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Semiconductor compounds are widely used for water splitting applications, where photo-generated electron-hole pairs are exploited to induce catalysis. Recently, powders of a metallic oxide (Sr$_{1-x}$NbO$_3$, 0.03 < x < 0.20) have shown competitive photocatalytic efficiency, opening up the material space available for finding optimizing performance in water-splitting applications. The origin of the visible light absorption in these powders was reported to be due to an interband transition and the charge carrier separation was proposed to be due to the high carrier mobility of this material. In the current work we have prepared epitaxial thin films of Sr$_{0.94}$NbO$_{3+{\delta}}$ and found that the bandgap of this material is ~4.1 eV, which is very large. Surprisingly the carrier density of the conducting phase reaches 10$^{22}$ cm$^{-3}$, which is only one order smaller than that of elemental metals and the carrier mobility is only 2.47 cm$^2$/(V$\cdot$s). Contrary to earlier reports, the visible light absorption at 1.8 eV (~688 nm) is due to the bulk plasmon resonance, arising from the large carrier density, instead of an interband transition. Excitation of the plasmonic resonance results in a multifold enhancement of the lifetime of charge carriers. Thus we propose that the hot charge carriers generated from decay of plasmons produced by optical absorption is responsible for the water splitting efficiency of this material under visible light irradiation.

Titanium dioxide (TiO$_2$) has rich physical properties with potential implications in both fundamental physics and new applications. Up-to-date, the main focus of applied research is to tune its optical properties, which is usually done via doping and/or nano-engineering. However, understanding the role of $d$-electrons in materials and possible functionalization of $d$-electron properties are still major challenges. Herewith, within a combination of an innovative experimental technique, high energy optical conductivity, and of the state-of-the-art {\it ab initio} electronic structure calculations, we report an emerging, novel resonant exciton in the deep ultraviolet region of the optical response. The resonant exciton evolves upon low concentration Ta-substitution in anatase TiO$_{2}$ films. It is surprisingly robust and related to strong electron-electron and electron-hole interactions. The $d$- and $f$- orbitals localization, due to Ta-substitution, plays an unexpected role, activating strong electronic correlations and dominating the optical response under photoexcitation. Our results shed light on a new optical phenomenon in anatase TiO$_{2}$ films and on the possibility of tuning electronic properties by Ta substitution.

The observation of magnetic interaction at the interface between nonmagnetic oxides has attracted much attention in recent years. In this report, we show that the Kondo-like scattering at the SrTiO3-based conducting interface is enhanced by increasing the lattice mismatch and growth oxygen pressure PO2. For the 26-unit-cell LaAlO3/SrTiO3 (LAO/STO) interface with lattice mismatch being 3.0%, the Kondo-like scattering is observed when PO2 is beyond 1 mTorr. By contrast, when the lattice mismatch is reduced to 1.0% at the (La0.3Sr0.7)(Al0.65Ta0.35)O3/SrTiO3 (LSAT/STO) interface, the metallic state is always preserved up to PO2 of 100 mTorr. The data from Hall measurement and X-ray absorption near edge structure (XANES) spectroscopy reveal that the larger amount of localized Ti3+ ions are formed at the LAO/STO interface compared to LSAT/STO. Those localized Ti3+ ions with unpaired electrons can be spin-polarized to scatter mobile electrons, responsible for the Kondo-like scattering observed at the LAO/STO interface., Comment: 25 pages, 5 figure

Electric field effect in electronic double layer transistor (EDLT) configuration with ionic liquids as the dielectric materials is a powerful means of exploring various properties in different materials. Here we demonstrate the modulation of electrical transport properties and extremely high mobility of two-dimensional electron gas at LaAlO$_3$/SrTiO$_3$ (LAO/STO) interface through ionic liquid-assisted electric field effect. By changing the gate voltages, the depletion of charge carrier and the resultant enhancement of electron mobility up to 19380 cm$^2$/Vs are realized, leading to quantum oscillations of the conductivity at the LAO/STO interface. The present results suggest that high-mobility oxide interfaces which exhibit quantum phenomena could be obtained by ionic liquid-assisted field effect., Comment: 22 pages, 4 figures, ACS Nano, March 09, 2016

The conducting gas that forms at the interface between LaAlO$_3$ and SrTiO$_3$ has proven to be a fertile playground for a wide variety of physical phenomena. The bulk of previous research has focused on the (001) and (110) crystal orientations. Here we report detailed measurements of the low-temperature electrical properties of (111) LAO/STO interface samples. We find that the low-temperature electrical transport properties are highly anisotropic, in that they differ significantly along two mutually orthogonal crystal orientations at the interface. While anisotropy in the resistivity has been reported in some (001) samples and in (110) samples, the anisotropy in the (111) samples reported here is much stronger, and also manifests itself in the Hall coefficient as well as the capacitance. In addition, the anisotropy is not present at room temperature and at liquid nitrogen temperatures, but only at liquid helium temperatures and below. The anisotropy is accentuated by exposure to ultraviolet light, which disproportionately affects transport along one surface crystal direction. Furthermore, analysis of the low-temperature Hall coefficient and the capacitance as a function of back gate voltage indicates that in addition to electrons, holes contribute to the electrical transport., Comment: 11 pages, 9 figures

The problem of counting occurrences of query graphs in a large data graph, known as subgraph counting, is fundamental to several domains such as genomics and social network analysis. Many important special cases (e.g. triangle counting) have received significant attention. Color coding is a very general and powerful algorithmic technique for subgraph counting. Color coding has been shown to be effective in several applications, but scalable implementations are only known for the special case of {\em tree queries} (i.e. queries of treewidth one). In this paper we present the first efficient distributed implementation for color coding that goes beyond tree queries: our algorithm applies to any query graph of treewidth $2$. Since tree queries can be solved in time linear in the size of the data graph, our contribution is the first step into the realm of colour coding for queries that require superlinear running time in the worst case. This superlinear complexity leads to significant load balancing problems on graphs with heavy tailed degree distributions. Our algorithm structures the computation to work around high degree nodes in the data graph, and achieves very good runtime and scalability on a diverse collection of data and query graph pairs as a result. We also provide theoretical analysis of our algorithmic techniques, showing asymptotic improvements in runtime on random graphs with power law degree distributions, a popular model for real world graphs.

Wetting behaviour of surfaces is believed to be affected by van der Waals (vdW) forces, however, there is no clear demonstration of this. With the isolation of two-dimensional vdW layered materials it is possible to test this hypothesis. In this paper, we report the wetting behaviour of vdW heterostructures which include, chemical vapor deposition (CVD) grown graphene, molybdenum disulfide (MoS2) and tungsten disulfide (WS2) on few layers of hexagon boron nitride (h-BN) and SiO2/Si. Our study clearly shows that while this class of two-dimensional materials are not wetting transparent, there seems to be a significant amount of influence on their wetting properties by the underlying substrate due to dominant vdW forces. Contact angle measurements indicate that graphene and graphene-like layered transitional metal dichalcogenides invariably have intrinsically dispersive surfaces with a dominating London-vdW force-mediated wettability. Electric field controlled wetting studies of MoS2/WS2/SiO2/Si heterostructures were performed and no notable changes to the water contact angle was seen with applied voltage although two orders of magnitude change in resistance was observed. We postulate that the highly dispersive nature of these surfaces arising from the predominant London-vdW forces could be the reason for such observation.

Since the discovery of two-dimensional electron gas (2DEG) at the oxide interface of LaAlO3/SrTiO3, improving carrier mobility has become an important issue for device applications. In this paper, by using an alternate polar perovskite insulator (La0.3Sr0.7)(Al0.65Ta0.35)O3 (LSAT) for reducing lattice mismatch from 3.0% to 1.0%, the low-temperature carrier mobility has been increased 30 fold to 35,000 cm2V-1s-1. Moreover, two critical thicknesses for the LSAT/SrTiO3 (001) interface are found: one at 5 unit cell for appearance of the 2DEG, the other at 12 unit cell for a peak in the carrier mobility. By contrast, the conducting (110) and (111) LSAT/STO interfaces only show a single critical thickness of 8 unit cells. This can be explained in terms of polar fluctuation arising from LSAT chemical composition. In addition to lattice mismatch and crystal symmetry at the interface, polar fluctuation arising from composition has been identified as an important variable to be tailored at the oxide interfaces to optimise the 2DEG transport., Comment: 17 pages, 4 figures

We use ionic liquid-assisted electric field effect to tune the carrier density in an electron-doped cuprate ultrathin film and cause a two-dimensional superconductor-insulator transition (SIT). The low upper critical field in this system allows us to perform magnetic field (B)-induced SIT in the liquid-gated superconducting film. Finite-size scaling analysis indicates that SITs induced both by electric and magnetic field are quantum phase transitions and the transitions are governed by percolation effects - quantum mechanical in the former and classical in the latter case. Compared to the hole-doped cuprates, the SITs in electron-doped system occur at critical sheet resistances (Rc) much lower than the pair quantum resistance RQ=h/(2e)2=6.45 k{\Omega}, suggesting the possible existence of fermionic excitations at finite temperature at the insulating phase near SITs., Comment: Manuscript including supplementary materials

Graphene is a rising star in nonlinear optics due to its saturable absorption and giant Kerr nonlinearity, these properties are useful in digital optics based on optical nonlinear devices. However, practical applications require large optical nonlinearities and these are inherently limited by the interaction length of atomically thin graphene. Here, we demonstrate optical bistability in a Fabry Perot cavity containing monolayer and bilayer graphene which have been restructured to form nanobubbles. We find that graphene nanobubble can act as a new type of optical nonlinear media due to its vertical side wall as well as added curvature, which enable strong non linear dispersive effects leading to a large optically induced phase change. Unlike thermally induced bistability, the all optical switching between two transmission states happens within a time scale of tens of nanoseconds. Nanobubble based optical devices with intrinsic optical nonlinearity help to overcome the optical path length limitation of atomically thin two dimensional films and allow us to explore the promise of using such elements as the building block of digital all-optical circuitry., Comment: 17 pages, 4 figures

In condensed matter physics the quasi two-dimensional electron gas at the interface of two different insulators, polar LaAlO3 on non-polar SrTiO3 (LaAlO3/SrTiO3) is a spectacular and surprising observation. This phenomenon is LaAlO3 film thickness-dependent and may be explained by the polarization catastrophe model, in which a charge transfer of 0.5 electron from the LaAlO3 film into the LaAlO3/SrTiO3 interface is expected. Here we show that in conducting samples (more than 4 unit cells of LaAlO3) there is indeed a 0.5 electron transfer from LaAlO3 into the LaAlO3/SrTiO3 interface by studying the optical conductivity in a broad energy range (0.5-35 eV). Surprisingly, in insulating samples (less than 4 unit cells of LaAlO3) a redistribution of charges within the polar LaAlO3 sub-layers (from AlO2 to LaO) as large as 0.5 electron is observed, with no charge transfer into the interface. Hence, our results reveal the different mechanisms for the polarization catastrophe compensation in insulating and conducting LaAlO3/SrTiO3 interfaces., Comment: Main Article (33 pages, 7 figures, 1 table); Supplementary Materials (19 pages, 8 figures)

We present evidence of a drastic renormalization of the optical conductivity of graphene on SrTiO$_3$ resulting in almost full transparency in the ultraviolet region. These findings are attributed to resonant excitonic effects further supported by \emph{ab initio} Bethe-Salpeter equation and density functional theory calculations. The ($\pi$,$\pi$*)-orbitals of graphene and Ti-3\textit{d} $t_{2g}$ orbitals of SrTiO$_3$ are strongly hybridized and the interactions of electron-hole states residing in those orbitals play dominant role in the graphene optical conductivity. These interactions are present much below the optical band gap of bulk SrTiO$_3$. These results open a possibility of manipulating interaction strengths in graphene via \textit {d}-orbitals which could be crucial for optical applications., Comment: 9 pages, 11 figures, Phys. Rev. B (accepted)

A detailed defect energy level map was investigated for heterostructures of 26 unit cells of LaAlO3 on SrTiO3 prepared at a low oxygen partial pressure of 10-6 mbar. The origin is attributed to the presence of dominating oxygen defects in SrTiO3 substrate. Using femtosecond laser spectroscopy, the transient absorption and relaxation times for various transitions were determined. An ultrafast relaxation process of 2-3 picosecond from the conduction band to the closest defect level and a slower process of 70-92 picosecond from conduction band to intra-band defect level were observed. The results are discussed on the basis of propose defect-band diagram., Comment: 11 pages, 4 figures

Atomically sharp oxide heterostructures often exhibit unusual physical properties that are absent in the constituent bulk materials. The interplay between electrostatic boundary conditions, strain and dimensionality in ultrathin epitaxial films can result in monolayer-scale transitions in electronic or magnetic properties. Here we report an atomically sharp antiferromagnetic-to-ferromagnetic phase transition when atomically growing polar antiferromagnetic LaMnO3 (001) films on SrTiO3 substrates. For a thickness of five unit cells or less, the films are antiferromagnetic, but for six unit cells or more, the LaMnO3 film undergoes a phase transition to a ferromagnetic state 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 how new emergent functionalities can be visualized and engineered in atomically thick oxide films at the atomic level.

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., Comment: 35 pages, 6 figures in the main text,13 figures in the supporting information. To be appearing in Advanced Materials Interfaces soon

We report that in unannealed LaAlO3/SrTiO3 (LAO/STO) heterostructures the critical thickness for the appearance of the two-dimensional electron gas can be less than 4 unit cell (uc), the interface is conducting even for STO substrates with mixed terminations and the low-temperature resistance upturn in LAO/STO heterostructures with thick LAO layers strongly depends on laser fluence. Our experimental results provide fundamental insights into the different roles played by oxygen vacancies and polarization catastrophe in the two-dimensional electron gas in crystalline LAO/STO heterostructures., Comment: 4 pages, 3 figures. To be appearing in Journal of Applied Physics

In this paper, we study a class of set cover problems that satisfy a special property which we call the {\em small neighborhood cover} property. This class encompasses several well-studied problems including vertex cover, interval cover, bag interval cover and tree cover. We design unified distributed and parallel algorithms that can handle any set cover problem falling under the above framework and yield constant factor approximations. These algorithms run in polylogarithmic communication rounds in the distributed setting and are in NC, in the parallel setting., Comment: Full version of FSTTCS'13 paper

Manipulating spin-orbit coupling (SOC) is important for devices such as spin-orbit torque based memory and its understanding is neccessary to answer several fundamental open questions in triplet state superconductivity, topological insulators and Majorana fermions. Here we report spin splitting of 25 meV at the LaAlO3/SrTiO3 (110) interface for in-plane spins at a current density of 1.4x104 A/cm2, which is large compared to that found in semiconductor heterostructures or the LaAlO3/SrTiO3 (100) interface, and in addition it is anisotropic. The anisotropy arises from the difference in electron effective mass along the [001] and [1-10] directions. Our study predicts a spin splitting energy > 1000 meV at a current density of 107 A/cm2, which is enormous compared to metallic systems and will be an ideal spin polarized source. In addition to the in-plane effect, there is an unexpected gate-tunable out-of-plane SOC at the LaAlO3/SrTiO3 (110) interface when the spins lie out-of-plane due to broken symmetry in the plane of the interface. We demonstrate that this can be manipulated by varying the LaAlO3 thickness showing that this interface can be engineered for spin-orbit torque devices., Comment: 17 pages, 5 figures in Advanced Electronic Materials (Wiley) Vol. 1, Issue 8, 2015

Localization of electrons in the two-dimensional electron gas at the LaAlO$_3$/SrTiO$_3$ interface is investigated by varying the channel thickness in order to establish the nature of the conducting channel. Layers of SrTiO$_3$ were grown on NdGaO$_3$ (110) substrates and capped with LaAlO$_3$. When the SrTiO$_3$ thickness is $\leq 6$ unit cells, most electrons at the interface are localized, but when the number of SrTiO$_3$ layers is 8-16, the free carrier density approaches $3.3 \times 10^{14}$ cm$^{-2}$, the value corresponding to charge transfer of 0.5 electron per unit cell at the interface. The number of delocalized electrons decreases again when the SrTiO$_3$ thickness is $\geq 20$ unit cells. The $\sim{4}$ nm conducting channel is therefore located significantly below the interface. The results are explained in terms of Anderson localization and the position of the mobility edge with respect to the Fermi level., Comment: Main: 19 pages, 4 figures Supplementary: 14 pages, 10 figures

Coherent radiation with frequencies ranging from 0.3 to 30 THz has recently become accessible by femtosecond laser technology. Terahertz (THz) waves have already found many applications in spectroscopy and imaging, and they can be manipulated using static optical elements such as lenses, polarizers, and filters. However, ultrafast modulation of THz radiation is required as well, for instance in short-range wireless communication or for preparing shaped THz transients for coherent control of numerous material excitations. Here, we demonstrate an all-optically created transient metamaterial that permits to manipulate the polarization of THz waveforms with sub-cycle precision. The polarization-modulated pulses are potentially interesting for controlling elementary motions such as vibrations of crystal lattices, rotations of molecules, and the precession of spins., Comment: 14 pages, 7 Figures

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., Comment: 9 pages, 6 figures

The confinement of the two dimensional electron gas (2DEG), preferential occupancy of the Ti 3d orbital and strong spin-orbit coupling at the LaAlO$_3$/SrTiO$_3$ interface play a significant role in its emerging properties. Here we report a fourfold oscillation in the anisotropic magneto resistance (AMR) and the observation of planar Hall effect (PHE) at the LaAlO$_3$/SrTiO$_3$ heterointerface. We evaluate the carrier confinement effects on the AMR and find that the fourfold oscillation appears only for the case of 2DEG system while it is twofold for the 3D system. As the fourfold oscillation fits well to the phenomenological model for a cubic symmetry system, we attribute this oscillation to the anisotropy in the magnetic scattering arising from the interaction of electrons with the localized magnetic moments coupled to the crystal symmetry. The AMR behavior is further found to be sensitive to applied gate electric field, emphasizing the significance of spin-orbit coupling at the interface. These confinement effects suggest that the magnetic interactions are predominant at the interface, and the gate electric field modulation of AMR suggest the possible gate tunable magnetic interactions in these systems. The observed large PHE further indicates that the in plane nature of magnetic ordering arises from the in-plane Ti 3dxy orbitals., Comment: Main manuscript: 20 pages, Figures: 5, Supplementary Information: 5 pages

The electronic properties of SrRuO3/LaAlO3 (SRO/LAO) superlattices with different interlayer thicknesses of SRO layers were studied. As the thickness of SRO layers is reduced, the superlattices exhibit a metal-insulator transition implying transformation into a more localized state from its original bulk metallic state. The strain effect on the metal-insulator transition was also examined. The origin of the metal-insulator transition in ultrathin SRO film is discussed. All the superlattices, even those with SRO layers as thin as 2 unit cells, are ferromagnetic at low temperatures. Moreover, we demonstrate field effect devices based on such multilayer superlattice structures., Comment: 19 pages, 5 figures, 1 table

We report evolution of the two-dimensional electron gas behavior at the NdAlO3/SrTiO3 heterointerfaces with varying thicknesses of the NdAlO3 overlayer. The samples with a thicker NdAlO3 show strong localizations at low temperatures and the degree of localization is found to increase with the NdAlO3 thickness. The T -1/3 temperature dependence of the sheet resistance at low temperatures and the magnetoresistance study reveal that the conduction is governed by a two-dimensional variable range hopping mechanism in this strong localized regime. We attribute this thickness dependence of the transport properties of the NdAlO3/SrTiO3 interfaces to the interface strain induced by the overlayers., Comment: 15 pages, 4 figures

Molybdenum disulphide, a diamagnetic layered dichalcogenide solid, is found to show magnetic ordering at room temperature when exposed to a 2 MeV proton beam. The temperature dependence of magnetization displays ferrimagnetic behavior with a Curie temperature of 895 K. A disorder mode corresponding to a zone-edge phonon and a Mo valence higher than +4, have been detected in the irradiated samples using Raman and X-ray photoelectron spectroscopy, respectively. The possible origins of long-range magnetic ordering in irradiated MoS2 samples are discussed.

The observation of a two dimensional electron gas (2DEG) (1, 2), superconductivity (3, 4), magnetic effects (5) and electronic phase separation (6-8) at the interfaces of insulating oxides, especially LaAlO3/SrTiO3, has further enhanced the potential of complex oxides for novel electronics. The occurrence of the 2DEG is strongly believed to be driven by the polarization discontinuity (9) at the interface between the two oxides. In this scenario, the crystal orientation plays an important role and no conductivity would be expected for e.g., the interface between LaAlO3 and (110)-oriented SrTiO3, which should not have a polarization discontinuity (10, 11). Here, we report the observation of unexpected conductivity at the LaAlO3/SrTiO3 interface prepared on (110)-oriented SrTiO3. The conductivity was further found to be strongly anisotropic, with the ratio of the conductance along the different directions parallel to the substrate surface showing a remarkable dependence on the oxygen pressure during deposition. The conductance and its anisotropy are discussed based on the atomic structure at the interface, as revealed by Scanning Transmission Electron Microscopy (STEM) and further supported by density functional theory (DFT) calculations., Comment: 17 pages, 5 figures

The PERCS system was designed by IBM in response to a DARPA challenge that called for a high-productivity high-performance computing system. The IBM PERCS architecture is a two level direct network having low diameter and high bisection bandwidth. Mapping and routing strategies play an important role in the performance of applications on such a topology. In this paper, we study mapping strategies for PERCS architecture, that examine how to map tasks of a given job on to the physical processing nodes. We develop and present fundamental principles for designing good mapping strategies that minimize congestion. This is achieved via a theoretical study of some common communication patterns under both direct and indirect routing mechanisms supported by the architecture., Comment: Full version of paper at HiPC 2012