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Semiconductor compounds are widely used for photocatalytic hydrogen production applications, where photogenerated electron–hole pairs are exploited to induce catalysis. Recently, powders of a metallic oxide (Sr 1− x NbO 3 , 0.03< x <0.20) were reported to show competitive photocatalytic efficiencies under visible light, which was attributed to interband absorption. This discovery expanded the range of materials available for optimized performance as photocatalysts. Here we study epitaxial thin films of SrNbO 3+ δ and find that their bandgaps are ∼4.1 eV. Surprisingly, the carrier density of the conducting phase exceeds 10 22  cm −3 and the carrier mobility is only 2.47 cm 2  V −1  s −1 . Contrary to earlier reports, the visible light absorption at 1.8 eV (∼688 nm) is due to the plasmon resonance, arising from the large carrier density. We propose that the hot electron and hole carriers excited via Landau damping (during the plasmon decay) are responsible for the photocatalytic property of this material under visible light irradiation. Metallic oxide SrNbO 3 has been identified as an efficient hydrogen evolution photocatalyst. Here, Venkatesan and co-workers show that its visible light absorption stems from plasmon resonance, thanks to its large carrier density (despite a large 4.1 eV bandgap), as opposed to from an interband transition.

In condensed matter physics the quasi two-dimensional electron gas at the interface of two different insulators, polar LaAlO 3 on nonpolar SrTiO 3 (LaAlO 3 /SrTiO 3 ) is a spectacular and surprising observation. This phenomenon is LaAlO 3 film thickness dependent and may be explained by the polarization catastrophe model, in which a charge transfer of 0.5 e − from the LaAlO 3 film into the LaAlO 3 /SrTiO 3 interface is expected. Here we show that in conducting samples (≥4 unit cells of LaAlO 3 ) there is indeed a ~0.5 e − transfer from LaAlO 3 into the LaAlO 3 /SrTiO 3 interface by studying the optical conductivity in a broad energy range (0.5–35 eV). Surprisingly, in insulating samples (≤3 unit cells of LaAlO 3 ) a redistribution of charges within the polar LaAlO 3 sublayers (from AlO 2 to LaO) as large as ~0.5 e − 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 LaAlO 3 /SrTiO 3 interfaces. The origin of the two-dimensional electron gas at complex oxide interfaces is often explained by the polar catastrophe model, which involves a charge transfer mechanism. Using optical conductivity analysis, the authors assign and quantify the charge transfer, corroborating the polar catastrophe scenario.

The fabrication of an intriguing nano-fiber network interconnected to crystalline spherical shaped nanoparticles of HfO 2 has been achieved by femtosecond (fs) pulsed laser ablation in liquids. Understanding the fundamental reasons behind the formation of such heterostructures is important to scale up such process for other varieties of electronic materials. The present work has been designed to verify the impact of initial grain size on the final heterostructures formed. The overall plasma density and its composition were varied since the laser interaction with the matter is affected by the initial grain/particle size. This work covers the effects of initial grain sizes on HfO 2 hetero-nanomaterials formed by a controlled ball-milling process. The ablation was performed with fs laser pulses on HfO 2 pellets with two different initial grain sizes in distilled water and ethanol. The formed nanoparticles (NPs) had a spherical shape along with an interesting nano-fiber-like structure. The NPs were found to be polycrystalline in nature, and the fiber-like structures were found to be amorphous in nature. Further, the formation of high-temperature and high-pressure phases of HfO x NPs (tetragonal/cubic HfO x ) was observed along with a room-temperature phase (monoclinic HfO 2 ). A combination of ball milling and ultrafast laser ablation appears to be a preferred method for synthesizing smaller NPs of exotic non-equilibrium phases.

We report the observation of spatially separated Kondo scattering and ferromagnetism in anatase Ta 0.06 Ti 0.94 O 2 thin films as a function of thickness (10–200 nm). The Kondo behavior observed in thicker films is suppressed on decreasing thickness and vanishes below ~25 nm. In 200 nm film, transport data could be fitted to a renormalization group theory for Kondo scattering though the carrier density in this system is lower by two orders of magnitude, the magnetic entity concentration is larger by a similar magnitude and there is strong electronic correlation compared to a conventional system such as Cu with magnetic impurities. However, ferromagnetism is observed at all thicknesses with magnetic moment per unit thickness decreasing beyond 10 nm film thickness. The simultaneous presence of Kondo and ferromagnetism is explained by the spatial variation of defects from the interface to surface which results in a dominantly ferromagnetic region closer to substrate-film interface while the Kondo scattering is dominant near the surface and decreasing towards the interface. This material system enables us to study the effect of neighboring presence of two competing magnetic phenomena and the possibility for tuning them.

We show here a new phenomenon in La 0.5 Sr 0.5 TiO 3 /SrTiO 3 (LSTO/STO) heterostructures; that is a coexistence of three-dimensional electron liquid (3DEL) and 2D electron gas (2DEG), separated by an intervening insulating LSTO layer. The two types of carriers were revealed through multi-channel analysis of the evolution of nonlinear Hall effect as a function of film thickness, temperature and back gate voltage. We demonstrate that the 3D electron originates from La doping in LSTO film and the 2D electron at the surface of STO is due to the polar field in the intervening insulating layer. As the film thickness is reduced below a critical thickness of 6 unit cells (uc), an abrupt metal-to-insulator transition (MIT) occurs without an intermediate semiconducting state. The properties of the LSTO layer grown on different substrates suggest that the insulating phase of the intervening layer is a result of interface strain induced by the lattice mismatch between the film and substrate. Further, by fitting the magnetoresistance (MR) curves, the 6 unit cell thick LSTO is shown to exhibit spin-orbital coupling. These observations point to new functionalities, in addition to magnetism and superconductivity in STO-based systems, which could be exploited in a multifunctional context.

We report room-temperature ferromagnetism (FM) in highly conducting, transparent anatase Ti1−xTaxO2 (x∼0.05) thin films grown by pulsed laser deposition on LaAlO3 substrates. Rutherford backscattering spectrometry (RBS), X-ray diffraction, proton-induced X-ray emission, X-ray absorption spectroscopy (XAS) and time-of-flight secondary-ion mass spectrometry indicated negligible magnetic contaminants in the films. The presence of FM with concomitant large carrier densities was determined by a combination of superconducting quantum interference device magnetometry, electrical transport measurements, soft X-ray magnetic circular dichroism (SXMCD), XAS and optical magnetic circular dichroism, and was supported by first-principles calculations. SXMCD and XAS measurements revealed a 90 per cent contribution to FM from the Ti ions, and a 10 per cent contribution from the O ions. RBS/channelling measurements show complete Ta substitution in the Ti sites, though carrier activation was only 50 per cent at 5 per cent Ta concentration, implying compensation by cationic defects. The role of the Ti vacancy (VTi) and Ti3+ was studied via XAS and X-ray photoemission spectroscopy, respectively. It was found that, in films with strong FM, the VTi signal was strong while the Ti3+ signal was absent. We propose (in the absence of any obvious exchange mechanisms) that the localized magnetic moments, VTi sites, are ferromagnetically ordered by itinerant carriers. Cationic-defect-induced magnetism is an alternative route to FM in wide-band-gap semiconducting oxides without any magnetic elements.

Here, we report the presence of defect-related states with magnetic degrees of freedom in crystals of LaAlO 3 and several other rare-earth based perovskite oxides using inelastic light scattering (Raman spectroscopy) at low temperatures in applied magnetic fields of up to 9 T. Some of these states are at about 140 meV above the valence band maximum while others are mid-gap states at about 2.3 eV. No magnetic impurity could be detected in LaAlO 3 by Proton-Induced X-ray Emission Spectroscopy. We, therefore, attribute the angular momentum-like states in LaAlO 3 to cationic/anionic vacancies or anti-site defects. Comparison with the other rare earth perovskites leads to the empirical rule that the magnetic-field-sensitive transitions require planes of heavy elements (e.g. lanthanum) and oxygen without any other light cations in the same plane. These magnetic degrees of freedom in rare earth perovskites with useful dielectric properties may be tunable by appropriate defect engineering for magneto-optic applications.

Strongly correlated electronic systems such as Transition Metal Oxides often possess various mid-gap states originating from intrinsic defects in these materials. In this paper, we investigate an extremely sharp Photoluminescence (PL) transition originating from such defect states in two widely used perovskites, LaAlO 3 and SrTiO 3 . A detailed study of the PL as a function of temperature and magnetic field has been conducted to understand the behavior and origin of the transition involved. The temperature dependence of the PL peak position for SrTiO 3 is observed to be opposite to that in LaAlO 3 . Our results reveal the presence of a spin/orbital character in these transitions which is evident from the splitting of these defect energy levels under a high magnetic field. These PL transitions have the potential for enabling non-contact thermal and field sensors.

In this study we report the existence of novel ultraviolet (UV) and blue emission in rare-earth based perovskite NdGaO 3 (NGO) and the systematic quench of the NGO photoluminescence (PL) by Ce doping. Study of room temperature PL was performed in both single-crystal and polycrystalline NGO (substrates and pellets) respectively. Several NGO pellets were prepared with varying Ce concentration and their room temperature PL was studied using 325 nm laser. It was found that the PL intensity shows a systematic quench with increasing Ce concentration. XPS measurements indicated that nearly 50% of Ce atoms are in the 4+ state. The PL quench was attributed to the novel concept of super hydrogenic dopant (SHD)”, where each Ce 4+ ion contributes an electron which forms a super hydrogenic atom with an enhanced Bohr radius, due to the large dielectric constant of the host. Based on the critical Ce concentration for complete quenching this SHD radius was estimated to be within a range of 0.85 nm and 1.15 nm whereas the predicted theoretical value of SHD radius for NdGaO3 is ~1.01 nm.

We report room-temperature ferromagnetism (FM) in highly conducting, transparent anatase Ti 1− x Ta x O 2  ( x ∼0.05) thin films grown by pulsed laser deposition on LaAlO 3 substrates. Rutherford backscattering spectrometry (RBS), X-ray diffraction, proton-induced X-ray emission, X-ray absorption spectroscopy (XAS) and time-of-flight secondary-ion mass spectrometry indicated negligible magnetic contaminants in the films. The presence of FM with concomitant large carrier densities was determined by a combination of superconducting quantum interference device magnetometry, electrical transport measurements, soft X-ray magnetic circular dichroism (SXMCD), XAS and optical magnetic circular dichroism, and was supported by first-principles calculations. SXMCD and XAS measurements revealed a 90 per cent contribution to FM from the Ti ions, and a 10 per cent contribution from the O ions. RBS/channelling measurements show complete Ta substitution in the Ti sites, though carrier activation was only 50 per cent at 5 per cent Ta concentration, implying compensation by cationic defects. The role of the Ti vacancy ( V Ti ) and Ti 3+ was studied via XAS and X-ray photoemission spectroscopy, respectively. It was found that, in films with strong FM, the V Ti signal was strong while the Ti 3+ signal was absent. We propose (in the absence of any obvious exchange mechanisms) that the localized magnetic moments, V Ti sites, are ferromagnetically ordered by itinerant carriers. Cationic-defect-induced magnetism is an alternative route to FM in wide-band-gap semiconducting oxides without any magnetic elements.