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Register a new userOrigin of interfacial conductivity at complex oxide heterointerfaces: possibility of electron transfer from water chemistry at surface oxygen vacancies
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Variety of conducting heterointerfaces have been made between SrTiO3 substrates and thin capping layers of distinctly different oxide materials that can be classified into polar band insulators (e.g. LaAlO3), polar Mott insulators (e.g. LaTiO3), apparently non-polar band insulators (e.g. {gamma}-Al2O3), and amorphous oxides (e.g. amorphous SrTiO3). A fundamental question to ask is if there is a common mechanism that governs interfacial conductivity in all these heterointerfaces. Here, we examined the conductivity of different kinds of heterointerfaces by annealing in oxygen and surface treatment with water. It was found that the conductivity of all the heterointerfaces show a strong dependence on annealing, and can be universally tuned by surface treatment whose effect is determined by the annealing condition. These observations, together with ambient-pressure X-ray photoelectron spectroscopy measurements, suggest that water chemistry at surface oxygen vacancies is a common mechanism that supplies electrons to the interface.
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Two-dimensional charge carrier accumulation at oxide heterointerfaces presents a paradigm shift for oxide electronics. Like a capacitor, interfacial charge buildup couples to an electric field across the dielectric medium. To prevent the so-called polar catastrophe, several charge screening mechanisms emerge, including polar distortions and interfacial intermixing which reduce the sharpness of the interface. Here, we examine how atomic intermixing at oxide interfaces affect the balance between polar distortions and electric potential across the dielectric medium. We find that intermixing moves the peak charge distribution away from the oxide/oxide interface; thereby changing the direction of polar distortions away from this boundary with minimal effect on the electric field. This opposing electric field and polar distortions is equivalent to the transient phase transition tipping point observed in double well ferroelectrics; resulting in an anomalous dielectric response -- a possible signature of local negative differential capacitance, with implications for designing dissipationless oxide electronics.
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 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.
Perovskite oxide heteroepitaxy receives much attention because of the possibility to com- bine the diverse functionalities of perovskite oxide building blocks. A general boundary con- dition for the epitaxy is the presence of polar discontinuities at heterointerfaces. These polar discontinuities result in reconstructions, often creating new functionalities at the interface. However, for a significant number of materials these reconstructions are unwanted as they alter the intrinsic materials properties at the interface. Therefore, a strategy to eliminate this reconstruction of the polar discontinuity at the interfaces is required. We show that the use of compositional interface engineering can prevent the reconstruction at the La0.67Sr0.33MnO3/SrTiO3 (LSMO/STO) interface. The polar discontinuity at this interface can be removed by the insertion of a single La0.33Sr0.67O layer, resulting in improved interface magnetization and electrical conductivity.
The predictions of the polar catastrophe scenario to explain the occurrence of a metallic interface in heterostructures of the solid solution(LaAlO$_3$)$_{x}$(SrTiO$_3$)$_{1-x}$ (LASTO:x) grown on (001) SrTiO$_3$ were investigated as a function of film thickness and $x$. The films are insulating for the thinnest layers, but above a critical thickness, $t_c$, the interface exhibits a constant finite conductivity which depends in a predictable manner on $x$. It is shown that $t_c$ scales with the strength of the built-in electric field of the polar material, and is immediately understandable in terms of an electronic reconstruction at the nonpolar-polar interface. These results thus conclusively identify the polar-catastrophe model as the intrinsic origin of the doping at this polar oxide interface.
Here we study the electronic properties of cuprate/manganite interfaces. By means of atomic resolution electron microscopy and spectroscopy, we produce a subnanometer scale map of the transition metal oxidation state profile across the interface between the high $T_c$ superconductor YBa$_2$Cu$_3$O$_{7-delta}$ and the colossal magnetoresistance compound (La,Ca)MnO$_3$. A net transfer of electrons from manganite to cuprate with a peculiar non-monotonic charge profile is observed. Model calculations rationalize the profile in terms of the competition between standard charge transfer tendencies (due to band mismatch), strong chemical bonding effects across the interface, and Cu substitution into the Mn lattice, with different characteristic length scales.
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