A Dipole Polarizable Potential for Reduced and Doped CeO$_2$ from First-Principles

TL;DR

This paper introduces a new dipole-polarizable interionic potential for CeO$_2$ that accurately reproduces key properties, enabling large-scale simulations where ab initio methods are impractical.

Contribution

The paper develops and parameterizes a novel DIPPIM potential for CeO$_2$, validated against experimental data, improving predictive capabilities for atomic-scale properties.

Findings

Achieves 10-15% accuracy in key properties

Reproduces thermal and chemical expansion coefficients

Matches experimental lattice parameters and elastic constants

Abstract

In this paper we present the parameterization of a new interionic potential for stoichiometric, reduced and doped CeO$_2$. We use a dipole-polarizable potential (DIPPIM) and optimize its parameters by fitting them to a series of DFT calculations. The resulting potential was tested by calculating a series of fundamental properties for CeO$_2$ and by comparing them to experimental values. The agreement for all the calculated properties (thermal and chemical expansion coefficients, lattice parameters, oxygen migration energies, local crystalline structure and elastic constants) is within 10-15% of the experimental one, an accuracy comparable to that of ab initio calculations. This result suggests the use of this new potential for reliably predicting atomic-scale properties of CeO$_2$ in problems where ab initio calculations are not feasible due to their size-limitations.