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We present a massive-parallel implementation of the resolution-of-identity (RI) coupled-cluster approach that includes single, double and perturbatively triple excitations, namely RI-CCSD(T), in the FHI-aims package for molecular systems. A…

Computational Physics · Physics 2018-10-19 Tonghao Shen , Igor Ying Zhang , Matthias Scheffler

The issue of orbital relaxation in computational core-hole spectroscopy, specifically x-ray absorption, has been a major problem for methods such as equation-of-motion coupled cluster with singles and doubles (EOM-CCSD). The…

Chemical Physics · Physics 2025-03-26 Megan Simons , Devin A. Matthews

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

Time-dependent density-functional theory (TDDFT) is widely used to describe electronic excitations in complex finite systems with large numbers of atoms, such as biomolecules and nanocrystals. The first part of this paper will give a simple…

Materials Science · Physics 2008-08-15 C. A. Ullrich , V. Turkowski

We develop a coupled-cluster theory for bosonic mixtures of binary species in external traps, providing a promising theoretical approach to demonstrate highly accurately the many-body physics of mixtures of Bose-Einstein condensates. The…

Quantum Gases · Physics 2024-02-01 Anal Bhowmik , Ofir E. Alon

Multi-configurational approaches yield universal wave function parameterizations that can qualitatively well describe electronic structures along reaction pathways. For quantitative results, multi-reference perturbation theory is required…

Chemical Physics · Physics 2016-09-08 Christopher J. Stein , Vera von Burg , Markus Reiher

We study possible optically excited bound states in monolayer MoS2: excitons and trions. For this purpose we formulate and apply a generalized time-dependent density-matrix functional approach for bound states of multiple excitations. The…

Mesoscale and Nanoscale Physics · Physics 2014-02-18 Alfredo Ramirez-Torres , Volodymyr Turkowski , Talat S. Rahman

The atomistic resolution recently achieved by ultrafast spectroscopies demands corresponding theoretical advances. Real-time time-dependent density-functional theory (RT-TDDFT) with Ehrenfest dynamics offers an optimal trade-off between…

Materials Science · Physics 2022-10-19 Jannis Krumland , Matheus Jacobs , Caterina Cocchi

In this work, we introduce a differentiable implementation of the local natural orbital coupled cluster (LNOCC) method within the automatic differentiation framework of the PySCFAD package. The implementation is comprehensively tuned for…

Chemical Physics · Physics 2024-07-08 Xing Zhang , Chenghan Li , Hong-Zhou Ye , Timothy C. Berkelbach , Garnet Kin-Lic Chan

The impact of residual electron correlation beyond the equation-of-motion coupled-cluster singles and doubles approximation (EOM-CCSD) on positions and widths of electronic resonances is investigated. To establish a method that accomplishes…

Chemical Physics · Physics 2018-02-14 Thomas-C. Jagau

Coupled cluster theory has had a momentous impact on the ab initio prediction of molecular properties, and remains a staple ingratiate in high-accuracy thermochemical model chemistries. However, these methods require inclusion of at least…

Chemical Physics · Physics 2025-03-26 James H. Thorpe , Zachary W. Windom , Rodney J. Bartlett , Devin A. Matthews

We introduce an analytical framework to calculate the values of key observables in a strongly disordered discrete time crystal (DTC) without fitting parameter. The perturbatively obtained closed-form formulae show quantitative agreement…

Disordered Systems and Neural Networks · Physics 2025-12-25 Yang-Ren Liu , Biao Huang

The coupled cluster iteration scheme for determining the cluster amplitudes involves a set of nonlinearly coupled difference equations. In the space spanned by the amplitudes, the set of equations are analysed as a multivariate…

With growing demand for time-domain simulations of correlated many-body systems, the development of efficient and stable integration schemes for the time-dependent Schr\"odinger equation is of keen interest in modern electronic structure…

Chemical Physics · Physics 2023-08-22 David B. Williams-Young , Stephen Yuwono , A. Eugene DePrince , Chao Yang

We introduce a generic scheme to perform non-perturbative linked cluster expansions in long-range ordered quantum phases. Clusters are considered to be surrounded by an ordered reference state leading to effective edge-fields in the exact…

Strongly Correlated Electrons · Physics 2016-11-22 D. Ixert , K. P. Schmidt

We present an ab initio study of electronically excited states of three-dimensional solids using Gaussian-based periodic equation-of-motion coupled-cluster theory with single and double excitations (EOM-CCSD). The explicit use of…

Materials Science · Physics 2020-01-31 Xiao Wang , Timothy C. Berkelbach

The recent quantum information boom has effected a resurgence of interest in unitary coupled cluster (UCC) theory. Our group's interest in local energy landscapes of unitary ans\"atze prompted us to investigate the classical approach of…

Chemical Physics · Physics 2022-11-01 Harper R. Grimsley , Nicholas J. Mayhall

We extend our assessment of the potential of perturbative coupled cluster (CC) expansions for a test set of open-shell atoms and organic radicals to the description of quadruple excitations. Namely, the second- through sixth-order models of…

Chemical Physics · Physics 2016-05-17 Janus J. Eriksen , Devin A. Matthews , Poul Jørgensen , Jürgen Gauss

We examine the contributions from triple excitation cluster operators in the relativistic coupled-cluster theory in atoms and ions. For this, we propose a tensor representation of the triple cluster operator. Based on this representaion and…

Atomic Physics · Physics 2015-03-19 B. K. Mani , Dilip Angom

We derive and implement a new way of solving coupled cluster equations with lower computational scaling. Our method is based on decomposition of both amplitudes and two electron integrals, using a combination of tensor hypercontraction and…

Chemical Physics · Physics 2020-05-14 Roman Schutski , Jinmo Zhao , Thomas M. Henderson , Gustavo E. Scuseria