We report magnetic, dielectric and magnetodielectric responses of pure monoclinic bulk phase of partially-disordered La2NiMnO6, exhibiting a spectrum of unusual properties and establish that this system intrinsically is a true multiglass with a large
magnetodielectric coupling (8-20%) over a wide range of temperatures (150 - 300 K). Specifically, our results establish a unique way to obtain colossal magnetodielectricity, independent of any striction effects, by engineering the asymmetric hopping contribution to the dielectric constant via the tuning of the relative spin orientations between neighboring magnetic ions in a transition metal oxide system. We discuss the role of anti-site (Ni-Mn) disorder in emergence of these unusual properties.
Combining experiments with first principles calculations, we show that site-specific doping of Mn into SrTiO3 has a decisive influence on the dielectric properties of these doped systems. We find that phonon contributions to the dielectric constant i
nvariably decrease sharply on doping at any site. However, a sizable, random dipolar contribution only for Mn at the Sr site arises from a strong off-centric displacement of Mn in spite of Mn being in a non-d0 state; this leads to a large dielectric constant at higher temperatures and gives rise to a relaxor ferroelectric behavior at lower temperatures. We also investigate magnetic properties in detail and critically reevaluate the possibility of a true multi-glass state in such systems.
