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The study and prediction of chemical reactivity is one of the most important application areas of molecular quantum chemistry. Large-scale, fully error-tolerant quantum computers could provide exact or near-exact solutions to the underlying…

Quantum Physics · Physics 2019-09-12 Michael Kühn , Sebastian Zanker , Peter Deglmann , Michael Marthaler , Horst Weiß

State-of-the-art many-body wave function techniques rely on heuristics to achieve high accuracy at an attainable cost to solve the many-body Schr\"odinger equation. By far the most common property used to assess accuracy has been the total…

Chemical Physics · Physics 2022-11-30 Shunyue Yuan , Yueqing Chang , Lucas K. Wagner

Accurately treating strong electron correlation in quantum chemistry typically requires multireference wave-function methods with steep computational scaling. The recently proposed i-DMFT method promises near configuration-interaction…

Chemical Physics · Physics 2026-04-23 Paul G. Graf , Florian Matz , Lexin Ding , Julia Liebert , Markus Penz , Christian Schilling

We introduce a theoretical approach to study the quantum-dissipative dynamics of electronic excitations in macromolecules, which enables to perform calculations in large systems and cover long time intervals. All the parameters of the…

Mesoscale and Nanoscale Physics · Physics 2016-07-20 S. A Beccara , F. Mascherpa , E. Schneider , P. Faccioli

By splitting the Coulomb interaction into long-range and short-range components, we decompose the energy of a quantum electronic system into long-range and short-range contributions. We show that the long-range part of the energy can be…

Chemical Physics · Physics 2009-11-10 Julien Toulouse , Francois Colonna , Andreas Savin

The expensive cost of computing exact exchange in periodic systems limits the application range of density functional theory with hybrid functionals. To reduce the computational cost of exact change, we present a range-separated algorithm…

Chemical Physics · Physics 2023-07-26 Qiming Sun

We propose a general approach to reducing basis set incompleteness error in electron correlation energy calculations. The correction is computed alongside the correlation energy in a single calculation by modifying the electron interaction…

A way to account for correlations between the chemically active (valence) and innermore (core) electrons in the framework of the generalized relativistic effective core potential (GRECP) method is suggested. The "correlated" GRECP's…

Chemical Physics · Physics 2009-11-10 N. S. Mosyagin , A. V. Titov

Separating the Coulomb potential into short-range and long-range components enables the use of different electron repulsion integral algorithms for each component. The short-range part can be efficiently computed using the analytical…

Chemical Physics · Physics 2023-09-27 Qiming Sun

In this chapter we focus first on the theoretical methods and relevant computational approaches to calculate the electronic structure of atoms, molecules, and clusters containing heavy elements for which relativistic effects become…

Chemical Physics · Physics 2021-10-05 Simone Taioli , Stefano Simonucci

We present a realistic study for electronic and magnetic properties in dilute magnetic semiconductor (Ga,Mn)As. A multi-orbital Haldane-Anderson model parameterized by density-functional calculations is presented and solved with the…

The cluster-in-molecule (CIM) local correlation approach with an accurate distant pair correlation energy correction is presented. For large systems, the inclusion of distant pair correlation energies is essential for the accurate…

Chemical Physics · Physics 2020-08-06 Zhigang Ni , Yang Guo , Frank Neese , Wei Li , Shuhua Li

We propose a Jastrow factor for electron-electron correlations that interpolates between the radial symmetry of the Coulomb interaction at short inter-particle distance and the space-group symmetry of the simulation cell at large…

Strongly Correlated Electrons · Physics 2016-08-10 T. M. Whitehead , M. H. Michael , G. J. Conduit

A model subspace configuration interaction method is developed to obtain chemically accurate electron correlations by diagonalising a very compact effective Hamiltonian of realistic molecule. The construction of the effective Hamiltonian is…

Chemical Physics · Physics 2022-10-18 Jiasheng Li , Jun Yang

With a transcorrelated Hamiltonian, we perform a many body perturbation (MBPT) calculation on the uniform electron gas in the high density regime. By using a correlation factor optimised for a single determinant Jastrow ansatz, the second…

Computational Physics · Physics 2024-06-19 Hongjun Luo , Ali Alavi

We propose a general method for constructing system-dependent basis functions for correlated quantum chemical calculations. Our construction combines features from several traditional approaches: plane waves, localized basis functions, and…

Chemical Physics · Physics 2018-02-28 Thomas E. Baker , Kieron Burke , Steven R. White

Calculations of transition energies between low-lying states of mercury atom are performed in the frame of combined CI/MBPT2 method. Results of all-electron relativistic calculations (using the Dirac-Coulomb Hamiltonian) are compared with…

Atomic Physics · Physics 2007-05-23 N. Mosyagin , M. Kozlov , A. Titov

A method and codes for two-step correlation calculation of heavy-atom molecules have been developed, employing the generalized relativistic effective core potential and relativistic coupled cluster (RCC) methods at the first step, followed…

Chemical Physics · Physics 2009-11-07 A. N. Petrov , N. S. Mosyagin , T. A. Isaev , A. V. Titov , V. F. Ezhov , E. Eliav , U. Kaldor

A range-separated double-hybrid (RSDH) scheme which generalizes the usual range-separated hybrids and double hybrids is developed. This scheme consistently uses a two-parameter Coulomb-attenuating-method (CAM)-like decomposition of the…

Chemical Physics · Physics 2018-05-23 Cairedine Kalai , Julien Toulouse

Evaluating multi-center molecular integrals with Cartesian Gaussian-type basis sets has been a long-standing bottleneck in electronic structure theory calculation for solids and molecules. We have developed a vector-coupling and…

Quantum Physics · Physics 2024-05-17 Hang Hu , Gilles Peslherbe , Hsu Kiang Ooi , Anguang Hu