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Diradical molecules are essential species involved in many organic and inorganic chemical reactions. The computational study of their electronic structure is often challenging, because a reliable description of the correlation, and in…

Chemical Physics · Physics 2014-06-18 Andrea Zen , Emanuele Coccia , Ye Luo , Sandro Sorella , Leonardo Guidoni

A method is developed that allows analysis of quantum Monte Carlo simulations to identify errors in trial wave functions. The purpose of this method is to allow for the systematic improvement of variational wave functions by identifying…

Strongly Correlated Electrons · Physics 2016-08-03 Kiel T. Williams , Lucas K. Wagner

A quantum Monte Carlo method of determining Jastrow-Slater wave functions for which the energy is stationary with respect to variations in the single-particle orbitals is presented. A potential is determined by a least-squares fitting of…

Condensed Matter · Physics 2007-05-23 Stephen Fahy , Claudia Filippi

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

The variational and diffusion quantum Monte Carlo methods are used to calculate the correlation energy of the paramagnetic three-dimensional homogeneous electron gas at intermediate to high density. Ground state energies in finite cells are…

Strongly Correlated Electrons · Physics 2023-03-29 Sam Azadi , N. D. Drummond , S. M. Vinko

We report all-electron and pseudopotential calculations of the ground-stateenergies of the neutral Ne atom and the Ne+ ion using the variational and diffusion quantum Monte Carlo (DMC) methods. We investigate different levels of…

Materials Science · Physics 2008-01-03 N. D. Drummond , P. Lopez Rios , A. Ma , J. R. Trail , G. Spink , M. D. Towler , R. J. Needs

In this work, we investigate the fidelity of orbital optimization in variational Monte Carlo to improve diffusion Monte Carlo results on correlated magnetic systems, using CrSBr as a model system. We compare the performance of different…

Strongly Correlated Electrons · Physics 2026-04-27 Cody A. Melton , Jaron T. Krogel

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

Accurate ab initio calculations of 3d transition metal monoxide molecules have attracted extensive attention because of its relevance in physical and chemical science, as well as theoretical challenges in treating strong electron…

Strongly Correlated Electrons · Physics 2021-11-02 Tonghuan Jiang , Yilin Chen , Nikolay Bogdanov , Enge Wang , Ali Alavi , Ji Chen

Achieving chemical accuracy for strongly correlated molecules is a defining milestone for first-generation, fault-tolerant quantum computers, yet the factorial growth of three, four, and six-index tensor contractions in coupled-cluster…

The time-dependent complete-active-space self-consistent-field (TD-CASSCF) method for the description of multielectron dynamics in intense laser fields is presented, and a comprehensive description of the method is given. It introduces the…

Atomic Physics · Physics 2015-06-15 Takeshi Sato , Kenichi L. Ishikawa

Multicomponent methods seek to treat select nuclei, typically protons, fully quantum mechanically and equivalent to the electrons of a chemical system. In such methods, it is well known that due to the neglect of electron-proton…

Chemical Physics · Physics 2020-12-21 O. Jonathan Fajen , Kurt R. Brorsen

In quantum chemistry, one of the most important challenges is the static correlation problem when solving the electronic Schr\"odinger equation for molecules in the Born--Oppenheimer approximation. In this article, we analyze the tailored…

Numerical Analysis · Mathematics 2019-11-21 Fabian M. Faulstich , Andre Laestadius , Örs Legeza , Reinhold Schneider , Simen Kvaal

In this work, we developed an efficient approach to compute ensemble averages in systems with pairwise-additive energetic interactions between the entities. Methods involving full enumeration of the configuration space result in exponential…

Biomolecules · Quantitative Biology 2020-10-13 Arun V. Sathanur , Nathan A. Baker

A quantum Monte Carlo method is presented for determining multi-determinantal Jastrow-Slater wave functions for which the energy is stationary with respect to the simultaneous optimization of orbitals and configuration interaction…

Other Condensed Matter · Physics 2009-11-10 Friedemann Schautz , Claudia Filippi

We present a simple, robust and efficient method for varying the parameters in a many-body wave function to optimize the expectation value of the energy. The effectiveness of the method is demonstrated by optimizing the parameters in…

Other Condensed Matter · Physics 2016-08-31 C. J. Umrigar , Claudia Filippi

This work introduces Jacobian-scaled K-means (JSK-means) clustering, which is a physics-informed clustering strategy centered on the K-means framework. The method allows for the injection of underlying physical knowledge into the clustering…

Computational Physics · Physics 2024-06-25 Shivam Barwey , Venkat Raman

We report the formulation of a new, cost-effective approximation method in the time-dependent optimized coupled-cluster (TD-OCC) framework [T. Sato et al., J. Chem. Phys. 148, 051101 (2018)] for first-principles simulations of multielectron…

Chemical Physics · Physics 2022-08-11 Himadri Pathak , Takeshi Sato , Kenichi L. Ishikawa

Highly accurate experimental structure factors of silicon are available in the literature, and these provide the ideal test for any \emph{ab initio} method for the construction of the all-electron charge density. In a recent paper [J. R.…

Materials Science · Physics 2015-05-14 J. R. Trail , D. M. Bird

Quantum-mechanical methods are widely used for understanding molecular interactions throughout biology, chemistry, and materials science. Quantum diffusion Monte Carlo (DMC) and coupled cluster with single, double, and perturbative triple…

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