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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

Introducing an active space approximation is inevitable for the quantum computations of chemical systems. However, this approximation ignores the electron correlations related to non-active orbitals. Here, we propose a computational method…

Quantum Physics · Physics 2024-06-06 Luca Erhart , Yuichiro Yoshida , Viktor Khinevich , Wataru Mizukami

We present a perturbative triples correction to the relativistic quadratic unitary coupled cluster singles and doubles (qUCCSD) method, denoted as qUCCSD[T]. The method builds upon the Hermitian structure of the unitary ansatz and employs a…

Chemical Physics · Physics 2025-10-08 Kamal Majee , Ján Šimunek , Jozef Noga , Achintya Kumar Dutta

Excited states exhibiting double excitation character are notoriously difficult to model using conventional single-reference methods, such as adiabatic time-dependent density-functional theory (TD-DFT) or equation-of-motion coupled cluster…

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)…

Chemical Physics · Physics 2026-04-17 Rahul Chakraborty , Paweł Tecmer

We present the first application to real molecular systems of the recently proposed linear-response theory for the density-based basis-set correction method [J. Chem. Phys. 158, 234107 (2023)]. We apply this approach to accelerate the…

Chemical Physics · Physics 2024-02-27 Diata Traore , Julien Toulouse , Emmanuel Giner

The accurate description of doubly-excited states using conventional electronic structure methods is remarkably challenging, primarily because such excited states require the inclusion of doubly or higher excited configurations or the…

Chemical Physics · Physics 2019-05-01 Katharina Boguslawski

We consider the sampling of the coupled cluster expansion within stochastic coupled cluster theory. Observing the limitations of previous approaches due to the inherently non-linear behaviour of a coupled cluster wavefunction representation…

Chemical Physics · Physics 2018-08-14 Charles J. C. Scott , Alex J. W. Thom

A unitary coupled-cluster (UCC)-based self-consistent electron propagator theory (EPT) is proposed for the description of electron-detached and electron-attached states. Two practical schemes, termed IP/EA-UCC3 and IP/EA-qUCCSD, are…

Chemical Physics · Physics 2026-03-03 Yu Zhang , Junzi Liu

We consider a system of two purely capacitively-coupled singlet-triplet qubits, and numerically simulate the energy structure of four electrons in two double quantum dots with a large potential barrier between them. We calculate the…

Mesoscale and Nanoscale Physics · Physics 2019-08-14 Donovan Buterakos , Robert E. Throckmorton , S. Das Sarma

We present an extension of the pair coupled cluster doubles (p-CCD) method to quasiparticles and apply it to the attractive pairing Hamiltonian. Near the transition point where number symmetry gets spontaneously broken, the proposed…

We introduce a black-box auxiliary field quantum Monte Carlo (AFQMC) approach to perform highly accurate electronic structure calculations using configuration interaction singles and doubles (CISD) trial states. This method consistently…

We propose a streamlined combination scheme of the transcorrelation (TC) and coupled cluster (CC) theory, which not only increases the convergence rate with respect to the basis set, but also extends the applicability of the lowest order CC…

Strongly Correlated Electrons · Physics 2021-07-28 Ke Liao , Thomas Schraivogel , Hongjun Luo , Daniel Kats , Ali Alavi

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…

Chemical Physics · Physics 2014-05-06 James J. Shepherd , Thomas. M. Henderson , Gustavo E. Scuseria

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 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

The coupled cluster method is considered a gold standard in quantum chemistry, reliably giving energies that are exact within chemical accuracy (1.6 mHartree). However, even in the CCSD approximation, where the cluster operator is truncated…

Chemical Physics · Physics 2023-03-10 Simon Elias Schrader , Simen Kvaal

Coupled cluster theory is a vital cornerstone of electronic structure theory and is being applied to ever-larger systems. Stochastic approaches to quantum chemistry have grown in importance and offer compelling advantages over traditional…

Cluster states, a special type of highly entangled states, are a universal resource for measurement-based quantum computation. Here, we propose an efficient one-step generation scheme for cluster states in semiconductor quantum dot…

Quantum Physics · Physics 2009-11-13 Guo-Ping Guo , Hui Zhang , Tao Tu , Guang-Can Guo

In this work, we derive working equations for the Linear Response pair Coupled Cluster Doubles (LR-pCCD) ansatz and its extension to singles (S), LR-pCCD+S. These methods allow us to compute electronic excitation energies and transition…

Chemical Physics · Physics 2025-03-18 Somayeh Ahmadkhani , Katharina Boguslawsk , Paweł Tecmer