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Achieving chemical accuracy for strongly correlated molecules is a defining milestone for first-generation, fault-tolerant quantum computers, yet the factorial growth of three, four, and six-index tensor contractions in coupled-cluster…

Coupled cluster theory is an attractive tool to solve the quantum many-body problem because its singles and doubles (CCSD) approximation is computationally affordable and yields about 90% of the correlation energy. Capturing the remaining…

Nuclear Theory · Physics 2024-02-16 Z. H. Sun , C. A. Bell , G. Hagen , T. Papenbrock

A new method that accurately describes strongly correlated states and captures dynamical correlation is presented. It is derived as a modification of coupled-cluster theory with single and double excitations (CCSD) through consideration of…

Chemical Physics · Physics 2013-07-15 Daniel Kats , Frederick R. Manby

We develop a quartic-scaling implementation of coupled-cluster singles and doubles based on low-rank tensor hypercontraction (THC) factorizations of both the electron repulsion integrals (ERIs) and the doubles amplitudes. This extends our…

Chemical Physics · Physics 2024-06-19 Edward G. Hohenstein , B. Scott Fales , Robert M. Parrish , Todd J. Martinez

The factorized form of unitary coupled cluster theory (UCC) is a promising wave-function ansatz for the variational quantum eigensolver algorithm. Here, we present a quantum inspired algorithm for UCC based on an exact operator identity for…

Strongly Correlated Electrons · Physics 2020-09-24 Jia Chen , Hai-Ping Cheng , James Freericks

While limited coupled cluster theory is \textit{formally} nonvariational, it is not broadly appreciated whether this is a major issue \textit{in practice}. We carried out a detailed comparison with \textit{de facto} full CI energies for a…

Chemical Physics · Physics 2024-10-03 Jan M. L. Martin , Emmanouil Semidalas

We investigate the basis-set convergence of electronic correlation energies calculated using coupled cluster theory and a recently proposed finite basis-set correction technique. The correction is applied to atomic and molecular systems and…

Chemical Physics · Physics 2019-10-03 Andreas Irmler , Andreas Grüneis

We investigate the use of orbital-optimized references in conjunction with single-reference coupled-cluster theory with single and double substitutions (CCSD) for the study of core excitations and ionizations of 18 small organic molecules,…

High-accuracy composite wavefunction methods like Weizmann-4 (W4) theory, high-accuracy extrapolated \textit{ab initio} thermochemistry (HEAT), and Feller-Peterson-Dixon (FPD) enable sub-kJ/mol accuracy in gas-phase thermochemical…

Chemical Physics · Physics 2024-04-12 Emmanouil Semidalas , Amir Karton , Jan M. L. Martin

Quantum-mechanical methods are widely used for understanding molecular interactions throughout biology, chemistry, and materials science. Quantum diffusion Monte Carlo (DMC) and coupled cluster with single, double, and perturbative triple…

Computationally efficient and accurate quantum mechanical approximations to solve the many-electron Schr\"odinger equation are at the heart of computational materials science. In that respect the coupled cluster hierarchy of methods plays a…

Materials Science · Physics 2022-01-11 Tina N. Mihm , Tobias Schäfer , Sai Kumar Ramadugu , Andreas Grüneis , James J. Shepherd

Coupled cluster methods based exclusively on double excitations are comparatively "cheap" and interesting model chemistries, as they are typically able to capture the bulk of the dynamical electron correlation effects. The trade-off in such…

Quantum Physics · Physics 2024-06-14 Zachary W. Windom , Daniel Claudino , Rodney J. Bartlett

The coupled cluster method (CCM) is a method of quantum many-body theory that may provide accurate results for the ground-state properties of lattice quantum spin systems even in the presence of strong frustration and for lattices of…

Strongly Correlated Electrons · Physics 2009-11-11 D. J. J. Farnell , J. Schulenburg , J. Richter , K. A. Gernoth

In the molecular quantum chemistry community, coupled-cluster (CC) methods are well-recognized for their systematic convergence and reliability. The extension of the theory to extended systems has been comparably recent, so that…

Chemical Physics · Physics 2024-10-31 Andreas Grüneis , Evgeny Moerman , Matthias Scheffler , Tonghao Shen , Igor Ying Zhang

The thermochemistry of the carbon clusters C$_n$ (n=2--10) has been revisited by means of W4 theory and W3.2lite theory. Particularly the larger clusters exhibit very pronounced post-CCSD(T) correlation effects. Despite this, our best…

Chemical Physics · Physics 2010-08-26 Amir Karton , Alex Tarnopolsky , Jan M. L. Martin

A unitary coupled-cluster (UCC) form for the wavefunction in the variational quantum eigensolver has been suggested as a systematic way to go beyond the mean-field approximation and include electron correlation in solving quantum chemistry…

Quantum Physics · Physics 2018-09-12 Ilya G. Ryabinkin , Tzu-Ching Yen , Scott N. Genin , Artur F. Izmaylov

Slater determinants have underpinned quantum chemistry for nearly a century, yet their full potential has remained challenging to exploit. In this work, we show that a variational wavefunction composed of a few hundred optimized…

Chemical Physics · Physics 2026-04-17 Clemens Giuliani , Jannes Nys , Rocco Martinazzo , Giuseppe Carleo , Riccardo Rossi

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 incorporate a solver for the fragment problem with accuracy beyond coupled cluster singles and doubles (CCSD) into the previously proposed static embedding framework, MPCC. To this end, we employ a CCSDT solver for the fragment…

Chemical Physics · Physics 2026-02-16 Avijit Shee , Fabian M. Faulstich , K. Birgitta Whaley , Lin Lin , Martin Head-Gordon

Elastic-scattering phase shifts for four-nucleon systems are studied in an $ab$-$initio$ type cluster model in order to clarify the role of the tensor force and to investigate cluster distortions in low energy $d+d$ and $t+p$ scattering. In…

Nuclear Theory · Physics 2015-05-28 S. Aoyama , K. Arai , Y. Suzuki , P. Descouvemont , D. Baye