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Register a new userCharge transfer in iridate-manganite superlattices
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Charge transfer in superlattices consisting of SrIrO$_3$ and SrMnO$_3$ is investigated using density functional theory. Despite the nearly identical work function and non-polar interfaces between SrIrO$_3$ and SrMnO$_3$, rather large charge transfer was experimentally reported at the interface between them. Here, we report a microscopic model that captures the mechanism behind this phenomenon, providing a qualitative understanding of the experimental observation. This leads to unique strain dependence of such charge transfer in iridate-manganite superlattices. The predicted behavior is consistently verified by experiment with soft x-ray and optical spectroscopy. Our work thus demonstrates a new route to control electronic states in non-polar oxide heterostructures.
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Motivated by recent experiments, we use the $+U$ extension of the generalized gradient approximation to density functional theory to study superlattices composed of alternating layers of LaNiO$_3$ and LaMnO$_3$. For comparison we also study a rocksalt ((111) double perovskite) structure and bulk LaNiO$_3$ and LaMnO$_3$. A Wannier function analysis indicates that band parameters are transferable from bulk to superlattice situations with the exception of the transition metal d-level energy, which has a contribution from the change in d-shell occupancy. The charge transfer from Mn to Ni is found to be moderate in the superlattice, indicating metallic behavior, in contrast to the insulating behavior found in recent experiments, while the rocksalt structure is found to be insulating with a large Mn-Ni charge transfer. We suggest a high density of cation antisite defects may account for the insulating behavior experimentally observed in short-period superlattices.
(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.
Charge transfer is of particular importance in manipulating the interface physics in transition-metal oxide heterostructures. In this work, we have fabricated epitaxial bilayers composed of polar 3d LaMnO3 and nonpolar 5d SrIrO3. Systematic magnetic measurements reveal an unexpectedly large exchange bias effect in the bilayer, together with a dramatic enhancement of the coercivity of LaMnO3. Based on first-principles calculations and x-ray absorption spectroscopy measurements, such a strong interfacial magnetic coupling is found closely associated with the polar nature of LaMnO3 and the strong spin-orbit interaction in SrIrO3, which collectively drives an asymmetric interfacial charge transfer and leads to the emergence of an interfacial spin glass state. Our study provides new insight into the charge transfer in transition-metal oxide heterostructures and offers a novel means to tune the interfacial exchange coupling for a variety of device applications.
Interfaces between correlated complex oxides are promising avenues to realize new forms of magnetism that arise as a result of charge transfer, proximity effects and locally broken symmetries. We report upon the discovery of a non-collinear magnetic structure in superlattices of the ferromagnetic metallic oxide La2/3Sr1/3MnO3 (LSMO) and the correlated metal LaNiO3 (LNO). The exchange interaction between LSMO layers is mediated by the intervening LNO, such that the angle between the magnetization of neighboring LSMO layers varies in an oscillatory manner with the thickness of the LNO layer. The magnetic field, temperature, and spacer thickness dependence of the non-collinear structure are inconsistent with the bilinear and biquadratic interactions that are used to model the magnetic structure in conventional metallic multilayers. A model that couples the LSMO layers to a helical spin state within the LNO fits the observed behavior. We propose that the spin-helix results from the interaction between a spatially varying spin susceptibility within the LNO and interfacial charge transfer that creates localized Ni2+ states. This provides a new approach to engineering non-collinear spin textures in metallic oxide heterostructures that can be exploited in devices based on both spin and charge transport.
We report a modulation of the in-plane magnetotransport in artificial manganite superlattice (SL) [(NdMnO3)n /(SrMnO3)n /(LaMnO3)n]m by varying the layer thickness n while keeping the total thickness of the structure constant. Charge transport in these heterostructures is confined to the interfaces and occurs via variable range hopping (VRH). Upon increasing n, the interfacial separation rises, leading to a suppression of the electrostatic screening between carriers of neighboring interfaces and the opening of a Coulomb gap at the Fermi level (EF). The high-field magnetoresistance (MR) is universally negative due to progressive spin alignment. However at a critical thickness of n=5 unit cells (u.c.), an exchange field coupling between ferromagnetically ordered interfaces results in positive MR at low magnetic field (H). Our results demonstrate the ability to geometrically tune the electrical transport between regimes dominated by either charge or spin correlations.
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