相关论文: Full optimization of Jastrow-Slater wave functions…
We propose a new Monte Carlo algorithm for the numerical study of general lattice models in Hamiltonian form. The algorithm is based on an initial Ansatz for the ground state wave function depending on a set of free parameters which are…
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…
The study of alloys using computational methods has been a difficult task due to the usually unknown stoichiometry and local atomic ordering of the different structures experimentally. In order to combat this, first-principles methods have…
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…
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…
All-electron variational and diffusion quantum Monte Carlo calculations of the ground state energies of the first row atoms (Li to Ne) are reported. We use trial wavefunctions of four types: single determinant Slater-Jastrow wavefunctions;…
This paper proposes several novel optimization algorithms for minimizing a nonlinear objective function. The algorithms are enlightened by the optimal state trajectory of an optimal control problem closely related to the minimized objective…
Quantum mechanics for many-body systems may be reduced to the evaluation of integrals in 3N dimensions using Monte-Carlo, providing the Quantum Monte Carlo ab initio methods. Here we limit ourselves to expectation values for trial…
Large scale optimization problems are ubiquitous in machine learning and data analysis and there is a plethora of algorithms for solving such problems. Many of these algorithms employ sub-sampling, as a way to either speed up the…
Joint diagonalization, the process of finding a shared set of approximate eigenvectors for a collection of matrices, arises in diverse applications such as multidimensional harmonic analysis or quantum information theory. This task is…
The hydrogen molecules $H_2$ and $(H_2)_2$ are analyzed with electronic correlations taken into account between the $1s$ electrons exactly. The optimal single-particle Slater orbitals are evaluated in the correlated state of $H_2$ by…
A fast and reliable geometry optimization algorithm is presented that optimizes atomic positions and lattice vectors simultaneously. Using a series of benchmarks, it is shown that the method presented in this paper outperforms in most cases…
Quantum Monte Carlo (QMC) algorithms have long relied on Jastrow factors to incorporate dynamic correlation into trial wave functions. While Jastrow-type wave functions have been widely employed in real-space algorithms, they have seen…
The accuracy and precision of high-energy spallation models are key issues for the design and development of new applications and experiments. We present a method to estimate model parameters and associated uncertainties by leveraging the…
We have employed the steepest descent method to optimise the variational ground state quantum Monte Carlo wave function for He, Li, Be, B and C atoms. We have used both the direct energy minimisation and the variance minimisation…
We introduce an efficient method to construct optimal and system adaptive basis sets for use in electronic structure and quantum Monte Carlo calculations. The method is based on an embedding scheme in which a reference atom is singled out…
Algorithms for bilevel optimization often encounter Hessian computations, which are prohibitive in high dimensions. While recent works offer first-order methods for unconstrained bilevel problems, the constrained setting remains relatively…
Quantum Monte Carlo simulations of interacting electrons in solids often use Slater-Jastrow trial wave functions. The Jastrow function takes into account correlations between pairs of electrons. In simulations of solids, it is common to use…
We employ quantum Monte Carlo to obtain chemically accurate vertical and adiabatic excitation energies, and equilibrium excited-state structures for the small, yet challenging, formaldehyde and thioformaldehyde molecules. A key ingredient…
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…