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We derive an automatic procedure for generating a set of highly localized, non-orthogonal orbitals for linear scaling quantum Monte Carlo calculations. We demonstrate the advantage of these orbitals in calculations of the total energy of…

Materials Science · Physics 2007-05-23 F. A. Reboredo , A. J. Williamson

Choosing a basis set is the first step of a quantum chemistry calculation and it sets its maximum accuracy. This choice of orbitals is limited by strong technical constraints as one must be able to compute a large number of six dimensional…

Strongly Correlated Electrons · Physics 2026-02-04 Nicolas Jolly , Yuriel Núñez Fernández , Xavier Waintal

Quantum Monte Carlo (QMC) techniques are used to calculate the one-body density matrix and excitation energies for the valence electrons of bulk silicon. The one-body density matrix and energies are obtained from a Slater-Jastrow wave…

Condensed Matter · Physics 2009-10-31 P. R. C. Kent , Randolph Q. Hood , M. D. Towler , R. J. Needs , G. Rajagopal

We present a scalable implementation of the $GW$ approximation using Gaussian atomic orbitals to study the valence and core ionization spectroscopies of molecules. The implementation of the standard spectral decomposition approach to the…

Chemical Physics · Physics 2021-12-06 Daniel Mejia-Rodriguez , Alexander Kunitsa , Edoardo Aprà , Niranjan Govind

Basis sets of atomic orbitals are very efficient for density functional calculations but lack a systematic variational convergence. We present a variational method to optimize numerical atomic orbitals using a single parameter to control…

Condensed Matter · Physics 2009-11-07 E. Anglada , J. Soler , J. Junquera , E. Artacho

Representations of atomic orbitals based on Monte-Carlo (MC) approaches are not always correct when using various sets of orthogonal coordinates other than Cartesian coordinates. The analysis proposed here gives elements for a proper use of…

Chemical Physics · Physics 2016-08-24 Jean Hoarau , Jean-Claude Rayez

We introduce a mixed density fitting scheme that uses both a Gaussian and a plane-wave fitting basis to accurately evaluate electron repulsion integrals in crystalline systems. We use this scheme to enable efficient all-electron Gaussian…

Chemical Physics · Physics 2017-11-22 Qiming Sun , Timothy C. Berkelbach , James D. McClain , Garnet Kin-Lic Chan

Quantum Monte Carlo methods are accurate and promising many body techniques for electronic structure calculations which, in the last years, are encountering a growing interest thanks to their favorable scaling with the system size and their…

Chemical Physics · Physics 2014-02-17 Andrea Zen , Ye Luo , Sandro Sorella , Leonardo Guidoni

The ionization by photon or electron impact of the inner (2a1) and outer (1t2) valence orbitals of the CH4 molecule is investigated theoretically. In spite of a number of approximations, including a monocentric approach and a rather simple…

Chemical Physics · Physics 2024-05-15 Abdallah Ammar , Arnaud Leclerc , Lorenzo Ugo Ancarani

The method of McCurdy, Baertschy, and Rescigno, J. Phys. B, 37, R137 (2004) is generalized to obtain a straightforward, surprisingly accurate, and scalable numerical representation for calculating the electronic wave functions of molecules.…

Quantum Monte Carlo (QMC) methods can very accurately compute ground state properties of quantum systems. We applied these methods to a system of boson hard spheres to get exact, infinite system size results for the ground state at several…

Computational Physics · Physics 2016-09-08 Mark Dewing

In this paper, we consider the Dirac-Coulomb equation for many-particles, to describe the interaction between electrons in the system having many electrons. The four-component wave function will expanding into a finite basis-set, using…

Quantum Physics · Physics 2019-12-10 Bilal K. Jasim , Ayad A. Al-Ani , Saad N. Abood

We investigate the inclusion of variable spins in electronic structure quantum Monte Carlo, with a focus on diffusion Monte Carlo with Hamiltonians that include spin-orbit interactions. Following our previous introduction of fixed-phase…

Computational Physics · Physics 2016-07-27 Cody A. Melton , M. Chandler Bennett , Lubos Mitas

We suggest an efficient method to resolve electronic cusps in electronic structure calculations by using an effective transcorrelated Hamiltonian. This effective Hamiltonian takes a simple form for plane wave bases, containing up to…

Computational Physics · Physics 2018-02-14 Hongjun Luo , Ali Alavi

Variational Monte Carlo (VMC) methods are used to sample classically from distributions corresponding to quantum states which have an efficient classical description. VMC methods are based on performing a number of steps of a Markov chain…

Quantum Physics · Physics 2023-10-27 Ashley Montanaro , Stasja Stanisic

Obtaining accurate solutions to the Schr\"odinger equation is the key challenge in computational quantum chemistry. Deep-learning-based Variational Monte Carlo (DL-VMC) has recently outperformed conventional approaches in terms of accuracy,…

Chemical Physics · Physics 2023-07-19 Michael Scherbela , Leon Gerard , Philipp Grohs

Certain point defects in solids can efficiently be used as qubits for applications in quantum technology. They have spin states that are initializable, readable, robust, and can be manipulated optically. New theoretical methods are needed…

Computational Physics · Physics 2023-09-20 Kristoffer Simula , Ilja Makkonen

The scale and complexity of quantum system to which real-space quantum Monte Carlo (QMC) can be applied in part depends on the representation and memory usage of the trial wavefunction. B-splines, the computationally most efficient basis…

Materials Science · Physics 2018-09-05 Ye Luo , Kenneth P. Esler , Paul R. C. Kent , Luke Shulenburger

A paramount goal in the field of nuclear physics is to unify ab-initio treatments of bound and unbound states. The position-space quantum Monte Carlo (QMC) methods have a long history of successful bound state calculations in light systems…

Nuclear Theory · Physics 2023-08-29 Abraham R. Flores , Kenneth M. Nollett

A quantum Monte Carlo study of the atomization energies for the G2 set of molecules is presented. Basis size dependence of diffusion Monte Carlo atomization energies is studied with a single determinant Slater-Jastrow trial wavefunction…

Chemical Physics · Physics 2015-06-04 F. R. Petruzielo , Julien Toulouse , C. J. Umrigar