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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 present a variational function that targets excited states directly based on their position in the energy spectrum, along with a Monte Carlo method for its evaluation and minimization whose cost scales polynomially for a wide class of…

Strongly Correlated Electrons · Physics 2016-01-22 Luning Zhao , Eric Neuscamman

In this work, we report potential energy surfaces (PESs) of the sodium dimer calculated by variational (VMC) and lattice regularized diffusion Monte Carlo (LRDMC). The VMC calculation is accurate for determining the equilibrium distance and…

Chemical Physics · Physics 2020-06-02 Kousuke Nakano , Ryo Maezono , Sandro Sorella

We review our calculation method, Gaussian expansion method (GEM), and its applications to various few-body (3- to 5-body) systems such as 1) few-nucleon systems, 2) few-body structure of hypernuclei, 3) clustering structure of light nuclei…

Nuclear Theory · Physics 2018-09-14 Emiko Hiyama , Masayasu Kamimura

An efficient method for calculating the electronic structure of systems that need a very fine sampling of the Brillouin zone is presented. The method is based on the variational optimization of a "single" (i.e. common to all points in the…

Materials Science · Physics 2009-10-31 Sandro Scandolo , Jorge Kohanoff

In this work, we introduce an original self-consistent scheme based on the one-body reduced density matrix ($\gamma$) formalism. A significant feature of this methodology is the utilization of an optimal unitary transformation of the…

Strongly Correlated Electrons · Physics 2023-11-10 Quentin Marécat , Benjamin Lasorne , Emmanuel Fromager , Matthieu Saubanère

We introduce highly local basis sets for electronic structure which are very efficient for correlation calculations near the complete basis set limit. Our approach is based on gausslets, recently introduced wavelet-like smooth orthogonal…

Chemical Physics · Physics 2019-02-20 Steven R. White , E. Miles Stoudenmire

We present a novel specialization of the variational Monte Carlo linear method for the optimization of the recently introduced cluster Jastrow antisymmetric geminal power ansatz, achieving a lower-order polynomial cost scaling than would be…

Chemical Physics · Physics 2016-03-23 Eric Neuscamman

A diffusion Monte Carlo algorithm is introduced that can determine the correct nodal structure of the wave function of a few-fermion system and its ground-state energy without an uncontrolled bias. This is achieved by confining signed…

Computational Physics · Physics 2020-02-05 Alexander A. Kunitsa , So Hirata

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

We propose here a single Pfaffian correlated variational ansatz, that dramatically improves the accuracy with respect to the single determinant one, while remaining at a similar computational cost. A much larger correlation energy is indeed…

Chemical Physics · Physics 2020-07-28 Claudio Genovese , Tomonori Shirakawa , Kousuke Nakano , Sandro Sorella

The idea of using fragment embedding to circumvent the high computational scaling of accurate electronic structure methods while retaining high accuracy has been a long-standing goal for quantum chemists. Traditional fragment embedding…

Chemical Physics · Physics 2022-10-11 Hong-Zhou Ye , Matthew Welborn , Nathan D. Ricke , Troy Van Voorhis

Since in periodic systems, a given element may be present in different spatial arrangements displaying vastly different physical and chemical properties, an elemental basis set that is independent of physical properties of materials may…

Chemical Physics · Physics 2021-05-04 Yanbing Zhou , Emanuel Gull , Dominika Zgid

Diffusion Monte Carlo (DMC) is an exact technique to project out the ground state (GS) of a Hamiltonian. Since the GS is always bosonic, in fermionic systems the projection needs to be carried out while imposing anti-symmetric constraints,…

Computational Physics · Physics 2025-01-08 Kousuke Nakano , Sandro Sorella , Dario Alfè , Andrea Zen

Gibbs-ensemble Monte Carlo (GEMC) is a powerful method for calculating the gas-liquid binodals of simple models and small molecules, but is too demanding computationally for realistic models of proteins. Here we discover that the main…

Chemical Physics · Physics 2025-12-23 Sanbo Qin , Huan-Xiang Zhou

The Slater-type F12 geminal lengthscales originally tuned for the second-order M{\o}ller-Plesset F12 method are too large for higher-order F12 methods formulated using the SP (diagonal fixed-coefficient spin-adapted) F12 ansatz. The new…

Chemical Physics · Physics 2025-10-13 Samuel R. Powell , Kshitijkumar A. Surjuse , Bimal Gaudel , Edward F. Valeev

We report an extensive theoretical study of the protonated water dimer (Zundel ion) by means of the highly correlated variational Monte Carlo and lattice regularized Monte Carlo approaches. This system represents the simplest model for…

Chemical Physics · Physics 2013-12-11 Mario Dagrada , Michele Casula , Antonino M. Saitta , Sandro Sorella , Francesco Mauri

We present a conjugate-gradient method for the ground-state optimization of projected entangled-pair states (PEPS) in the thermodynamic limit, as a direct implementation of the variational principle within the PEPS manifold. Our…

Strongly Correlated Electrons · Physics 2016-11-08 Laurens Vanderstraeten , Jutho Haegeman , Philippe Corboz , Frank Verstraete

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

The Markov chain Monte Carlo method is a versatile tool in statistical physics to evaluate multi-dimensional integrals numerically. For the method to work effectively, we must consider the following key issues: the choice of ensemble, the…

Statistical Mechanics · Physics 2014-01-07 Synge Todo , Hidemaro Suwa