Yasuyuki Hikita

Direct imaging of the coexistence of ferromagnetism and superconductivity at the LaAlO3/SrTiO3 interface

LaAlO{sub 3} and SrTiO{sub 3} are insulating, nonmagnetic oxides, yet the interface between them exhibits a two-dimensional electron system with high electron mobility, superconductivity at low temperatures, and electric-field-tuned metal-insulator and superconductor-insulator phase transitions. Bulk magnetization and magnetoresistance measurements also suggest some form of magnetism depending on preparation conditions and suggest a tendency towards nanoscale electronic phase separation. Here we use local imaging of the magnetization and magnetic susceptibility to directly observe a landscape of ferromagnetism, paramagnetism, and superconductivity. We find submicron patches of ferromagnetism in a uniform background of paramagnetism, with a nonuniform, weak diamagnetic superconducting susceptibility at low temperature. These results demonstrate the existence of nanoscale phase separation as suggested by theoretical predictions based on nearly degenerate interface subbands associated with the Ti orbitals. The magnitude and temperature dependence of the paramagnetic response suggests that the vast majority of the electrons at the interface are localized, and do not contribute to transport measurements. In addition to the implications for magnetism, the existence of a 2D superconductor at an interface with highly broken inversion symmetry and a ferromagnetic landscape in the background suggests the potential for exotic superconducting phenomena.

Polarization-sensitive broadband photodetector using a black phosphorus vertical p–n junction

The ability to detect light over a broad spectral range is central for practical optoelectronic applications, and has been successfully demonstrated with photodetectors of two-dimensional layered crystals such as graphene and MoS2. However, polarization sensitivity within such a photodetector remains elusive. Here we demonstrate a linear-dichroic broadband photodetector with layered black phosphorus transistors, using the strong intrinsic linear dichroism arising from the in-plane optical anisotropy with respect to the atom-buckled direction, which is polarization sensitive over a broad bandwidth from 400 nm to 3750 nm. Especially, a perpendicular build-in electric field induced by gating in black phosphorus transistors can spatially separate the photo-generated electrons and holes in the channel, effectively reducing their recombination rate, and thus enhancing the efficiency and performance for linear dichroism photodetection. This provides new functionality using anisotropic layered black phosphorus, thereby enabling novel optical and optoelectronic device applications.The ability to detect light over a broad spectral range is central to practical optoelectronic applications and has been successfully demonstrated with photodetectors of two-dimensional layered crystals such as graphene and MoS2. However, polarization sensitivity within such a photodetector remains elusive. Here, we demonstrate a broadband photodetector using a layered black phosphorus transistor that is polarization-sensitive over a bandwidth from ∼400 nm to 3,750 nm. The polarization sensitivity is due to the strong intrinsic linear dichroism, which arises from the in-plane optical anisotropy of this material. In this transistor geometry, a perpendicular built-in electric field induced by gating can spatially separate the photogenerated electrons and holes in the channel, effectively reducing their recombination rate and thus enhancing the performance for linear dichroism photodetection. The use of anisotropic layered black phosphorus in polarization-sensitive photodetection might provide new functionalities in novel optical and optoelectronic device applications.

A highly active and stable IrOx/SrIrO3 catalyst for the oxygen evolution reaction

Oxygen electrochemistry plays a key role in renewable energy technologies such as fuel cells and electrolyzers, but the slow kinetics of the oxygen evolution reaction (OER) limit the performance and commercialization of such devices. Here we report an iridium oxide/strontium iridium oxide (IrOx/SrIrO3) catalyst formed during electrochemical testing by strontium leaching from surface layers of thin films of SrIrO3. This catalyst has demonstrated specific activity at 10 milliamps per square centimeter of oxide catalyst (OER current normalized to catalyst surface area), with only 270 to 290 millivolts of overpotential for 30 hours of continuous testing in acidic electrolyte. Density functional theory calculations suggest the formation of highly active surface layers during strontium leaching with IrO3 or anatase IrO2 motifs. The IrOx/SrIrO3 catalyst outperforms known IrOx and ruthenium oxide (RuOx) systems, the only other OER catalysts that have reasonable activity in acidic electrolyte.

Titaniumdxy ferromagnetism at the LaAlO3/SrTiO3 interface

A number of recent transport and magnetization studies have shown signs of ferromagnetism in the LaAlO3/SrTiO3 heterostructure, an unexpected property with no bulk analogue in the constituent materials. However, no experiment thus far has provided direct information on the host of the magnetism. Here we report spectroscopic investigations of the magnetism using element-specific techniques, including X-ray magnetic circular dichroism and X-ray absorption spectroscopy, along with corresponding model calculations. We find direct evidence for in-plane ferromagnetic order at the interface, with Ti(3+) character in the dxy orbital of the anisotropic t2g band. These findings establish a striking example of emergent phenomena at oxide interfaces.

Control of electronic conduction at an oxide heterointerface using surface polar adsorbates

The interface between LaAlO(3) and SrTiO(3) possesses a range of intriguing properties, notably a proposed connection between the surface state of the LaAlO(3) and the conductivity buried in the SrTiO(3). Here we study the effect of the surface adsorption of a variety of common laboratory solvents on the conductivity at the interface between LaAlO(3) and SrTiO(3). We show that the application of chemicals such as acetone, ethanol, and water can induce a large change in the conductivity, and, in particular, an insulator to metal transition around the critical LaAlO(3) thickness. This phenomenon is observed only for polar solvents. These data provide experimental evidence for a general polarization-facilitated electronic transfer mechanism.

Critical thickness for ferromagnetism in LaAlO3/SrTiO3 heterostructures

In LaAlO(3)/SrTiO(3) heterointerfaces, charge carriers migrate from the LaAlO(3) to the interface in an electronic reconstruction. Magnetism has been observed in LaAlO(3)/SrTiO(3), but its relationship to the interface conductivity is unknown. Here we show that reconstruction is necessary, but not sufficient, for the formation of magnetism. Using scanning superconducting quantum interference device microscopy we find that magnetism appears only above a critical LaAlO(3) thickness, similar to the conductivity. We observe no change in ferromagnetism with gate voltage, and detect ferromagnetism in a non-conducting p-type sample. These observations indicate that the carriers at the interface do not need to be itinerant to generate magnetism. The ferromagnetism appears in isolated patches whose density varies greatly between samples. This inhomogeneity strongly suggests that disorder or local strain generates magnetism in a population of the interface carriers.

Charge Writing at the LaAlO3/SrTiO3 Surface

Biased conducting-tip atomic force microscopy (AFM) has been shown to write and erase nanoscale metallic lines at the LaAlO(3)/SrTiO(3) interface. Using various AFM modes, we show the mechanism of conductivity switching is the writing of surface charge. These charges are stably deposited on a wide range of LaAlO(3) thicknesses, including bulk crystals. A strong asymmetry with writing polarity was found for 1 and 2 unit cells of LaAlO(3), providing experimental evidence for a theoretically predicted built-in potential.

Locally enhanced conductivity due to the tetragonal domain structure in LaAlO3/SrTiO3 heterointerfaces.

The ability to control materials properties through interface engineering is demonstrated by the appearance of conductivity at the interface of certain insulators, most famously the {001} interface of the band insulators LaAlO3 and TiO2-terminated SrTiO3 (STO; refs 1, 2). Transport and other measurements in this system show a plethora of diverse physical phenomena. To better understand the interface conductivity, we used scanning superconducting quantum interference device microscopy to image the magnetic field locally generated by current in an interface. At low temperature, we found that the current flowed in conductive narrow paths oriented along the crystallographic axes, embedded in a less conductive background. The configuration of these paths changed on thermal cycling above the STO cubic-to-tetragonal structural transition temperature, implying that the local conductivity is strongly modified by the STO tetragonal domain structure. The interplay between substrate domains and the interface provides an additional mechanism for understanding and controlling the behaviour of heterostructures.

Subband Structure of a Two-Dimensional Electron Gas Formed at the Polar Surface of the Strong Spin-Orbit Perovskite KTaO3

We demonstrate the formation of a two-dimensional electron gas (2DEG) at the (100) surface of the 5d transition-metal oxide KTaO3. From angle-resolved photoemission, we find that quantum confinement lifts the orbital degeneracy of the bulk band structure and leads to a 2DEG composed of ladders of subband states of both light and heavy carriers. Despite the strong spin-orbit coupling, our measurements provide a direct upper bound for the potential Rashba spin splitting of only Δk(parallel)}~0.02 Å(-1) at the Fermi level. The polar nature of the KTaO3(100) surface appears to help mediate the formation of the 2DEG as compared to nonpolar SrTiO3(100).

Termination control of the interface dipole in La 0.7 Sr 0.3 MnO 3 / Nb : SrTiO 3 (001) Schottky junctions

In order to investigate the interface termination dependence of perovskite band alignments, we have studied the Schottky barrier height at