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Register a new userBand-Order Anomaly at the {gamma}-Al2O3/SrTiO3 Interface Drives the Electron-Mobility Boost
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Rich functionalities of transition-metal oxides and their interfaces bear an enormous technological potential. Its realization in practical devices requires, however, a significant improvement of yet relatively low electron mobility in oxide materials. Recently, a mobility boost of about two orders of magnitude has been demonstrated at the spinel/perovskite {gamma}-Al2O3/SrTiO3 interface compared to the paradigm perovskite/perovskite LaAlO3/SrTiO3. We explore the fundamental physics behind this phenomenon from direct measurements of the momentum-resolved electronic structure of this interface using resonant soft-X-ray angle-resolved photoemission. We find an anomaly in orbital ordering of the mobile electrons in {gamma}-Al2O3/SrTiO3 which depopulates electron states in the top STO layer. This rearrangement of the mobile electron system pushes the electron density away from the interface that reduces its overlap with the interfacial defects and weakens the electron-phonon interaction, both effects contributing to the mobility boost. A crystal-field analysis shows that the band order alters owing to the symmetry breaking between the spinel {gamma}-Al2O3 and perovskite SrTiO3. The band-order engineering exploiting the fundamental symmetry properties emerges as another route to boost the performance of oxide devices.
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Herein, we reported giant tunability of the physical properties of 2DEGs at the spinel/perovskite interface of {gamma}-Al2O3/SrTiO3 (GAO/STO). By modulating the carrier density thus the band filling with ionic-liquid gating, the system experiences a Lifshitz transition at a critical carrier density of 3E13 cm-2, where a remarkably strong enhancement of Rashba spin-orbit interaction and an emergence of Kondo effect at low temperatures are observed. Moreover, as the carrier concentration depletes with decreasing gating voltage, the electron mobility is enhanced by more than 6 times in magnitude, leading to the observation of clear quantum oscillations. The great tunability of GAO/STO interface by EDLT gating not only shows promise for design of oxide devices with on-demand properties, but also sheds new light on the electronic structure of 2DEG at the non-isostructural spinel/perovskite interface.
The discovery of two-dimensional electron gases (2DEGs) at the heterointerface between two insulating perovskite-type oxides, such as LaAlO3 and SrTiO3, provides opportunities for a new generation of all-oxide electronic and photonic devices. However, significant improvement of the interfacial electron mobility beyond the current value of approximately 1,000 cm2V-1s-1 (at low temperatures), remains a key challenge for fundamental as well as applied research of complex oxides. Here, we present a new type of 2DEG created at the heterointerface between SrTiO3 and a spinel {gamma}-Al2O3 epitaxial film with excellent quality and compatible oxygen ions sublattices. This spinel/perovskite oxide heterointerface exhibits electron mobilities more than one order of magnitude higher than those of perovskite/perovskite oxide interfaces, and demonstrates unambiguous two-dimensional conduction character as revealed by the observation of quantum magnetoresistance oscillations. Furthermore, we find that the spinel/perovskite 2DEG results from interface-stabilized oxygen vacancies and is confined within a layer of 0.9 nm in proximity to the heterointerface. Our findings pave the way for studies of mesoscopic physics with complex oxides and design of high-mobility all-oxide electronic devices.
The two-dimensional electron gas (2DEG) at the non-isostructural interface between spinel gamma-Al2O3 and perovskite SrTiO3 is featured by a record electron mobility among complex oxide interfaces in addition to a high carrier density up to the order of 1E15 cm-2. Herein, we report on the patterning of 2DEG at the gamma-Al2O3/SrTiO3 interface grown at 650 {deg}C by pulsed laser deposition using a hard mask of LaMnO3. The patterned 2DEG exhibits a critical thickness of 2 unit cells of gamma-Al2O3 for the occurrence of interface conductivity, similar to the unpatterned sample. However, its maximum carrier density is found to be approximately 3E13 cm-2, much lower than that of the unpatterned sample (1E15 cm-2). Remarkably, a high electron mobility of approximately 3,600 cm2V-1s-1 was obtained at low temperatures for the patterned 2DEG at a carrier density of 7E12 cm-2, which exhibits clear Shubnikov-de Hass quantum oscillations. The patterned high-mobility 2DEG at the gamma-Al2O3/SrTiO3 interface paves the way for the design and application of spinel/perovskite interfaces for high-mobility all-oxide electronic devices.
The magnetic and electronic nature of the gamma-Al2O3/SrTiO3 spinel/perovskite interface is explored by means of x-ray absorption spectroscopy. Polarized x-ray techniques combined with atomic multiplet calculations reveal localized magnetic moments assigned to Ti3+ at the interface with equivalent size for in- and out-of-plane magnetic field directions. Although magnetic fingerprints are revealed, the Ti3+ magnetism can be explained by a paramagnetic response at low temperature under applied magnetic fields. Modeling the x-ray linear dichroism results in a delta0 = 1.9 eV splitting between the t2g and eg states for the Ti4+ 3d0 orbitals. In addition these results indicate that the lowest energy states have the out-of-plane dxz/dyz symmetry. The isotropic magnetic moment behavior and the lowest energy dxz/dyz states are in contrast to the observations for the two-dimensional electron gas at the perovskite/perovskite interface of LaAlO3/SrTiO3, that exhibits an anisotropic magnetic dxy ground state.
Interplay of spin, charge, orbital and lattice degrees of freedom in oxide heterostructures results in a plethora of fascinating properties, which can be exploited in new generations of electronic devices with enhanced functionalities. The paradigm example is the interface between the two band insulators LaAlO3 and SrTiO3 (LAO/STO) that hosts two-dimensional electron system (2DES). Apart from the mobile charge carriers, this system exhibits a range of intriguing properties such as field effect, superconductivity and ferromagnetism, whose fundamental origins are still debated. Here, we use soft-X-ray angle-resolved photoelectron spectroscopy to penetrate through the LAO overlayer and access charge carriers at the buried interface. The experimental spectral function directly identifies the interface charge carriers as large polarons, emerging from coupling of charge and lattice degrees of freedom, and involving two phonons of different energy and thermal activity. This phenomenon fundamentally limits the carrier mobility and explains its puzzling drop at high temperatures.
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