Algorithmic differentiations; Dynamical correlations; Efficient implementation; Many body wave functions; Optimization procedures; Quantum Monte Carlo simulations; Resonating valence bonds; Variational Monte Carlo; Physics and Astronomy (all); Physical and Theoretical Chemistry; Physics - Computational Physics; Physics - Materials Science; Physics - Strongly Correlated Electrons; Physics - Chemical Physics
Abstract :
[en] TurboRVB is a computational package for 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 (WFs), capable of describing several materials with very high accuracy, even when standard mean-field approaches [e.g., density functional theory (DFT)] fail. The electronic 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 power with spin-singlet pairing or as a Pfaffian, including both singlet and triplet correlations. This WF can be viewed as an efficient implementation of the so-called resonating valence bond (RVB) Ansatz, first proposed by Pauling and Anderson in quantum chemistry [L. Pauling, The Nature of the Chemical Bond (Cornell University Press, 1960)] and condensed matter physics [P.W. Anderson, Mat. Res. Bull 8, 153 (1973)], 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. Therefore, its application to large systems is computationally feasible. The WF is expanded in a localized basis set. Several basis set functions are implemented, such as Gaussian, Slater, and mixed types, with no restriction on the choice of their contraction. 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 (Jastrow and antisymmetric parts together) is made possible, thanks to state-of-the-art stochastic algorithms for energy minimization. In the optimization procedure, the first guess can be obtained at the mean-field level by a built-in DFT driver. The code has been efficiently parallelized by using a hybrid MPI-OpenMP protocol, which is also an ideal environment for exploiting the computational power of modern Graphics Processing Unit accelerators.
Disciplines :
Physics
Author, co-author :
Nakano, Kousuke ; International School for Advanced Studies (SISSA), Via Bonomea 265, 34136 Trieste, Italy
Attaccalite, Claudio ; Aix-Marseille Université, CNRS, CINaM UMR 7325, Campus de Luminy, 13288 Marseille, France
BARBORINI, Matteo ; University of Luxembourg > Faculty of Science, Technology and Medicine (FSTM) > HPC Platform ; CNR-NANO, Via Campi 213/a, 41125 Modena, Italy
Capriotti, Luca ; New York University, Tandon School of Engineering, 6 MetroTech Center, Brooklyn, New York 11201, USA
Casula, Michele ; Institut de Minéralogie, de Physique des Matériaux et de Cosmochimie (IMPMC), Sorbonne Université, CNRS UMR 7590, IRD UMR 206, MNHN, 4 Place Jussieu, 75252 Paris, France
Coccia, Emanuele ; Department of Chemical and Pharmaceutical Sciences, University of Trieste, Via L. Giorgieri 1, 34127 Trieste, Italy
Dagrada, Mario; Forescout Technologies, John F. Kennedylaan 2, 5612AB Eindhoven, The Netherlands
Genovese, Claudio ; International School for Advanced Studies (SISSA), Via Bonomea 265, 34136 Trieste, Italy
Luo, Ye ; Computational Science Division, Argonne National Laboratory, 9700 S. Cass Avenue, Lemont, Illinois 60439, USA
Mazzola, Guglielmo ; IBM Research Zurich, Säumerstrasse 4, 8803 Rüschlikon, Switzerland
Zen, Andrea ; Department of Earth Sciences, University College London, Gower Street, London WC1E 6BT, United Kingdom
Sorella, Sandro ; International School for Advanced Studies (SISSA), Via Bonomea 265, 34136 Trieste, Italy
External co-authors :
yes
Language :
English
Title :
TurboRVB: A many-body toolkit for ab initio electronic simulations by quantum Monte Carlo.
Progetti di Rilevante Interesse Nazionale Air Force Office of Scientific Research European Cooperation in Science and Technology Simons Foundation Grand Équipement National de Calcul Intensif Partnership for Advanced Computing in Europe AISBL RIKEN Seventh Framework Program
Funding text :
The submitted manuscript has been created by UChicago Argonne, LLC, Operator of Argonne National Laboratory (“Argonne”). Argonne, a U.S. Department of Energy Office of Science laboratory, is operated under Contract No. DE-AC02-06CH11357. The U.S. Government retains for itself, and others acting on its behalf, a paid-up nonexclusive, irrevocable world-wide license in said article to reproduce, prepare derivative works, distribute copies to the public, and perform publicly and display publicly, by or on behalf of the Government. The Department of Energy will provide public access to these results of federally sponsored research in accordance with the DOE Public Access Plan. http://energy.gov/downloads/doe-public-access-plan.K.N. is grateful for computational resources from PRACE, Project No. 2019204934, and those from the facilities of the Research Center for Advanced Computing Infrastructure at Japan Advanced Institute of Science and Technology (JAIST). K.N. also acknowledges financial support from the Simons Foundation and that from Grant-in-Aid for Scientific Research on Innovative Areas (No. 16H06439). C.A. acknowledges funding from the European Union Seventh Framework Program under Grant Agreement No. 785219 Graphene Core 2 and COST Action TUMIEE CA17126. M.C. is grateful to the French grand équipement national de cal-cul intensif (GENCI) for the computational time provided through these years under Project No. 0906493; for the funded PRACE Project Nos. 2012061116, 2015133179, and 2016163936; and for the access to the Hokusai and K-computer granted by the Institute of Physical and Chemical Research (RIKEN). Y.L. was supported by the Argonne Leadership Computing Facility, which is a U.S. Department of Energy Office of Science User Facility operated under Contract No. DE-AC02-06CH11357. A.Z.’s work was sponsored by the Air Force Office of Scientific Research, Air Force Material Command, U.S. Air Force, under Grant No. FA9550-19-1-7007. S.S. acknowledges financial support from PRIN 2017BZPKSZ and computational resources from PRACE, Project No. 2019204934. S.S. is also grateful to his wife L. Urgias for bearing the too many weekends spent on the development of TURBORVB.
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