Direct coupling of first-principles calculations with replica exchange Monte Carlo sampling of ion disorder in solids

Abstract

We demonstrate the feasibility of performing sufficient configurational sampling of disordered oxides directly from first principles without resorting to the use of fitted models such as cluster expansion. This is achieved by harnessing the power of modern-day cluster supercomputers using the replica exchange Monte Carlo method coupled directly with structural relaxation and energy calculation performed by density functional codes. The idea is applied successfully to the calculation of the temperature-dependence of the degree of inversion in the cation sublattice of MgAl${}_2$O${}_4$ spinel oxide. The possibility of bypassing fitting models will lead to investigation of disordered systems where cluster expansion is known to perform badly: for example, systems with large lattice deformation due to defects, or systems where long-range interactions dominate such as electrochemical interfaces.

arXiv comment6 pages, 4 figures

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Cited by in corpus (3)

• Anodic Decomposition of Surface Films on High Voltage Spinel Surfaces -- Density Function Theory and Experimental Study
• Optimization of basis functions for the multi-configuration mixing using the Replica Exchange Monte-Carlo method and its application to ${}^{12}$C
• Facilitating {\it ab initio} configurational sampling of multicomponent solids using an on-lattice neural network model and active learning