Fast and accurate quantum Monte Carlo for molecular crystals

Abstract

Computer simulation plays a central role in modern day materials science. The utility of a given computational approach depends largely on the balance it provides between accuracy and computational cost. Molecular crystals are a class of materials of great technological importance which are challenging for even the most sophisticated \emph{ab initio} electronic structure theories to accurately describe. This is partly because they are held together by a balance of weak intermolecular forces but also because the primitive cells of molecular crystals are often substantially larger than those of atomic solids. Here, we demonstrate that diffusion quantum Monte Carlo (DMC) delivers sub-chemical accuracy for a diverse set of molecular crystals at a surprisingly moderate computational cost. As such, we anticipate that DMC can play an important role in understanding and predicting the properties of a large number of molecular crystals, including those built from relatively large molecules which are far beyond reach of other high accuracy methods.

References in corpus (18)

• Perspective on density functional theory
• Perspective: Advances and challenges in treating van der Waals dispersion forces in density functional theory
• Continuum variational and diffusion quantum Monte Carlo calculations
• Twist-averaged Boundary Conditions in Continuum Quantum Monte Carlo
• Hydrogen bonds and van der Waals forces in ice at ambient and high pressures
• The Finite Size Error in Many-body Simulations with long-Ranged Interactions
• Finite-size errors in continuum quantum Monte Carlo calculations
• Beyond the Random Phase Approximation for the Electron Correlation Energy: The Importance of Single Excitations
• Smooth relativistic Hartree-Fock pseudopotentials for H to Ba and Lu to Hg
• Norm-conserving Hartree-Fock pseudopotentials and their asymptotic behavior
• An efficient localized basis set for quantum Monte Carlo calculations on condensed matter
• Finite-size correction in many-body electronic structure calculations
• Finite size errors in quantum many-body simulations of extended systems
• Boosting the accuracy and speed of quantum Monte Carlo: size-consistency and time-step
• Energy benchmarks for water clusters and ice structures from an embedded many-body expansion
• Ab initio investigation of intermolecular interactions in solid benzene
• Lattice energies of molecular solids from the random phase approximation with singles corrections
• Pseudopotentials for correlated electron systems

Cited by in corpus (39)

• Deep neural network solution of the electronic Schrödinger equation
• QMCPACK : An open source ab initio Quantum Monte Carlo package for the electronic structure of atoms, molecules, and solids
• The first-principles phase diagram of monolayer nanoconfined water
• r2SCAN-D4: Dispersion corrected meta-generalized gradient approximation for general chemical applications
• Interactions between Large Molecules: Puzzle for Reference Quantum-Mechanical Methods
• Variational and Diffusion Quantum Monte Carlo Calculations with the CASINO Code
• On the physisorption of water on graphene: Sub-chemical accuracy from many-body electronic structure methods
• KITE: high-performance accurate modelling of electronic structure and response functions of large molecules, disordered crystals and heterostructures
• BIGDML: Towards Exact Machine Learning Force Fields for Materials
• A complete description of thermodynamic stabilities of molecular crystals
• Interaction between water and carbon nanostructures: How good are current density functional approximations?
• Excited states with selected CI-QMC: chemically accurate excitation energies and geometries
• A new scheme for fixed node diffusion quantum Monte Carlo with pseudopotentials: improving reproducibility and reducing the trial-wave-function bias
• Hydration of NH${}_4^{+}$ in Water: Bifurcated Hydrogen Bonding Structures and Fast Rotational Dynamics
• How accurate are simulations and experiments for the lattice energies of molecular crystals?
• DMC-ICE13: ambient and high pressure polymorphs of ice from Diffusion Monte Carlo and Density Functional Theory
• Accurate Predictions of Electron Binding Energies of Dipole-Bound Anions via Quantum Monte Carlo Methods
• The importance of nuclear quantum effects for NMR crystallography
• Efficient and accurate description of adsorption in zeolites
• Space-warp coordinate transformation for efficient ionic force calculations in quantum Monte Carlo
• An efficient method for grand-canonical twist averaging in quantum Monte Carlo calculations
• Diffusion Monte Carlo Study on Relative Stabilities of Boron Nitride Polymorphs
• Random Phase Approximation Applied to Many-Body Noncovalent Systems
• Random phase approximation with exchange for an accurate description of crystalline polymorphism
• A pathway towards high throughput Quantum Monte Carlo simulations for alloys: A case study of two-dimensional (2D) $Ga{S}_{x}S{e}_{1-x}$
• Assessment of random-phase approximation and second order Møller-Plesset perturbation theory for many-body interactions in solid ethane, ethylene, and acetylene
• Accurate and efficient machine learning interatomic potentials for finite temperature modeling of molecular crystals
• Systematic discrepancies between reference methods for non-covalent interactions within the S66 dataset
• Quantum Monte Carlo calculations of van der Waals interactions between aromatic benzene rings
• Basis set incompleteness errors in fixed-node diffusion Monte Carlo calculations on non-covalent interactions
• Binding energies of molecular solids from fragment and periodic approaches
• Efficient calculation of unbiased atomic forces in ab initio Variational Monte Carlo
• Reproducibility of fixed-node diffusion Monte Carlo across diverse community codes: The case of water-methane dimer
• An efficient hybrid orbital representation for quantum Monte Carlo calculations
• Efficient Implementation of the Random Phase Approximation with Domain-based Local Pair Natural Orbitals
• Linear-scale simulations of quench dynamics
• Beyond single-reference fixed-node approximation in ab initio Diffusion Monte Carlo using antisymmetrized geminal power applied to systems with hundreds of electrons
• The effects of dispersion damping and three-body interactions for accurate layered-material exfoliation energies
• Assessing the accuracy of compound formation energies with quantum Monte Carlo