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Doubly occupied configuration interaction (DOCI) with optimized orbitals often accurately describes strong correlations while working in a Hilbert space much smaller than that needed for full configuration interaction. However, the scaling…

Chemical Physics · Physics 2016-02-25 Thomas M. Henderson , Ireneusz W. Bulik , Tamar Stein , Gustavo E. Scuseria

The (T) and [T] perturbative corrections are derived for multicomponent coupled-cluster theory with single and double excitations (CCSD). Benchmarking shows that multicomponent CCSD methods that include the perturbative corrections are more…

Chemical Physics · Physics 2022-07-01 Dylan Fowler , Kurt R. Brorsen

Hybrid quantum-classical approaches offer potential solutions to quantum chemistry problems, yet they often manifest as constrained optimization problems. Here, we explore the interconnection between constrained optimization and generalized…

Quantum Physics · Physics 2025-03-27 Muqing Zheng , Bo Peng , Ang Li , Xiu Yang , Karol Kowalski

Coupled-cluster theory with single and double excitations (CCSD) is a promising ab initio method for the electronic structure of three-dimensional metals, for which second-order perturbation theory (MP2) diverges in the thermodynamic limit.…

Materials Science · Physics 2021-06-16 James M. Callahan , Malte F. Lange , Timothy C. Berkelbach

The variational quantum eigensolver (or VQE) uses the variational principle to compute the ground state energy of a Hamiltonian, a problem that is central to quantum chemistry and condensed matter physics. Conventional computing methods are…

The atmospheric reaction of H$_2$S with Cl has been reinvestigated to check if, as previously suggested, only explicit dynamical computations can lead to an accurate evaluation of the reaction rate because of strong recrossing effects and…

Chemical Physics · Physics 2020-07-21 Jacopo Lupi , Cristina Puzzarini , Carlo Cavallotti , Vincenzo Barone

Intensity enhancement in vibrational circular dichroism (VCD) arises in open-shell transition metal complexes from coupling between ground-state vibrational transitions and magnetic dipole-allowed transitions to low-lying excited states…

Chemical Physics · Physics 2025-07-08 Mariia Sapova , Chandan Kumar , Sahar Ashtari-Jafari , Wybren J. Buma , Lucas Visscher

A method is presented in which the ground-state subspace is projected out of a Hamiltonian representation. As a result of this projection, an effective Hamiltonian is constructed where its ground-state coincides with an excited-state of the…

Quantum Physics · Physics 2023-08-14 P. Jouzdani , S. Bringuier , M. Kostuk

We present relativistic coupled-cluster (CC) calculations of energies, magnetic-dipole hyperfine constants, and electric-dipole transition amplitudes for low-lying states of atomic boron. The trivalent boron atom is computationally treated…

Atomic Physics · Physics 2015-06-05 H. Gharibnejad , A. Derevianko

We present a comprehensive relativistic coupled cluster study of the electronic structures of the ThO and ThS molecules in the spinor basis. Specifically, we use the single-reference coupled cluster and the multi-reference Fock Space…

Chemical Physics · Physics 2020-02-18 Paweł Tecmer , Cristina E. González-Espinoza

This chapter gives an introduction to qualitative and quantitative topological analyses of molecular electronic transitions. Among the possibilities for qualitatively describing how the electronic structure of a molecule is reorganized upon…

Chemical Physics · Physics 2018-11-27 Thibaud Etienne

In quantum chemistry, the variational quantum eigensolver (VQE) is a promising algorithm for molecular simulations on near-term quantum computers. However, VQEs using hardware-efficient circuits face scaling challenges due to the barren…

Quantum Physics · Physics 2024-09-27 Rui Mao , Guojing Tian , Xiaoming Sun

We present the working equations for a reduced-scaling method of evaluating the perturbative triples (T) energy in coupled-cluster theory, through the tensor hypercontraction (THC) of the triples amplitudes ($t_{ijk}^{abc}$). Through our…

Chemical Physics · Physics 2024-06-12 Andy Jiang , Justin M. Turney , Henry F. Schaefer

We develop strong-coupling series expansion methods to study two-particle spectra of quantum lattice models. At the heart of the method lies the calculation of an effective Hamiltonian in the two-particle subspace. We explicitly consider an…

Strongly Correlated Electrons · Physics 2008-03-26 Weihong Zheng , C. J. Hamer , R. R. P. Singh , Simon Trebst , Hartmut Monien

Time-dependent coupled-cluster method with time-varying orbital functions, called time-dependent optimized coupled- cluster (TD-OCC) method, is formulated for multielectron dynamics in an intense laser field. We have successfully derived…

Chemical Physics · Physics 2018-03-14 Takeshi Sato , Himadri Pathak , Yuki Orimo , Kenichi L. Ishikawa

Convergence properties of the variational cluster approach with respect to the variational parameter space, cluster size, and boundary conditions of the reference system are investigated and discussed for bosonic many-body systems.…

Strongly Correlated Electrons · Physics 2010-06-21 Michael Knap , Enrico Arrigoni , Wolfgang von der Linden

The curse of dimensionality (COD) limits the current state-of-the-art {\it ab initio} propagation methods for non-relativistic quantum mechanics to relatively few particles. For stationary structure calculations, the coupled-cluster (CC)…

Quantum Physics · Physics 2015-06-03 Simen Kvaal

We use non-perturbative linked-cluster expansions to determine the ground-state energy per site of the spin-one Heisenberg model on the kagome lattice. To this end, a parameter is introduced allowing to interpolate between a fully…

Strongly Correlated Electrons · Physics 2015-12-09 D. Ixert , T. Tischler , K. P. Schmidt

We implement the Fock-space perturbed relativistic coupled-cluster theory to compute the electric dipole polarizability of ground and low lying excited states, and nuclear spin-dependent parity violating (NSD-PNC) transition amplitudes in…

Atomic Physics · Physics 2024-12-17 Suraj Pandey , Ravi Kumar , D. Angom , B. K. Mani

We introduce and benchmark a systematically improvable route for excited-state calculations, state-specific configuration interaction ($\Delta$CI), \alert{which is a particular realization of multiconfigurational self-consistent field and…

Chemical Physics · Physics 2023-08-31 Fábris Kossoski , Pierre-François Loos