Magnetostriction as the origin of the magnetodielectric effect in La2CoMnO6

The La₂CoMnO₆ (LCMO) perovskite has received a lot of attention due to its near-room-temperature magnetodielectric effect. Despite the recent efforts, the mechanism ruling the correlation between its magnetic and dielectric properties is not yet fully understood. In order to address this issue, we conducted a detailed investigation of the coupling between the structural, electronic, and magnetic properties of a polycrystalline LCMO sample. Using magnetic field-dependent x-ray powder diffraction and measurements with a capacitive dilatometer, we show that applying an external magnetic field decreases the unit cell volume, thereby modifying the octahedral distortions. Experiments involving temperature and field-dependent x-ray absorption spectroscopy at the Co-L2,3 edges provide further evidence that the spin-orbit interaction of outermost Co $3d$ orbital and the field-induced enhancement of covalence effects are the key contributors to the magnetostrictive effects. From a detailed analysis using multiplet and density functional theory calculations, we propose that the field-induced modulations of the orbital hybridization and the ligand-to-metal charge transfer are responsible for the changes in the dielectric response of LCMO, thus enabling a direct coupling between magnetic, elastic, and dielectric properties in this material.