Debraj Choudhury

Near-Room-Temperature Colossal Magnetodielectricity and Multiglass Properties in Partially Disordered La2NiMnO6

We report magnetic, dielectric, and magnetodielectric responses of the pure monoclinic bulk phase of partially disordered La2NiMnO6, exhibiting a spectrum of unusual properties and establish that this compound is an intrinsically multiglass system 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 antisite (Ni-Mn) disorder in emergence of these unusual properties.

Tuning of dielectric properties and magnetism of SrTiO3 by site-specific doping of Mn

Combining experiments with first-principles calculations, we show that site-specific doping of Mn into SrTiO(3) has a decisive influence on the dielectric properties of these doped systems. We find that phonon contributions to the dielectric constant invariably 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-d(0) 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 multiglass state in such systems.

Engineered Mott ground state in a LaTiO3+δ/LaNiO3 heterostructure

In pursuit of creating cuprate-like electronic and orbital structures, artificial heterostructures based on LaNiO3 have inspired a wealth of exciting experimental and theoretical results. However, to date there is a very limited experimental understanding of the electronic and orbital states emerging from interfacial charge transfer and their connections to the modified band structure at the interface. Towards this goal, we have synthesized a prototypical superlattice composed of a correlated metal LaNiO3 and a doped Mott insulator LaTiO3+δ, and investigated its electronic structure by resonant X-ray absorption spectroscopy combined with X-ray photoemission spectroscopy, electrical transport and theory calculations. The heterostructure exhibits interfacial charge transfer from Ti to Ni sites, giving rise to an insulating ground state with orbital polarization and eg orbital band splitting. Our findings demonstrate how the control over charge at the interface can be effectively used to create exotic electronic, orbital and spin states.

Engineered Mott ground state in LaTiO

In pursuit of creating cuprate-like electronic and orbital structures, artificial heterostructures based on LaNiO3 have inspired a wealth of exciting experimental and theoretical results. However, to date there is a very limited experimental understanding of the electronic and orbital states emerging from interfacial charge transfer and their connections to the modified band structure at the interface. Towards this goal, we have synthesized a prototypical superlattice composed of a correlated metal LaNiO3 and a doped Mott insulator LaTiO3+δ, and investigated its electronic structure by resonant X-ray absorption spectroscopy combined with X-ray photoemission spectroscopy, electrical transport and theory calculations. The heterostructure exhibits interfacial charge transfer from Ti to Ni sites, giving rise to an insulating ground state with orbital polarization and eg orbital band splitting. Our findings demonstrate how the control over charge at the interface can be effectively used to create exotic electronic, orbital and spin states.

_{3+\delta}

We investigated the rare-earth transition-metal oxide series, Ln(2)CuTiO(6) (Ln = Y, Dy, Ho, Er, and Yb), crystallizing in the hexagonal structure with noncentrosymmetric P6(3)cm space group for possible occurrences of multiferroic properties. Our results show that while these compounds, except Ln = Y, exhibit a low-temperature antiferromagnetic transition due to the ordering of the rare-earth moments, the expected ferroelectric transition is frustrated by the large size difference between Cu and Ti at the B site. Interestingly, this leads these compounds to attain a rare and unique combination of desirable paraelectric properties with high dielectric constants, low losses, and weak temperature and frequency dependencies. First-principles calculations establish these exceptional properties result from a combination of two effects. A significant difference in the MO5 polyhedral sizes for M = Cu and M = Ti suppress the expected cooperative tilt pattern of these polyhedra, required for the ferroelectric transition, leading to relatively large values of the dielectric constant for every compound investigated in this series. Additionally, it is shown that the majority contribution to the dielectric constant arises from intermediate-frequency polar vibrational modes, making it relatively stable against any temperature variation. Changes in the temperature stability of the dielectric constant among different members of this series are shown to arise from changes in relative contributions from soft polar modes.

/LaNiO

We discover that hexagonal holmium copper titanate (Ho2CuTiO6), has a unique and highly desirable combination of high dielectric constant, low losses, very small temperature coefficient, and low frequency dependence. Our first-principles calculations indicate that these exceptional properties result from a size-difference at the Cu/Ti B-site that suppresses the expected ferroelectric transition, combined with the dominance of intermediate-frequency polar vibrational modes in the dielectric response. Our results suggest that the use of such B-site disorder in alloys of hexagonal transition-metal oxides should generally result in similar robust dielectrics.

_3

We report on the phase diagram of competing magnetic interactions at the nanoscale in engineered ultrathin trilayer heterostructures of LaTiO_{3}/SrTiO_{3}/YTiO_{3}, in which the interfacial inversion symmetry is explicitly broken. Combined atomic layer resolved scanning transmission electron microscopy with electron energy loss spectroscopy and electrical transport have confirmed the formation of a spatially separated two-dimensional electron liquid and high density two-dimensional localized magnetic moments at the LaTiO_{3}/SrTiO_{3} and SrTiO_{3}/YTiO_{3} interfaces, respectively. Resonant soft x-ray linear dichroism spectroscopy has demonstrated the presence of orbital polarization of the conductive LaTiO_{3}/SrTiO_{3} and localized SrTiO_{3}/YTiO_{3} electrons. Our results provide a route with prospects for exploring new magnetic interfaces, designing a tunable two-dimensional d-electron Kondo lattice, and potential spin Hall applications.

heterostructure

Mn-doped SrTiO3.0, when synthesized free of impurities, is a paramagnetic insulator with interesting dielectric properties. Since delocalized charge carriers are known to promote ferromagnetism in a large number of systems via diverse mechanisms, we have looked for the possibility of any intrinsic, spontaneous magnetization by simultaneous doping of Mn ions and electrons into SrTiO3 via oxygen vacancies, thereby forming SrTi1−xMnxO3−δ, to the extent of making the doped system metallic. We find an absence of any enhancement of the magnetization in the metallic sample when compared with a similarly prepared Mn doped, however, insulating sample. Our results, thus, are not in agreement with a recent observation of a weak ferromagnetism in metallic Mn doped SrTiO3 system.

Electric and magnetic polarizabilities of hexagonal Ln(2)CuTiO(6)(Ln = Y, Dy, Ho, Er, and Yb)

The magnetocaloric effect is a well-known phenomenon where the temperature of a magnetic material varies upon application or removal of a magnetic field. This effect is anticipated to be applied to magnetic refrigeration technology, which is environmentally benign. For practical applications, it is essential to explore and expand the materials horizon of novel magnets that exhibit giant magnetocaloric effects to achieve sufficient cooling efficiency. In this article, several attempts to enhance the magnetocaloric effect are reviewed from the viewpoint of the competition or cooperation between the ferromagnetic interaction and other magnetic, electronic, and structural instabilities in strongly correlated materials. The results indicate that both the competition and cooperation between them promote the first-order nature of the magnetic transition, leading to giant magnetocaloric effects. Therefore, exploiting multiple instabilities is a promising strategy for exploring new magnetocaloric materials.

Unusual dielectric response in B-site size-disordered hexagonal transition metal oxides

Using a combination of X-ray absorption spectroscopy experiments with first principle calculations, we demonstrate that insulating KCuO_2 contains Cu in an unusually-high formal-3+ valence state, the ligand-to-metal (O to Cu) charge transfer energy is intriguingly negative (Delta~ -1.5 eV) and has a dominant (~60%) ligand-hole character in the ground state akin to the high Tc cuprate Zhang-Rice state. Unlike most other formal Cu^{3+} compounds, the Cu 2p XAS spectra of KCuO_2 exhibits pronounced 3d^8 (Cu^{3+}) multiplet structures, which accounts for ~40% of its ground state wave-function. Ab-initio calculations elucidate the origin of the band-gap in KCuO_2 as arising primarily from strong intra-cluster Cu 3d - O 2p hybridizations (t_{pd}); the value of the band-gap decreases with reduced value of t_{pd}. Further, unlike conventional negative charge-transfer insulators, the band-gap in KCuO_2 persists even for vanishing values of Coulomb repulsion U, underscoring the importance of single-particle band-structure effects connected to the one-dimensional nature of the compound.