Mark Huijben

Magnetic effects at the interface between non-magnetic oxides

The electronic reconstruction at the interface between two insulating oxides can give rise to a highly conductive interface. Here we show how, in analogy to this remarkable interface-induced conductivity, magnetism can be induced at the interface between the otherwise non-magnetic insulating perovskites SrTiO3 and LaAlO3. A large negative magnetoresistance of the interface is found, together with a logarithmic temperature dependence of the sheet resistance. At low temperatures, the sheet resistance reveals magnetic hysteresis. Magnetic ordering is a key issue in solid-state science and its underlying mechanisms are still the subject of intense research. In particular, the interplay between localized magnetic moments and the spin of itinerant conduction electrons in a solid gives rise to intriguing many-body effects such as Ruderman-Kittel-Kasuya-Yosida interactions, the Kondo effect and carrier-induced ferromagnetism in diluted magnetic semiconductors. The conducting oxide interface now provides a versatile system to induce and manipulate magnetic moments in otherwise non-magnetic materials.

Multiferroics and magnetoelectrics: thin films and nanostructures

Multiferroic materials, or materials that simultaneously possess two or more ferroic order parameters, have returned to the forefront of materials research. Driven by the desire to achieve new functionalities—such as electrical control of ferromagnetism at room temperature—researchers have undertaken a concerted effort to identify and understand the complexities of multiferroic materials. The ability to create high quality thin film multiferroics stands as one of the single most important landmarks in this flurry of research activity. In this review we discuss the basics of multiferroics including the important order parameters and magnetoelectric coupling in materials. We then discuss in detail the growth of single phase, horizontal multilayer, and vertical heterostructure multiferroics. The review ends with a look to the future and how multiferroics can be used to create new functionalities in materials

Interface ferromagnetism and orbital reconstruction in BiFeO3-La0.7Sr0.3MnO3 heterostructures

We report the formation of a novel ferromagnetic state in the antiferromagnet BiFeO3 at the interface with ferromagnet La(0.7)Sr(0.3)MnO3. Using x-ray magnetic circular dichroism at Mn and Fe L(2,3) edges, we discovered that the development of this ferromagnetic spin structure is strongly associated with the onset of a significant exchange bias. Our results demonstrate that the magnetic state is directly related to an electronic orbital reconstruction at the interface, which is supported by the linearly polarized x-ray absorption measurement at the oxygen K edge.

Deterministic control of ferroelastic switching in multiferroic materials

Multiferroic materials showing coupled electric, magnetic and elastic orderings provide a platform to explore complexity and new paradigms for memory and logic devices. Until now, the deterministic control of non-ferroelectric order parameters in multiferroics has been elusive. Here, we demonstrate deterministic ferroelastic switching in rhombohedral BiFeO(3) by domain nucleation with a scanning probe. We are able to select among final states that have the same electrostatic energy, but differ dramatically in elastic or magnetic order, by applying voltage to the probe while it is in lateral motion. We also demonstrate the controlled creation of a ferrotoroidal order parameter. The ability to control local elastic, magnetic and torroidal order parameters with an electric field will make it possible to probe local strain and magnetic ordering, and engineer various magnetoelectric, domain-wall-based and strain-coupled devices.

Suppression of Octahedral Tilts and Associated Changes in Electronic Properties at Epitaxial Oxide Heterostructure Interfaces

Epitaxial oxide interfaces with broken translational symmetry have emerged as a central paradigm behind the novel behaviors of oxide superlattices. Here, we use scanning transmission electron microscopy to demonstrate a direct, quantitative unit-cell-by-unit-cell mapping of lattice parameters and oxygen octahedral rotations across the BiFeO3-La0.7 Sr0.3 MnO3 interface to elucidate how the change of crystal symmetry is accommodated. Combined with low-loss electron energy loss spectroscopy imaging, we demonstrate a mesoscopic antiferrodistortive phase transition near the interface in BiFeO3 and elucidate associated changes in electronic properties in a thin layer directly adjacent to the interface.

Nanoscale Control of Exchange Bias with BiFeO3 Thin Films

We demonstrate a direct correlation between the domain structure of multiferroic BiFeO3 thin films and exchange bias of Co 0.9Fe 0.1/BiFeO3 heterostructures. Two distinct types of interactions - an enhancement of the coercive field ( exchange enhancement) and an enhancement of the coercive field combined with large shifts of the hysteresis loop ( exchange bias) - have been observed in these heterostructures, which depend directly on the type and crystallography of the nanoscale ( approximately 2 nm) domain walls in the BiFeO3 film. We show that the magnitude of the exchange bias interaction scales with the length of 109 degrees ferroelectric domain walls in the BiFeO 3 thin films which have been probed via piezoresponse force microscopy and X-ray magnetic circular dichroism.

Orbital Reconstruction and the Two-Dimensional Electron Gas at the LaAlO3/SrTiO3 Interface

In 2004, Ohtomo and Hwang discovered that an electron gas is created at the interface between insulating LaAlO3 and SrTiO3 compounds. Here we show that the generation of a conducting electron gas is related to an orbital reconstruction occurring at the LaAlO3/SrTiO3 interface. Our results are based on extensive investigations of the electronic properties and of the orbital structure of the interface using x-ray absorption spectroscopy. In particular, we find that the degeneracy of the Ti 3d states is fully removed and that the Ti 3d xy levels become the first available states for conducting electrons.

Ferroelectric size effects in multiferroic BiFeO3 thin films

Ferroelectric size effects in multiferroic BiFeO3 have been studied using a host of complementary measurements. The structure of such epitaxial films has been investigated using atomic force microscopy, transmission electron microscopy, and x-ray diffraction. The crystal structure of the films has been identified as a monoclinic phase, which suggests that the polarization direction is close to ⟨111⟩. Such behavior has also been confirmed by piezoforce microscopy measurements. That also reveals that the ferroelectricity is down to at least 2 nm

Thermal conductivity reduction in oxygen-deficient strontium titanates

We report significant thermal conductivity reduction in oxygen-deficient lanthanum-doped strontium titanate (Sr1−xLaxTiO3−δ) films as compared to unreduced strontium titanates. Our experimental results suggest that the oxygen vacancies could have played an important role in the reduction. This could be due to the nature of randomly distributed and clustered vacancies, which would be very effective to scatter phonons. Our results could provide a pathway for tailoring the thermal conductivity of complex oxides, which is very beneficial to various applications including thermoelectrics

Controlled lateral anisotropy in correlated manganite heterostructures by interface-engineered oxygen octahedral coupling

Controlled in-plane rotation of the magnetic easy axis in manganite heterostructures by tailoring the interface oxygen network could allow the development of correlated oxide-based magnetic tunnelling junctions with non-collinear magnetization, with possible practical applications as miniaturized high-switching-speed magnetic random access memory (MRAM) devices. Here, we demonstrate how to manipulate magnetic and electronic anisotropic properties in manganite heterostructures by engineering the oxygen network on the unit-cell level. The strong oxygen octahedral coupling is found to transfer the octahedral rotation, present in the NdGaO3 (NGO) substrate, to the La2/3Sr1/3MnO3 (LSMO) film in the interface region. This causes an unexpected realignment of the magnetic easy axis along the short axis of the LSMO unit cell as well as the presence of a giant anisotropic transport in these ultrathin LSMO films. As a result we possess control of the lateral magnetic and electronic anisotropies by atomic-scale design of the oxygen octahedral rotation.