Rationalizing accurate structure prediction in the meta-GGA SCAN functional
Abstract
The ability of first-principles computational methods to reproduce ground-state crystal structure selection is key to their application in the discovery of new materials, and yet presents a formidable challenge due to the low-energy scale of the problem and lack of systematic error cancellation. The recently developed Strongly Constrained and Appropriately Normed (SCAN) functional is notable for accurately calculating physical properties such as formation energies and in particular, correctly predicting ground-state structures. Here in this paper, we attempt to rationalize the improved structure prediction accuracy in SCAN by investigating the relationship between preferred coordination environments, the description of attractive van der Waals (vdW) interactions, and the overall ground-state prediction in bulk main-group solids. We observe a systematic undercoordination error in the traditional Perdew, Burke, and Ernzerhof (PBE) functional which is not present in SCAN results and find that semiempirical dispersion corrections in the form of PBE + D 3 fail to correct this error in a consistent or physical manner. We conclude that the medium-range vdW interaction is correctly parametrized in SCAN and yields meaningful relative energies between coordination environments.
- Authors:
-
- Univ. of California, Berkeley, CA (United States). Dept. of Materials Science and Engineering; Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). Materials Science Division
- Univ. of California, Santa Barbara, CA (United States). Materials Dept.
- Publication Date:
- Research Org.:
- Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
- Sponsoring Org.:
- USDOE Office of Science (SC), Basic Energy Sciences (BES)
- OSTI Identifier:
- 1572034
- Alternate Identifier(s):
- OSTI ID: 1545429
- Grant/Contract Number:
- AC02-05CH11231; AC02-05-CH11231
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Physical Review B
- Additional Journal Information:
- Journal Volume: 100; Journal Issue: 3; Journal ID: ISSN 2469-9950
- Publisher:
- American Physical Society (APS)
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 36 MATERIALS SCIENCE
Citation Formats
Yang, Julia H., Kitchaev, Daniil A., and Ceder, Gerbrand. Rationalizing accurate structure prediction in the meta-GGA SCAN functional. United States: N. p., 2019.
Web. doi:10.1103/physrevb.100.035132.
Yang, Julia H., Kitchaev, Daniil A., & Ceder, Gerbrand. Rationalizing accurate structure prediction in the meta-GGA SCAN functional. United States. doi:https://doi.org/10.1103/physrevb.100.035132
Yang, Julia H., Kitchaev, Daniil A., and Ceder, Gerbrand. Fri .
"Rationalizing accurate structure prediction in the meta-GGA SCAN functional". United States. doi:https://doi.org/10.1103/physrevb.100.035132. https://www.osti.gov/servlets/purl/1572034.
@article{osti_1572034,
title = {Rationalizing accurate structure prediction in the meta-GGA SCAN functional},
author = {Yang, Julia H. and Kitchaev, Daniil A. and Ceder, Gerbrand},
abstractNote = {The ability of first-principles computational methods to reproduce ground-state crystal structure selection is key to their application in the discovery of new materials, and yet presents a formidable challenge due to the low-energy scale of the problem and lack of systematic error cancellation. The recently developed Strongly Constrained and Appropriately Normed (SCAN) functional is notable for accurately calculating physical properties such as formation energies and in particular, correctly predicting ground-state structures. Here in this paper, we attempt to rationalize the improved structure prediction accuracy in SCAN by investigating the relationship between preferred coordination environments, the description of attractive van der Waals (vdW) interactions, and the overall ground-state prediction in bulk main-group solids. We observe a systematic undercoordination error in the traditional Perdew, Burke, and Ernzerhof (PBE) functional which is not present in SCAN results and find that semiempirical dispersion corrections in the form of PBE + D 3 fail to correct this error in a consistent or physical manner. We conclude that the medium-range vdW interaction is correctly parametrized in SCAN and yields meaningful relative energies between coordination environments.},
doi = {10.1103/physrevb.100.035132},
journal = {Physical Review B},
number = 3,
volume = 100,
place = {United States},
year = {2019},
month = {7}
}
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Works referenced in this record:
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
Temperature-induced structural changes in , and : A synchrotron x-ray powder diffraction study
journal, December 2005
- Howard, Christopher J.; Kennedy, Brendan J.; Curfs, Caroline
- Physical Review B, Vol. 72, Issue 21
The Crystal Structure of Cesium Monoxide
journal, March 1956
- Tsai, Khi-Ruey; Harris, P. M.; Lassettre, E. N.
- The Journal of Physical Chemistry, Vol. 60, Issue 3
Calculation of the lattice constant of solids with semilocal functionals
journal, February 2009
- Haas, Philipp; Tran, Fabien; Blaha, Peter
- Physical Review B, Vol. 79, Issue 8
TlBr and TlBrxI1−x crystals for γ-ray detectors
journal, April 2010
- Churilov, Alexei V.; Ciampi, Guido; Kim, Hadong
- Journal of Crystal Growth, Vol. 312, Issue 8
From semilocal density functionals to random phase approximation renormalized perturbation theory: A methodological assessment of structural phase transitions
journal, June 2018
- Sengupta, Niladri; Bates, Jefferson E.; Ruzsinszky, Adrienn
- Physical Review B, Vol. 97, Issue 23
Performance of various density-functional approximations for cohesive properties of 64 bulk solids
journal, June 2018
- Zhang, Guo-Xu; Reilly, Anthony M.; Tkatchenko, Alexandre
- New Journal of Physics, Vol. 20, Issue 6
Data Mined Ionic Substitutions for the Discovery of New Compounds
journal, January 2011
- Hautier, Geoffroy; Fischer, Chris; Ehrlacher, Virginie
- Inorganic Chemistry, Vol. 50, Issue 2
Machine-learning the configurational energy of multicomponent crystalline solids
journal, November 2018
- Natarajan, Anirudh Raju; Van der Ven, Anton
- npj Computational Materials, Vol. 4, Issue 1
Evaluating transition metal oxides within DFT-SCAN and frameworks for solar thermochemical applications
journal, September 2018
- Sai Gautam, Gopalakrishnan; Carter, Emily A.
- Physical Review Materials, Vol. 2, Issue 9
Atomic Radii and Interatomic Distances in Metals
journal, March 1947
- Pauling, Linus
- Journal of the American Chemical Society, Vol. 69, Issue 3
Improved lower bound on the indirect Coulomb energy
journal, March 1981
- Lieb, Elliott H.; Oxford, Stephen
- International Journal of Quantum Chemistry, Vol. 19, Issue 3
Construction of a generalized gradient approximation by restoring the density-gradient expansion and enforcing a tight Lieb–Oxford bound
journal, May 2008
- Zhao, Yan; Truhlar, Donald G.
- The Journal of Chemical Physics, Vol. 128, Issue 18
A Fractionally Ionic Approach to Polarizability and van der Waals Many-Body Dispersion Calculations
journal, November 2016
- Gould, Tim; Lebègue, Sébastien; Ángyán, János G.
- Journal of Chemical Theory and Computation, Vol. 12, Issue 12
VESTA 3 for three-dimensional visualization of crystal, volumetric and morphology data
journal, October 2011
- Momma, Koichi; Izumi, Fujio
- Journal of Applied Crystallography, Vol. 44, Issue 6
Accurate Molecular Van Der Waals Interactions from Ground-State Electron Density and Free-Atom Reference Data
journal, February 2009
- Tkatchenko, Alexandre; Scheffler, Matthias
- Physical Review Letters, Vol. 102, Issue 7
An X-ray diffraction study of the SrBrxI2−x system
journal, March 1983
- Hodorowicz, Stanislaw A.; Eick, Harry A.
- Journal of Solid State Chemistry, Vol. 46, Issue 3
New developments in the Inorganic Crystal Structure Database (ICSD): accessibility in support of materials research and design
journal, May 2002
- Belsky, Alec; Hellenbrandt, Mariette; Karen, Vicky Lynn
- Acta Crystallographica Section B Structural Science, Vol. 58, Issue 3
Polymorphism, compressibility and thermal expansion of thallous iodide
journal, October 1967
- Samara, G. A.; Walters, L. C.; Northrop, David A.
- Journal of Physics and Chemistry of Solids, Vol. 28, Issue 10
Energetics of polymorphs in density functional theory
journal, January 2016
- Kitchaev, Daniil A.; Peng, Haowei; Liu, Yun
- Physical Review B, Vol. 93, Issue 4
The structure of a metastable form of SrI2 by the X-Ray rietveld procedure
journal, December 1989
- Liu, Guo; Eick, H. A.
- Journal of the Less Common Metals, Vol. 156, Issue 1-2
Evaluation of van der Waals density functionals for layered materials
journal, March 2018
- Tawfik, Sherif Abdulkader; Gould, Tim; Stampfl, Catherine
- Physical Review Materials, Vol. 2, Issue 3
Evaluating structure selection in the hydrothermal growth of FeS2 pyrite and marcasite
journal, December 2016
- Kitchaev, Daniil A.; Ceder, Gerbrand
- Nature Communications, Vol. 7, Issue 1
A consistent and accurate ab initio parametrization of density functional dispersion correction (DFT-D) for the 94 elements H-Pu
journal, April 2010
- Grimme, Stefan; Antony, Jens; Ehrlich, Stephan
- The Journal of Chemical Physics, Vol. 132, Issue 15
Strongly Constrained and Appropriately Normed Semilocal Density Functional
journal, July 2015
- Sun, Jianwei; Ruzsinszky, Adrienn; Perdew, John P.
- Physical Review Letters, Vol. 115, Issue 3
Self-Consistent Equations Including Exchange and Correlation Effects
journal, November 1965
- Kohn, W.; Sham, L. J.
- Physical Review, Vol. 140, Issue 4A, p. A1133-A1138
A generalized-gradient approximation exchange hole model for dispersion coefficients
journal, January 2011
- Steinmann, Stephan N.; Corminboeuf, Clemence
- The Journal of Chemical Physics, Vol. 134, Issue 4
Efficient first-principles prediction of solid stability: Towards chemical accuracy
journal, March 2018
- Zhang, Yubo; Kitchaev, Daniil A.; Yang, Julia
- npj Computational Materials, Vol. 4, Issue 1
Ferroelastic phase transition in CaCl2 studied by Raman spectroscopy
journal, February 1992
- Unruh, H. -G.; M�hlenberg, D.; Hahn, Ch.
- Zeitschrift f�r Physik B Condensed Matter, Vol. 86, Issue 1
Applicability of the Strongly Constrained and Appropriately Normed Density Functional to Transition-Metal Magnetism
journal, November 2018
- Fu, Yuhao; Singh, David J.
- Physical Review Letters, Vol. 121, Issue 20
Prescription for the design and selection of density functional approximations: More constraint satisfaction with fewer fits
journal, August 2005
- Perdew, John P.; Ruzsinszky, Adrienn; Tao, Jianmin
- The Journal of Chemical Physics, Vol. 123, Issue 6
Efficiency of ab-initio total energy calculations for metals and semiconductors using a plane-wave basis set
journal, July 1996
- Kresse, G.; Furthmüller, J.
- Computational Materials Science, Vol. 6, Issue 1, p. 15-50
Accurate critical pressures for structural phase transitions of group IV, III-V, and II-VI compounds from the SCAN density functional
journal, March 2018
- Shahi, Chandra; Sun, Jianwei; Perdew, John P.
- Physical Review B, Vol. 97, Issue 9
Erratum: Restoring the Density-Gradient Expansion for Exchange in Solids and Surfaces [Phys. Rev. Lett. 100 , 136406 (2008)]
journal, January 2009
- Perdew, John P.; Ruzsinszky, Adrienn; Csonka, Gábor I.
- Physical Review Letters, Vol. 102, Issue 3
Completely numerical calculations on diatomic molecules in the local-density approximation
journal, April 1986
- Becke, A. D.
- Physical Review A, Vol. 33, Issue 4
Molecular excitation energies to high-lying bound states from time-dependent density-functional response theory: Characterization and correction of the time-dependent local density approximation ionization threshold
journal, March 1998
- Casida, Mark E.; Jamorski, Christine; Casida, Kim C.
- The Journal of Chemical Physics, Vol. 108, Issue 11
Efficient iterative schemes for ab initio total-energy calculations using a plane-wave basis set
journal, October 1996
- Kresse, G.; Furthmüller, J.
- Physical Review B, Vol. 54, Issue 16, p. 11169-11186
Relative stability of FeS 2 polymorphs with the random phase approximation approach
journal, January 2018
- Zhang, Min-Ye; Cui, Zhi-Hao; Jiang, Hong
- Journal of Materials Chemistry A, Vol. 6, Issue 15
Commentary: The Materials Project: A materials genome approach to accelerating materials innovation
journal, July 2013
- Jain, Anubhav; Ong, Shyue Ping; Hautier, Geoffroy
- APL Materials, Vol. 1, Issue 1
Inhomogeneous Electron Gas
journal, November 1964
- Hohenberg, P.; Kohn, W.
- Physical Review, Vol. 136, Issue 3B, p. B864-B871
Density Functionals that Recognize Covalent, Metallic, and Weak Bonds
journal, September 2013
- Sun, Jianwei; Xiao, Bing; Fang, Yuan
- Physical Review Letters, Vol. 111, Issue 10
The Polymorphism of Thallium and Other Halides at Low Temperatures
journal, February 1961
- Blackman, M.; Khan, I. H.
- Proceedings of the Physical Society, Vol. 77, Issue 2
Accurate and Efficient Method for Many-Body van der Waals Interactions
journal, June 2012
- Tkatchenko, Alexandre; DiStasio, Robert A.; Car, Roberto
- Physical Review Letters, Vol. 108, Issue 23
Inhomogeneous Electron Gas
journal, March 1973
- Rajagopal, A. K.; Callaway, J.
- Physical Review B, Vol. 7, Issue 5
Predicting accurate cathode properties of layered oxide materials using the SCAN meta-GGA density functional
journal, November 2018
- Chakraborty, Arup; Dixit, Mudit; Aurbach, Doron
- npj Computational Materials, Vol. 4, Issue 1
Identifying promising metal–organic frameworks for heterogeneous catalysis via high‐throughput periodic density functional theory
journal, February 2019
- Rosen, Andrew S.; Notestein, Justin M.; Snurr, Randall Q.
- Journal of Computational Chemistry, Vol. 40, Issue 12
Electronic structure and physical properties of early transition metal mononitrides: Density-functional theory LDA, GGA, and screened-exchange LDA FLAPW calculations
journal, March 2001
- Stampfl, C.; Mannstadt, W.; Asahi, R.
- Physical Review B, Vol. 63, Issue 15
Are DFT level calculations the answer to real-world molecular systems?
journal, March 2003
- Meier, Robert J.
- Computational Materials Science, Vol. 27, Issue 1-2
The role of decomposition reactions in assessing first-principles predictions of solid stability
journal, January 2019
- Bartel, Christopher J.; Weimer, Alan W.; Lany, Stephan
- npj Computational Materials, Vol. 5, Issue 1
Versatile van der Waals Density Functional Based on a Meta-Generalized Gradient Approximation
journal, October 2016
- Peng, Haowei; Yang, Zeng-Hui; Perdew, John P.
- Physical Review X, Vol. 6, Issue 4
Comparison of approximations in density functional theory calculations: Energetics and structure of binary oxides
journal, September 2017
- Hinuma, Yoyo; Hayashi, Hiroyuki; Kumagai, Yu
- Physical Review B, Vol. 96, Issue 9
The crystal structure of tin(II) iodide
journal, October 1972
- Howie, R. A.; Moser, W.; Trevena, I. C.
- Acta Crystallographica Section B Structural Crystallography and Crystal Chemistry, Vol. 28, Issue 10, p. 2965-2971
Subtlety of TiO 2 phase stability: Reliability of the density functional theory predictions and persistence of the self-interaction error
journal, January 2019
- Zhang, Yubo; Furness, James W.; Xiao, Bing
- The Journal of Chemical Physics, Vol. 150, Issue 1
Gedanken densities and exact constraints in density functional theory
journal, May 2014
- Perdew, John P.; Ruzsinszky, Adrienn; Sun, Jianwei
- The Journal of Chemical Physics, Vol. 140, Issue 18
The thermodynamic scale of inorganic crystalline metastability
journal, November 2016
- Sun, Wenhao; Dacek, Stephen T.; Ong, Shyue Ping
- Science Advances, Vol. 2, Issue 11
Assessing the quality of the random phase approximation for lattice constants and atomization energies of solids
journal, March 2010
- Harl, Judith; Schimka, Laurids; Kresse, Georg
- Physical Review B, Vol. 81, Issue 11
Density-functional calculations for III-V nitrides using the local-density approximation and the generalized gradient approximation
journal, February 1999
- Stampfl, C.; Van de Walle, C. G.
- Physical Review B, Vol. 59, Issue 8
Python Materials Genomics (pymatgen): A robust, open-source python library for materials analysis
journal, February 2013
- Ong, Shyue Ping; Richards, William Davidson; Jain, Anubhav
- Computational Materials Science, Vol. 68
Performance of the strongly constrained and appropriately normed density functional for solid-state materials
journal, June 2018
- Isaacs, Eric B.; Wolverton, Chris
- Physical Review Materials, Vol. 2, Issue 6
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- Si, Yitao; Li, Mingtao; Zhou, Zhaohui
- The Journal of Chemical Physics, Vol. 152, Issue 2
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journal, January 2020
- Koettgen, Julius; Bartel, Christopher J.; Ceder, Gerbrand
- Chemical Communications, Vol. 56, Issue 13