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تسجيل مستخدم جديدNature of electrons from oxygen vacancies and polar catastrophe at LaAlO3/SrTiO3 interfaces
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The relative significance of quantum conductivity correction and magnetic nature of electrons in understanding the intriguing low-temperature resistivity minimum and negative magnetoresistance of the two-dimensional electron gas at LaAlO3/SrTiO3 interfaces has been a long outstanding issue since its discovery. Here we report a comparative magnetotransport study on amorphous and oxygen-annealed crystalline LaAlO3/SrTiO3 heterostructures at a relatively high-temperature range, where the orbital scattering is largely suppressed by thermal fluctuations. Despite of a predominantly negative out-of-plane magnetoresistance effect for both, the magnetotransport is isotropic for amorphous LaAlO3/SrTiO3 while strongly anisotropic and well falls into a two-dimensional quantum correction frame for annealed crystalline LaAlO3/SrTiO3. These results clearly indicate that a large portion of electrons from oxygen vacancies are localized at low temperatures, serving as magnetic centers, while the electrons from the polar field are only weakly localized due to constructive interference between time-reversed electron paths in the clean limit and no signature of magnetic nature is visible.
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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 term
inations 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.
We formulate a model for magnetic and superconducting ordering at LaAlO3/SrTiO3 interfaces containing both localized magnetic moments and itinerant electrons. Though these both originate in Ti 3d orbitals, the former may be due to electrons more tigh
tly-bound to the interface while the latter are extended over several layers. Only the latter contribute significantly to metallic conduction and superconductivity. In our model, the interplay between the two types of electrons, which is argued to be ferromagnetic, combined with strong spin-orbit coupling of the itinerant electrons, leads to magnetic ordering. Furthermore, we propose a model for interfacial superconductivity, consisting of random superconducting grains in the bulk STO driven, via coupling to the interface conduction band, towards long-ranged or quasi-long-ranged order. Most interestingly, the magnetic order and strong spin orbit coupling can lead in this manner to unconventional interfacial superconductivity, yielding a possible realization of Majorana physics.
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 overl
ayers 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.
The so-called polar catastrophe, a sudden electronic reconstruction taking place to compensate for the interfacial ionic polar discontinuity, is currently considered as a likely factor to explain the surprising conductivity of the interface between t
he insulators LaAlO3 and SrTiO3. We applied optical second harmonic generation, a technique that a priori can detect both mobile and localized interfacial electrons, to investigating the electronic polar reconstructions taking place at the interface. As the LaAlO3 film thickness is increased, we identify two abrupt electronic rearrangements: the first takes place at a thickness of 3 unit cells, in the insulating state; the second occurs at a thickness of 4-6 unit cells, i.e., just above the threshold for which the samples become conducting. Two possible physical scenarios behind these observations are proposed. The first is based on an electronic transfer into localized electronic states at the interface that acts as a precursor of the conductivity onset. In the second scenario, the signal variations are attributed to the strong ionic relaxations taking place in the LaAlO3 layer.
Electronic phase separation is crucial for the fascinating macroscopic properties of the LaAlO3/SrTiO3 (LAO/STO) paradigm oxide interface, including the coexistence of superconductivity and ferromagnetism. We investigate this phenomenon using angle-r
esolved photoelectron spectroscopy (ARPES) in the soft-X-ray energy range, where the enhanced probing depth combined with resonant photoexcitation allow access to fundamental electronic structure characteristics (momentum-resolved spectral function, dispersions and ordering of energy bands, Fermi surface) of buried interfaces. Our experiment uses X-ray irradiation of the LAO/STO interface to tune its oxygen deficiency, building up a dichotomic system where mobile weakly correlated Ti t2g-electrons co-exist with localized strongly correlated Ti eg-ones. The ARPES spectra dynamics under X-ray irradiation shows a gradual intensity increase under constant Luttinger count of the Fermi surface. This fact identifies electronic phase separation (EPS) where the mobile electrons accumulate in conducting puddles with fixed electronic structure embedded in an insulating host phase, and allows us to estimate the lateral fraction of these puddles. We discuss the physics of EPS invoking a theoretical picture of oxygen-vacancy clustering, promoted by the magnetism of the localized Ti eg-electrons, and repelling of the mobile t2g-electrons from these clusters. Our results on the irradiation-tuned EPS elucidate the intrinsic one taking place at the stoichiometric LAO/STO interfaces.
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