Quantum Package 2.0: An Open-Source Determinant-Driven Suite of Programs

Abstract

\textsc{Quantum Package} is an open-source programming environment for quantum chemistry specially designed for wave function methods. Its main goal is the development of determinant-driven selected configuration interaction (sCI) methods and multi-reference second-order perturbation theory (PT2). The determinant-driven framework allows the programmer to include any arbitrary set of determinants in the reference space, hence providing greater methodological freedoms. The sCI method implemented in \textsc{Quantum Package} is based on the CIPSI (Configuration Interaction using a Perturbative Selection made Iteratively) algorithm which complements the variational sCI energy with a PT2 correction. Additional external plugins have been recently added to perform calculations with multireference coupled cluster theory and range-separated density-functional theory. All the programs are developed with the IRPF90 code generator, which simplifies collaborative work and the development of new features. \textsc{Quantum Package} strives to allow easy implementation and experimentation of new methods, while making parallel computation as simple and efficient as possible on modern supercomputer architectures. Currently, the code enables, routinely, to realize runs on roughly 2\,000 CPU cores, with tens of millions of determinants in the reference space. Moreover, we have been able to push up to 12\,288 cores in order to test its parallel efficiency. In the present manuscript, we also introduce some key new developments: i) a renormalized second-order perturbative correction for efficient extrapolation to the full CI limit, and ii) a stochastic version of the CIPSI selection performed simultaneously to the PT2 calculation at no extra cost.

21 pages, 8 figures

References in corpus (42)

• The Bravyi-Kitaev transformation for quantum computation of electronic structure
• Heat-bath Configuration Interaction: An efficient selected CI algorithm inspired by heat-bath sampling
• Semistochastic Heat-bath Configuration Interaction method: selected configuration interaction with semistochastic perturbation theory
• A Mountaineering Strategy to Excited States: Highly-Accurate Reference Energies and Benchmarks
• QMCPACK : An open source ab initio Quantum Monte Carlo package for the electronic structure of atoms, molecules, and solids
• An adaptive configuration interaction approach for strongly correlated electrons with tunable accuracy
• Cheap and near exact CASSCF with large active spaces
• Reference Energies for Double Excitations
• N-electron valence state perturbation theory based on a density matrix renormalization group reference function, with applications to the chromium dimer and poly-p-phenylene vinylene oligomer
• Excited states using semistochastic heat-bath configuration interaction
• Fast Semistochastic Heat-Bath Configuration Interaction
• Hybrid stochastic-deterministic calculation of the second-order perturbative contribution of multireference perturbation theory
• Excited States of Methylene, Polyenes, and Ozone from Heat-Bath Configuration Interaction
• Selected configuration interaction dressed by perturbation
• Adaptive multiconfigurational wave functions
• Machine Learning Configuration Interaction
• Fixed-Node Diffusion Monte Carlo potential energy curve of the fluorine molecule F2 using selected configuration interaction trial wavefunctions
• Excitation energies from diffusion Monte Carlo using selected Configuration Interaction nodes
• A time-dependent formulation of multi-reference perturbation theory
• Toward an improved control of the fixed-node error in quantum Monte Carlo: The case of the water molecule
• Time-dependent N-electron valence perturbation theory with matrix product state reference wavefunctions for large active spaces and basis sets: Applications to the chromium dimer and all-trans polyenes
• Curing basis-set convergence of wave-function theory using density-functional theory: a systematically improvable approach
• Deterministic construction of nodal surfaces within quantum Monte Carlo: the case of FeS
• Perturbatively selected configuration-interaction wave functions for efficient geometry optimization in quantum Monte Carlo
• An Auxiliary-Field Quantum Monte Carlo Study of the Chromium Dimer
• Unphysical Discontinuities in GW Methods
• Range-separated multideterminant density-functional theory with a short-range correlation functional of the on-top pair density
• Spin density distribution in open-shell transition metal systems: A comparative post-Hartree-Fock, Density Functional Theory and quantum Monte Carlo study of the CuCl2 molecule
• Green functions and self-consistency: insights from the spherium model
• Accurate nonrelativistic ground-state energies of 3d transition metal atoms
• Applying Monte Carlo configuration interaction to transition metal dimers: exploring the balance between static and dynamic correlation
• Quantum Monte Carlo with very large multideterminant wavefunctions
• Excited State Specific Multi-Slater Jastrow Wave Functions
• Using CIPSI nodes in diffusion Monte Carlo
• Three- and four-electron integrals involving Gaussian geminals: fundamental integrals, upper bounds and recurrence relations
• Multi-state effective Hamiltonian and size-consistency corrections in stochastic configuration interactions
• Understanding repulsively mediated superconductivity of correlated electrons via massively parallel DMRG
• Four-component relativistic range-separated density-functional theory: Short-range exchange local-density approximation
• Efficiency of a Multi-Reference Coupled Cluster method
• An efficient implementation of Slater-Condon rules
• Alternative definition of excitation amplitudes in Multi-Reference state-specific Coupled Cluster
• IRPF90: a programming environment for high performance computing

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