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A reliable and efficient computation of the entire single-particle spectrum of correlated molecules is an outstanding challenge in the field of quantum chemistry, with standard density functional theory approaches often giving an inadequate…

Chemical Physics · Physics 2021-10-08 Oliver J. Backhouse , Alejandro Santana-Bonilla , George H. Booth

Quantum computation is one of the most promising new paradigms for the simulation of physical systems composed of electrons and atomic nuclei, with applications in chemistry, solid-state physics, materials science, and molecular biology.…

Quantum Physics · Physics 2024-11-05 Jakob Günther , Alberto Baiardi , Markus Reiher , Matthias Christandl

We present a new implementation of DMRG-based tailored coupled clusters method (TCCSD), which employs the domain-based local pair natural orbital approach (DLPNO-TCCSD). Compared to the previous LPNO version of the method, the new…

Chemical Physics · Physics 2020-05-08 Jakub Lang , Andrej Antalík , Libor Veis , Jan Brandejs , Jiří Brabec , Örs Legeza , Jiří Pittner

We present a new model for the study of spin-orbit coupling in interacting quasi-one-dimensional systems and solve it exactly to find the spectral properties of such systems. We show that the combination of spin-orbit coupling and…

Mesoscale and Nanoscale Physics · Physics 2009-10-31 A. V. Moroz , K. V. Samokhin , C. H. W. Barnes

An electrodynamical coupled cluster (CC) methodology starting from a covariant formalism and an equal time approximation, and finally based on the Dirac-Fock picture of the electron and positron fields and Coulomb gauge, is given here. The…

Atomic Physics · Physics 2019-04-30 Sambhu N. Datta

The multi-reference Coupled Cluster method first proposed by Meller et al (J. Chem. Phys. 1996) has been implemented and tested. Guess values of the amplitudes of the single and double excitations (the ${\hat T}$ operator) on the top of the…

Chemical Physics · Physics 2016-04-11 Emmanuel Giner , Grégoire David , Anthony Scemama , Jean Paul Malrieu

Quantum mechanical calculations of core electron binding energies (CEBEs) leading to 2p hole states are relevant to interpreting L-edge x-ray photo-electron spectroscopy (XPS), as well as higher edges. Orbital-optimized density functional…

Chemical Physics · Physics 2025-07-31 Richard Kang , Leonardo A. Cunha , Diptarka Hait , Martin Head-Gordon

We incorporate explicit, non-perturbative treatment of spin-orbit coupling into ab initio auxiliary-field quantum Monte Carlo (AFQMC) calculations. The approach allows a general computational framework for molecular and bulk systems in…

Strongly Correlated Electrons · Physics 2023-02-16 Brandon Eskridge , Henry Krakauer , Hao Shi , Shiwei Zhang

Multi-configurational wave functions are known to describe electronic structure across a Born-Oppenheimer surface qualitatively correct. However, for quantitative reaction energies, dynamical correlation originating from the many…

Chemical Physics · Physics 2020-04-16 Christopher J. Stein , Markus Reiher

Numerical simulations of quantum spin models are crucial for a profound understanding of many-body phenomena in a variety of research areas in physics. An outstanding problem is the availability of methods to tackle systems that violate…

Quantum Physics · Physics 2023-05-31 Fabian Köhler , Rick Mukherjee , Peter Schmelcher

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

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

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…

A unitary coupled-cluster (UCC) form for the wavefunction in the variational quantum eigensolver has been suggested as a systematic way to go beyond the mean-field approximation and include electron correlation in solving quantum chemistry…

Quantum Physics · Physics 2018-09-12 Ilya G. Ryabinkin , Tzu-Ching Yen , Scott N. Genin , Artur F. Izmaylov

The tailored coupled cluster (TCC) approach is a promising ansatz that preserves the simplicity of single-reference coupled cluster theory, while incorporating a multi-reference wave function through amplitudes obtained from a preceding…

Chemical Physics · Physics 2021-01-07 Maximilian Mörchen , Leon Freitag , Markus Reiher

The dynamics of the nuclear-spin quantum computer with large number (L=1000) of qubits is considered using a perturbation approach, based on approximate diagonalization of exponentially large sparse matrices. Small parameters are introduced…

Quantum Physics · Physics 2007-05-23 G. P. Berman , D. I. Kamenev , V. I. Tsifrinovich

Perturbative and non-perturbative expansion methods already constitute a tool of choice to perform ab initio calculations over a significant part of the nuclear chart. In this context, the categories of accessible nuclei directly reflect…

Nuclear Theory · Physics 2022-01-28 Mikael Frosini , Thomas Duguet , Jean-Paul Ebran , Vittorio Somà

We developed a general theoretical approach and a user-ready computer code that permit to study the dynamics of collisional energy transfer and ro-vibrational energy exchange in complex molecule-molecule collisions. The method is a mixture…

Chemical Physics · Physics 2024-02-06 Carolin Joy , Bikramaditya Mandal , Dulat Bostan , Marie-Lise Dubernet , Dmitri Babikov

The d-wave pairing correlations along with spin correlation are calculated with quantum Monte Carlo method for the two-dimensional Hubbard model on lattice structures representing organic superconductors $\kappa$-(BEDT-TTF)$_2$X and…

Strongly Correlated Electrons · Physics 2009-10-31 Kazuhiko Kuroki , Hideo Aoki

We develop a static quantum embedding scheme that utilizes different levels of approximations to coupled cluster (CC) theory for an active fragment region and its environment. To reduce the computational cost, we solve the local fragment…

Chemical Physics · Physics 2024-11-13 Avijit Shee , Fabian M. Faulstich , Birgitta Whaley , Lin Lin , Martin Head-Gordon