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Yunzhong Chen

Publications and source records attributed to Yunzhong Chen.

16 recordsLinked to original sources

Light-Induced Giant Enhancement of the Nonlinear Hall Effect in Two-Dimensional Electron Gases at KTaO3 (111) Interfaces

The nonlinear Hall effect (NLHE), an emergent phenomenon in noncentrosymmetric systems, enables the generation of a transverse voltage without an external magnetic field through a second-order electrical response. However, achieving a sizable NLHE signal remains a critical challenge for its application in frequency-doubling and rectifying devices. Here, we report a light-induced giant enhancement of the NLHE in the two-dimensional electron gas (2DEG) at the CaZrO3/KTaO3 (111) interface. Under light illumination, the second harmonic Hall voltage (V2ω y) increases substantially and undergoes a sign reversal. Correspondingly,the second-order transverse conductivity increases by nearly five orders of magnitude, reaching 2.4 um V-1 omega-1, while also reversing its sign. Scaling analysis indicates that skew scattering is the dominant mechanism underlying the NLHE and is highly tunable via optical gating. Photoexcitation pumps electrons from in-gap states into the higher-lying Ta 5d conduction band, generating high-mobility photocarriers that significantly increase the cubic transport scattering time, thereby driving a dramatic enhancement of σ(2) yxx. First-principles calculations further reveal that the Berry curvature distribution on the Fermi surface strongly depends on band filling. As the Fermi level approaches a band crossing in the Ta 5d subband near the M point, the Berry curvature triple undergoes a sign change, accounting for the experimentally observed sign reversal of the nonlinear Hall response. Our work offers a new strategy to optically boost and tune the nonlinear Hall effect in oxide 2DEG systems, paving the way for applications in light-controlled rectification and nonlinear electronic devices.

cond-mat.mes-hall

Metal-organic Pulsed Laser Deposition for Complex Oxide Heterostructures

Point defects in complex oxide thin films play a critical role in determining material properties but remain challenging to control with precision. This study introduces metal-organic pulsed laser deposition (MOPLD) as a novel synthesis technique for the precise manipulation of these defects, using LaAlO3/SrTiO3 (LAO/STO) as a model system. By employing titanium tetraisopropoxide (TTIP) as the titanium precursor, MOPLD achieves refined stoichiometric control in STO layers while preserving their structural integrity, as confirmed by X-ray diffraction and Raman spectroscopy. Depth-resolved cathodoluminescence spectroscopy and density functional theory calculations reveal that increasing TTIP flux during STO growth enhances the [TiSr]/[VSr] ratio and reduces the [VO] concentration. These defect modifications lead to a significant improvement in the low-temperature mobility of the two-dimensional electron gas at the LAO/STO interface, evidenced by distinct Shubnikov-de Haas oscillations. This work underscores the potential of MOPLD to advance defect engineering in complex oxide heterostructures, opening new avenues for quantum material research.

cond-mat.mtrl-sci

Ferromagnetism in LaFeO3/LaNiO3 Superlattices with High Curie Temperature

Interfacing complex oxides in atomically engineered layered structures can give rise to a wealth of exceptional electronic and magnetic properties that surpass those of the individual building blocks. Herein, we demonstrate a ferromagnetic spin order with a high Curie temperature of 608 K in superlattices consisting of otherwise paramagnetic perovskite LaNiO3 (LNO) and antiferromagnetic LaFeO3 (LFO). The extraordinary ferromagnetism likely results from the covalent exchange due to interfacial charge transfer from Fe to Ni cations. By deliberately controlling the thickness of the LNO sublayers thus the amount of charge transfer, a robust ferromagnetism of 4 uB is realized for a stacking periodicity consisting of one single unit cell of both LNO and LFO, an emergent double perovskite phase of La2FeNiO6 with B-site layered ordering configurations. The ferromagnetic LFO/LNO superlattices offer great potential for the search of emergent magnetodielectric and/or multiferroic properties as well as applications in spintronics and electrocatalysts.

cond-mat.mtrl-sci

Band-Order Anomaly at the γ-Al2O3/SrTiO3 Interface Drives the Electron-Mobility Boost

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 γ-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 γ-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 γ-Al2O3 and perovskite SrTiO3. The band-order engineering exploiting the fundamental symmetry properties emerges as another route to boost the performance of oxide devices.

cond-mat.mtrl-sci

Strain induced stabilization of a static Jahn-Teller distortion in the O$^*$-phase of La$_{7/8}$Sr$_{1/8}$MnO$_3$

At room temperature, bulk La$_{7/8}$Sr$_{1/8}$MnO$_3$ is in the dynamic Jahn--Teller O$^*$ phase, but undergoes a transition to a static, magnetically ordered Jahn--Teller phase at lower temperatures. Here we study a $6$ unit cells thin film of this compound grown on SrTiO$_3$, resulting in small compressive strain due to a lattice mismatch of $\lesssim 0.2\%$. We combine X-ray absorption spectroscopy with multiplet ligand field theory to study the local electronic and magnetic properties of Mn in the film. We determine the Mn $d_{3z^2-r^2}$ orbital to be $0.13\;\text{eV}$ lower in energy than the $d_{x^2-y^2}$, which is a disproportionately large splitting given the small degree of compressive strain. We interpret this as resulting from the strain providing a preferential orientation for the MnO$_6$ octahedra, which are strongly susceptible to such a deformation in the vicinity of the phase transition. Hence, they collectively elongate along the $c$ axis into a static Jahn--Teller arrangement. Furthermore, we demonstrate the strongly covalent character of La$_{7/8}$Sr$_{1/8}$MnO$_3$, with a contribution of nearly $50\%$ of the one-ligand-hole configuration $d^{5} \underline{L}^1$ to the ground state wavefunction. Finally, we find the system to be in a high-spin configuration, with the projection of the local magnetic moment on the quantization axis being about $3.7\;μ_{\text{B}}/\text{Mn}$. We show, however, that the system is close to a high-spin--low-spin transition, which might be triggered by crystal field effects.

cond-mat.str-el

Gate-tunable Rashba spin-orbit coupling and spin polarization at diluted oxide interfaces

Diluted oxide interface of LaAl1-xMnxO/SrTiO3 (LAMO/STO) provides a new way of tuning the ground states of the interface between the two band insulators of LAO and STO from metallic/superconducting to highly insulating. Increasing the Mn doping level (x) leads to a delicate control of the carrier density as well as a raise in the electron mobility and spin polarization. Herein, we demonstrate a tunable Rashba spin-orbit coupling (SOC) and spin polarization of LAMO/STO (0.2 <= x <= 0.3) by applying a back gate. The presence of SOC causes the splitting of energy band into two branches by a spin splitting energy. The maximum spin splitting energy depends on the Mn doping and decreases with the increasing Mn content and then vanishes at x = 0.3. The carrier density dependence of the spin splitting energy for different compositions shows a dome-shaped behavior with a maximum at different normalized carrier density. These findings have not yet been observed in LAO/STO interfaces. A fully back-gate-tunable spin-polarized 2DEL is observed at the interface with x = 0.3 where only dxy orbits are populated (5.3E12 cm-2 <= ns <= 1.0E13 cm-2). The present results shed light on unexplored territory in SOC at STO-base oxide heterostructures and make LAMO/STO an intriguing platform for spin-related phenomena in 3d-electron systems.

cond-mat.str-el

On the emergence of conductivity at SrTiO3-based oxide interfaces -- an in-situ study

Heterostructures and crystal interfaces play a major role in state-of-the-art semiconductor devices and play a central role in the field of oxide electronics. In oxides the link between the microscopic properties of the interfaces and bulk properties of the resulting heterostructures challenge our fundamental understanding. Insights on the early growth stage of interfaces and its influence on resulting physical properties are scarce -- typically the information is inferred from post growth characterization. Here, we report on real time measurements of the transport properties of SrTiO3-based heterostructures while the crystal heterostructure is forming. Surprisingly, we detect a conducting interface already at the initial growth stage, much earlier than the well-established critical thickness limit for observing conductivity ex-situ after sample growth. We investigate how the conductivity depends on various physical processes occurring during pulsed laser depositions, including light illumination, particle bombardment by the plasma plume, interactions with the atmosphere and oxygen migration from SrTiO3 to the thin films of varying compositions. Using this approach, we propose a new design tool to control the electrical properties of interfaces in real time during their formation.

cond-mat.mtrl-sci

Towards Photoferroic Materials by Design: Recent Progresses and Perspective

The use of photoferroic materials that combine ferroelectric and light harvesting properties in a photovoltaic device is a promising route to significantly improve the efficiency of solar cells. These materials do not require the formation of a p-n junction and can produce photovoltages well above the value of the band gap, because of the spontaneous intrinsic polarization and the formation of domain walls. In this perspective, we discuss the recent experimental progresses and challenges for the synthesis of these materials and the theoretical discovery of novel photoferroic materials using a high-throughput approach.

cond-mat.mtrl-sci

Diluted Oxide Interfaces with Tunable Ground States

The metallic interface between two oxide insulators, such as LaAlO3/SrTiO3 (LAO/STO), provides new opportunities for electronics and spintronics. However, due to the presence of multiple orbital populations, tailoring the interfacial properties such as the ground state and metal-insulator transitions remains challenging. Here, we report an unforeseen tunability of the phase diagram of LAO/STO by alloying LAO with a ferromagnetic LaMnO3 insulator without forming lattice disorder and at the same time without changing the polarity of the system. By increasing the Mn-doping level, x, of LaAl1-xMnxO3/STO, the interface undergoes a Lifshitz transition at x = 0.225 across a critical carrier density of nc= 2.8E13 cm-2, where a peak TSC =255 mK of superconducting transition temperature is observed. Moreover, the LaAl1-xMnxO3 turns ferromagnetic at x >=0.25. Remarkably, at x = 0.3, where the metallic interface is populated by only dxy electrons and just before it becomes insulating, we achieve reproducibly a same device with both signatures of superconductivity and clear anomalous Hall effect. This provides a unique and effective way to tailor oxide interfaces for designing on-demand electronic and spintronic devices.

cond-mat.mtrl-sci

Direct demonstration of the emergent magnetism resulting from the multivalence Mn in a LaMnO3 epitaxial thin film system

Atomically engineered oxide heterostructures provide a fertile ground for creating novel states. For example, a two-dimensional electron gas at the interface between two oxide insulators, giant thermoelectric Seebeck coefficient, emergent ferromagnetism from otherwise nonmagnetic components, and colossal ionic conductivity. Extensive research efforts reveal that oxygen deficiency or lattice strain play an important role in determining these unexpected properties. Herein, by studying the abrupt presence of robust ferromagnetism (up to 1.5 uB/Mn) in LaMnO3-based heterostructures, we find the multivalence states of Mn that play a decisive role in the emergence of ferromagnetism in the otherwise antiferromagnetic LaMnO3 thin films. Combining spatially resolved electron energy-loss spectroscopy, X-ray absorption spectroscopy and X-ray magnetic circular dichroism techniques, we determine unambiguously that the ferromagnetism results from a conventional Mn3+-O-Mn4+ double-exchange mechanism rather than an interfacial effect. In contrast, the magnetic dead layer of 5 unit cell in proximity to the interface is found to be accompanied with the accumulation of Mn2+ induced by electronic reconstruction. These findings provide a hitherto-unexplored multivalence state of Mn on the emergent magnetism in undoped manganite epitaxial thin films, such as LaMnO3 and BiMnO3, and shed new light on all-oxide spintronic devices.

cond-mat.mtrl-sci

Quantization of Hall Resistance at the Metallic Interface between an Oxide Insulator and SrTiO$_{3}$

The two-dimensional metal forming at the interface between an oxide insulator and SrTiO3 provides new opportunities for oxide electronics. However, the quantum Hall effect, one of the most fascinating effects of electrons confined in two dimensions, remains underexplored at these complex oxide heterointerfaces. Here, we report the experimental observation of quantized Hall resistance in a SrTiO3 heterointerface based on the modulation-doped amorphous-LaAlO$_{3}$/SrTiO$_{3}$ heterostructure, which exhibits both high electron mobility exceeding 10000 cm$^{2}$/Vs and low carrier density on the order of ~10$^{12}$ cm$^{-2}$. Along with unambiguous Shubnikov-de Haas oscillations, the spacing of the quantized Hall resistance suggests that the interface is comprised of a single quantum well with ten parallel conducting two-dimensional subbands. This provides new insight into the electronic structure of conducting oxide interfaces and represents an important step towards designing and understanding advanced oxide devices.

cond-mat.mtrl-sci

Evidence of weak superconductivity at the room-temperature grown LaAlO$_{3}$/SrTiO$_3$ interface

The two-dimensional electron gas at the crystalline LaAlO$_{3}$/SrTiO$_{3}$ (c-LAO/STO) interface has sparked large interest due to its exotic properties including an intriguing gate-tunable superconducting phase. While there is growing evidence of pronounced spatial inhomogeneity in the conductivity at STO-based interfaces, the consequences for superconductivity remain largely unknown. We study interfaces based on amorphous LAO top layers grown at room temperature (a-LAO/STO) and demonstrate a superconducting phase similar to c-LAO/STO, however, with a gate-tunable critical temperature of $460 \, \mathrm{mK}$, higher than any previously reported values for c-LAO/STO. The dependence of the superconducting critical current on temperature, magnetic field and backgate-controlled doping is found to be consistently described by a model of a random array of Josephson-coupled superconducting domains.

cond-mat.mes-hall

Patterning of high mobility electron gases at complex oxide interfaces

Oxide interfaces provide an opportunity for electronics. However, patterning of electron gases at complex oxide interfaces is challenging. In particular, patterning of complex oxides while preserving a high electron mobility remains underexplored and inhibits the study of quantum mechanical effects where extended electron mean free paths are paramount. This letter presents an effective patterning strategy of both the amorphous-LaAlO$_3$/SrTiO$_3$ (a-LAO/STO) and modulation-doped amorphous- LaAlO$_3$/La$_{7/8}$Sr$_{1/8}$MnO$_3$/SrTiO$_3$ (a-LAO/LSM/STO) oxide interfaces. Our patterning is based on selective wet etching of amorphous-LSM (a-LSM) thin films which acts as a hard mask during subsequent depositions. Strikingly, the patterned modulation-doped interface shows electron mobilities up to ~8,700 cm$^2$/Vs at 2 K, which is among the highest reported values for patterned conducting complex oxide interfaces that usually are ~1,000 cm$^2$/Vs at 2 K.

cond-mat.mtrl-sci

Infrared ellipsometry study of the confined electrons in a high-mobility $γ$-Al$_2$O$_3$/SrTiO$_3$ heterostructure

With infrared ellipsometry we studied the response of the confined electrons in a $γ$-Al$_2$O$_3$/SrTiO$_3$ heterostructures in which they originate predominantly from oxygen vacancies. From the analysis of a so-called Berreman mode, that develops near the highest longitudinal optical phonon mode of SrTiO$_3$, we derive the sheet carrier density, ${N_{s}}$, the mobility, $μ$, and also the depth profile of the carrier concentration. Notably, we find that ${N_{s}}$ and the shape of the depth profile are similar as in LaAlO$_3$/SrTiO$_3$ heterostructures for which the itinerant carriers are believed to arise from a polar discontinuity. The main differences concern the higher mobility and a relatively stronger confinement of the electrons in $γ$-Al$_2$O$_3$/SrTiO$_3$

cond-mat.str-el

Creation of high mobility two-dimensional electron gases via strain induced polarization at an otherwise nonpolar complex oxide interface

The discovery of two-dimensional electron gases (2DEGs) in SrTiO3-based heterostructures provides new opportunities for nanoelectronics. Herein, we create a new type of oxide 2DEG by the epitaxial-strain-induced polarization at an otherwise nonpolar perovskite-type interface of CaZrO3/SrTiO3. Remarkably, this heterointerface is atomically sharp, and exhibits a high electron mobility exceeding 60,000 cm2V-1s-1 at low temperatures. The 2DEG carrier density exhibits a critical dependence on the film thickness, in good agreement with the polarization induced 2DEG scheme.

cond-mat.mtrl-sci

Metallic and insulating interfaces of amorphous SrTiO3-based oxide heterostructures

The conductance confined at the interface of complex oxide heterostructures provides new opportunities to explore nanoelectronic as well as nanoionic devices. Herein we show that metallic interfaces can be realized in SrTiO3-based heterostructures with various insulating overlayers of amorphous LaAlO3, SrTiO3 and yttria-stabilized zirconia films. On the other hand, samples of amorphous La7/8Sr1/8MnO3 films on SrTiO3 substrates remain insulating. The interfacial conductivity results from the formation of oxygen vacancies near the interface, suggesting that the redox reactions on the surface of SrTiO3 substrates play an important role.

cond-mat.mtrl-sci