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Unitary Coupled Cluster (UCC) theory is a promising variational method for electronic structure calculations, especially for strongly correlated systems and quantum computers. However, its practical application is limited by the steep…

Chemical Physics · Physics 2026-02-05 Prateek Vaish , Brenda Rubenstein

We present algebraic diagrammatic construction theory for simulating spin-orbit coupling and electron correlation in charged electronic states and photoelectron spectra. Our implementation supports Hartree-Fock and multiconfigurational…

Chemical Physics · Physics 2025-05-12 Rajat Majumder , Alexander Yu. Sokolov

A Cholesky decomposition (CD)-based implementation of relativistic two-component coupled-cluster (CC) and equation-of-motion CC (EOM-CC) methods using an exact two-component Hamiltonian augmented with atomic-mean-field spin-orbit integrals…

Chemical Physics · Physics 2023-09-19 Chaoqun Zhang , Filippo Lipparini , Stella Stopkowicz , Jürgen Gauss , Lan Cheng

We present a novel approach to spin-adapted coupled cluster theory. This approach is based on the entanglement of an open-shell molecule with electrons in a non-interacting bath; together they form a closed-shell state. For the total…

Chemical Physics · Physics 2023-05-22 Sarai Dery Folkestad , Bendik Støa Sannes , Henrik Koch

Lattice quantum chromodynamics (LQCD) has the promise of constraining low-energy constants (LECs) of nuclear effective field theories (EFTs) from first-principles calculations that incorporate the dynamics of quarks and gluons. Given the…

High Energy Physics - Lattice · Physics 2022-05-25 Zohreh Davoudi , Saurabh V. Kadam

We present a practical approach to treat static and dynamical correlation accurately in large multi-configurational systems. The static correlation is accounted for using the spin-flip approach which is well known for capturing static…

Strongly Correlated Electrons · Physics 2021-02-08 Oinam Romesh Meitei , Nicholas J. Mayhall

Coupled-cluster theory with single, double, and perturbative triple excitations (CCSD(T)) -- often considered the "gold standard" of main-group quantum chemistry -- is inapplicable to three-dimensional metals due to an infrared divergence,…

Materials Science · Physics 2023-03-21 Verena A. Neufeld , Timothy C. Berkelbach

We use perturbed relativistic coupled-cluster (PRCC) theory to calculate the electric dipole polarizability of noble gas atoms Ar, Kr, Xe and Rn. We also provide a detailed description of the nonlinear terms in the PRCC theory and consider…

Atomic Physics · Physics 2012-12-19 S. Chattopadhyay , B. K. Mani , D. Angom

We propose an approach to probe coherent spin-state dynamics of molecules using circularly polarized hard x-ray pulses. For the dynamically aligned nitric oxide molecules in a coherent superposition spin-orbit coupled electronic state that…

Optics · Physics 2024-01-02 Xiaoyu Mi , Ming Zhang , Zheng Li

We develop a method based on the relativistic coupled-cluster theory to incorporate a perturbative interaction to the no-pair Dirac-Coulomb atomic Hamiltonian. The method is general and suitable to incorporate any perturbation Hamiltonian…

Atomic Physics · Physics 2012-09-06 S. Chattopadhyay , B. K. Mani , D. Angom

Core-level spectra of 1s electrons of elements heavier than Ne show significant relativistic effects. We combine advances in orbital optimized DFT (OO-DFT) with the spin-free exact two-component (X2C) model for scalar relativistic effects,…

Chemical Physics · Physics 2022-04-19 Leonardo A. Cunha , Diptarka Hait , Richard Kang , Yuezhi Mao , Martin Head-Gordon

A relativistic coupled-cluster (RCC) theory is implemented to study electron impact excitations of atomic species. As a test case, the electron impact excitations of the $3s ~ ^2S_{1/2} - 3p ~ ^2P_{1/2;3/2}$ resonance transitions are…

Atomic Physics · Physics 2018-02-14 L. Sharma , B. K. Sahoo , P. Malkar , R. Srivastava

An implementation of coupled-cluster (CC) theory to treat atoms and molecules in finite magnetic fields is presented. The main challenges stem from the magnetic-field dependence in the Hamiltonian, or, more precisely, the appearance of the…

Chemical Physics · Physics 2015-09-02 Stella Stopkowicz , Jürgen Gauss , Kai K. Lange , Erik I. Tellgren , Trygve Helgaker

We present the quantum-selected configuration interaction-tailored coupled-cluster (QSCI-TCC) method, a hybrid quantum-classical scheme that tailors coupled-cluster (CC) theory with a quantum-selected configuration interaction (QSCI) wave…

Chemical Physics · Physics 2025-06-23 Luca Erhart , Yuichiro Yoshida , Wataru Mizukami

Machine learning is rapidly accelerating materials and chemical discovery, but most current models target energies, forces, or selected molecular properties rather than the underlying many-body electronic structure. Learning…

A relativistic description of the structure of heavy alkali atoms and alkali-like ions using S-spinors and L-spinors has been developed. The core wavefunction is defined by a Dirac-Fock calculation using an S-spinors basis. The S-spinor…

Atomic Physics · Physics 2017-01-05 Jun Jiang , J. Mitroy , Yongjun Cheng , Michael W. J. Bromley

We present a spin-free, size-extensive, and size-consistent coupled cluster method based on a generalised normal ordered exponential ansatz. This approach is a natural generalisation of single-reference coupled cluster theory for arbitrary…

Chemical Physics · Physics 2025-07-21 Nicholas Lee , David P. Tew

We introduce the electron attachment equation-of-motion pair coupled cluster doubles (EA-EOM-pCCD) ansatz, which allows us to inexpensively compute electron affinities, energies of unoccupied orbitals, and electron attachment spectra. We…

Chemical Physics · Physics 2024-06-24 Marta Gałyńska , Paweł Tecmer , Katharina Bogusławski

We present a precise fully relativistic numerical solution of the two-center Coulomb problem. The special case of unit nuclear charges is relevant for the accurate description of the ${\rm H}_2^+$ molecular ion and its isotopologues,…

Quantum Physics · Physics 2022-05-11 O. Kullie , S. Schiller

"Addition-by-subtraction" coupled cluster (CC) approaches provide a promising approach to treating the difficult strong correlation problem by simplifying the standard CC equations. In a separate vein, linearized CC methods have drawn…

Strongly Correlated Electrons · Physics 2026-03-02 Sylvia J. Bintrim , Ella R. Ransford , Kevin Carter-Fenk