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The exponential computational cost of describing strongly correlated electrons can be mitigated by adopting a reduced density-matrix (RDM)-based description of the electronic structure. While variational two-electron RDM (v2RDM) methods can…

化学物理 · 物理学 2026-01-06 Grier M. Jones , Run. R. Li , A. Eugene DePrince , Konstantinos D. Vogiatzis

Theory of one-electron transition density matrices has been formulated within the time-independent coupled cluster method for the polarization propagator [R. Moszynski, P. S. \.Zuchowski, and B. Jeziorski, Coll. Czech. Chem. Commun. {\bf…

化学物理 · 物理学 2014-09-25 Aleksandra M. Tucholska , Marcin Modrzejewski , Robert Moszynski

Tailored coupled cluster theory represents a computationally inexpensive way to describe static and dynamical electron correlation effects. In this work, we scrutinize the performance of various tailored coupled cluster methods externally…

化学物理 · 物理学 2021-03-24 Aleksandra Leszczyk , Mihály Máté , Örs Legeza , Katharina Boguslawski

Parametric two-electron reduced-density-matrix (p-2RDM) methods have enjoyed much success in recent years; the methods have been shown to exhibit accuracies greater than coupled cluster with single and double substitutions (CCSD) for both…

化学物理 · 物理学 2010-09-02 A. Eugene DePrince , David A. Mazziotti

We introduce a range-separation approximation to coupled cluster doubles (CCD) theory that successfully overcomes limitations of regular CCD when applied to the uniform electron gas. We combine the short-range ladder channel with the…

化学物理 · 物理学 2014-05-07 James J. Shepherd , Thomas M. Henderson , Gustavo E. Scuseria

Various properties of the general two-center two-electron integral over the explicitly correlated exponential function are analyzed for the potential use in high precision calculations for diatomic molecules. A compact one dimensional…

化学物理 · 物理学 2015-06-11 Krzysztof Pachucki

In this paper we show that 1-electron properties such as Compton profiles and structure factors of crystals can be asymptotically retrieved through cluster-based calculations, followed by an appropriate partition of the 1-electron reduced…

化学物理 · 物理学 2015-06-26 Sebastien Ragot , Jean-Michel Gillet , Pierre J Becker

Quantum embedding methods have recently developed significantly to model large molecular structures. This work proposes a novel wave function theory in density functional theory (WTF-in-DFT) embedding scheme based on pair-coupled cluster…

化学物理 · 物理学 2024-01-10 Rahul Chakraborty , Katharina Boguslawski , Paweł Tecmer

The pair-coupled-cluster doubles (pCCD) method has emerged as a viable approach for quantum-chemical studies of strongly correlated systems. Despite its lower formal scaling (O(N$^4$)) compared to other versions of coupled cluster (CC)…

化学物理 · 物理学 2026-04-17 Rahul Chakraborty , Paweł Tecmer

An efficient approach to calculate approximate pure-state and transition reduced density matrices in the framework of the multireference relativistic Fock-space coupled cluster (FS CC) theory is proposed. The method is based on the…

A combined density and first-order reduced-density-matrix (1RDM) functional method is proposed for the calculation of potential energy curves (PECs) of molecular multibond dissociation. Its 1RDM functional part, a pair density functional,…

化学物理 · 物理学 2020-09-23 Robert van Meer , Oleg Gritsenko , Jeng-Da Chai

We discuss diagrammatic modifications to the coupled cluster doubles (CCD) equations, wherein different groups of terms out of rings, ladders, crossed-rings and mosaics can be removed to form approximations to the coupled cluster method, of…

化学物理 · 物理学 2014-05-06 James J. Shepherd , Thomas. M. Henderson , Gustavo E. Scuseria

The $\Delta$NO two-electron density matrix (2-RDM) and energy expression are derived from a multideterminantal wave function. The approximate $\Delta$NO 2-RDM is combined with an on-top density functional and a double-counting correction to…

化学物理 · 物理学 2022-03-14 Ismael A. Elayan , Rishabh Gupta , Joshua W. Hollett

General theorem describing a relation between diagonal of one-electron density matrix and a certain class of many-electron ensembles of determinant states is proved. As a corollary to this theorem a constructive proof of sufficiency of…

化学物理 · 物理学 2007-05-23 A. I. Panin , A. N. Petrov

We present a new approach for simulating X-ray absorption spectra based on linear-response density cumulant theory (LR-DCT) [A. V. Copan and A. Yu. Sokolov, J. Chem. Theory Comput., 2018, 14, 4097 - 4108]. Our new method combines the…

化学物理 · 物理学 2019-06-03 Ruojing Peng , Andreas V. Copan , Alexander Yu. Sokolov

The computation of strongly correlated quantum systems is challenging because of its potentially exponential scaling in the number of electron configurations. Variational calculation of the two-electron reduced density matrix (2-RDM)…

量子物理 · 物理学 2021-04-01 David A. Mazziotti

Roles of electron correlation effects in the determination of attachment energies, magnetic dipole hyperfine structure constants and electric dipole (E1) matrix elements of the low-lying states in the singly charged cadmium ion (Cd$^+$)…

原子物理 · 物理学 2018-03-14 Cheng-Bin Li , Yan-Mei Yu , B. K. Sahoo

Machine learning is rapidly accelerating materials and chemical discovery, but most current models target energies, forces, or selected molecular properties rather than the underlying many-body electronic structure. Learning…

The previously proposed ansatz for density cumulant theory that combines orbital-optimization and a parameterization of the 2-electron reduced density matrix cumulant in terms of unitary coupled cluster amplitudes (OUDCT) is carefully…

The accurate and efficient description of strongly correlated systems remains an important challenge for computational methods. Doubly occupied configuration interaction (DOCI), in which all electrons are paired and no correlations which…

化学物理 · 物理学 2016-02-25 Thomas M. Henderson , Ireneusz W. Bulik , Gustavo E. Scuseria
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