arXiv subjects

Shiqing Deng

Publications and source records attributed to Shiqing Deng.

9 recordsLinked to original sources

arXiv2026

Multiferroicity in the two-dimensional limit in hexagonal LuFeO3 films

Multiferroic oxides, which combine coupled ferroelectric and magnetic orders, are central to understanding correlated quantum phenomena. Yet, as thickness approaches the two-dimensional (2D) limit, both ferroelectricity and magnetism are conventionally expected to vanish due to depolarization fields and finite-size effects, respectively. Here, we demonstrate that hexagonal LuFeO3 (h-LuFeO3) retains coupled ferroelectricity and magnetism at the 2D limit, with a thickness of just one and a half unit cells. Remarkably, the ferroelectric polarization remains comparable to bulk values at room temperature, while long-range magnetism and magnetoelectric coupling persist at low temperatures. We further show that the K3 phonon mode, which mediates the polarization-magnetism coupling, is stable down to the 2D limit. Our results establish h-LuFeO3 as the first oxide system to exhibit genuine 2D-limit multiferroicity, providing a fundamental breakthrough in the long-standing quest to understand and control coupled ferroic orders at the atomic scale.

cond-mat.mtrl-sci↗

arXiv2026

Nitrogen doping induced metal-insulator transition with iso-symmetric character in rutile VO2

Metal-insulator transitions (MITs) in correlated oxides offer immense potential for next-generation Mottronic devices. However, their integration into practical applications is often hindered by the coupling of MITs with symmetry-lowering structural phase transitions, which limits switching speed and endurance. In this study, we engineered an iso-symmetric MIT on average in epitaxial rutile VO2 thin films via an in-situ nitrogen doping strategy. Nitrogen incorporation effectively suppresses V-V dimerization, enabling an iso-symmetric MIT, while preserving the original crystal symmetry. Furthermore, in-operando time-resolved optical reflectivity measurements revealed a shortened switching time in nitrogen-doped films, highlighting their enhanced performance. Our findings provide critical insights into the underlying mechanisms of MITs and introduce anion doping as a powerful tool for tailoring phase transitions in strongly correlated electron systems. This approach opens new avenues for the development of high-performance electronic and photonic devices.

cond-mat.mtrl-sci↗

arXiv2026

Decoupling effects of the resistive-switching behavior on the polarization reversal in ultrathin ferroelectric Hf0.5Zr0.5O2 films

HfO2-based ferroelectric films have attracted considerable attention as their nanoscale ferroelectricity and compatibility with cmos technology, fulfilling demands of emerging memory technologies. However, as films scale down, resistive-switching behavior becomes increasingly pronounced, intricately intertwining with the polarization-switching process and affecting ferroelectric switching factors often overlooked yet crucial for device performance optimization. By characterizing resistive-switching behavior and oxygen vacancy motion using tailored electric pulse schemes, we decouple the resistive-switching behavior from the overall switching process in ultrathin ferroelectric HZO films, which would otherwise erroneously inflate polarization values and increase coercive fields. Building on this, we elucidate endurance degradation mechanisms from dual perspectives of resistive switching and defect migration. Furthermore, we demonstrate the mitigated resistive switching activity by designing HfO2-based devices with symmetric oxide electrodes, achieving reduced coercive fields and improved cycling performances. This work provides crucial insights into the origins of inflated polarizations and reliability challenges in HfO2-based devices while offering a viable strategy to enhance ferroelectric properties for advanced memory applications.

cond-mat.mtrl-sci↗

arXiv2025

Enhancing ferroelectric stability: Wide-range of adaptive control in epitaxial HfO2/ZrO2 superlattices

The metastability of the polar phase in HfO2, despite its excellent compatibility with the complementary metal-oxide-semiconductor process, remains a key obstacle for its industrial applications. Traditional stabilization approaches, such as doping, often induce crystal defects and impose constraints on the thickness of ferroelectric HfO2 thin films. These limitations render the ferroelectric properties vulnerable to degradation, particularly due to phase transitions under operational conditions. Here, we demonstrate robust ferroelectricity in high-quality epitaxial (HfO2)n/(ZrO2)n superlattices, which exhibit significantly enhanced ferroelectric stability across an extended thickness range. Optimized-period superlattices maintain stable ferroelectricity from up to 100 nm, excellent fatigue resistance exceeding 109 switching cycles, and a low coercive field of ~0.85 MV/cm. First-principles calculations reveal that the kinetic energy barrier of phase transition and interfacial formation energy are crucial factors in suppressing the formation of non-polar phases. This work establishes a versatile platform for exploring high-performance fluorite-structured superlattices and advances the integration of HfO2-based ferroelectrics into a broader range of applications.

cond-mat.mtrl-sci↗

arXiv2025

Designing Optimal Distorted-Octahedra Superlattices for Strong Topological Hall Effect

Topologically protected spin states hold great promise for applications in next generation of memory circuits and spintronic devices. These intriguing textures typically emerge in bulk materials or heterostructures with broken inversion symmetry, accompanied by an enhanced Dzyaloshinskii-Moriya interaction (DMI). In this study, we successfully induced the topological Hall effect (THE) in atomically designed (DyScO3)n/(SrRuO3)n (DnSn) superlattices over a significant range of temperatures (10~120K) and thicknesses (16~40nm). Using magnetic force microscopy (MFM), we observed the formation and stability of magnetic domains, such as topological skyrmions. By precisely controlling the interlayer thickness (n) and biaxial strain, we elucidated the mechanisms underlying the modulation and induction of magnetic topological states. Supporting evidence was provided by scanning transmission electron microscopy (STEM) and X-ray absorption spectroscopy (XAS), thereby lending further credence to our conclusions. These heterostructures offer a universal method for exploring topological phenomena driven by distorted octahedra, while enhancing the integrability and addressability of topologically protected functional devices.

cond-mat.mtrl-sci↗

arXiv2025

Ideal antiferroelectricity with large digital electrostrain in PbZrO3 epitaxial thin films

Antiferroelectrics exhibit reversible antipolar-polar phase transitions under electric fields, yielding large electrostrain suitable for electromechanical devices. Nevertheless, in thin-film form, the antiferroelectric behavior is often obscured by competing ferroic orders, resulting in slanted hysteresis loops with undesired remnant polarization, subsequently posing challenges in obtaining ideal antiferroelectricity and understanding their intrinsic electrical behavior. Here, atomistic models for controllable antiferroelectric-ferroelectric phase transition pathways are unveiled along specific crystallographic directions. Guided by the anisotropic phase transition and orientation design, we achieved ideal antiferroelectricity with square double hysteresis loop, large saturated polarization (~60 {\mu}C/cm2), near-zero remnant polarization, fast response time (~75 ns), and near-fatigue-free performance (~10^10 cycles) in (111)P-oriented PbZrO3 epitaxial thin films. Moreover, a bipolar and frequency-independent digital electrostrain (~0.83%) were demonstrated in this architype antiferroelectric system. In-situ X-ray diffraction studies further reveal that the large digital electrostrain results from intrinsic field-induced antiferroelectric-ferroelectric structural transition. This work demonstrates the anisotropic phase transition mechanism and ideal antiferroelectricity with large digital electrostrain in antiferroelectric thin films, offering a new avenue for applications of antiferroelectricity in nanoelectromechanical systems.

cond-mat.mtrl-sci↗

arXiv2025

Ferroelectricity in layered bismuth oxide down to 1 nanometer

Atomic-scale ferroelectrics are of great interest for high-density electronics, particularly field-effect transistors, low-power logic, and nonvolatile memories. We devised a film with a layered structure of bismuth oxide that can stabilize the ferroelectric state down to 1 nanometer through samarium bondage. This film can be grown on a variety of substrates with a cost-effective chemical solution deposition. We observed a standard ferroelectric hysteresis loop down to a thickness of ~1 nanometer. The thin films with thicknesses that range from 1 to 4.56 nanometers possess a relatively large remanent polarization from 17 to 50 microcoulombs per square centimeter. We verified the structure with first-principles calculations, which also pointed to the material being a lone pair-driven ferroelectric material. The structure design of the ultrathin ferroelectric films has great potential for the manufacturing of atomic-scale electronic devices.

cond-mat.mtrl-sci↗

arXiv2024

Progress in Computational Understanding of Ferroelectric Mechanisms in HfO$_2$

Since the first report of ferroelectricity in nanoscale HfO$_2$-based thin films in 2011, this silicon-compatible binary oxide has quickly garnered intense interest in academia and industry, and continues to do so. Despite its deceivingly simple chemical composition, the ferroelectric physics supported by HfO$_2$ is remarkably complex, arguably rivaling that of perovskite ferroelectrics. Computational investigations, especially those utilizing first-principles density functional theory (DFT), have significantly advanced our understanding of the nature of ferroelectricity in these thin films. In this review, we provide an in-depth discussion of the computational efforts to understand ferroelectric hafnia, comparing various metastable polar phases and examining the critical factors necessary for their stabilization. The intricate nature of HfO$_2$ is intimately related to the complex interplay among diverse structural polymorphs, dopants and their charge-compensating oxygen vacancies, and unconventional switching mechanisms of domains and domain walls, which can sometimes yield conflicting theoretical predictions and theoretical-experimental discrepancies. We also discuss opportunities enabled by machine-learning-assisted molecular dynamics and phase-field simulations to go beyond DFT modeling, probing the dynamical properties of ferroelectric HfO$_2$ and tackling pressing issues such as high coercive fields.

cond-mat.mtrl-sci↗

arXiv2023

Epitaxial ferroelectric hafnia stabilized by symmetry constraints

Ferroelectric memories experienced a revival in the last decade due to the discovery of ferroelectricity in HfO$_2$-based nanometer-thick thin films. These films exhibit exceptional silicon compatibility, overcoming the scaling and integration obstacles that impeded perovskite ferroelectrics' use in high-density integrated circuits. The exact phase responsible for ferroelectricity in hafnia films remains debated with no single factor identified that could stabilize the ferroelectric phase thermodynamically. Here, supported by density functional theory (DFT) high-throughput (HT) calculations that screen a broad range of epitaxial conditions, we demonstrate conclusively that specific epitaxial conditions achievable with common substrates such as yttria-stabilized zirconia (YSZ) and SrTiO$_3$ can favor the polar Pca2$_1$ phase thermodynamically over other polar phases such as R3m and Pmn2$_1$ and nonpolar P2$_1$/c phase. The substrate's symmetry constraint-induced shear strain is crucial for the preference of Pca2$_1$. The strain-stability phase diagrams resolve experiment-theory discrepancies and can guide the improvement of ferroelectric properties of epitaxial hafnia thin films.

cond-mat.mtrl-sci↗