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Exploring DFT$+U$ parameter space with a Bayesian calibration assisted by Markov chain Monte Carlo sampling

Materials Science 2021-09-17 v1 Strongly Correlated Electrons

Abstract

Density-functional theory is widely used to predict the physical properties of materials. However, it usually fails for strongly correlated materials. A popular solution is to use the Hubbard corrections to treat strongly correlated electronic states. Unfortunately, the exact values of the Hubbard UU and JJ parameters are initially unknown, and they can vary from one material to another. In this semi-empirical study, we explore the UU and JJ parameter space of a group of iron-based compounds to simultaneously improve the prediction of physical properties (volume, magnetic moment, and bandgap). We used a Bayesian calibration assisted by Markov chain Monte Carlo sampling for three different exchange-correlation functionals (LDA, PBE, and PBEsol). We found that LDA requires the largest UU correction. PBE has the smallest standard deviation and its UU and JJ parameters are the most transferable to other iron-based compounds. Lastly, PBE predicts lattice parameters reasonably well without the Hubbard correction.

Keywords

Cite

@article{arxiv.2109.07617,
  title  = {Exploring DFT$+U$ parameter space with a Bayesian calibration assisted by Markov chain Monte Carlo sampling},
  author = {Pedram Tavadze and Reese Boucher and Guillermo Avendaño-Franco and Keenan X. Kocan and Sobhit Singh and Viviana Dovale-Farelo and Wilfredo Ibarra-Hernández and Matthew B Johnson and David S. Mebane and Aldo H Romero},
  journal= {arXiv preprint arXiv:2109.07617},
  year   = {2021}
}
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