W. M. Lü

Origin of the Two-Dimensional Electron Gas at LaAlO3=SrTiO3 Interfaces: The Role of Oxygen Vacancies and Electronic Reconstruction

The relative importance of atomic defects and electron transfer in explaining conductivity at the crystalline LaAlO3/SrTiO3 interface has been a topic of debate. Metallic interfaces with similar electronic properties produced by amorphous oxide overlayers on SrTiO3 have called in question the original polarization catastrophe model. We resolve the issue by a comprehensive comparison of (100)-oriented SrTiO3 substrates with crystalline and amorphous overlayers of LaAlO3 of different thicknesses prepared under different oxygen pressures. For both types of overlayers, there is a critical thickness for the appearance of conductivity, but its value is always 4 unit cells (around 1.6 nm) for the oxygen-annealed crystalline case, whereas in the amorphous case, the critical thickness could be varied in the range 0.5 to 6 nm according to the deposition conditions. Subsequent ion milling of the overlayer restores the insulating state for the oxygen-annealed crystalline heterostructures but not for the amorphous ones. Oxygen post-annealing removes the oxygen vacancies, and the interfaces become insulating in the amorphous case. However, the interfaces with a crystalline overlayer remain conducting with reduced carrier density. These results demonstrate that oxygen vacancies are the dominant source of mobile carriers when the LaAlO3 overlayer is amorphous, while both oxygen vacancies and polarization catastrophe contribute to the interface conductivity in unannealed crystalline LaAlO3/SrTiO3 heterostructures, and the polarization catastrophe alone accounts for the conductivity in oxygen-annealed crystalline LaAlO3/SrTiO3 heterostructures. Furthermore, we find that the crystallinity of the LaAlO3 layer is crucial for the polarization catastrophe mechanism in the case of crystalline LaAlO3 overlayers.

Oxygen electrocatalysis on (001)-oriented manganese perovskite films: Mn valency and charge transfer at the nanoscale

We report that the oxygen reduction reaction (ORR) activities of (001)-oriented manganese perovskite films decrease from 10 to 1 nm by more than an order of magnitude, which can be attributed to the barrier associated with interfacial band bending that impedes electron transfer to the electrolyte, and reduction of Mn3+ due to charge transfer from the Nb:SrTiO3 substrate. Furthermore, we show by substitution in La1−x(Ca,Sr)xMnO3 that Mn3+, not Mn4+, is the active valence state for ORR.

Metal-insulator transition in SrTiO(3-x) thin films induced by frozen-out carriers.

Z. Q. Liu, D. P. Leusink, X. Wang, W. M. Lü, K. Gopinadhan, A. Annadi, Y. L. Zhao, X. H. Huang, S. W. Zeng, Z. Huang, A. Srivastava, S. Dhar, T. Venkatesan, and Ariando1,2∗ NUSNNI-Nanocore, Department of Physics, Department of Electrical and Computer Engineering, National University of Singapore, Singapore and Faculty of Science and Technology and MESA Institute for Nanotechnology, University of Twente, 7500 AE Enschede, The Netherlands (Dated: January 13, 2013)

Anisotropic two dimensional electron gas at the LaAlO3/SrTiO3(110) interface

The observation of a high-mobility two-dimensional electron gas between two insulating complex oxides, especially LaAlO3/SrTiO3, has enhanced the potential of oxides for electronics. The occurrence of this conductivity is believed to be driven by polarization discontinuity, leading to an electronic reconstruction. In this scenario, the crystal orientation has an important role and no conductivity would be expected, for example, for the interface between LaAlO3 and (110)-oriented SrTiO3, which should not have a polarization discontinuity. Here we report the observation of unexpected conductivity at the LaAlO3/SrTiO3 interface prepared on (110)-oriented SrTiO3, with a LaAlO3-layer thickness-dependent metal-insulator transition. Density functional theory calculation reveals that electronic reconstruction, and thus conductivity, is still possible at this (110) interface by considering the energetically favourable (110) interface structure, that is, buckled TiO2/LaO, in which the polarization discontinuity is still present. The conductivity was further found to be strongly anisotropic along the different crystallographic directions with potential for anisotropic superconductivity and magnetism, leading to possible new physics and applications.

Unexpected Anisotropic Two Dimensional Electron Gas at the LaAlO3/SrTiO3 (110) Interface

The observation of a high-mobility two-dimensional electron gas between two insulating complex oxides, especially LaAlO3/SrTiO3, has enhanced the potential of oxides for electronics. The occurrence of this conductivity is believed to be driven by polarization discontinuity, leading to an electronic reconstruction. In this scenario, the crystal orientation has an important role and no conductivity would be expected, for example, for the interface between LaAlO3 and (110)-oriented SrTiO3, which should not have a polarization discontinuity. Here we report the observation of unexpected conductivity at the LaAlO3/SrTiO3 interface prepared on (110)-oriented SrTiO3, with a LaAlO3-layer thickness-dependent metal-insulator transition. Density functional theory calculation reveals that electronic reconstruction, and thus conductivity, is still possible at this (110) interface by considering the energetically favourable (110) interface structure, that is, buckled TiO2/LaO, in which the polarization discontinuity is still present. The conductivity was further found to be strongly anisotropic along the different crystallographic directions with potential for anisotropic superconductivity and magnetism, leading to possible new physics and applications.

Imaging and control of ferromagnetism in LaMnO3/SrTiO3 heterostructures

Control of magnetism in heterostructures The interface between two different materials in a heterostructure can exhibit properties unique to either of the two materials alone. A well-known example is a conducting gas that forms when LaAlO3 is grown on SrTiO3, but only if the LaAlO3 layer is at least four unit cells thick. Wang et al. report a similarly abrupt magnetic transition in a heterostructure formed by another oxide (LaMnO3) on the same SrTiO3 substrate. Even though bulk LaMnO3 is an antiferromagnet, when six or more unit-cell layers of it were deposited on SrTiO3, it behaved like a ferromagnet. Science, this issue p. 716 Superconducting quantum interference device magnetometry is used to observe a magnetic transition in an oxide heterostructure. Oxide heterostructures often exhibit unusual physical properties that are absent in the constituent bulk materials. Here, we report an atomically sharp transition to a ferromagnetic phase when polar antiferromagnetic LaMnO3 (001) films are grown on SrTiO3 substrates. For a thickness of six unit cells or more, the LaMnO3 film abruptly becomes ferromagnetic over its entire area, which is visualized by scanning superconducting quantum interference device microscopy. The transition is explained in terms of electronic reconstruction originating from the polar nature of the LaMnO3 (001) films. Our results demonstrate that functionalities can be engineered in oxide films that are only a few atomic layers thick.

Magnetoresistance of two-dimensional and three-dimensional electron gas in LaAlO3/SrTiO3heterostructures: Influence of magnetic ordering, interface scattering, and dimensionality

Magnetoresistance (MR) anisotropy in LaAlO3/SrTiO3 (LAO/STO) interfaces is compared between samples prepared in high oxygen partial pressure (PO2) of 10-4 mbar exhibiting quasi-two-dimensional (quasi-2D) electron gas and low PO2 of 10-6 mbar exhibiting 3D conductivity. While MR of an order of magnitude larger was observed in low PO2 samples compared to those of high PO2 samples, large MR anisotropies were observed in both cases. The MR with the out-of-plane field is always larger compared to the MR with in-plane field suggesting lower dissipation of electrons from interface versus defect scattering. The quasi-2D interfaces show a negative MR at low temperatures while the 3D interfaces show positive MR for all temperatures. Furthermore, the angle relationship of MR anisotropy for these two different cases and temperature dependence of in-plane MR are also presented. Our study demonstrates that MR can be used to distinguish the dimensionality of the charge transport and various (defect, magnetic center, and interface boundary) scattering processes in this system.

Reversible room-temperature ferromagnetism in Nb-doped SrTiO3single crystals

The search for oxide-based room-temperature ferromagnetism has been one of the holy grails in condensed matter physics. Room-temperature ferromagnetism observed in Nb-doped SrTiO3 single crystals is reported in this Rapid Communication. The ferromagnetism can be eliminated by air annealing (making the samples predominantly diamagnetic) and can be recovered by subsequent vacuum annealing. The temperature dependence of magnetic moment resembles the temperature dependence of carrier density, indicating that the magnetism is closely related to the free carriers. Our results suggest that the ferromagnetism is induced by oxygen vacancies. In addition, hysteretic magnetoresistance was observed for magnetic field parallel to current, indicating that the magnetic moments are in the plane of the samples. The x-ray photoemission spectroscopy, the static time-of-flight and the dynamic secondary ion mass spectroscopy and proton induced x-ray emission measurements were performed to examine magnetic impurities, showing that the observed ferromagnetism is unlikely due to any magnetic contaminant.

Bandgap Control of the Oxygen-Vacancy-Induced Two-Dimensional Electron Gas in SrTiO3

We report very large bandgap enhancement in SrTiO3 (STO) films (fabricated by pulsed laser deposition below 800 {\deg}C), which can be up to 20% greater than the bulk value, depending on the deposition temperature. The origin is comprehensively investigated and finally attributed to Sr/Ti antisite point defects, supported by density functional theory calculations. More importantly, the bandgap enhancement can be utilized to tailor the electronic and magnetic phases of the two-dimensional electron gas (2DEG) in STO-based interface systems. For example, the oxygen-vacancy-induced 2DEG (2DEG-V) at the interface between amorphous LaAlO3 and STO films is more localized and the ferromagnetic order in the STO-film-based 2DEG-V can be clearly seen from low-temperature magnetotransport measurements. This opens an attractive path to tailor electronic, magnetic and optical properties of STO-based oxide interface systems under intensive focus in the oxide electronics community. Meanwhile, our study provides key insight into the origin of the fundamental issue that STO films are difficult to be doped into the fully metallic state by oxygen vacancies.

Magnetic-field induced resistivity minimum with in-plane linear magnetoresistance of the Fermi liquid in SrTiO3−xsingle crystals

We report novel magnetotransport properties of the low temperature Fermi liquid in SrTiO3-x single crystals. The classical limit dominates the magnetotransport properties for a magnetic field perpendicular to the sample surface and consequently a magnetic-field induced resistivity minimum emerges. While for the field applied in plane and normal to the current, the linear magnetoresistance (MR) starting from small fields (< 0.5 T) appears. The large anisotropy in the transverse MRs reveals the strong surface interlayer scattering due to the large gradient of oxygen vacancy concentration from the surface to the interior of SrTiO3-x single crystals. Moreover, the linear MR in our case was likely due to the inhomogeneity of oxygen vacancies and oxygen vacancy clusters, which could provide experimental evidences for the unusual quantum linear MR proposed by Abrikosov [A. A. Abrikosov, Phys. Rev. B 58, 2788 (1998)].