Marta Gibert

Exchange bias in LaNiO3-LaMnO3 superlattices.

The wide spectrum of exotic properties exhibited by transition-metal oxides stems from the complex competition between several quantum interactions. The capacity to select the emergence of specific phases at will is nowadays extensively recognized as key for the design of diverse new devices with tailored functionalities. In this context, interface engineering in complex oxide heterostructures has developed into a flourishing field, enabling not only further tuning of the exceptional properties of these materials, but also giving access to hidden phases and emergent physical phenomena. Here we demonstrate how interfacial interactions can induce a complex magnetic structure in a non-magnetic material. We specifically show that exchange bias can unexpectedly emerge in heterostructures consisting of paramagnetic LaNiO3 (LNO) and ferromagnetic LaMnO3 (LMO). The observation of exchange bias in (111)-oriented LNO-LMO superlattices, manifested as a shift of the magnetization-field loop, not only implies the development of interface-induced magnetism in the paramagnetic LNO layers, but also provides us with a very subtle tool for probing the interfacial coupling between the LNO and LMO layers. First-principles calculations indicate that this interfacial interaction may give rise to an unusual spin order, resembling a spin-density wave, within the LNO layers.

Metal-insulator transition in ultrathin LaNiO3 films.

Transport in ultrathin films of LaNiO(3) evolves from a metallic to a strongly localized character as the films thickness is reduced and the sheet resistance reaches a value close to h/e(2), the quantum of resistance in two dimensions. In the intermediate regime, quantum corrections to the Drude low-temperature conductivity are observed; they are accurately described by weak localization theory. Remarkably, the negative magnetoresistance in this regime is isotropic, which points to magnetic scattering associated with the proximity of the system to either a spin-glass state or the charge ordered antiferromagnetic state observed in other rare earth nickelates.

Interfacial Control of Magnetic Properties at LaMnO3/LaNiO3 Interfaces.

The functional properties of oxide heterostructures ultimately rely on how the electronic and structural mismatches occurring at interfaces are accommodated by the chosen materials combination. We discuss here LaMnO3/LaNiO3 heterostructures, which display an intrinsic interface structural asymmetry depending on the growth sequence. Using a variety of synchrotron-based techniques, we show that the degree of intermixing at the monolayer scale allows interface-driven properties such as charge transfer and the induced magnetic moment in the nickelate layer to be controlled. Further, our results demonstrate that the magnetic state of strained LaMnO3 thin films dramatically depends on interface reconstructions.

Ground-state oxygen holes and the metal–insulator transition in the negative charge-transfer rare-earth nickelates

The metal–insulator transition and the intriguing physical properties of rare-earth perovskite nickelates have attracted considerable attention in recent years. Nonetheless, a complete understanding of these materials remains elusive. Here we combine X-ray absorption and resonant inelastic X-ray scattering (RIXS) spectroscopies to resolve important aspects of the complex electronic structure of rare-earth nickelates, taking NdNiO3 thin film as representative example. The unusual coexistence of bound and continuum excitations observed in the RIXS spectra provides strong evidence for abundant oxygen holes in the ground state of these materials. Using cluster calculations and Anderson impurity model interpretation, we show that distinct spectral signatures arise from a Ni 3d8 configuration along with holes in the oxygen 2p valence band, confirming suggestions that these materials do not obey a conventional positive charge-transfer picture, but instead exhibit a negative charge-transfer energy in line with recent models interpreting the metal–insulator transition in terms of bond disproportionation.

Electronic transitions in strained SmNiO3 thin films

Nickelates are known for their metal to insulator transition (MIT) and an unusual magnetic ordering, occurring at T = TNeel. Here, we investigate thin films of SmNiO3 subjected to different levels of epitaxial strain. We find that the original bulk behavior (TNeel < TMI) is strongly affected by applying compressive strain to the films. For small compressive strains, a regime where TNeel = TMI is achieved, the paramagnetic insulating phase characteristic of the bulk compound is suppressed and the MIT becomes 1st order. Further increasing the in-plane compression of the SmNiO3 lattice leads to the stabilization of a single metallic paramagnetic phase.

Tailoring the electronic transitions of NdNiO3 films through (111)pc oriented interfaces

Bulk NdNiO3 and thin films grown along the pseudocubic (001)pc axis display a 1st order metal to insulator transition (MIT) together with a Neel transition at T = 200 K. Here, we show that for NdNiO3 films deposited on (111)pc NdGaO3, the MIT occurs at T = 335 K and the Neel transition at T = 230 K. By comparing transport and magnetic properties of layers grown on substrates with different symmetries and lattice parameters, we demonstrate a particularly large tuning when the epitaxy is realized on (111)pc surfaces. We attribute this effect to the specific lattice matching conditions imposed along this direction when using orthorhombic substrates.

Optically switched magnetism in photovoltaic perovskite CH3NH3(Mn:Pb)I3.

The demand for ever-increasing density of information storage and speed of manipulation boosts an intense search for new magnetic materials and novel ways of controlling the magnetic bit. Here, we report the synthesis of a ferromagnetic photovoltaic CH3NH3(Mn:Pb)I3 material in which the photo-excited electrons rapidly melt the local magnetic order through the Ruderman–Kittel–Kasuya–Yosida interactions without heating up the spin system. Our finding offers an alternative, very simple and efficient way of optical spin control, and opens an avenue for applications in low-power, light controlling magnetic devices.

Interlayer coupling through a dimensionality-induced magnetic state

Dimensionality is known to play an important role in many compounds for which ultrathin layers can behave very differently from the bulk. This is especially true for the paramagnetic metal LaNiO3, which can become insulating and magnetic when only a few monolayers thick. We show here that an induced antiferromagnetic order can be stabilized in the [111] direction by interfacial coupling to the insulating ferromagnet LaMnO3, and used to generate interlayer magnetic coupling of a nature that depends on the exact number of LaNiO3 monolayers. For 7-monolayer-thick LaNiO3/LaMnO3 superlattices, negative and positive exchange bias, as well as antiferromagnetic interlayer coupling are observed in different temperature windows. All three behaviours are explained based on the emergence of a (¼,¼,¼)-wavevector antiferromagnetic structure in LaNiO3 and the presence of interface asymmetry with LaMnO3. This dimensionality-induced magnetic order can be used to tailor a broad range of magnetic properties in well-designed superlattice-based devices.

Striped nanoscale phase separation at the metal-insulator transition of heteroepitaxial nickelates

Nucleation processes of mixed-phase states are an intrinsic characteristic of first-order phase transitions, typically related to local symmetry breaking. Direct observation of emerging mixed-phase regions in materials showing a first-order metal–insulator transition (MIT) offers unique opportunities to uncover their driving mechanism. Using photoemission electron microscopy, we image the nanoscale formation and growth of insulating domains across the temperature-driven MIT in NdNiO3 epitaxial thin films. Heteroepitaxy is found to strongly determine the nanoscale nature of the phase transition, inducing preferential formation of striped domains along the terraces of atomically flat stepped surfaces. We show that the distribution of transition temperatures is a local property, set by surface morphology and stable across multiple temperature cycles. Our data provide new insights into the MIT of heteroepitaxial nickelates and point to a rich, nanoscale phenomenology in this strongly correlated material.

Optical spectroscopy and the nature of the insulating state of rare-earth nickelates

Using a combination of spectroscopic ellipsometry and DC transport measurements, we determine the temperature dependence of the optical conductivity of NdNiO