Amar Srivastava

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.

Selective growth of single phase VO2(A, B, and M) polymorph thin films

We demonstrate the growth of high quality single phase films of VO2(A, B, and M) on SrTiO3 substrate by controlling the vanadium arrival rate (laser frequency) and oxidation of the V atoms. A phase diagram has been developed (oxygen pressure versus laser frequency) for various phases of VO2 and their electronic properties are investigated. VO2(A) phase is insulating VO2(B) phase is semi-metallic, and VO2(M) phase exhibits a metal-insulator transition, corroborated by photo-electron spectroscopic studies. The ability to control the growth of various polymorphs opens up the possibility for novel (hetero)structures promising new device functionalities.

New insights into the diverse electronic phases of a novel vanadium dioxide polymorph: a terahertz spectroscopy study.

A remarkable feature of vanadium dioxide is that it can be synthesized in a number of polymorphs. The conductivity mechanism in the metastable layered polymorph VO2(B) thin films has been investigated by terahertz time-domain spectroscopy (THz-TDS). In VO2(B), a critical temperature of 240 K marks the appearance of a non-zero Drude term in the observed complex conductivity, indicating the evolution from a pure insulating state towards a metallic state. In contrast, the THz conductivity of the well-known VO2(M1) is well fitted only by a modification of the Drude model to include backscattering. We also identified two different THz conductivity regimes separated by temperature in these two polymorphs. The electronic phase diagram is constructed, revealing that the width and onset of the metal-insulator transition in the B phase develop differently from the M1 phase.

Gate Tunable In- and Out-of-Plane Spin–Orbit Coupling and Spin-Splitting Anisotropy at LaAlO3/SrTiO3 (110) Interface

Manipulating spin–orbit coupling (SOC) is important for devices such as spin–orbit torque-based memory and its understanding is necessary to answer several fundamental open questions in triplet state superconductivity, topological insulators, and Majorana fermions. Here spin splitting of 25 meV is reported at the LaAlO3/SrTiO3 (110) interface for in-plane spins at a current density of 1.4 × 104 A cm−2, 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 cm−2, 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. It is demonstrated that this can be manipulated by varying the LaAlO3 thickness showing that this interface can be engineered for spin–orbit torque devices.

Evolution of variable range hopping in strongly localized two dimensional electron gas at NdAlO3/SrTiO3 (100) heterointerfaces

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.

Evidence for Photoinduced Insulator-to-Metal transition in B-phase vanadium dioxide

Ultrafast optical studies have been performed on epitaxial films of the novel B-phase of vanadium dioxide using temperature-dependent optical pump-probe technique. Signature of temperature-driven metal-to-insulator transition was distinctly observed in the ultrafast dynamics — the insulating phase showed two characteristic electronic relaxation times while the metallic phase showed only one. Beyond a threshold value of the pump fluence, the insulating state collapses into a ‘metallic-like’ phase which can be further subdivided into two regimes according to the lengths of the fast characteristic time. The first regime can be explained by lattice heating due to the optical pump; the other cannot be accounted by simple lattice heating effects alone, and thus offers evidence for a true photoinduced phase transition.

Coherently coupled ZnO and VO2 interface studied by photoluminescence and electrical transport across a phase transition

We have investigated the photoluminescence and electrical properties of a coherently coupled interface consisting of a ZnO layer grown on top of an oriented VO2 layer on sapphire across the phase transition of VO2. The band edge and defect luminescence of the ZnO overlayer exhibit hysteresis in opposite directions induced by the phase transition of VO2. Concomitantly the phase transition of VO2 was seen to induce defects in the ZnO layer. Such coherently coupled interfaces could be of use in characterizing the stability of a variety of interfaces in situ and also for novel device application.

Effect of Nb and Ta substitution on donor electron transport and ultrafast carrier dynamics in anatase TiO2 thin films

Ta and Nb substituted TiO2 are important transparent conducting oxides that have potential for applications in photovoltaics, photocatalysis, and water splitting/CO2 sequestration. In addition to donating electrons, what are the effects of Nb and Ta substitution? Here we observe strong experimental evidence that Ta and Nb substitution induces large and small polarons in anatase TiO2 epitaxial thin films. The degenerate donor electrons (from both Nb and Ta) show a high temperature T3 dependence on electrical resistivity, which confirms the presence of large polarons, along with room temperature metallic transport. This is further confirmed by the enhancement in the electron effective mass, which was estimated from thermopower measurements. Femtosecond transient absorption (fs-TA) reveals the life time of the Ti-t2g and eg levels and the separation of these levels are consistent with the X-ray absorption spectroscopy (XAS) measurement. In addition, fs-TA reveals the presence of small polarons with a life time substantially >1 ns, which arises from defect levels and is a consequence of Ta and Nb substitution. X-ray photoelectron spectroscopy (XPS) provides evidence of Ti3+, which may be identified as the defects responsible for the small polarons. These long-lived small polarons may provide a way to minimize recombination dynamics in TiO2-based electrodes for photo-excited devices.