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A global hybrid extension of variational two-electron reduced-density matrix (v2RDM)-driven multiconfiguration pair-density functional theory (MCPDFT) is developed. Using a linear decomposition of the electron-electron repulsion term, a…

Chemical Physics · Physics 2019-11-27 Mohammad Mostafanejad , Marcus Dante Liebenthal , A. Eugene DePrince

A major challenge in the molecular simulation of electric double layer capacitors (EDLCs) is the choice of an appropriate model for the electrode. Typically, in such simulations the electrode surface is modeled using a uniform fixed charge…

Computational Physics · Physics 2015-06-22 Zhenxing Wang , Yang Yang , David L. Olmsted , Mark Asta , Brian B. Laird

We have studied electron correlations in the doped two-dimensional (2D) Hubbard model by using the coupled-cluster method (CCM) to investigate whether or not the method can be applied to correct the independent particle approximations…

Strongly Correlated Electrons · Physics 2009-10-31 Yoshihiro Asai , Hideki Katagiri

Machine learning (ML) plays an important role in quantum chemistry, providing fast-to-evaluate predictive models for various properties of molecules. However, most existing ML models for molecular electronic properties use density…

Chemical Physics · Physics 2024-06-26 Hao Tang , Brian Xiao , Wenhao He , Pero Subasic , Avetik R. Harutyunyan , Yao Wang , Fang Liu , Haowei Xu , Ju Li

In this paper we demonstrate the performance of several density-based methods in predicting the inversion of S$_1$ and T$_1$ states of a few N-heterocyclic fused ring molecules (popularly known as INVEST molecules) with an eye to identify a…

Chemical Physics · Physics 2024-08-12 Shamik Chanda , Subhasish Saha , Sangita Sen

Linearized Coupled Cluster Doubles (LinCCD) often provides near-singular energies in small-gap systems that exhibit static correlation. This has been attributed to the lack of quadratic $T_2^2$ terms that typically balance out small energy…

Chemical Physics · Physics 2025-05-13 Kevin Carter-Fenk

Ground-state electronic structure calculations using Kohn-Sham density functional theory (KS-DFT) offer an unprecedented balance between efficiency and accuracy, now paradigmatic to the fields of quantum chemistry and condensed matter…

Chemical Physics · Physics 2026-04-14 Lucien Dupuy , Toni Chiti , Jérémy Morere , Emmanuel Fromager

We generalize the Aufbau suppressed coupled cluster formalism into the realm of doubly excited states by deriving, implementing, and testing a wave function initialization strategy that allows the zeroth order wave function to match the…

Chemical Physics · Physics 2026-05-11 Qasim Javed , Harrison Tuckman , Eric Neuscamman

Localized orbital coupled cluster theory has recently emerged as an nonempirical alternative to DFT for large systems. Intuitively, one might expect such methods to perform less well for highly delocalized systems. In the present work, we…

Chemical Physics · Physics 2020-10-16 Nitai Sylvetsky , Ambar Banerjee , Mercedes Alonso , Jan M. L. Martin

Accurately modeling chemical reactions at the atomistic level requires high-level electronic structure theory due to the presence of unpaired electrons and the need to properly describe bond breaking and making energetics. Commonly used…

Accurate many-body treatments of condensed-phase systems are challenging because correlated solvers such as full configuration interaction (FCI) and the density matrix renormalization group (DMRG) scale exponentially with system size.…

Metallic solids are a challenging target for wavefunction-based electronic structure theories and have not been studied in great detail by such methods. Here, we use coupled-cluster theory with single and double excitations (CCSD) to study…

Materials Science · Physics 2022-04-05 Verena A. Neufeld , Hong-Zhou Ye , Timothy C. Berkelbach

We apply a simple dynamical density functional theory, the phase-field-crystal (PFC) model, to describe homogeneous and heterogeneous crystal nucleation in 2d monodisperse colloidal systems and crystal nucleation in highly compressed Fe…

Materials Science · Physics 2015-05-18 László Gránásy , György Tegze , Gyula I. Tóth , Tamás Pusztai

Density matrix embedding theory (DMET) [Phys. Rev. Lett., 109, 186404 (2012)], introduced a new approach to quantum cluster embedding methods, whereby the mapping of strongly correlated bulk problems to an impurity with finite set of bath…

Strongly Correlated Electrons · Physics 2015-06-24 George H. Booth , Garnet Kin-Lic Chan

We present a linear-response formulation of density cumulant theory (DCT) that provides a balanced and accurate description of many electronic states simultaneously. In the original DCT formulation, only information about a single…

Chemical Physics · Physics 2018-09-10 Andreas V. Copan , Alexander Yu. Sokolov

In classical computational chemistry, the coupled-cluster ansatz is one of the most commonly used $ab~initio$ methods, which is critically limited by its non-unitary nature. The unitary modification as an ideal solution to the problem is,…

Quantum Physics · Physics 2017-03-01 Yangchao Shen , Xiang Zhang , Shuaining Zhang , Jing-Ning Zhang , Man-Hong Yung , Kihwan Kim

Linear-response quantum electrodynamical density functional theory (QEDFT) enables the description of molecular spectra under strong coupling to quantized photonic modes, such as those in optical cavities. Recently, this approach was…

Chemical Physics · Physics 2025-07-11 Lukas Konecny , Valeriia P. Kosheleva , Michael Ruggenthaler , Michal Repisky , Angel Rubio

In this paper, we have developed a unitary variant of a double exponential coupled cluster theory, which is capable of mimicking the effects of connected excitations of arbitrarily high rank, using only rank-one and rank-two parametrization…

Chemical Physics · Physics 2022-11-23 Dipanjali Halder , V. S. Prasannaa , Rahul Maitra

The unitary coupled cluster (UCC) approximation is one of the more promising wave-function ans\"atze for electronic structure calculations on quantum computers via the variational quantum eigensolver algorithm. However, for large systems…

Quantum Physics · Physics 2021-09-30 Jia Chen , Hai-Ping Cheng , James K. Freericks

We present a flexible, automated, and basis-set insensitive domain-based charge-transfer (CT) decomposition framework that can be combined with any CI-type excited-state wavefunction. Our approach is not based on excited-state densities and…

Chemical Physics · Physics 2026-05-15 Lena Szczuczko , Julia Szczuczko , Marta Gałyńska , Katharina Boguslawski
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