Abstract
A highly efficient computational approach for the screening of Li ion conducting materials is presented and its performance is demonstrated for olivine-type oxides and thiophosphates. The approach is based on a topological analysis of the electrostatic (Coulomb) potential obtained from a single density functional theory calculation augmented by a Born-Mayer-type repulsive term between Li ions and the anions of the material. This 3D-corrugation descriptor enables the automatic determination of diffusion pathways in one, two, and three dimensions and reproduces migration barriers obtained from density functional theory calculations using nudged elastic band method within approximately 0.1 eV. Importantly, it correlates with Li ion conductivity. This approach thus offers an efficient tool for evaluating, ranking, and optimizing materials with high Li-ion conductivity.
Highlights
A highly efficient computational approach for the screening of Li ion conducting materials is presented and its performance is demonstrated for olivine-type oxides and thiophosphates
The three-dimensional migration pathway can be determined by a percolation algorithm. Application of this approach to 14 olivine-type oxides shows a good correlation in the predicted barrier heights compared with density functional theory (DFT) results obtained with nudged elastic band (NEB) calculations, but deviations are relatively large, and the absolute values are systematically overestimated
A typical NEB calculation requires to optimize the supercell geometry of many images, which leads to a large number of DFT calculations on several images
Summary
A highly efficient computational approach for the screening of Li ion conducting materials is presented and its performance is demonstrated for olivine-type oxides and thiophosphates. The approach is based on a topological analysis of the electrostatic (Coulomb) potential obtained from a single density functional theory calculation augmented by a Born-Mayer-type repulsive term between Li ions and the anions of the material This 3D-corrugation descriptor enables the automatic determination of diffusion pathways in one, two, and three dimensions and reproduces migration barriers obtained from density functional theory calculations using nudged elastic band method within approximately 0.1 eV. The present method consists in (i) the construction of an effective potential experienced by diffusing Li ions, called 3D-corrugation descriptor, and (ii) its topological analysis to determine the descriptor barrier energies interpreted as the Li-ion diffusion barriers This approach maps out all diffusion pathways of a given structure without prior information of the topology of the system and it computes the related diffusion barriers using information from a single DFT calculation without the need for multiple NEB calculations. The proposed 3D-corrugation descriptor enables an efficient screening and ranking of Li ion conducting materials in terms of the descriptor barrier energies
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