gov/pmc/blobs/907e/11129316/a759596700af/jp4c00788_0004.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/907e/11129316/e6e1522b7451/jp4c00788_0001.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/907e/11129316/efc58a143fe5/jp4c00788_0002.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/907e/11129316/6292fb489173/jp4c00788_0003.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/907e/11129316/a759596700af/jp4c00788_0004.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/907e/11129316/e6e1522b7451/jp4c00788_0001.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/907e/11129316/efc58a143fe5/jp4c00788_0002.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/907e/11129316/6292fb489173/jp4c00788_0003.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/907e/11129316/a759596700af/jp4c00788_0004.jpg

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J Phys Chem Lett. 2023 Sep 28;14(38):8448-8459. doi: 10.1021/acs.jpclett.3c01832. Epub 2023 Sep 18.
2
Møller-Plesset and Density-Fixed Adiabatic Connections for a Model Diatomic System at Different Correlation Regimes.不同相关体系下双原子模型系统的莫勒-普莱塞特方法与密度固定绝热连接
J Chem Theory Comput. 2023 Sep 12;19(17):5835-5850. doi: 10.1021/acs.jctc.3c00529. Epub 2023 Aug 29.
3
Strong-weak duality via Jordan-Wigner transformation: Using fermionic methods for strongly correlated su(2) spin systems.
通过约旦-维格纳变换实现的强弱对偶性：将费米子方法应用于强关联的su(2)自旋系统。
J Chem Phys. 2022 Nov 21;157(19):194114. doi: 10.1063/5.0125124.
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DFT exchange: sharing perspectives on the workhorse of quantum chemistry and materials science.DFT 交换：对量子化学和材料科学的主力的观点分享。
Phys Chem Chem Phys. 2022 Dec 7;24(47):28700-28781. doi: 10.1039/d2cp02827a.
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Comparing correlation components and approximations in Hartree-Fock and Kohn-Sham theories via an analytical test case study.通过一个分析性案例研究比较哈特里-福克理论和科恩-沈理论中的相关分量及近似。
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Gradient Expansions for the Large-Coupling Strength Limit of the Møller-Plesset Adiabatic Connection.莫勒-普莱塞特绝热连接大耦合强度极限的梯度展开
J Chem Theory Comput. 2022 Mar 8;18(3):1584-1594. doi: 10.1021/acs.jctc.1c01206. Epub 2022 Feb 18.
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8
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9
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