A. Roy Barman

Electronic phase separation at the LaAlO3/SrTiO3 interface

There are many electronic and magnetic properties exhibited by complex oxides. Electronic phase separation (EPS) is one of those, the presence of which can be linked to exotic behaviours, such as colossal magnetoresistance, metal-insulator transition and high-temperature superconductivity. A variety of new and unusual electronic phases at the interfaces between complex oxides, in particular between two non-magnetic insulators LaAlO(3) and SrTiO(3), have stimulated the oxide community. However, no EPS has been observed in this system despite a theoretical prediction. Here, we report an EPS state at the LaAlO(3)/SrTiO(3) interface, where the interface charges are separated into regions of a quasi-two-dimensional electron gas, a ferromagnetic phase, which persists above room temperature, and a (superconductor like) diamagnetic/paramagnetic phase below 60 K. The EPS is due to the selective occupancy (in the form of 2D-nanoscopic metallic droplets) of interface sub-bands of the nearly degenerate Ti orbital in the SrTiO(3). The observation of this EPS demonstrates the electronic and magnetic phenomena that can emerge at the interface between complex oxides mediated by the Ti orbital.

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.

A new route to graphene layers by selective laser ablation

Selectively creating regions of spatially varying thickness may enable the utilization of the electronic properties of N-layer (N=1 or more) graphene and other similar layered materials (e.g., topological insulators or layered superconductors) for novel devices and functionalities on a single chip. The ablation threshold energy density increases dramatically for decreasing layer numbers of graphene originating from the dimensional crossover of the specific heat. For the 2D regime of graphite (up to N≈7) the dominant flexural mode specific heat (due to its N-1 dependence) gives rise to a strong layer number-dependence on the pulsed laser ablation threshold energy density, while for 3D regime (N>>7) the ablation threshold saturates due to dominant acoustic mode specific heat. As a result, several energy density windows exist between the minimum energy densities that are required for ablating single, bi, or more layers of graphene, allowing layer number selectivity.

Mega-electron-volt proton irradiation on supported and suspended graphene: A Raman spectroscopic layer dependent study

Graphene samples with 1, 2, and 4 layers and 1 + 1 folded bi-layers and graphite have been irradiated with 2 MeV protons at fluences ranging from 1 × 1015 to 6 × 1018 ions/cm2. The samples were characterized using visible and UV Raman spectroscopy and Raman microscopy. The ion-induced defects were found to decrease with increasing number of layers. Graphene samples suspended over etched holes in SiO2 have been fabricated and used to investigate the influence of the substrate SiO2 for defect creation in graphene. While Raman vibrational modes at 1460 cm−1 and 1555 cm−1 have been observed in the visible Raman spectra of substantially damaged graphene samples, these modes were absent in the irradiated-suspended monolayer graphene.

Cationic-vacancy-induced room-temperature ferromagnetism in transparent, conducting anatase Ti1-xTaxO2 (x~0.05) thin films.

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.

Multifunctional Ti1−xTaxO2: Ta doping or alloying?

Useful electronic, magnetic, and optical properties have been proposed and observed in thin films of Ti1−xMxO2 (M=Ta,Nb,V). In this work, we have studied phase formation for films of Ti1−xTaxO2 prepared by pulsed laser deposition. We show that substitutional Ta in TiO2 results in a different material system in terms of its electronic properties. Moss–Burstein shift is ruled out by comparing the electrical transport data of anatase and rutile TiO2. Vegard’s law fit to the blueshift data and the high energy optical reflectivity studies confirm the formation of an alloy with a distinct band structure.

Defect dynamics and spectral observation of twinning in single crystalline LaAlO3 under subbandgap excitation

We have investigated the photoluminescence and ultrafast dynamics of LaAlO3 crystal. The photoluminescence consists of a broad spectrum and two sharp peaks, which arise from various defect levels within the bandgap. A doublet splitting of roughly 6 nm is seen in these two sharp peaks. An Al displacement of 0.09 A in a sublattice, which is possible because of twinning, is adequate to explain the spectral splitting. Femtosecond pump probe experiments reveal further that many of these defect levels have a few picosecond decay times while the lowest defect states have decay times longer than nanosecond to the valence band.

Static and ultrafast dynamics of defects of SrTiO3 in LaAlO3/SrTiO3 heterostructures

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 ps from the conduction band to the closest defect level and a slower process of 70–92 ps from conduction band to intraband defect level were observed. The results are discussed on the basis of the proposed defect-band diagram.

Metal-insulator transition at a depleted LaAlO3/SrTiO3 interface: Evidence for charge transfer induced by SrTiO3 phase transitions

Two anomalous bias dependent resistive peaks induced by the SrTiO3 structural phase transitions at 55 and 110 K were observed in a LaAlO3/SrTiO3 and Nb:SrTiO3 rectifying junction when the LaAlO3/SrTiO3 was depleted under reverse bias. At these transition temperatures, the barrier between LaAlO3/SrTiO3 and Nb:SrTiO3 showed abrupt changes in the tunneling energy under forward bias. The peak at 110 K was an insulator-metal phase transition while the peak at 55 K was a metal-insulator one. We propose that the phase transitions of the SrTiO3 substrate influence the charge transfer to the LaAlO3/SrTiO3 layer, giving rise to these anomalous resistive peaks.