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Register a new userTuning the two-dimensional electron liquid at oxide interfaces by buffer-layer-engineered redox reactions
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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.
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Using tunneling spectroscopy we have measured the spectral density of states of the mobile, two-dimensional electron system generated at the LaAlO3-SrTiO3 interface. As shown by the density of states the interface electron system differs qualitatively, first, from the electron systems of the materials defining the interface and, second, from the two-dimensional electron gases formed at interfaces between conventional semiconductors.
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.
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.
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.
Modulation-doped oxide two-dimensional electron gas (2DEG) formed at the LaMnO3 (LMO) buffered disorderd-LaAlO3/SrTiO3 (d-LAO/LMO/STO) heterointerface, provides new opportunities for electronics as well as quantum physics. Herein, we studied the dependence of Sr-doping of La1-xSrxMnO3 (LSMO, x=0, 1/8, 1/3, 1/2, and 1) thus the filling of the Mn eg subbands as well as the LSMO polarity on the transport properties of d-LAO/LSMO/STO. Upon increasing the LSMO film thickness from 1 unit cell (uc) to 2 uc, a sharp metal to insulator transition of interface conduction was observed, independent of x. The resultant electron mobility is often higher than 1900 cm2V-1s-1 at 2 K, which increases upon decreasing x. The sheet carrier density, on the other hand, is in the range of 6.9E1012~1.8E1013 cm-2 (0.01~0.03 e/uc) and is largely independent on x for all the metallic d-LAO/LSMO (1 uc)/STO interfaces. These results are consistent with the charge transfer induced modulation doping scheme and clarify that the polarity of the buffer layer plays a trivial role on the modulation doping. The negligible tunability of the carrier density could result from the reduction of LSMO during the deposition of disordered LAO or that the energy levels of Mn 3d electrons at the interface of LSMO/STO are hardly varied even when changing the LSMO composition from LMO to SrMnO3.
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