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Quantum Monte Carlo (QMC) is a stochastic method which has been particularly successful for ground-state electronic structure calculations but mostly unexplored for the computation of excited-state energies. Here, we show that, within a…

Chemical Physics · Physics 2018-08-09 Anthony Scemama , Anouar Benali , Denis Jacquemin , Michel Caffarel , Pierre-François Loos

In this paper, we evaluate the accuracy of the Hermitian form of the downfolding procedure utilizing the double unitary coupled cluster Ansatz (DUCC) on the H6 and H8 benchmark systems. The computational infrastructure employs the…

Quantum Physics · Physics 2023-05-18 Karol Kowalski , Bo Peng , Nicholas P. Bauman

Fourth-order many-body corrections to matrix elements for atoms with one valence electron are derived. The obtained diagrams are classified using coupled-cluster-inspired separation into contributions from n-particle excitations from the…

Atomic Physics · Physics 2009-11-07 Andrei Derevianko , Erik D. Emmons

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

We investigate the accuracy of a number of wavefunction based methods at the heart of quantum chemistry for metallic systems. Using Hartree-Fock as a reference, perturbative (M{\o}ller-Plesset, MP) and coupled cluster (CC) theories are used…

Chemical Physics · Physics 2013-10-24 James J. Shepherd , Andreas Grüneis

We derive and implement a new way of solving coupled cluster equations with lower computational scaling. Our method is based on decomposition of both amplitudes and two electron integrals, using a combination of tensor hypercontraction and…

Chemical Physics · Physics 2020-05-14 Roman Schutski , Jinmo Zhao , Thomas M. Henderson , Gustavo E. Scuseria

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

State-specific approximations can provide an accurate representation of challenging electronic excitations by enabling relaxation of the electron density. While state-specific wave functions are known to be local minima or saddle points of…

Chemical Physics · Physics 2022-01-06 Hugh G. A. Burton

We calculate the energies of ground and three low lying excited states of confined helium atom centered in an impenetrable spherical box. We perform the calculation by employing variational method with two-parameter variational forms for…

Atomic Physics · Physics 2009-11-11 Arup Banerjee , C. Kamal , Avijit Chowdhury

We propose a multireference linearized coupled cluster theory using matrix product states (MPS-LCC) which provides remarkably accurate ground-state energies, at a computational cost that has the same scaling as multireference configuration…

Chemical Physics · Physics 2015-09-02 Sandeep Sharma , Ali Alavi

We explore the possibility of calculating electronic excited states by using perturbation theory along a range-separated adiabatic connection. Starting from the energies of a partially interacting Hamiltonian, a first-order correction is…

Chemical Physics · Physics 2014-12-15 Elisa Rebolini , Julien Toulouse , Andrew M. Teale , Trygve Helgaker , Andreas Savin

We present a variational Monte Carlo algorithm for estimating the lowest excited states of a quantum system which is a natural generalization of the estimation of ground states. The method has no free parameters and requires no explicit…

Computational Physics · Physics 2024-09-04 David Pfau , Simon Axelrod , Halvard Sutterud , Ingrid von Glehn , James S. Spencer

The variational quantum eigensolver has been proposed as a low-depth quantum circuit that can be employed to examine strongly correlated systems on today's noisy intermediate-scale quantum computers. We examine details associated with the…

Quantum Physics · Physics 2020-08-26 Luogen Xu , Joseph T. Lee , J. K. Freericks

Pair vibrations are studied for a Hamiltonian with neutron-neutron, proton-proton and neutron-proton pairing. The spectrum is found to be rich in strongly correlated, low-lying excited states. Changing theratio of diagonal to off-diagonal…

Nuclear Theory · Physics 2010-02-09 R. R. Chasman , P. Van Isacker

When the number of strongly correlated electrons becomes larger, the single-reference coupled-cluster (CC) CCSD, CCSDT, etc. hierarchy displays an erratic behavior, while traditional multi-reference approaches may no longer be applicable…

Chemical Physics · Physics 2025-12-12 Ilias Magoulas , Jun Shen , Piotr Piecuch

A balanced description of ground and excited states is essential for the description of many chemical processes. However, few methods can handle cases where static correlation is present, and often these scale very unfavourably with system…

Chemical Physics · Physics 2019-05-08 Hugh G. A. Burton , Alex J. W. Thom

This work presents a series of highly-accurate excited-state properties obtained using high-order coupled-cluster (CC) calculations performed with a series of diffuse containing basis sets, as well as extensive comparisons with experimental…

Chemical Physics · Physics 2021-06-14 Amara Chrayteh , Aymeric Blondel , Pierre-François Loos , Denis Jacquemin

We present a reduced-cost equation-of-motion coupled-cluster method for excited states, built on a new state-specific frozen natural orbital (SS-FNO) framework. This approach enables systematic and controllable truncation of the virtual…

Chemical Physics · Physics 2025-07-24 Amrita Manna , Achintya Kumar Dutta

The performance of quantum algorithms for ground-state energy estimation is directly impacted by the quality of the initial state, where quality is traditionally defined in terms of the overlap of the input state with the target state. An…

Variational calculations of excited electronic states are carried out by finding saddle points on the surface that describes how the energy of the system varies as a function of the electronic degrees of freedom. This approach has several…

Chemical Physics · Physics 2023-02-15 Yorick L. A. Schmerwitz , Gianluca Levi , Hannes Jónsson
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