Benchmarking density functional perturbation theory to enable high-throughput screening of materials for dielectric constant and refractive index

Abstract

We demonstrate a high-throughput density functional perturbation theory (DFPT) methodology capable of screening compounds for their dielectric properties. The electronic and ionic dielectric tensors are calculated for 88 compounds, where the eigenvalues of the total dielectric tensors are compared with single crystal and polycrystalline experimental values reported in the literature. We find that GGA/PBE has a smaller mean average deviation from experiments ($\text{MARD}=16.2$%) when compared to LDA. The prediction accuracy of DFPT is lowest for compounds that exhibit complex structural relaxation effects (e.g., octahedra rotation in perovskites) and/or strong anharmonicity. Despite some discrepancies between DFPT results and reported experimental values, the high-throughput methodology is found to be useful in identifying interesting compounds by ranking. This is demonstrated by the high Spearman correlation factor $(\ensuremath{\rho}=0.92)$. Finally, we demonstrate that DFPT provides a good estimate for the refractive index of a compound without calculating the frequency dependence of the dielectric matrix ($\text{MARD}=5.7$%).