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.
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 [Y. Chen et al., Nano Lett. 11, 3774 (2011); S. W. Lee et al., Nano Lett. 12, 4775 (2012)] have called in question the original polarization catastrophe model [N. Nakagawa et al., Nature Mater. 5, 204 (2006)]. 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 (∼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 restored 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, but 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, it was found that the crystallinity of the LaAlO3 layer is crucial for the polarization catastrophe mechanism in the case of crystalline LaAlO3 overlayers. PACS numbers: 73.20.-r 73.21.Ac 73.40.-c 71.23.CqThe two-dimensional electron gas (2DEG) appearing at the interface between the band insulators LaAlO 3 (LAO) and SrTiO 3 (STO) has attracted much attention since its discovery by Ohtomo and Hwang [1]. It has stimulated a substantial body of experimental and theoretical work [2-25], but, its origin is still controversial [26]. Three different mechanisms have been proposed. First is interface electronic reconstruction to avoid the polarization catastrophe induced by the discontinuity at the interface between polar LAO and nonpolar STO [2][3][4]. Second is doping by thermal interdiffusion of Ti/Al or La/Sr atoms at the interface [13]. A third possible mechanism is creation of oxygen vacancies in STO substrates during the deposition process [9][10][11]27,28]. Oxygen vacancies are known to introduce a shallow intragap donor level close to the conduction band of STO [29], and their action may be specific to this one substrate. The thermal interdiffusion mechanism was discounted in recent work [25], which studied the effect of a mixed interface layer. It i...
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.
In condensed matter physics the quasi two-dimensional electron gas at the interface of two different insulators, polar LaAlO3 on nonpolar 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 0.5e(-) from the LaAlO3 film into the LaAlO3/SrTiO3 interface is expected. Here we show that in conducting samples (≥ 4 unit cells of LaAlO3) there is indeed a ~0.5e(-) 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 (≤ 3 unit cells of LaAlO3) a redistribution of charges within the polar LaAlO3 sublayers (from AlO2 to LaO) as large as ~0.5e(-) 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.
SrTiO-based heterointerfaces support quasi-two-dimensional (2D) electron systems that are analogous to III-V semiconductor heterostructures, but also possess superconducting, magnetic, spintronic, ferroelectric, and ferroelastic degrees of freedom. Despite these rich properties, the relatively low mobilities of 2D complex-oxide interfaces appear to preclude ballistic transport in 1D. Here we show that the 2D LaAlO/SrTiO interface can support quantized ballistic transport of electrons and (nonsuperconducting) electron pairs within quasi-1D structures that are created using a well-established conductive atomic-force microscope (c-AFM) lithography technique. The nature of transport ranges from truly single-mode (1D) to three-dimensional (3D), depending on the applied magnetic field and gate voltage. Quantization of the lowest e/ h plateau indicate a ballistic mean-free path l ∼ 20 μm, more than 2 orders of magnitude larger than for 2D LaAlO/SrTiO heterostructures. Nonsuperconducting electron pairs are found to be stable in magnetic fields as high as B = 11 T and propagate ballistically with conductance quantized at 2 e/ h. Theories of one-dimensional (1D) transport of interacting electron systems depend crucially on the sign of the electron-electron interaction, which may help explain the highly ballistic transport behavior. The 1D geometry yields new insights into the electronic structure of the LaAlO/SrTiO system and offers a new platform for the study of strongly interacting 1D electronic systems.
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