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With the aim of establishing a framework to efficiently perform the practical application of quantum chemistry simulation on near-term quantum devices, we envision a hybrid quantum--classical framework for leveraging problem decomposition…

We present two machine learning methodologies that are capable of predicting diffusion Monte Carlo (DMC) energies with small datasets (~60 DMC calculations in total). The first uses voxel deep neural networks (VDNNs) to predict DMC energy…

Mesoscale and Nanoscale Physics · Physics 2022-11-02 Kevin Ryczko , Jaron T. Krogel , Isaac Tamblyn

Atomic forces are calculated for first-row monohydrides and carbon monoxide within electronic quantum Monte Carlo (QMC). Accurate and efficient forces are achieved by using an improved method for moving variational parameters in variational…

Chemical Physics · Physics 2009-11-10 Myung Won Lee , Massimo Mella , Andrew M. Rappe

We present a reformulation of QM/MM as a fully quantum mechanical theory of interacting subsystems, all treated at the level of density functional theory (DFT). For the MM subsystem, which lacks orbitals, we assign an ad hoc electron…

We propose improved versions of the standard diffusion Monte Carlo (DMC) and the lattice regularized diffusion Monte Carlo (LRDMC) algorithms. For the DMC method, we refine a scheme recently devised to treat non-local pseudopotential in a…

Other Condensed Matter · Physics 2015-05-18 Michele Casula , Saverio Moroni , Sandro Sorella , Claudia Filippi

The chemical diffusion master equation (CDME) describes the probabilistic dynamics of reaction--diffusion systems at the molecular level [del Razo et al., Lett. Math. Phys. 112:49, 2022]; it can be considered the master equation for…

Statistical Mechanics · Physics 2023-01-23 Mauricio J. del Razo , Stefanie Winkelmann , Rupert Klein , Felix Höfling

We present the first quantum-centric simulations of noncovalent interactions using a supramolecular approach. We simulate the potential energy surfaces (PES) of the water and methane dimers, featuring hydrophilic and hydrophobic…

Building on the success of Quantum Monte Carlo techniques such as diffusion Monte Carlo, alternative stochastic approaches to solve electronic structure problems have emerged over the last decade. The full configuration interaction quantum…

Reaction-diffusion processes play an important role in a variety of physical, chemical, and biological systems. Conventionally, the kinetics of these processes are described by the law of mass action. However, there are various cases where…

Chemical Physics · Physics 2026-05-06 Roman V. Li , Oleg A. Igoshin , Evgeny B. Krissinel , Pavel A. Frantsuzov

Colloids have a striking relevance in a wide spectrum of industrial formulations, spanning from personal care products to protective paints. Their behaviour can be easily influenced by extremely weak forces, which disturb their…

Soft Condensed Matter · Physics 2018-06-14 Daniel Corbett , Alejandro Cuetos , Matthew Dennison , Alessandro Patti

A unitary coupled-cluster (UCC) form for the wavefunction in the variational quantum eigensolver has been suggested as a systematic way to go beyond the mean-field approximation and include electron correlation in solving quantum chemistry…

Quantum Physics · Physics 2018-09-12 Ilya G. Ryabinkin , Tzu-Ching Yen , Scott N. Genin , Artur F. Izmaylov

Clay minerals are ubiquitous in nature, and the manner in which they interact with their surroundings has important industrial and environmental implications. Consequently, a molecular-level understanding of the adsorption of molecules on…

Chemical Physics · Physics 2016-12-07 Andrea Zen , Loïc M Roch , Stephen J Cox , Xiao L Hu , Sandro Sorella , Dario Alfè , Angelos Michaelides

Quantum Mechanics/Molecular Mechanics (QM/MM) simulations are a popular approach to study various features of large systems. A common application of QM/MM calculations is in the investigation of reaction mechanisms in condensed-phase and…

Chemical Physics · Physics 2020-10-29 Jorge Nochebuena , Sehr Naseem-Khan , G. Andrés Cisneros

Employing a classical density-functional description of liquid environments, we introduce a rigorous method for the diffusion quantum Monte Carlo calculation of free energies and thermodynamic averages of solvated systems that requires…

The search for two-dimensional (2D) magnetic materials has attracted a great deal of attention because of the experimental synthesis of 2D CrI$_3$, which has a measured Curie temperature of 45 K. Often times, these monolayers have a higher…

Strongly Correlated Electrons · Physics 2023-01-16 Daniel Wines , Kamal Choudhary , Francesca Tavazza

Polymorphs in molecular crystals are often very close in energy, yet they may possess markedly different physical and chemical properties. The understanding and prediction of polymorphism is of paramount importance for a variety of…

Multicomponent systems are defined as chemical systems that require a quantum mechanical description of two or more different types of particles. Non-Born-Oppenheimer electron-nuclear interactions in molecules, electron-hole interactions in…

Chemical Physics · Physics 2015-10-21 Benjamin H. Ellis , Somil Aggarwal , Arindam Chakraborty

This topical review describes the methodology of continuum variational and diffusion quantum Monte Carlo calculations. These stochastic methods are based on many-body wave functions and are capable of achieving very high accuracy. The…

Materials Science · Physics 2010-02-11 R. J. Needs , M. D. Towler , N. D. Drummond , P. Lopez Rios

Nuclear physics seeks to describe both bound and unbound states within a unified predictive framework. While coordinate-space Quantum Monte Carlo (QMC) methods have successfully computed bound states for systems with $A \leq 12$, their…

Nuclear Theory · Physics 2025-02-27 Abraham R. Flores , Kenneth M. Nollett , Maria Piarulli

The DCA$^+$ algortihm was recently introduced to extend the dynamic cluster approximation (DCA) with a continuous lattice self-energy in order to achieve better convergence with cluster size. Here we extend the DCA$^+$ algorithm to the…

Strongly Correlated Electrons · Physics 2015-06-18 Peter Staar , Thomas Maier , Thomas Schulthess