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Register a new userIntrinsic origin of the two-dimensional electron gas at polar oxide interfaces
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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.
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The discovery of two-dimensional electron gas (2DEG) at well-defined interfaces between insulating complex oxides provides the opportunity for a new generation of all-oxide electronics. Particularly, the 2DEG at the interface between two perovskite insulators represented by the formula of ABO3, such as LaAlO3 and SrTiO3, has attracted significant attention. In recent years, progresses have been made to decipher the puzzle of the origin of interface conduction, to design new types of oxide interfaces, and to improve the interfacial carrier mobility significantly. These achievements open the door to explore fundamental as well as applied physics of complex oxides. Here, we review our recent experimental work on metallic and insulating interfaces controlled by interfacial redox reactions in SrTiO3-based heterostructures. Due to the presence of oxygen-vacancies at the SrTiO3 surface, metallic conduction can be created at room temperature in perovskite-type interfaces when the overlayer oxide ABO3 involves Al, Ti, Zr, or Hf elements at the B-sites. Furthermore, relying on interface-stabilized oxygen vacancies, we have created a new type of 2DEG at the heterointerface between SrTiO3 and a spinel {gamma}-Al2O3 epitaxial film with compatible oxygen ions sublattices. The spinel/perovskite oxide 2DEG exhibits an electron mobility exceeding 100,000 cm2V-1s-1, more than one order of magnitude higher than those of hitherto investigated perovskite-type interfaces. Our findings pave the way for design of high-mobility all-oxide electronic devices and open a route towards studies of mesoscopic physics with complex oxides.
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.
Polar discontinuities and redox reactions provide alternative paths to create two-dimensional electron liquids (2DELs) at oxide interfaces. Herein, we report high mobility 2DELs at interfaces involving SrTiO3 (STO) achieved using polar La7/8Sr1/8MnO3 (LSMO) buffer layers to manipulate both polarities and redox reactions from disordered overlayers grown at room temperature. Using resonant x-ray reflectometry experiments, we quantify redox reactions from oxide overlayers on STO as well as polarity induced electronic reconstruction at epitaxial LSMO/STO interfaces. The analysis reveals how these effects can be combined in a STO/LSMO/disordered film trilayer system to yield high mobility modulation doped 2DELs, where the buffer layer undergoes a partial transformation from perovskite to brownmillerite structure. This uncovered interplay between polar discontinuities and redox reactions via buffer layers provides a new approach for the design of functional oxide interfaces.
Well-controlled sub-unit-cell layer-by-layer epitaxial growth of spinel alumina is achieved at room temperature on the TiO2-terminated SrTiO3 single crystalline substrate. By tailoring the interface redox reaction, two-dimensional electron gases with mobilities exceeding 3000 cm2V-1s-1 are achieved at this novel oxide interface.
A modulation-doping approach to control the carrier density of the high-density electron gas at a prototype polar/non-polar oxide interface is presented. It is shown that the carrier density of the electron gas at a GdTiO3/SrTiO3 interface can be reduced by up to 20% from its maximum value (~ 3x10^14 cm^-2) by alloying the GdTiO3 layer with Sr. The Seebeck coefficient of the two-dimensional electron gas increases concurrently with the decrease in its carrier density. The experimental results provide insight into the origin of charge carriers at oxide interfaces exhibiting a polar discontinuity.
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