Coordination Corrected ab Initio Formation Enthalpies
Abstract
The correct calculation of formation enthalpy is one of the enablers of ab-initio computational materials design. For several classes of systems (e.g. oxides) standard density functional theory produces incorrect values. Here we propose the coordination corrected enthalpies method (CCE), based on the number of nearest neighbor cationanion bonds, and also capable of correcting relative stability of polymorphs. CCE uses calculations employing the Perdew, Burke and Ernzerhof (PBE), local density approximation (LDA) and strongly constrained and appropriately normed (SCAN) exchange correlation functionals, in conjunction with a quasiharmonic Debye model to treat zero-point vibrational and thermal effects. The benchmark, performed on binary and ternary oxides (halides), shows very accurate room temperature results for all functionals, with the smallest mean absolute error of 27(24) meV/atom obtained with SCAN. The zero-point vibrational and thermal contributions to the formation enthalpies are small and with different signslargely canceling each other.
Document Details
- Document Type
- Technical Report
- Publication Date
- May 15, 2019
- Accession Number
- AD1105406
Entities
People
- Andrew Supka
- Corey Oses
- Cormac Toher
- Demet Usanmaz
- Marco B. Nardelli
- Marco Fornari
- Rico Friedrich
- Stefano Curtarolo
Organizations
- Duke University