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The mean-field solutions of electronic excited states are much less accessible than ground state (e.g.\ Hartree-Fock) solutions. Energy-based optimization methods for excited states, like $\Delta$-scf, tend to fall into the lowest solution…

Chemical Physics · Physics 2022-10-11 Hong-Zhou Ye , Matthew Wellborn , Nathan D. Ricke , Troy Van Voorhis

Obtaining sub-chemical accuracy (1 kJ mol${}^{-1}$) for reaction energies of medium-sized gas-phase molecules is a longstanding challenge in the field of thermochemical modeling. The perturbative triples correction to CCSD, CCSD(T),…

Chemical Physics · Physics 2025-03-26 Tingting Zhao , James H. Thorpe , Devin A. Matthews

Molecular ground-state simulation is one of the most promising fields for demonstrating practical quantum advantage on near-term quantum computers. However, the Variational Quantum Eigensolver (VQE), a leading algorithm for this task, still…

Quantum Physics · Physics 2025-07-08 Runhong He , Qiaozhen Chai , Xin Hong , Ji Guan , Guolong Cui , Shengbin Wang , Shenggang Ying

Using the ground-state energy of 16-O obtained with the realistic V_UCOM interaction as a test case, we present a comprehensive comparison of different configuration interaction (CI) and coupled-cluster (CC) methods, analyzing the intrinsic…

Nuclear Theory · Physics 2009-06-30 R. Roth , J. R. Gour , P. Piecuch

We report the core binding energies of K-edge and L-edge transitions in simple semiconducting and insulating solids using periodic equation-of-motion coupled-cluster theory with single and double excitations (EOM-CCSD). In our all-electron…

Chemical Physics · Physics 2025-08-04 Ethan A. Vo , Timothy C. Berkelbach

We introduce the multistate iterative qubit coupled cluster (MS-iQCC) method, a quantum-inspired algorithm that runs efficiently on classical hardware and is designed to predict both ground and excited electronic states of molecules.…

Chemical Physics · Physics 2026-01-05 Robert A. Lang , Shashank G. Mehendale , Ilya G. Ryabinkin , Artur F. Izmaylov

Non-unitary theories are commonly seen in the classical simulations of quantum systems. Among these theories, the method of moments of coupled-cluster equations (MMCCs) and the ensuing classes of the renormalized coupled-cluster (CC)…

Quantum Physics · Physics 2022-12-13 Bo Peng , Karol Kowalski

Newly developed coupled-cluster (CC) methods enable simulations of ionization potentials and spectral functions of molecular systems in a wide range of energy scales ranging from core-binding to valence. This paper discusses results…

The cluster-in-molecule (CIM) local correlation approach with an accurate distant pair correlation energy correction is presented. For large systems, the inclusion of distant pair correlation energies is essential for the accurate…

Chemical Physics · Physics 2020-08-06 Zhigang Ni , Yang Guo , Frank Neese , Wei Li , Shuhua Li

The coupled cluster method (CCM) is a powerful and widely applied technique of modern-day quantum many-body theory. It has been used with great success in order to understand the properties of quantum magnets at zero temperature. This is…

Strongly Correlated Electrons · Physics 2009-09-11 D. J. J. Farnell

Molecular fragment or embedding methods are powerful techniques for overcoming scalability limitations in electronic structure theory by dividing large molecular systems into individual units that are small enough to be treated using…

Chemical Physics · Physics 2017-08-14 Jason N. Byrd , Robert W. Molt, , Rodney J. Bartlett , Beverly A. Sanders

Here we demonstrate workably accurate estimation of optical excitation threshold for large systems comprising of hundreds of atoms through an anti-causally corrected(ACC) real-time dynamics(RTD) approach implemented in a minimal…

Materials Science · Physics 2023-06-13 Joydev De , Manoar Hossain , Joydeep Bhattacharjee

A practical high-accuracy relativistic method of atomic structure calculations for univalent atoms is presented. The method is rooted in the coupled-cluster formalism and includes non-perturbative treatment of single and double excitations…

Atomic Physics · Physics 2009-11-11 Sergey G. Porsev , Andrei Derevianko

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…

Computational Physics · Physics 2025-06-12 Alexander V. Oleynichenko , Andrei Zaitsevskii , Leonid V. Skripnikov , Ephraim Eliav

Quantum computing methods for excited-state calculations remain underexplored in Noisy Intermediate-Scale Quantum (NISQ) hardware, despite their critical role in photochemistry and material science. Herein, we propose a resource-efficient…

Quantum Physics · Physics 2025-06-16 Qianjun Yao , He Li

The cluster variation method (CVM) is a hierarchy of approximate variational techniques for discrete (Ising--like) models in equilibrium statistical mechanics, improving on the mean--field approximation and the Bethe--Peierls approximation,…

Statistical Mechanics · Physics 2007-07-16 Alessandro Pelizzola

We show that recently developed quantum Monte Carlo methods, which provide accurate vertical transition energies for single excitations, also successfully treat double excitations. We study the double excitations in medium-sized molecules,…

We present a basis set correction scheme for the coupled-cluster singles and doubles (CCSD) method. The scheme is based on employing frozen natural orbitals (FNOs) and diagrammatically decomposed contributions to the electronic correlation…

Materials Science · Physics 2021-06-18 Andreas Irmler , Alejandro Gallo , Andreas Grüneis

We aim to obtain accurate rate coefficients for the collisional excitation of CH+ by He for high gas temperatures. The ab initio coupled-cluster [CCSD(T)] approximation was used to compute the interaction potential energy. Cross sections…

Solar and Stellar Astrophysics · Physics 2015-05-14 K. Hammami , L. C. Owono Owono , P. Staeuber

Many-body Green's functions theory within the GW approximation and the Bethe-Salpeter Equation (BSE) is implemented in the open-source VOTCA-XTP software, aiming at the calculation of electronically excited states in complex molecular…