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Title: 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 » 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.« less

Authors:
ORCiD logo [1]; ORCiD logo [1];  [1];  [1]
  1. 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}
}

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