arXiv subjects

Ce-Wen Nan

Publications and source records attributed to Ce-Wen Nan.

17 recordsLinked to original sources

arXiv2025

Artificial ferroelectric-like hysteresis in antiferroelectrics with non-uniform disorder

Antiferroelectrics exhibit unique double-hysteresis polarization loops, which have garnered significant attention due to their potential applications such as energy storage, electromechanical transduction, as well as synapse devices. However, numerous antiferroelectric materials have been reported to display signs of hysteresis loops resembling those of ferroelectric materials, and a comprehensive understanding remains elusive. In this work, we provide a phenomenological model that reproduces such widely observed artificial ferroelectric hysteresis with a superposition of numerous disordered antiferroelectric loops that have varying antiferroelectric-to-ferroelectric transition fields, particularly when these field ranges intersect. Experimentally, we realized such artificial ferroelectric-like hysteresis loops in the prototypical antiferroelectric PbZrO$_3$ and PbHfO$_3$ thin films, by introducing non-uniform local disorder (e.g., defects) via fine-tuning of the film growth conditions. These ferroelectric-like states are capable of persisting for several hours prior to transitioning back into the thermodynamically stable antiferroelectric ground state. Those results provide insights into the fundamental impact of disorder on the AFE properties and new possibilities of disorder-tailored functions.

cond-mat.mtrl-sci↗

arXiv2025

Broad-temperature-range ultrafast terahertz excitation of collective dynamics in polar skyrmions

Ultrafast coherent control of electric dipoles using strong terahertz (THz) pulses provides a means to discover hidden phases of materials and potentially leads to applications in high-speed electro-optic devices. The effectiveness of this means, albeit demonstrated in architype (incipient) ferroelectric systems such as SrTiO3, hinges on a spectral overlapping between their soft phonon modes within the excitation bandwidth of THz pulses. Generally this can only induce an appreciable coupling close to the phase transition temperatures, where the lattice phonons substantially soften. Because of their emergent subterahertz collective dynamics, a fundamentally distinct and effective THz coupling mechanism can be envisaged in topological polar structures recently discovered in PbTiO3/SrTiO3 superlattices. Here, we show that polar skyrmions can be coherently driven into a hidden phase with transient macroscopic polarization, as probed based on THz field-induced second harmonic generation and optical Kerr effects. Such an ultrafast THz-driven phase transition is found to sustain across a broad temperature range of 4-470 K, in accordance with the equilibrium stability field of the skyrmions. Supplemented by dynamical phase-field simulations, we identify the spatial symmetries and relaxation behaviors of the excited collective modes, thereby revealing their correlation with the emergence of the polar phases. Our results unveil the exotic dynamical properties of topological polar structures, which could be technologically exploited given their remarkable flexibility in structure design and tunability under external fields.

cond-mat.mtrl-sci↗

arXiv2024

A Hidden Quantum Paraelectric Phase in SrTiO3 Induced by Terahertz Field

Coherent manipulation of lattice vibrations using ultrafast light pulses enables access to nonequilibrium 'hidden' phases with designed functionalities in quantum materials. However, expanding the understanding of nonlinear light-phonon interaction mechanisms remains crucial for developing new strategies. Here, we report re-entrant ultrafast phase transitions in SrTiO3 driven by intense terahertz excitation. As the terahertz field increases, the system transitions from the quantum paraelectric (QPE) ground state to an intermediate ferroelectric phase, and then unexpectedly reverts to a QPE state above ~500 kV/cm. The latter hidden QPE phase exhibits distinct lattice dynamics compared to the initial phases, highlighting activated antiferrodistortive phonon modes. Aided by first-principles dynamical calculations, we identify the mechanism for these complex behaviors as a superposition of multiple coherently excited eigenstates of the polar soft mode. Our results reveal a previously uncharted quantum facet of SrTiO3 and open pathways for harnessing high-order excitations to engineer quantum materials in the ultrafast regime.

cond-mat.mtrl-sci↗

arXiv2024

Flexomagnetoelectric effect in Sr2IrO4 thin films

Symmetry engineering is explicitly effective to manipulate and even create phases and orderings in strongly correlated materials. Flexural stress is universally practical to break the space-inversion or time-reversal symmetry. Here, by introducing strain gradient in a centrosymmetric antiferromagnet Sr2IrO4, the space-inversion symmetry is broken accompanying a non-equivalent O p-Ir d orbital hybridization along z axis. Thus, emergent polar phase and out-of-plane magnetic moment have been simultaneously observed in these asymmetric Sr2IrO4 thin films, which both are absent in its ground state. Furthermore, upon the application of magnetic field, such polarization can be controlled by modifying the occupied d orbitals through spin-orbit interaction, giving rise to a flexomagnetoelectric effect. This work provides a general strategy to artificially design multiple symmetries and ferroic orderings in strongly correlated systems.

cond-mat.str-el↗

arXiv2023

Multifunctional magnetic oxide-MoS$_2$ heterostructures on silicon

Correlated oxides and related heterostructures are intriguing for developing future multifunctional devices by exploiting their exotic properties, but their integration with other materials, especially on Si-based platforms, is challenging. Here, van der Waals heterostructures of La$_{0.7}$Sr$_{0.3}$MnO$_3$ (LSMO), a correlated manganite perovskite, and MoS$_2$ are demonstrated on Si substrates with multiple functions. To overcome the problems due to the incompatible growth process, technologies involving freestanding LSMO membranes and van der Waals force-mediated transfer are used to fabricate the LSMO-MoS$_2$ heterostructures. The LSMO-MoS$_2$ heterostructures exhibit a gate-tunable rectifying behavior, based on which metal-semiconductor field-effect transistors (MESFETs) with on-off ratios of over 104 can be achieved. The LSMO-MoS$_2$ heterostructures can function as photodiodes displaying considerable open-circuit voltages and photocurrents. In addition, the colossal magnetoresistance of LSMO endows the LSMO-MoS$_2$ heterostructures with an electrically tunable magnetoresponse at room temperature. This work not only proves the applicability of the LSMO-MoS$_2$ heterostructure devices on Si-based platform but also demonstrates a paradigm to create multifunctional heterostructures from materials with disparate properties.

cond-mat.str-el↗

arXiv2023

Deep Learning Illuminates Spin and Lattice Interaction in Magnetic Materials

Atomistic simulations hold significant value in clarifying crucial phenomena such as phase transitions and energy transport in materials science. Their success stems from the presence of potential energy functions capable of accurately depicting the relationship between system energy and lattice changes. In magnetic materials, two atomic scale degrees of freedom come into play: the lattice and the spin. However, accurately tracing the simultaneous evolution of both lattice and spin in magnetic materials at an atomic scale is a substantial challenge. This is largely due to the complexity involved in depicting the interaction energy precisely, and its influence on lattice and spin-driving forces, such as atomic force and magnetic torque, which continues to be a daunting task in computational science. Addressing this deficit, we present DeepSPIN, a versatile approach that generates high-precision predictive models of energy, atomic forces, and magnetic torque in magnetic systems. This is achieved by integrating first-principles calculations of magnetic excited states with deep learning techniques via active learning. We thoroughly explore the methodology, accuracy, and scalability of our proposed model in this paper. Our technique adeptly connects first-principles computations and atomic-scale simulations of magnetic materials. This synergy presents opportunities to utilize these calculations in devising and tackling theoretical and practical obstacles concerning magnetic materials.

cond-mat.mtrl-sci↗

arXiv2023

Significant Unconventional Anomalous Hall Effect in Heavy Metal/Antiferromagnetic Insulator Heterostructures

The anomalous Hall effect (AHE) is a quantum coherent transport phenomenon that conventionally vanishes at elevated temperatures because of thermal dephasing. Therefore, it is puzzling that the AHE can survive in heavy metal (HM)/antiferromagnetic (AFM) insulator (AFMI) heterostructures at high temperatures yet disappears at low temperatures. In this paper, we report that an unconventional high-temperature AHE in HM/AFMI is observed only around the Néel temperature of AFM, with large anomalous Hall resistivity up to 40 n$Ω$ cm. This mechanism is attributed to the emergence of a noncollinear AFM spin texture with a non-zero net topological charge. Atomistic spin dynamics simulation shows that such a unique spin texture can be stabilized by the subtle interplay among the collinear AFM exchange coupling, interfacial Dyzaloshinski-Moriya interaction, thermal fluctuation, and bias magnetic field.

cond-mat.mes-hall↗

arXiv2021

Tailoring magnetic order via atomically stacking 3d/5d electrons

The ability to tune magnetic orders, such as magnetic anisotropy and topological spin texture, is desired in order to achieve high-performance spintronic devices. A recent strategy has been to employ interfacial engineering techniques, such as the introduction of spin-correlated interfacial coupling, to tailor magnetic orders and achieve novel magnetic properties. We chose a unique polar-nonpolar LaMnO3/SrIrO3 superlattice because Mn (3d)/Ir (5d) oxides exhibit rich magnetic behaviors and strong spin-orbit coupling through the entanglement of their 3d and 5d electrons. Through magnetization and magnetotransport measurements, we found that the magnetic order is interface-dominated as the superlattice period is decreased. We were able to then effectively modify the magnetization, tilt of the ferromagnetic easy axis, and symmetry transition of the anisotropic magnetoresistance of the LaMnO3/SrIrO3 superlattice by introducing additional Mn (3d) and Ir (5d) interfaces. Further investigations using in-depth first-principles calculations and numerical simulations revealed that these magnetic behaviors could be understood by the 3d/5d electron correlation and Rashba spin-orbit coupling. The results reported here demonstrate a new route to synchronously engineer magnetic properties through the atomic stacking of different electrons, contributing to future applications.

cond-mat.str-el↗

arXiv2020

Electric-field-controllable high-spin SrRuO3 driven by a solid ionic junction

Controlling magnetism and spin structures in strongly correlated systems by using electric field is of fundamental importance but challenging. Here, a high-spin ruthenate phase is achieved via a solid ionic chemical junction at SrRuO3/SrTiO3 interface with distinct formation energies and diffusion barriers of oxygen vacancies, analogue to electronic band alignment in semiconductor heterojunction. Oxygen vacancies trapped within this interfacial SrRuO3 reconstruct Ru-4d electronic structure and orbital occupancy, leading to an enhanced magnetic moment. Furthermore, an interfacial magnetic phase can be switched reversibly by electric-field-rectifying oxygen migration in a solid-state ionic gating device, providing a framework for atomic design of functionalities in strongly correlated oxides using a way of solid chemistry.

cond-mat.str-el↗

arXiv2019

Large Magnetoelectric Response in Sr2IrO4/SrTiO3 superlattices with non-equivalent interfaces

Large magnetoelectric response in thin films is highly desired for high-throughput and high-density microelectronic applications. However, the d0 rule in single-phase compounds usually results in a weak interaction between ferroelectric and magnetic orders; the magnetoelectric coupling via elastic resonance in composites restricts their thin-film integration in broadband. Here, we effectuate a concurrence of ferroelectric-like and antiferromagnetic phase transitions in Sr2IrO4/SrTiO3 superlattices by artificial design periodically non-equivalent interfaces, where a maximum magnetoelectric coefficient of ~980 mV cm-1 Oe-1 can be measured. Evidenced by synchrotron X-ray absorption and electron energy loss spectroscopies, a lopsided electron occupation occurs at the interfacial Ti ions. From perturbative calculations and numerical results, a strong coupling of antiferromagnetism and asymmetric electron occupation mediated by spin-orbit interaction leads to a large bulk magnetoelectric response. This atomic tailoring of the quantum order parameters in 3d and 5d oxides provides an alternative pathway towards strong magnetoelectric effects with thin-film integrations.

cond-mat.str-el↗

arXiv2019

Electrical Control of Large Rashba Effect in Oxide Heterostructures

Large Rashba effect efficiently tuned by an external electric field is highly desired for spintronic devices. Using first-principles calculations, we demonstrate that large Rashba splitting is locked at conduction band minimum in ferroelectric Bi(Sc/Y/La/Al/Ga/In)O3/PbTiO3 heterostructures where the position of Fermi level is precisely controlled via its stoichiometry. Fully reversible Rashba spin texture and drastic change of Rashba splitting strength with ferroelectric polarization switching are realized in the symmetric and asymmetric heterostructures, respectively. By artificially tuning the local ferroelectric displacement and the orbital hybridization, the synergetic effect of local potential gradient and orbital overlap on the dramatic change of splitting strength is confirmed. These results improve the feasibility of utilizing Rashba spin-orbit coupling in spintronic devices.

cond-mat.mtrl-sci↗

arXiv2018

A protonated brownmillerite electrolyte for superior low-temperature proton conductivity

Design novel solid oxide electrolyte with enhanced ionic conductivity forms one of the Holy Grails in the field of materials science due to its great potential for wide range of energy applications. Conventional solid oxide electrolyte typically requires elevated temperature to activate the ionic transportation, while it has been increasing research interests to reduce the operating temperature due to the associated scientific and technological importance. Here, we report a conceptually new solid oxide electrolyte, HSrCoO2.5, which shows an exceptional enhanced proton conductivity at low temperature region (from room temperature to 140 oC). Combining both the experimental results and corresponding first-principles calculations, we attribute these intriguing properties to the extremely-high proton concentration as well as the well-ordered oxygen vacancy channels inherited from the novel crystalline structure of HSrCoO2.5. This result provides a new strategy to design novel solid oxide electrolyte with excellent proton conductivity for wide ranges of energy-related applications.

cond-mat.mtrl-sci↗

arXiv2018

Ionic Modulation of Interfacial Magnetism through Electrostatic Doping in Pt/YIG bilayer heterostructure

Voltage modulation of yttrium iron garnet (YIG) with compactness, high speed response, energy efficiency and both practical/theoretical siginificances can be widely applied to various YIG based spintronics such as spin Hall, spin pumping, spin Seeback effects. Here we initial an ionic modulation of interfacial magnetism process on YIG/Pt bilayer heterostructures, where the Pt capping would influence the ferromagnetic (FMR) field position significantly, and realize a significant magnetism enhancement in bilayer system. A large voltage induced FMR field shifts of 690 Oe has been achieved in YIG (13 nm)/Pt (3 nm) multilayer heterostructures under a small voltage bias of 4.5 V. The remarkable ME tunability comes from voltage induced extra FM ordering in Pt metal layer near the Pt/YIG interface. The first-principle theoretical simulation reveal that the electrostatic doping induced Pt5+ ions have strong magnetic ordering due to uncompensated d orbit electrons. The large voltage control of FMR change pave a foundation towards novel voltage tunable YIG based spintronics.

cond-mat.mtrl-sci↗

arXiv2017

Mechanical Switching of Nanoscale Multiferroic Phase Boundaries

Tuning the lattice degree of freedom in nanoscale functional crystals is critical to exploit the emerging functionalities such as piezoelectricity, shape-memory effect, or piezomagnetism, which are attributed to the intrinsic lattice-polar or lattice-spin coupling. Here it is reported that a mechanical probe can be a dynamic tool to switch the ferroic orders at the nanoscale multiferroic phase boundaries in BiFeO 3 with a phase mixture, where the material can be reversibly transformed between the "soft" tetragonal-like and the "hard" rhombohedrallike structures. The microscopic origin of the nonvolatile mechanical switching of the multiferroic phase boundaries, coupled with a reversible 180° rotation of the in-plane ferroelectric polarization, is the nanoscale pressure-induced elastic deformation and reconstruction of the spontaneous strain gradient across the multiferroic phase boundaries. The reversible control of the room-temperature multiple ferroic orders using a pure mechanical stimulus may bring us a new pathway to achieve the potential energy conversion and sensing applications.

cond-mat.mtrl-sci↗

arXiv2017

Nanoscale Bandgap Tuning across an Inhomogeneous Ferroelectric Interface

We report nanoscale bandgap engineering via a local strain across the inhomogeneous ferroelectric interface, which is controlled by the visible-light-excited probe voltage. Switchable photovolatic effects and the spectral response of the photocurrent were explore to illustrate the reversible bandgap variation (~0.3eV). This local-strain-engineered bandgap has been further revealed by in situ probe-voltage-assisted valence electron energy-loss spectroscopy (EELS). Phase-field simulations and first-principle calculations were also employed for illustration of the large local strain and the bandgap variation in ferroelectric perovskite oxides. This reversible bandgap tuning in complex oxides demonstrates a framework for the understanding of the opticallyrelated behaviors (photovoltaic, photoemission, and photocatalyst effects) affected by order parameters such as charge, orbital, and lattice parameters.

cond-mat.mes-hall↗

arXiv2017

Deterministic Role of Concentration Surplus of Cation Vacancy over Anion Vacancy in Bipolar Memristive NiO

Migration of oxygen vacancies has been proposed to play an important role in the bipolar memristive behaviors since oxygen vacancies can directly determine the local conductivity in many systems. However, a recent theoretical work demonstrated that both migration of oxygen vacancies and coexistence of cation and anion vacancies are crucial to the occurrence of bipolar memristive switching, normally observed in the small-sized NiO. So far, experimental work addressing this issue is still lacking. In this work, with conductive atomic force microscope and combined scanning transmission electron microscopy & electron energy loss spectroscopy, we reveal that concentration surplus of Ni vacancy over O vacancy determines the bipolar memristive switching of NiO films. Our work supports the dual-defects-based model, which is of fundamental importance for understanding the memristor mechanisms beyond the well-established oxygen-vacancy-based model. Moreover, this work provides a methodology to investigate the effect of dual defects on memristive behaviors.

cond-mat.mtrl-sci↗

arXiv2010

Size dependent electric voltage-controlled magnetic anisotropy in multiferroic heterostructures: Interface-charge and strain co-mediated magnetoelectric coupling

We present a phenomenological scheme to study the size-dependent electric voltage-controlled magnetic anisotropy in ferromagnetic (FM)/ferroelectric (FE) heterostructures. The FM layers are either metallic Fe(001), Ni(001), Co(0001), or half-metallic (La, Sr)MnO3 films. Two magnetoelectric mechanisms, i.e., interface-charge and strain-mediated couplings, are considered. We show that the interface-charge mediated coupling is the main mechanism for the magnetoelectic coupling when the FM film thickness is below a certain transition thickness dtr while the strain-mediated coupling dominates above dtr.

cond-mat.mtrl-sci↗