Benchmarking the pseudopotential and fixed-node approximations in diffusion Monte Carlo calculations of molecules and solids
Abstract
We performed diffusion Monte Carlo (DMC) calculations of the spectroscopic properties of a large set of molecules, assessing the effect of different approximations. In systems containing elements with large atomic numbers, we show that the errors associated with the use of nonlocal mean-field-based pseudopotentials in DMC calculations can be significant and may surpass the fixed-node error. In conclusion, we suggest practical guidelines for reducing these pseudopotential errors, which allow us to obtain DMC-computed spectroscopic parameters of molecules and equation of state properties of solids in excellent agreement with experiment.
- Authors:
-
- Lawrence Livermore National Lab. (LLNL), Livermore, CA (United States)
- Sandia National Lab. (SNL-NM), Albuquerque, NM (United States)
- Publication Date:
- Research Org.:
- Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States); Lawrence Livermore National Laboratory (LLNL), Livermore, CA (United States)
- Sponsoring Org.:
- USDOE Office of Science (SC), Basic Energy Sciences (BES); USDOE National Nuclear Security Administration (NNSA)
- OSTI Identifier:
- 1261352
- Alternate Identifier(s):
- OSTI ID: 1244158; OSTI ID: 1262188
- Report Number(s):
- LLNL-JRNL-676682
Journal ID: ISSN 2469-9950; KC0202030; ERKCK03
- Grant/Contract Number:
- AC05-00OR22725; AC52-07NA27344; AC04-94AL85000; LDRD 13- ERD-067
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Physical Review B
- Additional Journal Information:
- Journal Volume: 93; Journal Issue: 9; Journal ID: ISSN 2469-9950
- Publisher:
- American Physical Society (APS)
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND SUPERFLUIDITY; 74 ATOMIC AND MOLECULAR PHYSICS; 36 MATERIALS SCIENCE
Citation Formats
Nazarov, Roman, Shulenburger, Luke, Morales, Miguel A., and Hood, Randolph Q. Benchmarking the pseudopotential and fixed-node approximations in diffusion Monte Carlo calculations of molecules and solids. United States: N. p., 2016.
Web. doi:10.1103/PhysRevB.93.094111.
Nazarov, Roman, Shulenburger, Luke, Morales, Miguel A., & Hood, Randolph Q. Benchmarking the pseudopotential and fixed-node approximations in diffusion Monte Carlo calculations of molecules and solids. United States. https://doi.org/10.1103/PhysRevB.93.094111
Nazarov, Roman, Shulenburger, Luke, Morales, Miguel A., and Hood, Randolph Q. Mon .
"Benchmarking the pseudopotential and fixed-node approximations in diffusion Monte Carlo calculations of molecules and solids". United States. https://doi.org/10.1103/PhysRevB.93.094111. https://www.osti.gov/servlets/purl/1261352.
@article{osti_1261352,
title = {Benchmarking the pseudopotential and fixed-node approximations in diffusion Monte Carlo calculations of molecules and solids},
author = {Nazarov, Roman and Shulenburger, Luke and Morales, Miguel A. and Hood, Randolph Q.},
abstractNote = {We performed diffusion Monte Carlo (DMC) calculations of the spectroscopic properties of a large set of molecules, assessing the effect of different approximations. In systems containing elements with large atomic numbers, we show that the errors associated with the use of nonlocal mean-field-based pseudopotentials in DMC calculations can be significant and may surpass the fixed-node error. In conclusion, we suggest practical guidelines for reducing these pseudopotential errors, which allow us to obtain DMC-computed spectroscopic parameters of molecules and equation of state properties of solids in excellent agreement with experiment.},
doi = {10.1103/PhysRevB.93.094111},
journal = {Physical Review B},
number = 9,
volume = 93,
place = {United States},
year = {Mon Mar 28 00:00:00 EDT 2016},
month = {Mon Mar 28 00:00:00 EDT 2016}
}
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Works referenced in this record:
Improved semiconductor lattice parameters and band gaps from a middle-range screened hybrid exchange functional
journal, March 2012
- Lucero, M. J.; Henderson, T. M.; Scuseria, G. E.
- Journal of Physics: Condensed Matter, Vol. 24, Issue 14
Electronic surface error in the Si interstitial formation energy
journal, April 2008
- Mattsson, Ann E.; Wixom, Ryan R.; Armiento, Rickard
- Physical Review B, Vol. 77, Issue 15
Temperature-driven phase transitions from first principles including all relevant excitations: The fcc-to-bcc transition in Ca
journal, December 2011
- Grabowski, B.; Söderlind, P.; Hickel, T.
- Physical Review B, Vol. 84, Issue 21
Vacancies in Metals: From First-Principles Calculations to Experimental Data
journal, October 2000
- Carling, Karin; Wahnström, Göran; Mattsson, Thomas R.
- Physical Review Letters, Vol. 85, Issue 18
Ground State of the Electron Gas by a Stochastic Method
journal, August 1980
- Ceperley, D. M.; Alder, B. J.
- Physical Review Letters, Vol. 45, Issue 7, p. 566-569
Towards an exact description of electronic wavefunctions in real solids
journal, December 2012
- Booth, George H.; Grüneis, Andreas; Kresse, Georg
- Nature, Vol. 493, Issue 7432
Quantum Monte Carlo simulations of solids
journal, January 2001
- Foulkes, W. M. C.; Mitas, L.; Needs, R. J.
- Reviews of Modern Physics, Vol. 73, Issue 1
Applications of quantum Monte Carlo methods in condensed systems
journal, January 2011
- Kolorenč, Jindřich; Mitas, Lubos
- Reports on Progress in Physics, Vol. 74, Issue 2
Recent progress in the field of electron correlation
journal, April 1994
- Senatore, G.; March, N. H.
- Reviews of Modern Physics, Vol. 66, Issue 2
Continuous-time Monte Carlo methods for quantum impurity models
journal, May 2011
- Gull, Emanuel; Millis, Andrew J.; Lichtenstein, Alexander I.
- Reviews of Modern Physics, Vol. 83, Issue 2
Quantum Monte Carlo Method using Phase-Free Random Walks with Slater Determinants
journal, April 2003
- Zhang, Shiwei; Krakauer, Henry
- Physical Review Letters, Vol. 90, Issue 13
Path integrals in the theory of condensed helium
journal, April 1995
- Ceperley, D. M.
- Reviews of Modern Physics, Vol. 67, Issue 2
Linear-Scaling Quantum Monte Carlo Calculations
journal, November 2001
- Williamson, A. J.; Hood, Randolph Q.; Grossman, J. C.
- Physical Review Letters, Vol. 87, Issue 24
Effects of three-body and backflow correlations in the two-dimensional electron gas
journal, October 1993
- Kwon, Yongkyung; Ceperley, D. M.; Martin, Richard M.
- Physical Review B, Vol. 48, Issue 16
New stochastic method for systems with broken time-reversal symmetry: 2D fermions in a magnetic field
journal, October 1993
- Ortiz, G.; Ceperley, D. M.; Martin, R. M.
- Physical Review Letters, Vol. 71, Issue 17
Quantum Monte Carlo study of circular quantum dots in presence of Rashba interaction
journal, April 2011
- Ambrosetti, A.; Pederiva, F.; Lipparini, E.
- Physical Review B, Vol. 83, Issue 15
Twist-averaged boundary conditions in continuum quantum Monte Carlo algorithms
journal, June 2001
- Lin, C.; Zong, F. H.; Ceperley, D. M.
- Physical Review E, Vol. 64, Issue 1
The statistical error of green's function Monte Carlo
journal, June 1986
- Ceperley, D. M.
- Journal of Statistical Physics, Vol. 43, Issue 5-6
Valence quantum Monte Carlo with a b i n i t i o effective core potentials
journal, July 1987
- Hammond, Brian L.; Reynolds, Peter J.; Lester, William A.
- The Journal of Chemical Physics, Vol. 87, Issue 2
Relativistic Pseudopotentials: Their Development and Scope of Applications
journal, September 2011
- Dolg, Michael; Cao, Xiaoyan
- Chemical Reviews, Vol. 112, Issue 1
Chemically Motivated Pseudopotential for Sodium
journal, February 1973
- Topp, William C.; Hopfield, John J.
- Physical Review B, Vol. 7, Issue 4
New Method for Calculating Wave Functions in Crystals and Molecules
journal, October 1959
- Phillips, James C.; Kleinman, Leonard
- Physical Review, Vol. 116, Issue 2
Norm-Conserving Pseudopotentials
journal, November 1979
- Hamann, D. R.; Schlüter, M.; Chiang, C.
- Physical Review Letters, Vol. 43, Issue 20
Norm-conserving Hartree–Fock pseudopotentials and their asymptotic behavior
journal, January 2005
- Trail, J. R.; Needs, R. J.
- The Journal of Chemical Physics, Vol. 122, Issue 1
Smooth relativistic Hartree–Fock pseudopotentials for H to Ba and Lu to Hg
journal, May 2005
- Trail, J. R.; Needs, R. J.
- The Journal of Chemical Physics, Vol. 122, Issue 17
Energy-consistent pseudopotentials for quantum Monte Carlo calculations
journal, June 2007
- Burkatzki, M.; Filippi, C.; Dolg, M.
- The Journal of Chemical Physics, Vol. 126, Issue 23
Energy-consistent small-core pseudopotentials for 3d-transition metals adapted to quantum Monte Carlo calculations
journal, October 2008
- Burkatzki, M.; Filippi, Claudia; Dolg, M.
- The Journal of Chemical Physics, Vol. 129, Issue 16
Improved Pauli Hamiltonian for local-potential problems
journal, September 1978
- Wood, J. H.; Boring, A. Michael
- Physical Review B, Vol. 18, Issue 6
Pseudopotentials for correlated electron systems
journal, July 2013
- Trail, J. R.; Needs, R. J.
- The Journal of Chemical Physics, Vol. 139, Issue 1
Correlated electron pseudopotentials for 3d-transition metals
journal, February 2015
- Trail, J. R.; Needs, R. J.
- The Journal of Chemical Physics, Vol. 142, Issue 6
Generalized Gradient Approximation Made Simple
journal, October 1996
- Perdew, John P.; Burke, Kieron; Ernzerhof, Matthias
- Physical Review Letters, Vol. 77, Issue 18, p. 3865-3868
Generalized Gradient Approximation Made Simple [Phys. Rev. Lett. 77, 3865 (1996)]
journal, February 1997
- Perdew, John P.; Burke, Kieron; Ernzerhof, Matthias
- Physical Review Letters, Vol. 78, Issue 7
Variational Quantum Monte Carlo Nonlocal Pseudopotential Approach to Solids: Cohesive and Structural Properties of Diamond
journal, October 1988
- Fahy, S.; Wang, X. W.; Louie, Steven G.
- Physical Review Letters, Vol. 61, Issue 14
Erratum: Variational quantum Monte Carlo nonlocal pseudopotential approach to solids: Formulation and application to diamond, graphite, and silicon
journal, April 1991
- Fahy, S.; Wang, X. W.; Louie, Steven G.
- Physical Review B, Vol. 43, Issue 11
Quantum Monte Carlo applied to solids
journal, December 2013
- Shulenburger, Luke; Mattsson, Thomas R.
- Physical Review B, Vol. 88, Issue 24
Toward reliable density functional methods without adjustable parameters: The PBE0 model
journal, April 1999
- Adamo, Carlo; Barone, Vincenzo
- The Journal of Chemical Physics, Vol. 110, Issue 13
Hybrid functionals based on a screened Coulomb potential
journal, May 2003
- Heyd, Jochen; Scuseria, Gustavo E.; Ernzerhof, Matthias
- The Journal of Chemical Physics, Vol. 118, Issue 18
Comparison of Density Functional and MP2 Calculations on the Water Monomer and Dimer
journal, October 1994
- Kim, K.; Jordan, K. D.
- The Journal of Physical Chemistry, Vol. 98, Issue 40
Ab Initio Calculation of Vibrational Absorption and Circular Dichroism Spectra Using Density Functional Force Fields
journal, November 1994
- Stephens, P. J.; Devlin, F. J.; Chabalowski, C. F.
- The Journal of Physical Chemistry, Vol. 98, Issue 45, p. 11623-11627
A soft Hartree–Fock pseudopotential for carbon with application to quantum Monte Carlo
journal, August 1998
- Greeff, C. W.; Lester, W. A.
- The Journal of Chemical Physics, Vol. 109, Issue 5
Effective Core Potentials for DFT Calculations
journal, November 1995
- Russo, Thomas V.; Martin, Richard L.; Hay, P. Jeffrey
- The Journal of Physical Chemistry, Vol. 99, Issue 47
Fully relativistic correlated benchmark results for uranyl and a critical look at relativistic effective core potentials for uranium
journal, December 2001
- de Jong, W. A.; Harrison, R. J.; Nichols, J. A.
- Theoretical Chemistry Accounts: Theory, Computation, and Modeling (Theoretica Chimica Acta), Vol. 107, Issue 1
Nonlocal pseudopotentials and diffusion Monte Carlo
journal, September 1991
- Mitáš, Luboš; Shirley, Eric L.; Ceperley, David M.
- The Journal of Chemical Physics, Vol. 95, Issue 5
Efficient pseudopotentials for plane-wave calculations
journal, January 1991
- Troullier, N.; Martins, José Luriaas
- Physical Review B, Vol. 43, Issue 3
Transferable relativistic Dirac-Slater pseudopotentials
journal, July 2000
- Grinberg, Ilya; Ramer, Nicholas J.; Rappe, Andrew M.
- Physical Review B, Vol. 62, Issue 4
Architecture of Qbox: A scalable first-principles molecular dynamics code
journal, January 2008
- Gygi, F.
- IBM Journal of Research and Development, Vol. 52, Issue 1.2
Efficacious Form for Model Pseudopotentials
journal, May 1982
- Kleinman, Leonard; Bylander, D. M.
- Physical Review Letters, Vol. 48, Issue 20
QUANTUM ESPRESSO: a modular and open-source software project for quantum simulations of materials
journal, September 2009
- Giannozzi, Paolo; Baroni, Stefano; Bonini, Nicola
- Journal of Physics: Condensed Matter, Vol. 21, Issue 39, Article No. 395502
Beyond the locality approximation in the standard diffusion Monte Carlo method
journal, October 2006
- Casula, Michele
- Physical Review B, Vol. 74, Issue 16
Jastrow correlation factor for atoms, molecules, and solids
journal, December 2004
- Drummond, N. D.; Towler, M. D.; Needs, R. J.
- Physical Review B, Vol. 70, Issue 23
Continuum variational and diffusion quantum Monte Carlo calculations
journal, December 2009
- Needs, R. J.; Towler, M. D.; Drummond, N. D.
- Journal of Physics: Condensed Matter, Vol. 22, Issue 2
Diatomic Molecules According to the Wave Mechanics. II. Vibrational Levels
journal, July 1929
- Morse, Philip M.
- Physical Review, Vol. 34, Issue 1
The Compressibility of Media under Extreme Pressures
journal, September 1944
- Murnaghan, F. D.
- Proceedings of the National Academy of Sciences, Vol. 30, Issue 9
A universal equation of state for solids
journal, July 1986
- Vinet, P.; Ferrante, J.; Smith, J. R.
- Journal of Physics C: Solid State Physics, Vol. 19, Issue 20
An Introduction to the Bootstrap
book, January 1993
- Efron, Bradley; Tibshirani, Robert J.
- Chapman and Hall/CRC
The bond length of silver dimer
journal, November 1991
- Simard, Benoit; Hackett, Peter A.; James, Andrew M.
- Chemical Physics Letters, Vol. 186, Issue 4-5
Simulated annealing study of neutral and charged clusters: Al n and Ga n
journal, July 1993
- Jones, R. O.
- The Journal of Chemical Physics, Vol. 99, Issue 2
Potential-energy functions of diatomic molecules of the noble gases I. Like nuclear species
journal, October 1992
- Ogilvie, J. F.; Wang, Frank Y. H.
- Journal of Molecular Structure, Vol. 273
On the electronic spectrum of the Mo2 molecule observed after flash photolysis of Mo(CO)6
journal, December 1978
- Efremov, Yu. M.; Samoilova, A. N.; Kozhukhovsky, V. B.
- Journal of Molecular Spectroscopy, Vol. 73, Issue 3
Potential energy curves and dissociation energies of NbO, SiC, CP, PH+, SiF+, and NH+
journal, January 1992
- Reddy, R. R.; Rao, T. V. R.; Viswanath, R.
- Astrophysics and Space Science, Vol. 189, Issue 1
Dissociation energy and excited-state properties of diatomic Sn2
journal, January 1988
- Pak, K.; Cai, M. F.; Dzugan, T. P.
- Faraday Discussions of the Chemical Society, Vol. 86
Photoionization spectroscopy of dichromium and dimolybdenum: Ionization potentials and bond energies
journal, June 1998
- Simard, Benoit; Lebeault-Dorget, Marie-Ange; Marijnissen, Adrian
- The Journal of Chemical Physics, Vol. 108, Issue 23
Electronic structure and bonding in the Pd 2 molecule by all electron a b i n i t i o HF–CI calculations and mass spectrometric measurements
journal, May 1984
- Shim, Irene; Gingerich, Karl A.
- The Journal of Chemical Physics, Vol. 80, Issue 10
Thermodynamic investigation of the gaseous molecules TiRh, Rh 2 , and Ti 2 Rh by mass spectrometry
journal, March 1974
- Cocke, D. L.; Gingerich, K. A.
- The Journal of Chemical Physics, Vol. 60, Issue 5
Analysis of the E-X and C-X band system isotopically enriched of Ag2
journal, November 1981
- Srdanov, V. I.; Pešić, D. S.
- Journal of Molecular Spectroscopy, Vol. 90, Issue 1
Dissociation Energy of Pd 2
journal, September 1969
- Lin, Sin‐Shong; Strauss, Bernard; Kant, Arthur
- The Journal of Chemical Physics, Vol. 51, Issue 5
Spectroscopy of mass-selected rhodium dimers in argon matrices
journal, February 1997
- Wang, Huaiming; Haouari, Hanae; Craig, R.
- The Journal of Chemical Physics, Vol. 106, Issue 6
Electron structure calculations including CI for ten low lying states of Pb 2 and Sn 2 . Partition function and dissociation energy of Sn 2
journal, January 1983
- Balasubramanian, K.; Pitzer, Kenneth S.
- The Journal of Chemical Physics, Vol. 78, Issue 1
Spectroscopy of mass‐selected tantalum dimers in argon matrices
journal, June 1992
- Hu, Zhendong; Shen, Bo; Lombardi, J. R.
- The Journal of Chemical Physics, Vol. 96, Issue 12
Error Estimates for Solid-State Density-Functional Theory Predictions: An Overview by Means of the Ground-State Elemental Crystals
journal, October 2013
- Lejaeghere, K.; Van Speybroeck, V.; Van Oost, G.
- Critical Reviews in Solid State and Materials Sciences, Vol. 39, Issue 1
Atomic-environment classification of the chemical elements
journal, June 1993
- Villars, P.; Daams, J. L. C.
- Journal of Alloys and Compounds, Vol. 197, Issue 2
The crystal dynamics of grey (α) tin at 90°K
journal, October 1969
- Price, D. L.; Rowe, J. M.
- Solid State Communications, Vol. 7, Issue 19
Ab initio Quantum Monte Carlo Calculations of Spin Superexchange in Cuprates: The Benchmarking Case of
journal, July 2014
- Foyevtsova, Kateryna; Krogel, Jaron T.; Kim, Jeongnim
- Physical Review X, Vol. 4, Issue 3
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- Santana, Juan A.; Krogel, Jaron T.; Kent, Paul R. C.
- The Journal of Chemical Physics, Vol. 144, Issue 17
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journal, June 2016
- Melton, Cody A.; Bennett, M. Chandler; Mitas, Lubos
- The Journal of Chemical Physics, Vol. 144, Issue 24
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journal, March 2017
- Krongchon, Kittithat; Busemeyer, Brian; Wagner, Lucas K.
- The Journal of Chemical Physics, Vol. 146, Issue 12
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journal, June 2017
- Krogel, Jaron T.; Kent, P. R. C.
- The Journal of Chemical Physics, Vol. 146, Issue 24
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journal, July 2017
- Dzubak, Allison L.; Krogel, Jaron T.; Reboredo, Fernando A.
- The Journal of Chemical Physics, Vol. 147, Issue 2
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journal, December 2017
- Bennett, M. Chandler; Melton, Cody A.; Annaberdiyev, Abdulgani
- The Journal of Chemical Physics, Vol. 147, Issue 22
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journal, September 2018
- Bennett, M. Chandler; Wang, Guangming; Annaberdiyev, Abdulgani
- The Journal of Chemical Physics, Vol. 149, Issue 10
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journal, October 2018
- Zhang, Shuai; Malone, Fionn D.; Morales, Miguel A.
- The Journal of Chemical Physics, Vol. 149, Issue 16
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text, January 2016
- Santana, Juan A.; Krogel, Jaron T.; Kent, Paul R. C.
- arXiv
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- Ma, Fengjie; Zhang, Shiwei; Krakauer, Henry
- arXiv
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- Krogel, Jaron T.; Kent, Paul R. C.
- arXiv