TurboRVB: a many-body toolkit for {\it ab initio} electronic simulations by quantum Monte Carlo

Abstract

TurboRVB is a computational package for {\it ab initio} Quantum Monte Carlo (QMC) simulations of both molecular and bulk electronic systems. The code implements two types of well established QMC algorithms: Variational Monte Carlo (VMC), and Diffusion Monte Carlo in its robust and efficient lattice regularized variant. A key feature of the code is the possibility of using strongly correlated many-body wave functions. The electronic wave function (WF) is obtained by applying a Jastrow factor, which takes into account dynamical correlations, to the most general mean-field ground state, written either as an antisymmetrized geminal product with spin-singlet pairing, or as a Pfaffian, including both singlet and triplet correlations. This wave function can be viewed as an efficient implementation of the so-called resonating valence bond (RVB) ansatz, first proposed by L. Pauling and P. W. Anderson in quantum chemistry and condensed matter physics, respectively. The RVB ansatz implemented in TurboRVB has a large variational freedom, including the Jastrow correlated Slater determinant as its simplest, but nontrivial case. Moreover, it has the remarkable advantage of remaining with an affordable computational cost, proportional to the one spent for the evaluation of a single Slater determinant. The code implements the adjoint algorithmic differentiation that enables a very efficient evaluation of energy derivatives, comprising the ionic forces. Thus, one can perform structural optimizations and molecular dynamics in the canonical NVT ensemble at the VMC level. For the electronic part, a full WF optimization is made possible thanks to state-of-the-art stochastic algorithms for energy minimization. The code has been efficiently parallelized by using a hybrid MPI-OpenMP protocol, that is also an ideal environment for exploiting the computational power of modern GPU accelerators.

41 pages, 21 figures, 3 tables

References in corpus (90)

• Quantum ESPRESSO: a modular and open-source software project for quantum simulations of materials
• Perspective on density functional theory
• The Interiors of Giant Planets: Models and Outstanding Questions
• Electron Localization in the Insulating State
• Long range Neel order in the triangular Heisenberg model
• Efficient stochastic thermostatting of path integral molecular dynamics
• Continuum variational and diffusion quantum Monte Carlo calculations
• A Constrained Path Monte Carlo Method for Fermion Ground States
• Twist-averaged Boundary Conditions in Continuum Quantum Monte Carlo
• QMCPACK : An open source ab initio Quantum Monte Carlo package for the electronic structure of atoms, molecules, and solids
• The nature and strength of inter-layer binding in graphite
• Optimization of quantum Monte Carlo wave functions by energy minimization
• Green Function Monte Carlo with Stochastic Reconfiguration
• Wave function optimization in the variational Monte Carlo method
• Towards the solution of the many-electron problem in real materials: equation of state of the hydrogen chain with state-of-the-art many-body methods
• Inhomogeneous backflow transformations in quantum Monte Carlo calculations
• Weak binding between two aromatic rings: feeling the van der Waals attraction by quantum Monte Carlo methods
• The Finite Size Error in Many-body Simulations with long-Ranged Interactions
• Beyond the locality approximation in the standard diffusion Monte Carlo method
• Correlated geminal wave function for molecules: an efficient resonating valence bond approach
• Resonating Valence Bond Wave Functions for Strongly Frustrated Spin Systems
• Superconductivity in the two-dimensional t-J model
• Full optimization of Jastrow-Slater wave functions with application to the first-row atoms and homonuclear diatomic molecules
• Geminal wavefunctions with Jastrow correlation: a first application to atoms
• Variational description of Mott insulators
• Ab initio computations of molecular systems by the auxiliary-field quantum Monte Carlo method
• Pfaffian pairing wave functions in electronic structure quantum Monte Carlo
• Size-consistent variational approaches to non-local pseudopotentials: standard and lattice regularized diffusion Monte Carlo methods revisited
• Stable liquid Hydrogen at high pressure by a novel ab-initio molecular dynamics
• Finite-size correction in many-body electronic structure calculations
• Optimizing large parameter sets in variational quantum Monte Carlo
• A New Generation of Effective Core Potentials for Correlated Calculations
• Green Function Monte Carlo with Stochastic Reconfiguration: an effective remedy for the sign problem disease
• Diffusion Monte Carlo with lattice regularization
• Pfaffian pairing and backflow wave functions for electronic structure quantum Monte Carlo methods
• Density matrix quantum Monte Carlo
• Finite size errors in quantum many-body simulations of extended systems
• Proof for an upper bound in fixed-node Monte Carlo for lattice fermions
• Algorithmic differentiation and the calculation of forces by quantum Monte Carlo
• Phase diagram of hydrogen and a hydrogen-helium mixture at planetary conditions by Quantum Monte Carlo simulations
• Strong electronic correlation in the Hydrogen chain: a variational Monte Carlo study
• Resonating valence bond wave function with molecular orbitals: Application to first-row molecules
• New generation of effective core potentials from correlated calculations: 3d transition metal series
• Interaction Picture Density Matrix Quantum Monte Carlo
• Stochastic determination of effective Hamiltonian for the full configuration interaction solution of quasi-degenerate electronic states
• Benchmark all-electron ab initio quantum Monte Carlo calculations for small molecules
• Unexpectedly high pressure for molecular dissociation in liquid hydrogen by a reliable electronic simulation
• Boosting the accuracy and speed of quantum Monte Carlo: size-consistency and time-step
• New generation of effective core potentials from correlated calculations: 2nd row elements
• Ab-initio molecular dynamics simulation of liquid water by Quantum Monte Carlo
• Static and dynamical correlation in diradical molecules by Quantum Monte Carlo using the Jastrow Antisymmetrized Geminal Power ansatz
• Shape and Energy Consistent Pseudopotentials for Correlated Electron systems
• Charge fluctuations close to phase separation in the two dimensional t-J model
• Superconductivity, charge-density waves, antiferromagnetism, and phase separation in the Hubbard-Holstein model
• Spatially homogeneous ground state of the two-dimensional Hubbard model
• Electronic Origin of the Volume Collapse in Cerium
• Developments in Stochastic Coupled Cluster Theory: The initiator approximation and application to the Uniform Electron Gas
• Toward Accurate Adsorption Energetics on Clay Surfaces
• Correlation-Driven Dimerization and Topological Gap Opening in Isotropically Strained Graphene
• A new scheme for fixed node diffusion quantum Monte Carlo with pseudopotentials: improving reproducibility and reducing the trial-wave-function bias
• The HANDE-QMC project: open-source stochastic quantum chemistry from the ground state up
• Molecular properties by Quantum Monte Carlo: an investigation on the role of the wave function ansatz and the basis set in the water molecule
• Distinct metallization and atomization transitions in dense liquid hydrogen
• Finite temperature electronic simulations beyond the Born-Oppenheimer approximation
• Correlated Electron Pseudopotentials for 3d-Transition Metals
• A driven-dissipative quantum Monte Carlo method for open quantum systems
• The fate of the resonating valence bond in graphene
• Ab-initio calculations for the beta-tin diamond transition in Silicon: comparing theories with experiments
• Competing collinear magnetic structures in superconducting FeSe by first principles quantum Monte Carlo calculations
• Molecular hydrogen adsorbed on benzene: insights from a quantum Monte Carlo study
• Systematically convergent method for accurate total energy calculations with localized atomic orbitals
• Fate of the open-shell singlet ground state in the experimentally accessible acenes: a quantum Monte Carlo study
• Multi-state effective Hamiltonian and size-consistency corrections in stochastic configuration interactions
• Efficient Monte Carlo Calculations of the One-Body Density
• Accelerated ab-initio Molecular Dynamics: probing the weak dispersive forces in dense liquid hydrogen
• Exact special twist method for quantum Monte Carlo simulations
• Optimized structure and vibrational properties by error affected potential energy surfaces
• Assessing the Accuracy of the Jastrow Antisymmetrized Geminal Power in the H4 Model System
• All-electron quantum Monte Carlo with Jastrow single determinant Ansatz: application to the sodium dimer
• Geminal embedding scheme for optimal atomic basis set construction in correlated calculations
• Clock Quantum Monte Carlo: an imaginary-time method for real-time quantum dynamics
• The Resonating-Valence-Bond Ground State of Li Nanoclusters
• Speeding up the ab initio diffusion Monte Carlo by a smart lattice regularization
• Improper s-wave symmetry for the electronic pairing in iron-based superconductors by first-principles calculation
• Properties of Reactive Oxygen Species by Quantum Monte Carlo
• van der Waals forces stabilize low-energy polymorphism in B2O3: Implications for the crystallization anomaly
• Theoretical S1 <- S0 absorption energies of the anionic forms of oxyluciferin by Variational Monte Carlo and Many Body Green's Function Theory
• Resonating Valence Bond wave function: from lattice models to realistic systems
• The New Resonating Valence Bond Method for Ab-Initio Electronic Simulations
• General correlated geminal ansatz for electronic structure calculations: exploiting Pfaffians in place of determinants

Cited by in corpus (40)

• Interactions between Large Molecules: Puzzle for Reference Quantum-Mechanical Methods
• Quantum phase diagram of high-pressure hydrogen
• Quantum computing for chemistry and physics applications from a Monte Carlo perspective
• High pressure hydrogen by machine learning and quantum Monte Carlo
• TREXIO: A File Format and Library for Quantum Chemistry
• Atomic forces by quantum Monte Carlo: application to phonon dispersion calculation
• Artificial Neural Networks as Trial Wave Functions for Quantum Monte Carlo
• PyQMC: an all-Python real-space quantum Monte Carlo module in PySCF
• Space-warp coordinate transformation for efficient ionic force calculations in quantum Monte Carlo
• Interatomic force from neural network based variational quantum Monte Carlo
• Taming the fixed-node error in diffusion Monte Carlo via range separation
• Diffusion Monte Carlo Study on Relative Stabilities of Boron Nitride Polymorphs
• Normal liquid ${}^3$He studied by Path Integral Monte Carlo with a parametrized partition function
• Principal deuterium Hugoniot via Quantum Monte Carlo and $\Delta$-learning
• TurboGenius: Python suite for high-throughput calculations of ab initio quantum Monte Carlo methods
• Superconducting properties of the hole-doped three-band \emph{d-p} model studied with minimal-size real-space \emph{d}-wave pairing operators
• Towards chemical accuracy using the Jastrow correlated antisymmetrized geminal power ansatz
• Electronic structure and optical properties of quantum crystals from first principles calculations in the Born-Oppenheimer approximation
• Systematic discrepancies between reference methods for non-covalent interactions within the S66 dataset
• Training models using forces computed by stochastic electronic structure methods
• Ground-state properties of the narrowest zigzag graphene nanoribbon from quantum Monte Carlo and comparison with density functional theory
• Extending the reach of quantum computing for materials science with machine learning potentials
• Basis set incompleteness errors in fixed-node diffusion Monte Carlo calculations on non-covalent interactions
• Efficient calculation of unbiased atomic forces in ab initio Variational Monte Carlo
• A brief introduction to the diffusion Monte Carlo method and the fixed-node approximation
• Candidate structure for the H${}_2$-PRE phase of solid hydrogen
• Reproducibility of fixed-node diffusion Monte Carlo across diverse community codes: The case of water-methane dimer
• High-pressure II-III phase transition in solid hydrogen: Insights from state-of-the-art ab initio calculations
• Deep learning quantum Monte Carlo for solids
• Beyond single-reference fixed-node approximation in ab initio Diffusion Monte Carlo using antisymmetrized geminal power applied to systems with hundreds of electrons
• Equation of state of atomic solid hydrogen by stochastic many-body wave function methods
• Assessing many-body methods on the potential energy surface of the (H${}_2$)${}_2$ hydrogen dimer
• Shifting sands of hardware and software in exascale quantum mechanical simulations
• Accurate and thermodynamically consistent hydrogen equation of state for planetary modeling with flow matching
• Electron correlation effects and spin-liquid state in the Herbertsmithite Kagome lattice
• Self-consistency error correction for accurate machine learning potentials from variational Monte Carlo
• QMCkl: A Kernel Library for Quantum Monte Carlo Applications
• Acceleration of the CASINO quantum Monte Carlo software using graphics processing units and OpenACC
• A Denser Hydrogen Inferred from First-Principles Simulations Challenges Jupiter's Interior Models
• Fast Evaluation of Unbiased Atomic Forces in ab initio Variational Monte Carlo via the Lagrangian Technique