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Computer simulation plays a central role in modern day materials science. The utility of a given computational approach depends largely on the balance it provides between accuracy and computational cost. Molecular crystals are a class of…

A variational solution procedure is reported for the many-particle no-pair Dirac-Coulomb-Breit Hamiltonian aiming at a parts-per-billion (ppb) convergence of the atomic and molecular energies, described within the fixed nuclei…

Quantum Physics · Physics 2024-06-19 Péter Jeszenszki , Dávid Ferenc , Edit Mátyus

A simple yet general method for constructing basis sets for molecular electronic structure calculations is presented. These basis sets consist of atomic natural orbitals from a multi-configurational self-consistent field calculation…

Materials Science · Physics 2015-05-19 F. R. Petruzielo , Julien Toulouse , C. J. Umrigar

A general procedure for the optimization of atomic density-fitting basis functions is designed with the balance between accuracy and numerical stability in mind. Given one-electron wavefunctions and energies, weights are assigned to the…

Chemical Physics · Physics 2020-10-13 Dimitri N. Laikov

Diffusion quantum Monte Carlo calculations with partial and full optimization of the guide function are carried out for the dissociation of the FeS molecule. For the first time, quantum Monte Carlo orbital optimization for transition metal…

Chemical Physics · Physics 2017-07-31 Kaveh Haghighi Mood , Arne Lüchow

We examine the application of the Variational Monte Carlo (VMC) method to a cluster model for halo nuclei. Particular attention is paid to the error estimate in the presence of correlations in the underlying random walk. We analyse the…

Nuclear Theory · Physics 2009-11-10 Theodoros Leontiou , Niels R. Walet

In this paper, we consider the Dirac-Hartree-Fock equations for system has many-particles. The difficulties associated with Gaussians model are likely to be more complex in relativistic Dirac-Hartree-Fock calculations. To processing these…

Atomic Physics · Physics 2019-12-11 Bilal K. Jasim , Ayad A. Al-Ani. Saad N. Abood

We develop a quantum embedding method that enables accurate and efficient treatment of interactions between molecules and an environment, while explicitly including many-body correlations. The molecule is composed of classical nuclei and…

Chemical Physics · Physics 2023-03-30 Matej Ditte , Matteo Barborini , Leonardo Medrano Sandonas , Alexandre Tkatchenko

Variational Monte Carlo and Green's function Monte Carlo are powerful tools for calculations of properties of light nuclei using realistic two-nucleon and three-nucleon potentials. Recently the GFMC method has been extended to multiple…

Nuclear Theory · Physics 2009-11-10 Steven C. Pieper

Molecule-optimized basis sets, based on approximate natural orbitals, are developed for accelerating the convergence of quantum calculations with strongly correlated (multi-referenced) electrons. We use a low-cost approximate solution of…

Chemical Physics · Physics 2014-02-12 Gergely Gidofalvi , David A. Mazziotti

Quantum Monte Carlo approaches such as the diffusion Monte Carlo (DMC) method are among the most accurate many-body methods for extended systems. Their scaling makes them well suited for defect calculations in solids. We review the various…

Materials Science · Physics 2014-04-23 William D. Parker , John W. Wilkins , Richard G. Hennig

We extend the recently introduced phaseless auxiliary-field quantum Monte Carlo (QMC) approach to any single-particle basis, and apply it to molecular systems with Gaussian basis sets. QMC methods in general scale favorably with system…

Computational Physics · Physics 2007-05-23 W. A. Al-Saidi , Shiwei Zhang , Henry Krakauer

Quantum variational algorithms (QVAs) are increasingly potent tools for simulating quantum many-body systems on noisy intermediate-scale quantum (NISQ) devices. This work examines the application of the Variational Quantum Eigensolver (VQE)…

Nuclear Theory · Physics 2026-01-28 Dhritimalya Roy , Somnath Nag

The Coupled Cluster (CC) method is used to compute the electronic correlation energy in atoms and molecules and often leads to highly accurate results. However, due to its single-reference nature, standard CC in its projected form fails to…

We introduce a method for accurate quantum chemical calculations based on a simple variational wave function, defined by a single geminal that couples all the electrons into singlet pairs, combined with a real space correlation factor. The…

Materials Science · Physics 2009-10-22 M. Marchi , S. Azadi , M. Casula , S. Sorella

Quantum computing and quantum Monte Carlo (QMC) are respectively the state-of-the-art quantum and classical computing methods for understanding many-body quantum systems. Here, we propose a hybrid quantum-classical algorithm that integrates…

Quantum Physics · Physics 2025-11-17 Yukun Zhang , Yifei Huang , Jinzhao Sun , Dingshun Lv , Xiao Yuan

We introduce hybrid gausslet/Gaussian basis sets, where a standard Gaussian basis is added to a gausslet basis in order to increase accuracy near the nuclei while keeping the spacing of the grid of gausslets relatively large. The Gaussians…

Chemical Physics · Physics 2024-06-19 Yiheng Qiu , Steven R. White

Electronic structure calculation of atoms and molecules, in the past few decades has largely been dominated by density functional methods. This is primarily due to the fact that this can account for electron correlation effects in a…

Chemical Physics · Physics 2013-07-12 Amlan K. Roy

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

We report on the most recent applications of the Auxiliary Field Diffusion Monte Carlo (AFDMC) method. The equation of state (EOS) for pure neutron matter in both normal and BCS phase and the superfluid gap in the low--density regime are…