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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 an implementation of equation-of-motion oscillator strengths for the multilevel CCSD (MLCCSD) model where CCS is used as the lower level method (CCS/CCSD). In this model, the double excitations of the cluster operator are…

Chemical Physics · Physics 2020-09-21 Sarai D. Folkestad , Henrik Koch

We present an efficient implementation of the low-cost linear-response coupled-cluster singles and doubles (LR-CCSD) method for computing static and frequency-dependent polarizabilities in systems with significant relativistic and…

Chemical Physics · Physics 2026-04-15 Sudipta Chakraborty , Muskan Begom , Xubo Wang , Achintya Kumar Dutta

We investigate the coupling of different quantum-embedding approaches with a third molecular-mechanics layer, which can be either polarizable or non-polarizable. In particular, such a coupling is discussed for the multilevel families of…

Chemical Physics · Physics 2020-12-11 Linda Goletto , Tommaso Giovannini , Sarai D. Folkestad , Henrik Koch

Multicomponent systems are defined as chemical systems that require a quantum mechanical description of two or more different types of particles. Non-Born-Oppenheimer electron-nuclear interactions in molecules, electron-hole interactions in…

Chemical Physics · Physics 2015-10-21 Benjamin H. Ellis , Somil Aggarwal , Arindam Chakraborty

A novel implementation of the coupled-cluster singles and doubles (CCSD) approach is presented that is specifically tailored for the treatment of large, symmetric systems. It fully exploits Abelian point-group symmetry and the use of the…

Chemical Physics · Physics 2023-12-07 Tommaso Nottoli , Jürgen Gauss , Filippo Lipparini

In the present article, we introduce the relativistic Cholesky-decomposed density (CDD) matrix second-order M{\o}ller-Plesset perturbation theory (MP2) energies. The working equations are formulated in terms of the usual intermediates of…

Chemical Physics · Physics 2018-12-26 Benjamin Helmich-Paris , Michal Repisky , Lucas Visscher

We present a novel energy-based localization procedure able to localize molecular orbitals into specific spatial regions. The method is applied to several cases including both conjugated and non-conjugated systems. The obtained localized…

Chemical Physics · Physics 2022-09-13 Tommaso Giovannini , Henrik Koch

Localized orbital coupled cluster theory has recently emerged as an nonempirical alternative to DFT for large systems. Intuitively, one might expect such methods to perform less well for highly delocalized systems. In the present work, we…

Chemical Physics · Physics 2020-10-16 Nitai Sylvetsky , Ambar Banerjee , Mercedes Alonso , Jan M. L. Martin

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

A comprehensive theoretical understanding of electron-photon correlation is essential for describing the reshaping of molecular orbitals in quantum electrodynamics (QED) environments. The strong coupling QED Hartree-Fock (SC-QED-HF) theory…

Chemical Physics · Physics 2024-09-04 Yassir El Moutaoukal , Rosario R. Riso , Matteo Castagnola , Henrik Koch

Accurate many-body treatments of condensed-phase systems are challenging because correlated solvers such as full configuration interaction (FCI) and the density matrix renormalization group (DMRG) scale exponentially with system size.…

A fast stochastic method for calculating the 2nd order M{\o}ller-Plesset (MP2) correction to the correlation energy of large systems of electrons is presented. The approach is based on reducing the exact summation over occupied and…

Chemical Physics · Physics 2012-12-12 Daniel Neuhauser , Eran Rabani , Roi Baer

An efficient perturbational treatment of spin-orbit coupling within the framework of high-level multi-reference techniques has been implemented in the most recent version of the COLUMBUS quantum chemistry package, extending the existing…

An efficiency of the Tucker decomposition of amplitude tensors within the single-reference relativistic coupled cluster method with single and double excitations (RCCSD) was studied in a series of benchmark calculations for (AuCl)$_n$…

Computational Physics · Physics 2025-07-29 Alexander V. Oleynichenko , Artem S. Rumiantsev , Andrei Zaitsevskii , Ephraim Eliav

A second-order many-body perturbation correction to the relativistic Dirac-Hartree-Fock energy is evaluated stochastically by integrating 13-dimensional products of four-component spinors and Coulomb potentials. The integration in the real…

Quantum Physics · Physics 2022-06-16 J. César Cruz , Jorge Garza , Takeshi Yanai , So Hirata

We apply the microscopic coupled-cluster method (CCM) to the spin-$1\over2$ $XXZ$ models on both the one-dimensional chain and the two-dimensional square lattice. Based on a systematic approximation scheme of the CCM developed by us…

Condensed Matter · Physics 2017-08-24 R. F. Bishop , R. G. Hale , Y. Xian

We present an implementation and analysis of a stochastic high performance algorithm to calculate the correlation energy of three dimensional periodic systems in second-order M{\o}ller-Plesset perturbation theory (MP2). In particular we…

Chemical Physics · Physics 2018-02-12 Tobias Schäfer , Benjamin Ramberger , Georg Kresse

We present a new linear scaling method for the energy minimization step of semiempirical and first-principles Hartree-Fock and Kohn-Sham calculations. It is based on the self-consistent calculation of the optimum localized orbitals of any…

Materials Science · Physics 2009-11-10 Luis Seijo , Zoila Barandiaran

We present second-order molecular cluster perturbation theory (MCPT(2)), a linear scaling methodology to calculate arbitrarily large systems with explicit calculation of individual wavefunctions in a coupled-cluster framework. This new…

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