Formation energy puzzle in intermetallic alloys: Random phase approximation fails to predict accurate formation energies
Abstract
We performed density functional calculations to estimate the formation energies of intermetallic alloys. We used two semilocal approximations, the generalized gradient approximation (GGA) by Perdew-Burke- Ernzerhof (PBE) and the strongly constrained and appropriately normed (SCAN) meta-GGA. In addition, we utilized two nonlocal DFT functionals, the hybrid HSE06, and the state-of-the-art random phase approximation (RPA). The nonlocal functionals such as HSE06 and RPA yield accurate formation energies of binary alloys with completely-filled d-band metals, where semilocal functionals underperform. The accuracy at the nonlocal functionals is greatly reduced when a partially-filled d-band metal is present in an alloy, while PBE-GGA outperforms in these cases. We show that the accurate prediction of formation energies by any DFT method depends on its ability to predict the accurate electronic properties, e.g., valence d-band contribution to the density of states (DOS). The SCAN meta-GGA often corrects the PBE-DOS, however, it does not provide accurate formation energies compared to PBE. This is assumed to be due to the lack of proper error cancellation that should be expected due to the similar bulk nature of both alloys and their constituents, which may improve with the modification of meta-GGA ingredients. RPA yields too negative formation energies of alloys withmore »
- Authors:
-
- Temple Univ., Philadelphia, PA (United States)
- Publication Date:
- Research Org.:
- Temple Univ., Philadelphia, PA (United States); Central Michigan Univ., Mount Pleasant, MI (United States)
- Sponsoring Org.:
- USDOE Office of Science (SC), Basic Energy Sciences (BES); National Science Foundation (NSF)
- OSTI Identifier:
- 1851699
- Grant/Contract Number:
- SC0012575; SC0018331; DMR-1553022; 1625061; W911NF-16-2-0189.
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Physical Review. B
- Additional Journal Information:
- Journal Volume: 102; Journal Issue: 20; 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; 36 MATERIALS SCIENCE
Citation Formats
Nepal, Niraj K., Adhikari, Santosh, Neupane, Bimal, and Ruzsinszky, Adrienn. Formation energy puzzle in intermetallic alloys: Random phase approximation fails to predict accurate formation energies. United States: N. p., 2020.
Web. doi:10.1103/physrevb.102.205121.
Nepal, Niraj K., Adhikari, Santosh, Neupane, Bimal, & Ruzsinszky, Adrienn. Formation energy puzzle in intermetallic alloys: Random phase approximation fails to predict accurate formation energies. United States. https://doi.org/10.1103/physrevb.102.205121
Nepal, Niraj K., Adhikari, Santosh, Neupane, Bimal, and Ruzsinszky, Adrienn. Sun .
"Formation energy puzzle in intermetallic alloys: Random phase approximation fails to predict accurate formation energies". United States. https://doi.org/10.1103/physrevb.102.205121. https://www.osti.gov/servlets/purl/1851699.
@article{osti_1851699,
title = {Formation energy puzzle in intermetallic alloys: Random phase approximation fails to predict accurate formation energies},
author = {Nepal, Niraj K. and Adhikari, Santosh and Neupane, Bimal and Ruzsinszky, Adrienn},
abstractNote = {We performed density functional calculations to estimate the formation energies of intermetallic alloys. We used two semilocal approximations, the generalized gradient approximation (GGA) by Perdew-Burke- Ernzerhof (PBE) and the strongly constrained and appropriately normed (SCAN) meta-GGA. In addition, we utilized two nonlocal DFT functionals, the hybrid HSE06, and the state-of-the-art random phase approximation (RPA). The nonlocal functionals such as HSE06 and RPA yield accurate formation energies of binary alloys with completely-filled d-band metals, where semilocal functionals underperform. The accuracy at the nonlocal functionals is greatly reduced when a partially-filled d-band metal is present in an alloy, while PBE-GGA outperforms in these cases. We show that the accurate prediction of formation energies by any DFT method depends on its ability to predict the accurate electronic properties, e.g., valence d-band contribution to the density of states (DOS). The SCAN meta-GGA often corrects the PBE-DOS, however, it does not provide accurate formation energies compared to PBE. This is assumed to be due to the lack of proper error cancellation that should be expected due to the similar bulk nature of both alloys and their constituents, which may improve with the modification of meta-GGA ingredients. RPA yields too negative formation energies of alloys with partially-filled d-band metals. RPA results can be corrected by restoring the exchange-correlation kernel, thereby improving the short-range electron-electron correlation in metallic densities.},
doi = {10.1103/physrevb.102.205121},
journal = {Physical Review. B},
number = 20,
volume = 102,
place = {United States},
year = {Sun Nov 01 00:00:00 EDT 2020},
month = {Sun Nov 01 00:00:00 EDT 2020}
}
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
Photoemission from Cu, Ag, and Au in the 10- to 27-eV Energy Range
journal, February 1970
- Eastman, D. E.; Cashion, J. K.
- Physical Review Letters, Vol. 24, Issue 7
The XPS valence band spectra of Hf metal and HfC x N y O z compounds and the correlation to their superconductivity
journal, September 1979
- Steiner, P.; H�chst, H.; Schneider, J.
- Zeitschrift f�r Physik B Condensed Matter and Quanta, Vol. 33, Issue 3
Exchange-Correlation Catastrophe in Cu-Au: A Challenge for Semilocal Density Functional Approximations
journal, August 2016
- Tian, Li-Yun; Levämäki, Henrik; Ropo, Matti
- Physical Review Letters, Vol. 117, Issue 6
Projector augmented-wave method
journal, December 1994
- Blöchl, P. E.
- Physical Review B, Vol. 50, Issue 24, p. 17953-17979
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
Accurate surface and adsorption energies from many-body perturbation theory
journal, July 2010
- Schimka, L.; Harl, J.; Stroppa, A.
- Nature Materials, Vol. 9, Issue 9
Accurate Ground-State Energies of Solids and Molecules from Time-Dependent Density-Functional Theory
journal, May 2014
- Olsen, Thomas; Thygesen, Kristian S.
- Physical Review Letters, Vol. 112, Issue 20
Standard Enthalpies of Formation of Ni3V, Ni3Hf, Pd3Hf, and Pt3Sc and Systematics of .DELTA.H.degree.f for Ni3Me (Me .ident. La, Hf, Ta), Pd3Me (Me .ident. La, Hf, Ta) and Pt3Me (Me .ident. Sc, Ti, V or Y, Zr, Nb) Alloys
journal, March 1995
- Guo, Qiti; Kleppa, O. J.
- The Journal of Physical Chemistry, Vol. 99, Issue 9
Effects of atomic order in - and -phase Ag-Cd alloys studied by x-ray photoelectron spectroscopy
journal, December 1978
- Crecelius, G.; Wertheim, G. K.
- Physical Review B, Vol. 18, Issue 12
Ab-initio simulations of materials using VASP: Density-functional theory and beyond
journal, October 2008
- Hafner, Jürgen
- Journal of Computational Chemistry, Vol. 29, Issue 13
Adiabatic-connection fluctuation-dissipation DFT for the structural properties of solids—The renormalized ALDA and electron gas kernels
journal, September 2015
- Patrick, Christopher E.; Thygesen, Kristian S.
- The Journal of Chemical Physics, Vol. 143, Issue 10
Electronic structures of perovskite-type ScRh3Bx (0≤x≤1): X-ray photoelectron and nuclear magnetic resonance spectroscopies and ab initio band calculation
journal, June 2002
- Oku, Masaoki; Shishido, Toetsu; Shinohara, Takeshi
- Journal of Alloys and Compounds, Vol. 339, Issue 1-2
Thermochemistry of binary alloys of transition metals: The Me-Ti, Me-Zr, and Me-Hf(Me = Ag, Au) systems
journal, March 1992
- Fitzner, K.; Kleppa, O. J.
- Metallurgical Transactions A, Vol. 23, Issue 3
Intrinsically selective absorption in alloys of early with late transition metals
journal, November 1986
- Vogelzang, E.; Sikkens, M.; Sawatzky, G. A.
- Solar Energy Materials, Vol. 14, Issue 3-5
From ultrasoft pseudopotentials to the projector augmented-wave method
journal, January 1999
- Kresse, G.; Joubert, D.
- Physical Review B, Vol. 59, Issue 3, p. 1758-1775
Finite Elastic Strain of Cubic Crystals
journal, June 1947
- Birch, Francis
- Physical Review, Vol. 71, Issue 11
Density functional theory for transition metals and transition metal chemistry
journal, January 2009
- Cramer, Christopher J.; Truhlar, Donald G.
- Physical Chemistry Chemical Physics, Vol. 11, Issue 46
Standard enthalpies of formation of scandium alloys, Sc+Me (MeFe, Co, Ni, Ru, Rh, Pd, Ir, Pt), by high-temperature calorimetry
journal, January 1993
- Selhaoui, N.; Kleppa, O. J.
- Journal of Alloys and Compounds, Vol. 191, Issue 1
Random phase approximation applied to solids, molecules, and graphene-metal interfaces: From van der Waals to covalent bonding
journal, February 2013
- Olsen, Thomas; Thygesen, Kristian S.
- Physical Review B, Vol. 87, Issue 7
The Variation of the Adiabatic Elastic Constants of KCl, NaCl, CuZn, Cu, and Al with Pressure to 10,000 Bars
journal, August 1949
- Lazarus, David
- Physical Review, Vol. 76, Issue 4
Thermochemistry of alloys of transition metals: Part IV. Alloys of copper with scandium, yttrium, lanthanum, and lutetium
journal, June 1984
- Watanabe, Shunroku; Kleppa, O. J.
- Metallurgical Transactions B, Vol. 15, Issue 2
Standard enthalpies of formation of Ptti, Ptzr, and Pthf
journal, July 1988
- Topor, Letitia; Kleppa, O. J.
- Metallurgical Transactions A, Vol. 19, Issue 7
An effective interaction potential model for the shape memory alloy AuCd
journal, July 2009
- Guthikonda, Venkata Suresh; Elliott, Ryan S.
- Continuum Mechanics and Thermodynamics, Vol. 21, Issue 4
Electronic densities of states from x-ray photoelectron spectroscopy
journal, July 1970
- Fadley, C. S.; Shirley, D. A.
- Journal of Research of the National Bureau of Standards Section A: Physics and Chemistry, Vol. 74A, Issue 4
Theory of nonuniform electronic systems. I. Analysis of the gradient approximation and a generalization that works
journal, June 1980
- Langreth, David C.; Perdew, John P.
- Physical Review B, Vol. 21, Issue 12
The exchange-correlation energy of a metallic surface
journal, December 1975
- Langreth, D. C.; Perdew, J. P.
- Solid State Communications, Vol. 17, Issue 11
Ultraviolet photoelectron spectra of the outer d bands of Ag-In and Ag-Cd alloys
journal, February 1976
- Riley, J. D.; Leckey, R. C. G.; Jenkin, J. G.
- Journal of Physics F: Metal Physics, Vol. 6, Issue 2
Bulk Properties of Transition Metals: A Challenge for the Design of Universal Density Functionals
journal, August 2014
- Janthon, Patanachai; Luo, Sijie (Andy); Kozlov, Sergey M.
- Journal of Chemical Theory and Computation, Vol. 10, Issue 9
Erratum: “Hybrid functionals based on a screened Coulomb potential” [J. Chem. Phys. 118, 8207 (2003)]
journal, June 2006
- Heyd, Jochen; Scuseria, Gustavo E.; Ernzerhof, Matthias
- The Journal of Chemical Physics, Vol. 124, Issue 21
XPS-valence bands of iron, cobalt, palladium and platinum
journal, June 1976
- Höchst, H.; Hüfner, S.; Goldmann, A.
- Physics Letters A, Vol. 57, Issue 3
Constraint-based wave vector and frequency dependent exchange-correlation kernel of the uniform electron gas
journal, June 2020
- Ruzsinszky, Adrienn; Nepal, Niraj K.; Pitarke, J. M.
- Physical Review B, Vol. 101, Issue 24
X-ray photoelectron spectroscopy of some Cu-Zn alloys
journal, August 1975
- Andrews, P. T.; Hisscott, L. A.
- Journal of Physics F: Metal Physics, Vol. 5, Issue 8
Lattice constants and cohesive energies of alkali, alkaline-earth, and transition metals: Random phase approximation and density functional theory results
journal, June 2013
- Schimka, Laurids; Gaudoin, René; Klimeš, Jiří
- Physical Review B, Vol. 87, Issue 21
Electron correlation energies from scaled exchange-correlation kernels: Importance of spatial versus temporal nonlocality
journal, May 2000
- Lein, Manfred; Gross, E. K. U.; Perdew, John P.
- Physical Review B, Vol. 61, Issue 20
Cohesive energy curves for noble gas solids calculated by adiabatic connection fluctuation-dissipation theory
journal, January 2008
- Harl, Judith; Kresse, Georg
- Physical Review B, Vol. 77, Issue 4
Tests of a ladder of density functionals for bulk solids and surfaces
journal, February 2004
- Staroverov, Viktor N.; Scuseria, Gustavo E.; Tao, Jianmin
- Physical Review B, Vol. 69, Issue 7
Pseudoelasticity in Au-Cd thermoelastic martensite
journal, August 1973
- Nakanishi, N.; Mori, T.; Miura, S.
- Philosophical Magazine, Vol. 28, Issue 2
Predicting the formation enthalpies of binary intermetallic compounds
journal, July 2007
- Zhang, R. F.; Sheng, S. H.; Liu, B. X.
- Chemical Physics Letters, Vol. 442, Issue 4-6
An object-oriented scripting interface to a legacy electronic structure code
journal, January 2002
- Bahn, S. R.; Jacobsen, K. W.
- Computing in Science & Engineering, Vol. 4, Issue 3
van der Waals Bonding in Layered Compounds from Advanced Density-Functional First-Principles Calculations
journal, June 2012
- Björkman, T.; Gulans, A.; Krasheninnikov, A. V.
- Physical Review Letters, Vol. 108, Issue 23
Real-space grid implementation of the projector augmented wave method
journal, January 2005
- Mortensen, J. J.; Hansen, L. B.; Jacobsen, K. W.
- Physical Review B, Vol. 71, Issue 3
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
Thermochemistry of binary alloys of transition metals: The Me-Sc, Me-Y, and Me-La (Me = Ag,Au) systems
journal, May 1991
- Fitzner, K.; Jung, W. -G.; Kleppa, O. J.
- Metallurgical Transactions A, Vol. 22, Issue 5
Ultraviolet photoemission from intermetallic compounds with CsCl structure: ScAg, ScPd, ScIr and ScRu
journal, April 1978
- Battye, F. L.; Schulz, H.; Goldmann, A.
- Journal of Physics F: Metal Physics, Vol. 8, Issue 4
An XPS investigation of the electronic structure in AgZn
journal, September 1989
- Jordan, R. G.; Zehner, D. M.; Harrison, N. M.
- Zeitschrift f�r Physik B Condensed Matter, Vol. 75, Issue 3
Extending the random-phase approximation for electronic correlation energies: The renormalized adiabatic local density approximation
journal, August 2012
- Olsen, Thomas; Thygesen, Kristian S.
- Physical Review B, Vol. 86, Issue 8
Exchange-correlation energy of a metallic surface: Wave-vector analysis
journal, March 1977
- Langreth, David C.; Perdew, John P.
- Physical Review B, Vol. 15, Issue 6
Electronic structures of AuMg and AuZn
journal, February 2001
- Leiro, J. A.; Kokko, K.; Laihia, R.
- Journal of Electron Spectroscopy and Related Phenomena, Vol. 113, Issue 2-3
Time-dependent density-functional theory in the projector augmented-wave method
journal, June 2008
- Walter, Michael; Häkkinen, Hannu; Lehtovaara, Lauri
- The Journal of Chemical Physics, Vol. 128, Issue 24
On the crystal chemistry of normal valence compounds
journal, December 1959
- Mooser, E.; Pearson, W. B.
- Acta Crystallographica, Vol. 12, Issue 12
Random-phase approximation and its applications in computational chemistry and materials science
journal, June 2012
- Ren, Xinguo; Rinke, Patrick; Joas, Christian
- Journal of Materials Science, Vol. 47, Issue 21
Structure and stability of Laves phases. Part I. Critical assessment of factors controlling Laves phase stability
journal, July 2004
- Stein, F.; Palm, M.; Sauthoff, G.
- Intermetallics, Vol. 12, Issue 7-9
Nonlocal First-Principles Calculations in Cu-Au and Other Intermetallic Alloys
journal, February 2014
- Zhang, Yongsheng; Kresse, Georg; Wolverton, C.
- Physical Review Letters, Vol. 112, Issue 7
Inhomogeneous Electron Gas
journal, November 1964
- Hohenberg, P.; Kohn, W.
- Physical Review, Vol. 136, Issue 3B, p. B864-B871
Ab initio calculation of bulk and defect properties of ductile rare-earth intermetallic compounds
journal, September 2004
- Morris, James R.; Ye, Yiying; Lee, Yong-Bin
- Acta Materialia, Vol. 52, Issue 16
The temperature dependence of the elastic constants of gold-cadmium alloys
journal, March 1956
- Zirinsky, Stanley
- Acta Metallurgica, Vol. 4, Issue 2
Electronic structure of yttrium hydride studied by X-ray photoemission spectroscopy
journal, January 1984
- Fujimori, A.; Schlapbach, L.
- Journal of Physics C: Solid State Physics, Vol. 17, Issue 2
The standard enthalpies of formation of the compounds of early transition metals with late transition metals and with noble metals as determined by Kleppa and co-workers at the University of Chicago — A review
journal, June 2001
- Guo, Qiti; Kleppa, Ole Jakob
- Journal of Alloys and Compounds, Vol. 321, Issue 2
Cu-Au, Ag-Au, Cu-Ag, and Ni-Au intermetallics: First-principles study of temperature-composition phase diagrams and structures
journal, March 1998
- Ozoliņš, V.; Wolverton, C.; Zunger, Alex
- Physical Review B, Vol. 57, 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
Electron correlation methods based on the random phase approximation
journal, January 2012
- Eshuis, Henk; Bates, Jefferson E.; Furche, Filipp
- Theoretical Chemistry Accounts, Vol. 131, Issue 1
Calorimetric study of the Hf–Os and Os–Ti systems
journal, August 1998
- Mahdouk, Kamal; Gachon, Jean-Claude
- Journal of Alloys and Compounds, Vol. 278, Issue 1-2
Electronic structure of Ni and Pd alloys. I. X-ray photoelectron spectroscopy of the valence bands
journal, February 1983
- Fuggle, John C.; Hillebrecht, F. Ulrich; Zeller, R.
- Physical Review B, Vol. 27, Issue 4