LaAlO3/SrTiO3 Research Articles

Second-order charge and spin transport in LaO/STO system in the presence of cubic Rashba spin orbit couplings

Under an applied electric field, certain non-centrosymmetric materials with broken time-reversal symmetry may exhibit non-reciprocal transport behavior in which the charge and spin currents contain components that are second order in the electric field. In this study, we investigate the second-order spin accumulation and charge and spin responses in the LaAlO3/SrTiO3 (LaO/STO) system with magnetic dopants under the influence of linear and cubic Rashba spin–orbit coupling (RSOC) terms. We explain the physical origin of the second-order response and perform a symmetry analysis of the first- and second-order responses for different dopant magnetization directions relative to the applied electric field. We then numerically solve the Boltzmann transport equation by extending the approach of Schliemann and Loss (2003 Phys. Rev. B 68 165311) to higher orders in the electric field. We show that the sign of the second-order responses can be switched by varying the magnetization direction of the magnetic dopants or relative strengths of the two cubic RSOC terms and explain these trends by considering the Fermi surfaces of the respective systems. These findings provide insights into the interplay of multiple SOC effects in the LaO/STO system and how the resulting first- and second-order charge and spin responses can be engineered by exploiting the symmetries of the system.

Stoichiometric control of electron mobility and 2D superconductivity at LaAlO3-SrTiO3 interfaces

SrTiO3-based conducting interfaces, which exhibit coexistence of gate-tunable 2D superconductivity and strong Rashba spin-orbit coupling (RSOC), are candidates to host topological superconductive phases. Yet, superconductivity is usually in the dirty limit, which tends to suppress nonconventional pairing and therefore challenges these expectations. Here we report on LaAlO3/SrTiO3 (LAO/STO) interfaces with large mobility and mean free paths comparable to the superconducting coherence length, approaching the clean limit for superconductivity. We further show that the carrier density, mobility, and formation of the superconducting condensate are controlled by the fine-tuning of La/Al chemical ratio in the LAO film. We find a region in the superconducting phase diagram where the critical temperature is not suppressed below the Lifshitz transition, at odds with previous experimental investigations. These findings point out the relevance of achieving a clean-limit regime to enhance the observation of unconventional pairing mechanisms in these systems.

Optoelectronic Synapse Based on 2D Electron Gas in Stoichiometry-Controlled Oxide Heterostructures.

Emulating synaptic functionalities in optoelectronic devices is significant in developing artificial visual-perception systems and neuromorphic photonic computing. Persistent photoconductivity (PPC) in metal oxides provides a facile way to realize the optoelectronic synaptic devices, but the PPC performance is often limited due to the oxygen vacancy defects that release excess conduction electrons without external stimuli. Herein, a high-performance optoelectronic synapse based on the stoichiometry-controlled LaAlO3/SrTiO3 (LAO/STO) heterostructure is developed. By increasing La/Al ratio up to 1.057:1, the PPC is effectively enhanced but suppressed the background conductivity at the LAO/STO interface, achieving strong synaptic behaviors. The spectral noise analyses reveal that the synaptic behaviors are attributed to the cation-related point defects and their charge compensation mechanism near the LAO/STO interface. The short-term and long-term plasticity is demonstrated, including the paired-pulse facilitation, in the La-rich LAO/STO device upon exposure to UV light pulses. As proof of concepts, two essential synaptic functionalities, the pulse-number-dependent plasticity and the self-noise cancellation, are emulated using the 5×5 array of La-rich LAO/STO synapses. Beyond the typical oxygen deficiency control, the results show how harnessing the cation stoichiometry can be used to design oxide heterostructures for advanced optoelectronic synapses and neuromorphic applications.

LaAlO3/SrTiO3 Heterointerface: 20 Years and Beyond

AbstractThis year marks the 20th anniversary of the discovery of LaAlO3/SrTiO3 (LAO/STO) oxide heterointerfaces. Since their discovery, transition metal oxide (TMO) interfaces have emerged as a fascinating and fast‐growing area of research, offering a variety of unique and exotic physical properties which has provided a strong impetus for the rapid advances and actualization of oxide electronics. This review revisits the fundamental mechanisms accounting for the two‐dimensional (2D) conducting interfaces, and how new models proposed to better account for the unique interfacial effects. Recent breakthroughs in the theoretical and experimental domains of oxide interfaces are also discussed including the detection and investigation of 2D quasiparticle. Moving beyond the well‐known LAO/STO interface, this review delves into other systems where unconventional interfacial superconductivity, interfacial magnetism, and spin polarization are dealt with in greater detail. In terms of device applications, this review proceeds with a treatment on the recent developments in domains including field effect transistors and freestanding heterostructure membranes. By emphasizing the opportunities and challenges of integrating oxide interfaces with existing technologies, the review will end off with an outlook projecting the progress and the trajectory of this research domain in the years to come.

Plasma-Induced 2D Electron Transport at Hetero-Phase Titanium Oxide Interface.

Interfaces of metal oxide heterojunctions display a variety of intriguing physical properties that enable novel applications in spintronics, quantum information, neuromorphic computing, and high-temperature superconductivity. One such LaAlO3 /SrTiO3 (LAO/STO) heterojunction hosts a 2D electron liquid (2DEL) presenting remarkable 2D superconductivity and magnetism. However, these remarkable properties emerge only at very low temperatures, while the heterostructure fabrication is challenging even at the laboratory scale, thus impeding practical applications. Here, a novel plasma-enabled fabrication concept is presented to develop the TiO2 /Ti3 O4 hetero-phase bilayer with a 2DEL that exhibits features of a weakly localized Fermi liquid even at room temperature. The hetero-phase bilayer is fabricated by applying a rapid plasma-induced phase transition that transforms a specific portion of anatase TiO2 thin film into vacancy-prone Ti3 O4 in seconds. The underlying mechanism relies on the screening effect of the achieved high-density electron liquid that suppresses the electron-phonon interactions. The achieved "adiabatic" electron transport in the hetero-phase bilayer offers strong potential for low-loss electric or plasmonic circuits and hot electron harvesting and utilization. These findings open new horizons for fabricating diverse multifunctional metal oxide heterostructures as an innovative platform for emerging clean energy, integrated photonics, spintronics, and quantum information technologies.

Conductivity and photo-response of amorphous-LaAlO3/SrTiO3 (001) grown by on-axis radio-frequency magnetron sputtering

LaAlO3/SrTiO3 (LAO/STO) possesses many novel properties. To pursue its application in future electronic devices, studying of its mass production and controllability by external stimuli are indispensable. Here, we fabricate conducting amorphous-LAO/STO (001) (a-LAO/STO) for the first time by on-axis radio-frequency (RF) magnetron sputtering. The properties of sputtered a-LAO/STO dependent strongly on growth parameters, with low electroconductibility but strong photo-response in samples sputtered at large target-to-substrate distance and/or under high Ar gas pressure. Using X-ray photoelectron spectroscopy (XPS) to investigate the film's stoichiometry, we find that this is related to Al deficiency (Al/La<1) in a-LAO among these samples. Our work demonstrates that sputtering is a feasible method for controllable, large-scale and low-cost fabrication of oxide interfaces.

Electron pairing and nematicity in LaAlO3/SrTiO3 nanostructures

Strongly correlated electronic systems exhibit a wealth of unconventional behavior stemming from strong electron-electron interactions. The LaAlO3/SrTiO3 (LAO/STO) heterostructure supports rich and varied low-temperature transport characteristics including low-density superconductivity, and electron pairing without superconductivity for which the microscopic origins is still not understood. LAO/STO also exhibits inexplicable signatures of electronic nematicity via nonlinear and anomalous Hall effects. Nanoscale control over the conductivity of the LAO/STO interface enables mesoscopic experiments that can probe these effects and address their microscopic origins. Here we report a direct correlation between electron pairing without superconductivity, anomalous Hall effect and electronic nematicity in quasi-1D ballistic nanoscale LAO/STO Hall crosses. The characteristic magnetic field at which the Hall coefficient changes directly coincides with the depairing of non-superconducting pairs showing a strong correlation between the two distinct phenomena. Angle-dependent Hall measurements further reveal an onset of electronic nematicity that again coincides with the electron pairing transition, unveiling a rotational symmetry breaking due to the transition from paired to unpaired phases at the interface. The results presented here highlights the influence of preformed electron pairs on the transport properties of LAO/STO and provide evidence of the elusive pairing “glue” that gives rise to electron pairing in SrTiO3-based systems.

Reversible Photomodulation of Two-Dimensional Electron Gas in LaAlO3/SrTiO3 Heterostructures.

Long-lived photoinduced conductance changes in LaAlO3/SrTiO3 (LAO/STO) heterostructures enable their use in optoelectronic memory applications. However, it remains challenging to quench the persistent photoconductivity (PPC) instantly and reproducibly, which limits the reversible optoelectronic switching. Herein, we demonstrate a reversible photomodulation of two-dimensional electron gas (2DEG) in LAO/STO heterostructures with high reproducibility. By irradiating UV pulses, the 2DEG at the LAO/STO interface is gradually transformed to the PPC state. Notably, the PPC can be completely removed by water treatment when two key requirements are met: (1) the moderate oxygen deficiency in STO and (2) the minimal band edge fluctuation at the interface. Through our X-ray photoelectron spectroscopy and electrical noise analysis, we reveal that the reproducible change in the conductivity of 2DEG is directly attributed to the surface-driven electron relaxation in the STO. Our results provide a stepping-stone toward developing optically tunable memristive devices based on oxide 2DEG systems.

Nonlinear optical phonon spectroscopy revealing polaronic signatures of the LaAlO3/SrTiO3 interface.

We report the direct observation of lattice phonons confined at LaAlO3/SrTiO3 (LAO/STO) interfaces and STO surfaces using the sum-frequency phonon spectroscopy. This interface-specific nonlinear optical technique unveiled phonon modes localized within a few monolayers at the interface, with inherent sensitivity to the coupling between lattice and charge degrees of freedom. Spectral evolution across the insulator-to-metal transition at LAO/STO interface revealed an electronic reconstruction at the subcritical LAO thickness, as well as strong polaronic signatures upon formation of the two-dimensional electron gas. We further discovered a characteristic lattice mode from interfacial oxygen vacancies, enabling us to probe such important structural defects in situ. Our study provides a unique perspective on many-body interactions at the correlated oxide interfaces.

A comparative study of superconductivity at LaAlO3/SrTiO3 and BaTiO3/LaAlO3/SrTiO3 heterointerfaces

Lead-free BaTiO3 (BTO) film was fabricated by pulsed laser deposition on LaAlO3/SrTiO3 (LAO/STO) heterostructure in oxygen pressure of 2 × 10−3 Pa, which is experimentally required for ensuring the two-dimensional electron gas at LAO/STO heterointerface. Modulation of back-gate voltage on the superconductivity of LAO/STO and BTO/LAO/STO heterointerfaces was studied. The results indicate that the back-gate voltage can adjust the resistance at high temperatures around 300 mK, while it does not modulate the superconducting transition temperature of LAO/STO, which occurs at 160 mK. As for BTO/LAO/STO, it still shows a superconducting transition-like behavior at 110 mK. However, when a negative back-gate voltage is applied, the superconducting transition-like behavior disappears, and after removing the voltage, unlike what was observed for LAO/STO, the superconductivity cannot be recovered. Given this, some underlying mechanisms are proposed.

Collective Control of Potential-Constrained Oxygen Vacancies in Oxide Heterostructures for Gradual Resistive Switching.

Filamentary resistive switching in oxides is one of the key strategies for developing next-generation non-volatile memory devices. However, despite numerous advantages, their practical applications in neuromorphic computing are still limited due to non-uniform and indeterministic switching behavior. Given the inherent stochasticity of point defect migration, the pursuit of reliable switching likely demands an innovative approach. Herein, a collective control of oxygen vacancies is introduced in LaAlO3 /SrTiO3 (LAO/STO) heterostructures to achieve reliable and gradual resistive switching. By exploiting an electrostatic potential constraint in ultrathin LAO/STO heterostructures, the formation of conducting filaments is suppressed, but instead precisely control the concentration of oxygen vacancies. Since the conductance of the LAO/STO device is governed by the ensemble concentration of oxygen vacancies, not their individual probabilistic migrations, the resistive switching is more uniform and deterministic compared to conventional filamentary devices. It provides direct evidence for the collective control of oxygen vacancies by spectral noise analysis and modeling by Monte-Carlo simulation. As a proof of concept, the significantly-improved analog switching performance of the filament-free LAO/STO devices is demonstrated, revealing potential for neuromorphic applications. The results establish an approach to store information by point defect concentration, akin to biological ionic channels, for enhancing switching characteristics of oxide materials.

Semiclassical spin transport in LaO/STO system in the presence of multiple Rashba spin-orbit couplings

The interaction between linear and cubic spin–orbit couplings with magnetic moments and mobile spin-polarized carriers in the LaAlO3/SrTiO3 (LaO/STO) system provides new avenues for spin transport applications. We study the interplay between linear and cubic Rashba spin orbit coupling (RSOC) on in-plane magnetic moments in the LaO/STO system using the Boltzmann transport theory based on the relaxation time approximation (RTA) and the more refined Schliemann-Loss (SL) delta-potential scattering model. In general, both methods yield a linear (quadratic) relationship in the spin accumulation (spin current) when one of the three RSOC strengths is varied and the other two fixed. The simultaneous presence of multiple types of RSOC with distinct angular dependencies facilitates the breaking of the k-space symmetry of the Fermi surface, thus ensuring a finite spin accumulation upon integration over the entire Fermi surface. While the oft-used RTA method is sufficiently accurate for spin accumulation calculations, the more refined SL model is required for spin current calculations because the RTA method neglects the anisotropy of the Fermi contour arising from the cubic RSOC terms. Based on the refined SL model and under optimal tuning of the RSOC parameters, the spin charge conversion in LaO/STO is predicted to reach a remarkable efficiency of 30%.

Probing oxygen vacancy distribution in oxide heterostructures by deep Learning-based spectral analysis of current noise

Exploiting oxygen vacancies has emerged as a versatile tool to tune the electronic and optoelectronic properties of complex oxide heterostructures. For the precise manipulation of the oxygen vacancies, the capability of directly probing the defect distribution in nanoscale is essential, but still lacking. Here we estimate the spatial distribution of oxygen vacancies in LaAlO3/SrTiO3 (LAO/STO) heterostructures by deep learning-based spectral analysis of current noise. The Monte-Carlo simulation and the specifically-designed deep learning model allow us to evaluate the defect distribution from current noise signals, measured through two-dimensional electron gas at the LAO/STO interface. We show that the oxygen vacancies are uniformly distributed over ∼ 100 nm from the interface in the as-grown LAO/STO heterostructure, while they can be migrated and confined to the interface within ∼ 14 nm by a vertical electric field at room temperature. These results introduce a powerful strategy to quantitatively probe the spatial distribution of point defects in oxide heterostructures with nm-scale precision.

A Two-Dimensional Superconducting Electron Gas in Freestanding LaAlO3/SrTiO3 Micromembranes

Freestanding oxide membranes constitute an intriguing material platform for new functionalities and allow integration of oxide electronics with technologically important platforms such as silicon. Sambri et al. recently reported a method to fabricate freestanding LaAlO3/SrTiO3 (LAO/STO) membranes by spalling of strained heterostructures. Here, we first develop a scheme for the high-yield fabrication of membrane devices on silicon. Second, we show that the membranes exhibit metallic conductivity and a superconducting phase below ∼200 mK. Using anisotropic magnetotransport we extract the superconducting phase coherence length ξ ≈ 36-80 nm and establish an upper bound on the thickness of the superconducting electron gas d ≈ 17-33 nm, thus confirming its two-dimensional character. Finally, we show that the critical current can be modulated using a silicon-based backgate. The ability to form superconducting nanostructures of LAO/STO membranes, with electronic properties similar to those of the bulk counterpart, opens opportunities for integrating oxide nanoelectronics with silicon-based architectures.

Light-enhanced gating effect at the interface of oxide heterostructure

In semiconducting materials, electrostatic gating and light illumination are widely used stimuli to tune the electronic properties of the system. Here, we show a significant enhancement of photoresponse at the conducting interface of LaVO3–SrTiO3 under the simultaneous application of light and negative gate bias voltage, in comparison to their individual application. On the other hand, the illuminated LaVO3-SrTiO3 interface does not show any enhancement, when a positive gate bias voltage is applied. Our x-ray diffractometer, Raman spectroscopy and photoemission measurements show that unlike the LaAlO3–SrTiO3 interface, migration of oxygen vacancies may not be the prime mechanism for the enhanced photoresponse. Rather, we suggest that the photoresponse of our system is intrinsic and this intrinsic mechanism is a complex interplay between band filling, electric field at the interface and modification of conducting channel width.

Robust Electronic Structure of Manganite-Buffered Oxide Interfaces with Extreme Mobility Enhancement.

The electronic structure as well as the mechanism underlying the high-mobility two-dimensional electron gases (2DEGs) at complex oxide interfaces remain elusive. Herein, using soft X-ray angle-resolved photoemission spectroscopy (ARPES), we present the band dispersion of metallic states at buffered LaAlO3/SrTiO3 (LAO/STO) heterointerfaces where a single-unit-cell LaMnO3 (LMO) spacer not only enhances the electron mobility but also renders the electronic structure robust toward X-ray radiation. By tracing the evolution of band dispersion, orbital occupation, and electron-phonon interaction of the interfacial 2DEG, we find unambiguous evidence that the insertion of the LMO buffer strongly suppresses both the formation of oxygen vacancies as well as the electron-phonon interaction on the STO side. The latter effect makes the buffered sample different from any other STO-based interfaces and may explain the maximum mobility enhancement achieved at buffered oxide interfaces.

A Laser‐ARPES View of the 2D Electron Systems at LaAlO3/SrTiO3 and Al/SrTiO3 Interfaces

AbstractThe electronic structure of the two‐dimensional electron system (2DES) found at the Al/SrTiO3 (Al/STO) and LaAlO3/SrTiO3 (LAO/STO) interfaces is measured by means of laser angle resolved photoemission spectroscopy, taking advantage of the large photoelectron escape depth at low photon energy to probe these buried interfaces. The possibility of tuning the electronic density in Al/STO by varying the Al layer thickness is demonstrated, and it is shown that the electronic structure evolution is well described by self‐consistent tight binding supercell calculations, but differs qualitatively from a rigid band shift model. It is shown that both 2DES are strongly coupled to longitudinal optical phonons, in agreement with previous reports of a polaronic ground state in similar STO based 2DESs. Tuning the electronic density in Al/STO to match that of LAO/STO and comparing both systems, it is estimated that the intrinsic LAO/STO 2DES has a bare band width of ≈60 meV and a carrier density of ≈6 × 1013 cm−2.

Electronic reconstruction at the polar (111)-oriented oxide interface

Atomically flat (111) interfaces between insulating perovskite oxides provide a landscape for new electronic phenomena. For example, the graphene-like coordination between interfacial metallic ion layer pairs can lead to topologically protected states [Xiao et al., Nat. Commun. 2, 596 (2011) and A. Rüegg and G. A. Fiete, Phys. Rev. B 84, 201103 (2011)]. The metallic ion/metal oxide bilayers that comprise the unit cell of the perovskite (111) heterostructures require the interface to be polar, generating an intrinsic polar discontinuity [Chakhalian et al., Nat. Mater. 11, 92 (2012)]. Here, we investigate epitaxial heterostructures of (111)-oriented LaAlO3/SrTiO3 (LAO/STO). We find that during heterostructure growth, the LAO overlayer eliminates the structural reconstruction of the STO (111) surface with an electronic reconstruction, which determines the properties of the resulting two-dimensional conducting gas. This is confirmed by transport measurements, direct determination of the structure and atomic charge from coherent Bragg rod analysis, and theoretical calculations of electronic and structural characteristics. Interfacial behaviors of the kind discussed here may lead to new growth control parameters useful for electronic devices.

Dimensionality of mobile electrons at x-ray-irradiated LaAlO3/SrTiO3 interfaces

Electronic structure of LaAlO3/SrTiO3 (LAO/STO) samples, grown at low oxygen pressure and post-annealed ex situ, was investigated by soft-x-ray ARPES focussing on the Fermi momentum (k F) of the mobile electron system (MES). X-ray irradiation of these samples at temperatures below 100 K creates oxygen vacancies (VOs) injecting Ti t 2g-electrons into the MES. At this temperature the oxygen out-diffusion is suppressed, and the VOs should appear mostly in the top STO layer. The x-ray generated MES demonstrates, however, a pronounced three-dimensional (3D) behavior as evidenced by variations of its experimental k F over different Brillouin zones. Identical to bare STO, this behavior indicates an unexpectedly large extension of the x-ray generated MES into the STO depth. The intrinsic MES in the standard LAO/STO samples annealed in situ, in contrast, demonstrates purely two-dimensional (2D) behaviour. The relevance of our ARPES data analysis is supported by model calculations to compare the intensity vs gradient methods of the k F determination as a function of the energy resolution ratio to the bandwidth. Based on self-interaction-corrected DFT calculations of the MES induced by VOs at the interface and in STO bulk, we discuss possible scenarios of the puzzling 3D-ity. It may involve either a dense ladder of quantum-well states formed in a long-range interfacial potential or, more likely, x-ray-induced bulk metallicity in STO accessed in the ARPES experiment through a short-range interfacial barrier. The mechanism of this metallicity may involve remnant VOs and photoconductivity-induced metallic states in the STO bulk, and even more exotic mechanisms such as x-ray induced formation of Frenkel pairs.

Tunable Rashba spin-orbit coupling and its interplay with multiorbital effect and magnetic ordering at oxide interfaces

The complex oxide heterostructures such as LaAlO3/SrTiO3 (LAO/STO) interface are paradigmatic platforms to explore emerging multi-degrees of freedom coupling and the associated exotic phenomena. In this study, we reveal the effects of multiorbital and magnetic ordering on Rashba spin-orbit coupling (SOC) at the LAO/STO (001) interface. Based on first-principles calculations, we show that the Rashba spin splitting near the conduction band edge can be tuned substantially by the interfacial insulator-metal transition due to the multiorbital effect of the lowest t_2g bands. We further unravel a competition between Rashba SOC and intrinsic magnetism, in which the Rashba SOC induced spin polarization is suppressed by the interfacial magnetic ordering. These results deepen our understanding of intricate electronic and magnetic reconstruction at the perovskite oxide interfaces and shed light on the engineering of oxide heterostructures for all-oxides-based spintronic devices.