Anand Bhattacharya

Quantifying octahedral rotations in strained perovskite oxide films

We have measured the oxygen positions in

Metal-Insulator Transition and Its Relation to Magnetic Structure in (LaMnO3)2n/(SrMnO3)n Superlattices

{\text{LaNiO}}_{3}

Enhanced ordering temperatures in antiferromagnetic manganite superlattices

films to elucidate the coupling between epitaxial strain and oxygen octahedral rotations. The oxygen positions are determined by comparing the measured and calculated intensities of half-order Bragg peaks, arising from the octahedral rotations. Combining ab initio density-functional calculations with these experimental results, we show how strain systematically modifies both bond angles and lengths in this functional perovskite oxide.

Non-volatile ferroelastic switching of the Verwey transition and resistivity of epitaxial Fe3O4/PMN-PT (011).

Superlattices of (LaMnO3){2n}/(SrMnO3){n} (1<or=n<or=5), composed of the gapped insulators LaMnO3 and SrMnO3, undergo a metal-insulator transition as a function of n, being metallic for n<or=2 and insulating for n>or=3. Measurements of transport, magnetization, and polarized neutron reflectivity reveal that the ferromagnetism is relatively uniform in the metallic state, and is strongly modulated in the insulating state, being high in LaMnO3 and suppressed in SrMnO3. The modulation is consistent with a Mott transition driven by the proximity between the (LaMnO3)/(SrMnO3) interfaces. The insulating state for n>or=3 obeys variable range hopping at low temperatures. We suggest that this is due to states at the Fermi level that emerge at the (LaMnO3)/(SrMnO3) interfaces and are localized by disorder.

Dynamic layer rearrangement during growth of layered oxide films by molecular beam epitaxy

The disorder inherent to doping by cation substitution in the complex oxides can have profound effects on collective-ordered states. Here, we demonstrate that cation-site ordering achieved through digital-synthesis techniques can dramatically enhance the antiferromagnetic ordering temperatures of manganite films. Cation-ordered (LaMnO3)m/(SrMnO3)2m superlattices show Néel temperatures (TN) that are the highest of any La(1-x)Sr(x)MnO3 compound, approximately 70 K greater than compositionally equivalent randomly doped La(1/3)Sr(2/3)MnO3. The antiferromagnetic order is A-type, consisting of in-plane double-exchange-mediated ferromagnetic sheets coupled antiferromagnetically along the out-of-plane direction. Through synchrotron X-ray scattering, we have discovered an in-plane structural modulation that reduces the charge itinerancy and hence the ordering temperature within the ferromagnetic sheets, thereby limiting TN. This modulation is mitigated and driven to long wavelengths by cation ordering, enabling the higher TN values of the superlattices. These results provide insight into how cation-site ordering can enhance cooperative behaviour in oxides through subtle structural phenomena.

Probing Interfacial Electronic Structures in Atomic Layer LaMnO3 and SrTiO3 Superlattices

A central goal of electronics based on correlated materials or ‘Mottronics’ is the ability to switch between distinct collective states with a control voltage. Small changes in structure and charge density near a transition can tip the balance between competing phases, leading to dramatic changes in electronic and magnetic properties. In this work, we demonstrate that an electric field induced two-step ferroelastic switching pathway in (011) oriented 0.71Pb(Mg1/3Nb2/3)O3-0.29PbTiO3 (PMN-PT) substrates can be used to tune the Verwey metal-insulator transition in epitaxial Fe3O4 films in a stable and reversible manner. We also observe robust non-volatile resistance switching in Fe3O4 up to room temperature, driven by ferroelastic strain. These results provides a framework for realizing non-volatile and reversible tuning of order parameters coupled to lattice-strain in epitaxial oxide heterostructures over a broad range of temperatures, with potential device applications.

Charge transfer and interfacial magnetism in (LaNiO3)n/(LaMnO3)2superlattices

The A(n+1)B(n)O(3n+1) Ruddlesden-Popper homologous series offers a wide variety of functionalities including dielectric, ferroelectric, magnetic and catalytic properties. Unfortunately, the synthesis of such layered oxides has been a major challenge owing to the occurrence of growth defects that result in poor materials behaviour in the higher-order members. To understand the fundamental physics of layered oxide growth, we have developed an oxide molecular beam epitaxy system with in situ synchrotron X-ray scattering capability. We present results demonstrating that layered oxide films can dynamically rearrange during growth, leading to structures that are highly unexpected on the basis of the intended layer sequencing. Theoretical calculations indicate that rearrangement can occur in many layered oxide systems and suggest a general approach that may be essential for the construction of metastable Ruddlesden-Popper phases. We demonstrate the utility of the new-found growth strategy by performing the first atomically controlled synthesis of single-crystalline La3Ni2O7.

Control of octahedral rotations in (LaNiO{sub 3}){sub n}/(SrMnO{sub 3}){sub m} superlattices

The interfacial electronic structure characterization of a m x (LaMnO{sub 3})/n x (SrTiO{sub 3}) superlattice based on scanning transmission electron microscopy and electron energy loss spectroscopy. Evidence of interfacial band alignment and electron transfer are presented based on the observation of O K edge of individual transition metal and oxygen atomic columns. Electron probe aberration correction was essential for the high spatial resolution mapping of interfacial electronic states.

Electronic Reconstruction at SrMnO3-LaMnO3 Superlattice Interfaces

(LaNiO3)n/(LaMnO3)2 superlattices were grown using ozone-assisted molecular beam epitaxy, where LaNiO3 is a paramagnetic metal and LaMnO3 is an antiferromagnetic insulator. The superlattices exhibit excellent crystallinity and interfacial roughness of less than 1 unit cell. X-ray spectroscopy and dichroism measurements indicate that electrons are transferred from the LaMnO3 to the LaNiO3, inducing magnetism in LaNiO3. Magnetotransport measurements reveal a transition from metallic to insulating behavior as the LaNiO3 layer thickness is reduced from 5 unit cells to 2 unit cells and suggest a modulated magnetic structure within LaNiO3.

Correlating interfacial octahedral rotations with magnetism in (LaMnO3+δ)N/(SrTiO3)N superlattices

Oxygen octahedral rotations have been measured in short-period (LaNiO{sub 3}){sub n}/(SrMnO{sub 3}){sub m} superlattices using synchrotron diffraction. The in-plane and out-of-plane bond angles and lengths are found to systematically vary with superlattice composition. Rotations are suppressed in structures with m > n, producing a nearly unrotated form of LaNiO{sub 3}. Large rotations are present in structures with m < n, leading to reduced bond angles in SrMnO{sub 3}. The metal-oxygen-metal bond lengths decrease as rotations are reduced, in contrast to behavior previously observed in strained, single-layer films. This result demonstrates that superlattice structures can be used to stabilize nonequilibrium octahedral behavior in a manner distinct from epitaxial strain, providing a novel means to engineer the electronic and ferroic properties of oxide heterostructures.