arXiv subjects

Jiaou Wang

Publications and source records attributed to Jiaou Wang.

At least 19 recordsLinked to original sources

arXiv2026

Two-Dimensional Altermagnetism in Epitaxial CrSb Ultrathin Films

Altermagnets constitute an emerging class of collinear magnets that exhibit zero net magnetization yet host spin-split electronic bands arising from non-relativistic spin-space-group symmetries. Realization of altermagnetism in the two-dimensional (2D) limit remains an outstanding challenge because dimensional reduction suppresses kZ dispersion and destabilizes the symmetry operations essential for spin compensation. Here, we investigate ultrathin CrSb films grown epitaxially on Bi2Te3 substrate and uncover the evolution of altermagnetism in the 2D limit. Scanning tunneling microscopy (STM), quasiparticle interference (QPI), angle-resolved photoemission spectroscopy (ARPES), and density functional theory (DFT) calculations show that interfacial symmetry breaking in the one-unit-cell (1 UC) limit gives rise to localized electronic states and uncompensated magnetic moments. These interfacial effects become weakened from 7/4 UC, accompanied by the recovery of a bulk-like coordination environment and the emergence of altermagnetic electronic characteristics. Our results show that the essential altermagnetic electronic structure of CrSb survives at a thickness of only ~1.05 nm, demonstrating the robustness of altermagnetism in the 2D limit and opening opportunities for integrating stray-field-free spin order into low dimensional spintronic architectures.

cond-mat.mtrl-sci↗

arXiv2026

Discovery of d-orbital order in Tb2CoAl4Ge2

Orbital order describes a quantum state where occupied orbitals line up in a periodic pattern. While orbital physics plays a fundamental and universal role in strongly correlated electron systems, the existence and particularly the band structure fingerprint of orbital order remain a long-standing mystery. Here, we report the discovery of rare earth 5d-orbital order developed by the surface states of intermetallic compound Tb2CoAl4Ge2. Angle-resolved photoemission spectroscopy reveals characteristic nematic features like Fermi surface deformation and band split. These experimental observations can be described by a ferro-orbital order term in the mean-field Hamiltonian. The structural and magnetic origin of such order is excluded by systematic high-resolution neutron powder diffraction and scanning tunnelling microscopy measurements. Our results provide strong evidence for a pure surface orbital order scenario avoiding complications from structural distortion as in colossal magnetoresistance manganites, magnetic order as in iron-based superconductors, and charge transfer p-orbital order in cuprates.

cond-mat.str-el↗

arXiv2026

Curvature-driven revival of charge density waves in non-Euclidean space

Strongly correlated quantum states, such as charge density waves (CDWs), are exquisitely sensitive to Fermi surface topology and lattice symmetry, and are typically quenched by heavy carrier doping. In two-dimensional (2D) systems, however, macroscopic geometric curvature emerges as a novel structural degree of freedom to modulate microscopic quantum coherence. This raises a compelling physical question: can non-Euclidean geometric deformations compete with extreme electronic perturbations to reshape, or even revive, a quenched macroscopic quantum order? Here, by constructing monolayer TiSe$_2$-NbSe$_2$ heterostructure on a BLG/SiC substrate for the first time, we report the curvature-driven revival of a frustrated charge order in a non-Euclidean space. Low-temperature angle-resolved photoemission spectroscopy (ARPES) reveals a massive interfacial charge transfer, which destroys the global Fermi surface nesting and completely suppresses the long-range CDW order in Euclidean flat regions. Strikingly, high-resolution scanning tunneling microscopy (STM) reveals that a novel, non-linear CDW state miraculously survives, remaining strictly localized within morphologically distorted, non-Euclidean nanoscale curved regions. Atomistic simulations unravel the structural origin of this phenomenon, demonstrating that interfacial twist and lattice mismatch spontaneously generate a corrugated superlattice.

cond-mat.mtrl-sci↗

arXiv2025

In-plane polar domains enhanced energy storage

Relaxor ferroelectric thin films are recognized for their ultrahigh power density, rendering them highly promising for energy storage applications in electrical and electronic systems. However, achieving high energy storage performance with chemically homogeneous, environmentally friendly and compositionally stable materials remains challenging. In this work, we present a design of dielectrics with high energy storage performance via an in-plane polar domains incorporating polar nanoregions mechanism. Guided by phase-field simulations, we synthesized La/Si co-doping BaTiO3 solid-solution thin films with high chemical homogeneity to realize high energy storage performance. Given that, we achieve a high energy density of 203.7J/cm3 and an energy efficiency of approximately 80% at an electric field of 6.15MV/cm. This mechanism holds significant promise for the design of next-generation high-performance dielectric materials for energy storage and other advanced functional materials.

cond-mat.mtrl-sci↗

arXiv2024

Ultralarge polarization in ferroelectric hafnia-based thin films

Hafnia-based ferroelectrics have become a valuable class of electronic functional materials at the nanoscale, showing great potential for next-generation memory and logic devices. However, more robust ferroelectric properties and better understanding of the polarization mechanisms are currently needed both in technology and science. Herein, we report the properties of oxygen-deficient Hf0.5Zr0.5O2 films with ultralarge remanent polarization (Pr) of 387 uC cm-2 at room temperature (1 kHz). Structure characterizations identify a new ferroelectric monoclinic Pc phase in these Hf0.5Zr0.5O2 films. The in-situ STEM measurements evidence polar displacements of the oxygen atoms, which move up and down in the Pc structure under applied DC bias fields, showing a huge displacement (1.6 A). DFT calculations optimized the Pc structure and also predicted a large polarization. The coexistence of the ferroelectric monoclinic (Pc) phases and orthorhombic (Pca21) is responsible for this superior ferroelectric properties. These findings are promising for hafnia-based ferroelectric applications in integrated ferroelectric devices, energy harvesting and actuators, etc.

cond-mat.mtrl-sci↗

arXiv2023

Non-Equilibrium Spark Plasma Reactive Doping Enables Highly Adjustable Metal to Insulator Transitions and Improved Mechanical Stability for VO2

Although vanadium dioxide (VO2) exhibits the most abrupt metal to insulator transition (MIT) properties near room-temperature, the present regulation of their MIT functionalities is insufficient owing to the high complexity and susception associated with V4+. Herein, we demonstrate a spark plasma assisted reactive sintering (SPARS) approach to simultaneously achieve in situ doping and sintering of VO2 within largely short period (~10 minutes). This enables high convenience and flexibility in regulating the electronic structure of VO2 via dopant elements covering Ti, W, Nb, Mo, Cr and Fe, leading to a wide adjustment in their metal to insulator transition temperature (TMIT) and basic resistivity. Furthermore, the mechanical strengths of the doped-VO2 were meanwhile largely improved via the compositing effect of high melting-point dopant oxide. The high adjustability in MIT properties and improved mechanical properties further paves the way towards practical applications of VO2 in power electronics, thermochromism and infrared camouflage.

cond-mat.mtrl-sci↗

arXiv2022

Atomically engineered cobaltite layers for robust ferromagnetism

Emergent phenomena at heterointerfaces are directly associated with the bonding geometry of adjacent layers. Effective control of accessible parameters, such as the bond length and bonding angles, offers an elegant method to tailor competing energies of the electronic and magnetic ground states. In this study, we construct unit thick syntactic layers of cobaltites within a strongly tilted octahedral matrix via atomically precise synthesis. The octahedral tilt patterns of adjacent layers propagate into cobaltites, leading to a continuation of octahedral tilting while maintaining significant misfit tensile strain. These effects induce severe rumpling within an atomic plane of neighboring layers triggers the electronic reconstruction between the splitting orbitals. First-principles calculations reveal that the cobalt ions transits to a higher spin state level upon octahedral tilting, resulting in robust ferromagnetism in ultrathin cobaltites. This work demonstrates a design methodology for fine-tuning the lattice and spin degrees of freedom in correlated quantum heterostructures by exploiting epitaxial geometric engineering.

cond-mat.mtrl-sci↗

arXiv2021

Hydrogen induced electronic transition within correlated perovskite nickelates with heavy rare-earth composition

Although discovery in hydrogen induced electronic transition within perovskite family of rare-earth nickelate (ReNiO3) opens up a new paradigm in exploring both the new materials functionality and device applications, the existing research stays at ReNiO3 with light rare-earth compositions. To further extend the cognition towards heavier rare-earth, herein we demonstrate the hydrogen induced electronic transitions for quasi-single crystalline ReNiO3/LaAlO3 (001) heterostructures, covering a large variety of the rare-earth composition from Nd to Er. The hydrogen induced elevations in the resistivity of ReNiO3 (RH/R0) show an unexpected non-monotonic tendency with the atomic number of the rare-earth composition, e.g., firstly increase from Nd to Dy and afterwards decreases from Dy to Er. Although ReNiO3 with heavy rare-earth composition (e.g. DyNiO3) exhibits large RH/R0 up to 107, their hydrogen induced electronic transition is not reversible. Further probing the electronic structures via near edge X-ray absorption fine structure analysis clearly demonstrates the respective transition in electronic structures of ReNiO3 from Ni3+ based electron itinerant orbital configurations towards the Ni2+ based electron localized state. Balancing the hydrogen induced transition reversibility with the abruption in the variations of material resistivity, we emphasize that the ReNiO3 with middle rare-earth compositions (e.g. Sm) to be most suitable that caters for the potential applications in correlated electronic devices.

cond-mat.mtrl-sci↗

arXiv2021

Revealing the role of interfacial heterogeneous nucleation in metastable thin film growth of rare earth nickelates electronic transition materials

Although rare earth nickelates (ReNiO3) exhibit abundant electronic phases and widely adjustable metal to insulator electronic transition properties, their practical electronic applications are largely impeded by their intrinsic meta stability. Apart from elevating oxygen reaction pressures, heterogeneous nucleation is expected as an alternative strategy that enables the crystallization of ReNiO3 at low meta stability. In this work, the respective roles of high oxygen pressure and heterogeneous interface in triggering ReNiO3 thin films growth at metastable state are revealed. The ReNiO3 (Re:Nd, Sm, Eu, Gd, and Dy) heterogeneous thin films growth on LaAlO3 single crystal substrate have an effective crystallization at atmosphere without the necessity to apply high oxygen pressures, suggesting the interfacial bonding between the ReNiO3 and substrates can sufficiently reduce the positive Gibbs formation energy of ReNiO3, which is further verified by the first principles calculations. Nevertheless, the abrupt electronic transitions only appear in ReNiO3 thin films grown at high oxygen pressures, in which cases the oxygen vacancies are effectively eliminated via high oxygen pressure reactions as indicated by near edge X ray absorption fine structure (NEXAFS). This work unveils the synergistic effects of heterogeneous nucleation and high oxygen pressure on the growth of high quality ReNiO3 thin films.

cond-mat.mtrl-sci↗

arXiv2021

Facet Dependent Topological Phase Transition in Bi4Br4

The realization of the coexistence of various topologically nontrivial surface states in one material is expected to lay a foundation for new electric applications with selective robust spin current. Here we apply the magnetoconductivity characteristic and angle-resolved photoemission spectroscopy (ARPES) to visualize the surface-selected electronic features evolution of quasi-one-dimensional material Bi4Br4. The transport measurements indicate the quantum interference correction to conductivity possesses symbolic spin rotational characteristic correlated to the value of Berry phase with the effects of weak localization and weak antilocalization for (001) and (100) surfaces, respectively. The ARPES spectra provide the experimental evidence for quasi-one-dimensional massless Dirac surface state at the side (100) surface and anisotropic massive Dirac surface state at the top (001) surface, respectively, which is highly coincide with the angle-dependent scaling behavior of magnetoconductivity. Our results reveal the facet dependent topological phases in quasi-one-dimensional Bi4Br4, stimulating the further investigations of this dual topology classes and the applications of the feasible technologies of topological spintronics.

cond-mat.mtrl-sci↗

arXiv2021

Large-Gap Quantum Spin Hall State and Temperature-Induced Lifshitz Transition in Bi4Br4

Searching for new quantum spin Hall insulators with large fully opened energy gap to overcome the thermal disturbance at room temperature has attracted tremendous attention due to the one-dimensional (1D) spin-momentum locked topological edge states serving as dissipationless channels for the practical applications in low consumption electronics and high performance spintronics. Here, we report the investigation of topological nature of monolayer Bi4Br4 by the techniques of scanning tunneling microscopy and angle-resolved photoemission spectroscopy (ARPES). The topological non-triviality of 1D edge state integrals within the large bulk energy gap (~ 0.2 eV) is revealed by the first-principle calculations. The ARPES measurements at different temperature show a temperature-induced Lifshitz transition, corresponding to the resistivity anomaly caused by the shift of chemical potential. The connection between the emergency of superconductivity and the Lifshitz transition is discussed.

cond-mat.mtrl-sci↗

arXiv2021

Emergent Magnetic Phenomenon with Unconventional Structure in Epitaxial Manganate Thin Films

A variety of emergent phenomena has been enabled by interface engineering in the complex oxides heterostructures. While extensive attention has been attracted to LaMnO3 (LMO) thin films for observing the control of functionalities at its interface with substrate, the nature of the magnetic phases in the thin film is, however,controversial. Here, it is reported that the ferromagnetism in 2 and 5 unit cells thick LMO films epitaxially deposited (001)-SrTiO3 substrates ferromagnetic/ferromagnetic coupling in 8 and 10-unit-cell ones, and a striking ferromagnetic/antiferromagnetic pinning effect with apparent positive exchange bias in 15 and 20-unit-cell ones are observed. This novel phenomenon in both 15 and 20-unit-cell films indicates a coexistence of three magnetic orderings in a single LMO film.The high-resolution scanning transmission electron microscopy suggests a P21/n to Pbnm symmetry transition from interface to surface, with the spatial stratification of MnO6 octahedral morphology, corresponding to different magnetic orderings. These results should shed some new lights on manipulating the functionality of oxides by interface engineering.

cond-mat.str-el↗

arXiv2020

AC-frequency switchable correlated transports in rare-earth perovskite nickelates

Whilst electron correlations were previously recognized to trigger beyond conventional direct current (DC) electronic transportations (e.g. metal-to-insulator transitions, bad metal, thermistors), their respective influences to the alternation current (AC) transport are largely overlooked. Herein, we demonstrate active regulations in the electronic functionalities of d-band correlated rare-earth nickelate (ReNiO3) thin films, by simply utilizing their electronic responses to AC-frequencies (fAC). Assisted by temperature dependent near edge X-ray absorption fine structure analysis, we discovered positive temperature dependences in Coulomb viscosity of ReNiO3 that moderates their AC impedance. Distinguished crosslinking among R(Real)-fAC measured in nearby temperatures is observed that differs to conventional oxides. It enables active adjustability in correlated transports of ReNiO3, among NTCR-, TDelta- and PTCR- thermistors, via fAC from the electronic perspective without varying materials or device structures. The TDelta-fAC relationship can be further widely adjusted via Re composition and interfacial strains. The AC-frequency sensitivity discovered in ReNiO3 brings in a new freedom to regulating and switching the device working states beyond the present semiconductor technologies. It opens a new paradigm for enriching novel electronic applications catering automatic transmission or artificial intelligence in sensing temperatures and frequencies.

cond-mat.mtrl-sci↗

arXiv2020

Experimental Realization of Two-Dimensional Buckled Lieb lattice

Two-dimensional (2D) materials with a Lieb lattice can host exotic electronic band structures. Such a system does not exist in nature, and it is also difficult to obtain in the laboratory due to its structural instability. Here, we experimentally realized a 2D system composed of a tin overlayer on an aluminum substrate by molecular beam epitaxy. The specific arrangement of Sn atoms on the Al(100) surface, which benefits from favorable interface interactions, forms a stabilized buckled Lieb lattice. Our theoretical calculations indicate a partially broken nodal line loop protected by its mirror reflection symmetry and a topologically nontrivial insulating state with a spin-orbital coupling (SOC) effect in the band structure of this Lieb lattice. The electronic structure of this system has also been experimentally characterized by scanning tunnelling spectroscopy and angle-resolved photoemmision spectroscopy. Our work provides an appealing method for constructing 2D quantum materials based on the Lieb lattice.

cond-mat.mtrl-sci↗

arXiv2019

Overlooked transportation anisotropies in d-band correlated rare-earth perovskite nickelates

Anisotropies in electronic transportations conventionally originate from the nature of low symmetries in crystal structures, and were not anticipated for perovskite oxides, the crystal asymmetricity of which is far below, e.g. van der Waals or topological crystal. Beyond conventional expectations, herein we demonstrate pronounced anisotropies in the inter-band coulomb repulsion dominated electronic transportation behaviors under low-dimensional confinement for the perovskite family of rare-earth nickelates (ReNiO3). From one aspect, imparting bi-axial interfacial strains upon various lattice planes results in extrinsic anisotropies in the abrupt orbital transitions of ReNiO3, and their metal to insulator transition behaviors that elevates the transition temperature beyond the existing merit. From the other aspect, the in-plane orbital entropy associated to the in-plane symmetry of the NiO6 octahedron within ReNiO3 causes intrinsic anisotropies for the gradually orbital transition with temperature to further improve their thermistor transportation properties. The present work unveils the overlooked role of the electronic orbital directionality within low dimensional correlated perovskites that can trigger anisotropic transportation behaviors, in spite of their relatively symmetric crystal structures. Establishing anisotropic transportations integrating the electron correlation and quantum confinement effects will bring in a new freedom for achieving further improvement in transportation properties of multi-functional perovskite oxides.

cond-mat.mtrl-sci↗

arXiv2019

Magnetoresistance in Metallic Ferroelectrics

Polar metals with ferroelectric-like displacements in metals have been achieved recently, half century later than Anderson and Blount's prediction. However, the genuine ferroelectricity with electrical dipolar switching has not yet been attained experimentally in the conducting materials, especially the ones possessing magnetic responses. Here we report the coexistence of ferroelectricity and magnetoresistance (MR) in the metallic PbNb0.12Ti0.88O3 (PNTO) thin films. We found that the conducting and magnetic responses of PNTO films are highly asymmetric. Negative MR up to 50% is observed under an in-plane magnetic field; the MR switches to positive with the magnetic field applied parallel to the surface normal. Such unique behavior is attributed to the moving electron caused effective magnetic field which couples with the spins of electrons, which form a dynamic multiferroic state in the metallic PNTO. These findings break a path to multiferroic metal and offer a great potential to the multi-functional devices.

cond-mat.mtrl-sci↗

arXiv2019

Entropy driven reverse-metal-to-insulator transition and delta-temperatural transports in metastable perovskites of correlated rare-earth nickelate

The metal to insulator transition (MIT) in Mott-Hubbard systems is one of the most important discoveries in condensed matter physics, and results in abrupt orbital transitions from the insulating to metallic phases by elevating temperature across a critical point (TMIT). Although the MIT was previously expected to be mainly driven by the orbital Coulomb repulsion energy, the entropy contribution to the orbital free energy that also determines the relative stability of the metallic and insulating phases was largely overlooked. Herein, we demonstrate an orbital-entropy dominated reversible electronic phase transition in the metastable perovskite family of correlated rare-earth nicklates (ReNiO3), in addition to their previously known MIT driven by orbital Coulomb energies. In reverse to MIT, the resistivity of ReNiO3 abruptly increases by 2-3 orders by elevating T across another critical point (TR-MIT) below TMIT, and such transition is named as reverse-metal to insulator transition (R-MIT). Combining the afterwards exponentially decreasing resistivity in the insulating phase of ReNiO3 at further temperature elevation, a distinguished delta-temperatural transport character is established, which is potentially applicable for locking the working temperatures range for electric devices. The TR-MIT is shown to be enhanced via reducing the compositional complexity and size of Re or imparting bi-axial compressive strains, and meanwhile the transition sharpness of delta-temperatural transport is reduced. Our discovery indicates that temperature range for a thermodynamically stable insulating phase of ReNiO3 is in between of TR-MIT and TMIT, while a new conductive phase with high orbital entropy is formed by further descending temperature below TR-MIT.

physics.app-ph↗

arXiv2018

Electronic nature of coverage-dependent nanosurface effect by cooperative orbital redistribution

Nanomaterial surface states can effectively modify or even dominate their physical and chemical properties due to large surface-to-volume ratios. Such surface effects are highly dependent on particle size and ligand coverage, yet the underlying electronic-level mechanism still remains unknown. Using TiO2 nanosheet as a model system, we reveal the electronic nature of coverage-dependent nanosurface effects through varying ligand coverage and probing the modified surface bonding and electronic band structures with near-edge X-ray absorption fine structure. We discover experimentally that surface ligands can competitively polarize the 3d orbitals of surface Ti atoms into chemisorption states, which is cooperative with increased ligand coverages. Such coverage-dependent cooperative orbital redistribution accounts for various nanosurface effects on regulating the electronic structure, surface reactivity, optical property, and chemisorption of nanomaterials.

cond-mat.mtrl-sci↗