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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

Variational quantum Monte Carlo calculations are reported for the bulk GaAs semiconductor in order to present values for the ground-state energy, the lattice constant, the bulk modulus, and some derived properties. The statistical accuracy…

mtrl-th · Physics 2009-10-30 H. Eckstein , W. Schattke , M. Reigrotzki , R. Redmer

We present an improved formalism for quantum Monte Carlo calculations of energy derivatives and properties (e.g. the interatomic forces), with a multideterminant Jastrow-Slater function. As a function of the number $N_e$ of Slater…

Chemical Physics · Physics 2017-06-26 Roland Assaraf , Saverio Moroni , Claudia Filippi

We study the efficiency, precision and accuracy of all-electron variational and diffusion quantum Monte Carlo calculations using Slater basis sets. Starting from wave functions generated by Hartree-Fock and density functional theory, we…

Materials Science · Physics 2010-02-11 Norbert Nemec , Michael D. Towler , R. J. Needs

Compact and accurate wave functions can be constructed by quantum Monte Carlo methods. Typically, these wave functions consist of a sum of a small number of Slater determinants multiplied by a Jastrow factor. In this paper we study the…

Condensed Matter · Physics 2009-10-30 Chien-Jung Huang , C. J. Umrigar , M. P. Nightingale

The rapidly growing interest in simulating condensed-phase materials using quantum chemistry methods calls for a library of high-quality Gaussian basis sets suitable for periodic calculations. Unfortunately, most standard Gaussian basis…

Chemical Physics · Physics 2022-06-07 Hong-Zhou Ye , Timothy C. Berkelbach

We investigate the use of optimized correlation consistent gaussian basis sets for the study of insulating solids with auxiliary-field quantum Monte Carlo (AFQMC). The exponents of the basis set are optimized through the minimization of the…

Chemical Physics · Physics 2021-02-03 Miguel A. Morales , Fionn D. Malone

We develop a quantum Monte Carlo method for many fermions that allows the use of any one-particle basis. It projects out the ground state by random walks in the space of Slater determinants. An approximate approach is formulated to control…

Condensed Matter · Physics 2009-02-20 Shiwei Zhang , Henry Krakauer

We describe a method for imposing the correct electron-nucleus (e-n) cusp in molecular orbitals expanded as a linear combination of (cuspless) Gaussian basis functions. Enforcing the e-n cusp in trial wave functions is an important asset in…

Chemical Physics · Physics 2020-06-05 Pierre-François Loos , Anthony Scemama , Michel Caffarel

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

This tutorial paper introduces quantum approaches to Monte Carlo computation with applications in computational finance. We outline the basics of quantum computing using Grover's algorithm for unstructured search to build intuition. We then…

Quantum Physics · Physics 2025-09-24 Jose Blanchet , Mark S. Squillante , Mario Szegedy , Guanyang Wang

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

We review the use of continuum quantum Monte Carlo (QMC) methods for the calculation of energy gaps from first principles, and present a broad set of excited-state calculations carried out with the variational and fixed-node diffusion QMC…

Materials Science · Physics 2018-08-22 Ryan J. Hunt , Marcin Szyniszewski , Genki I. Prayogo , Ryo Maezono , Neil D. Drummond

We present a simple and general formalism to compute efficiently the derivatives of a multi-determinant Jastrow-Slater wave function, the local energy, the interatomic forces, and similar quantities needed in quantum Monte Carlo. Through a…

Materials Science · Physics 2016-06-22 Claudia Filippi , Roland Assaraf , Saverio Moroni

Quantum Monte Carlo methods are used to calculate various ground state properties of charged bosons in two dimensions, throughout the whole density range where the fluid phase is stable. Wigner crystallization is predicted at $r_s\simeq…

Condensed Matter · Physics 2018-05-01 S. De Palo , S. Conti , S. Moroni

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 Monte Carlo (QMC) methods such as variational Monte Carlo and fixed node diffusion Monte Carlo depend heavily on the quality of the trial wave function. Although Slater-Jastrow wave functions are the most commonly used variational…

Materials Science · Physics 2015-05-28 Bryan K. Clark , Miguel A. Morales , Jeremy McMinis , Jeongnim Kim , Gustavo E. Scuseria

With our recently proposed effective Hamiltonian via Monte Carlo, we are able to compute low energy physics of quantum systems. The advantage is that we can obtain not only the spectrum of ground and excited states, but also wave functions.…

High Energy Physics - Lattice · Physics 2015-06-25 Xiang-Qian Luo , C. Q. Huang , J. Q. Jiang , H. Jirari , H. Kroeger , K. Moriarty

For qubits, Monte Carlo estimation of the average fidelity of Clifford unitaries is efficient -- it requires a number of experiments that is independent of the number $n$ of qubits and classical computational resources that scale only…

Quantum Physics · Physics 2014-10-23 Giulia Gualdi , David Licht , Daniel M. Reich , Christiane P. Koch

Various strategies to implement efficiently QMC simulations for large chemical systems are presented. These include: i.) the introduction of an efficient algorithm to calculate the computationally expensive Slater matrices. This novel…

Performance · Computer Science 2019-05-28 Anthony Scemama , Michel Caffarel , Emmanuel Oseret , William Jalby
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