arXiv subjects

Changming Ke

Publications and source records attributed to Changming Ke.

13 recordsLinked to original sources

arXiv2026

Revisiting Ferroelectricity Beyond Polar Space Groups

Ferroelectricity, a hallmark of spontaneous inversion-symmetry breaking, has been a central concept in condensed matter physics and functional materials research, yet recent discoveries are revealing that switchable polarization can emerge in forms far richer than allowed by the conventional symmetry-based paradigm. Fractional quantum ferroelectricity and ionic-conductor ferroelectricity challenge the long-standing association of ferroelectricity exclusively with polar space groups. In this Review, we reconcile these emerging phenomena within the Berry-phase modern theory of polarization. We emphasize that polarization in insulating periodic crystals is not a single-valued vector, but a multivalued lattice quantity defined modulo a polarization quantum. Consequently, nonpolar crystals may possess nonzero formal polarization, and adiabatic paths connecting symmetry-equivalent structures can produce quantized changes in polarization without violating symmetry principles. The symmetry of this multivalued formal polarization is governed by a generalized Neumann principle. We further show that the large polarization changes induced by long-range ion migration in both fractional quantum ferroelectrics and ionic-conductor ferroelectrics can be naturally understood through the topological definition of oxidation state, which links ionic transport to quantized charge transfer and polarization change. We discuss the physical accessibility of these unconventional polarization states, highlighting the roles of switching pathways, boundary conditions, and domain-wall dynamics, particularly in systems such as $\alpha$-In$_2$Se$_3$. Finally, we suggest that the most promising functionality of these materials may lie not in conventional bulk ferroelectric switching, but in the creation and control of charged interfaces and domain walls arising from discontinuities in formal polarization.

cond-mat.mtrl-sci↗

arXiv2026

Proximity Ferroelectricity Driven by Mobile High-Miller-Index Domain Walls

Wurtzite ferroelectrics such as scandium-doped aluminum nitride (AlScN) are promising for next-generation memory because of their compatibility with semiconductor processes and strong spontaneous polarization. Ferroelectric switching in these materials is typically attributed to doping-induced softening of the bulk switching barrier. However, recent reports of proximity ferroelectricity, in which undoped AlN layers up to 500 nm thick fully switch in AlN/AlScN multilayers, challenge this view. Here, we reveal an alternative switching mechanism mediated by high-Miller-index domain walls, long overlooked due to their complex geometry and presumed instability. Using first-principles calculations and machine-learning molecular dynamics simulations, we show that these walls, once nucleated, migrate with exceptionally low barriers. The Sc dopants play a dual role: they stabilize high-index walls and thereby promote nucleation, while also introducing pinning that hinders wall motion. In multilayers, our simulations demonstrate that mobile domain walls nucleated in AlScN can propagate deep into adjacent AlN, where they move easily without dopant pinning, enabling low-field switching across thick undoped layers. This microscopic divide-and-conquer mechanism resolves the puzzle of proximity ferroelectricity and highlights high-index interfaces as an underexplored lever for controlling ferroelectric switching.

cond-mat.mtrl-sci↗

arXiv2025

Topological Control of Transition Metal Networks for Reversible High-Capacity Li-rich Cathodes

Developing high-energy-density batteries is essential for advancing sustainable energy technologies. However, leading cathode materials such as Li-rich oxides, including Li$_2$MnO$_3$, suffer from capacity loss due to irreversible oxygen release and structural degradation, both consequences of the oxygen redox activity that also enables their high capacity. The atomic-scale mechanisms behind this degradation, and whether it can be made reversible, remain open questions. Here, using submicrosecond-scale molecular dynamics simulations with first-principles accuracy, we directly visualize the entire charge-discharge cycle of Li$_2$MnO$_3$, uncovering the full lifecycle of the O$_2$-filled nanovoids responsible for degradation and identifying the critical size limit for voids to remain fully repairable upon discharge. Our results reveal that the topology of the Mn cation network is the key factor governing void growth, coalescence, and reparability. Based on a structural topology-informed design principle, we computationally develop a novel Li$_2$MnO$_3$ structure featuring a Mn lattice with a Kagome-like pattern, demonstrating full electrochemical reversibility even under extreme 80% delithiation. Our work establishes a new paradigm for designing high-energy cathodes, shifting the focus from mitigating damage to engineering inherent stability through atomic-level topological control of transition metal network.

cond-mat.mtrl-sci↗

arXiv2025

Rippled Moire Superlattices for Decoupled Ferroelectric Bits

Symmetry considerations suggest that moire superlattices formed by twisted two-dimensional materials should preserve overall inversion symmetry. However, experiments consistently report robust ferroelectricity in systems such as twisted bilayer h-BN, posing a fundamental discrepancy between theory and experiment regarding its microscopic origin. Here, using large-scale finite-field molecular dynamics simulations, we challenge the prevailing defect-pinning hypothesis and instead identify an out-of-plane bending field, induced by in-plane compressive strain, as the key symmetry-breaking mechanism. This strain-induced rippling drives spatially heterogeneous interlayer sliding and distorts the moire domain wall network, resulting in a four-state ferroelectric system. Remarkably, we show this mechanism can be harnessed at the nanoscale, where localized nanobubbles designate the moire lattice's fundamental hexagonal domain clusters as the smallest individually addressable ferroelectric bits, thereby imposing local control on an otherwise globally defined structure. Our findings establish a geometry-driven framework for understanding and engineering moire ferroelectrics, offering not only a route toward ultra-high-density, rewritable memory, but also a strategy for locally tuning the moire potential itself, a critical step for manipulating emergent correlated and topological quantum phases.

physics.comp-ph↗

arXiv2025

Superlubric Motion of Wave-like Domain Walls in Sliding Ferroelectrics

Sliding ferroelectrics constructed from stacked nonpolar monolayers enable out-of-plane polarization in two dimensions with exceptional properties, including ultrafast switching speeds and fatigue-free behavior. However, the widely accepted switching mechanism, which posits synchronized long-distance in-plane translation of entire atomic layers driven by an out-of-plane electric field, has shown inconsistencies with experimental observations. We demonstrate that this spinodal decomposition-like homogeneous switching process violates Neumann's principle and is unlikely to occur due to symmetry constraint. Instead, symmetry-breaking domain walls (DWs) and the tensorial nature of Born effective charges are critical for polarization reversal, underscoring the quantum nature of sliding ferroelectrics. Using the Bernal-stacked $h$-BN bilayer as a model system, we discover that the coherent propagation of wide, wave-like domain walls is the key mechanism for ferroelectric switching. This mechanism fundamentally differs from the layer-by-layer switching associated with narrow domain walls, which has been established for over sixty years in perovskite ferroelectrics. Moreover, these wave-like DWs exhibit superlubric dynamics, achieving ultrahigh velocities of approximately 4000 m/s at room temperature and displaying an anomalous cooling-promoted switching speed. The unexpected emergence of DW superlubricity in sliding ferroelectrics presents new avenues for enhancing key performance metrics and offers exciting opportunities for applications in cryogenic environments.

cond-mat.mtrl-sci↗

arXiv2024

Sliding-Reversible Bandgap Modulation in Irreversible Asymmetric Multilayers

The electronic bandgap of a material is often fixed after fabrication. The capability to realize on-demand and non-volatile control over the bandgap will unlock exciting opportunities for adaptive devices with enhanced functionalities and efficiency. We introduce a general design principle for on-demand and non-volatile control of bandgap values, which utilizes reversible sliding-induced polarization driven by an external electric field to modulate the irreversible background polarization in asymmetric two-dimensional (2D) multilayers. The structural asymmetry can be conveniently achieved in homobilayers of Janus monolayers and heterobilayers of nonpolar monolayers, making the design principle applicable to a broad range of 2D materials. We demonstrate the versatility of this design principle using experimentally synthesized Janus metal dichalcogenide (TMD) multilayers as examples. Our first-principles calculations show that the bandgap modulation can reach up to 0.3 eV and even support a semimetal-to-semiconductor transition. By integrating a ferroelectric monolayer represented by 1T$'''$-MoS$_2$ into a bilayer, we show that the combination of intrinsic ferroelectricity and sliding ferroelectricity leads to multi-bandgap systems coupled to multi-step polarization switching. The sliding-reversible bandgap modulation offers an avenue to dynamically adjust the optical, thermal, and electronic properties of 2D materials through mechanical and electrical stimuli.

cond-mat.mtrl-sci↗

arXiv2023

Competing charge transfer and screening effects in two-dimensional ferroelectric capacitors

Two-dimensional (2D) ferroelectrics offer the potential for ultrathin flexible nanoelectronics, typically utilizing a metal-ferroelectric-metal sandwich structure as the functional unit. Electrodes can either contribute free carriers to screen the depolarization field, enhancing nanoscale ferroelectricity, or they can induce charge doping, disrupting the long-range crystalline order. Here, we explore the dual roles of electrodes in 2D ferroelectric capacitors, supported by extensive first-principles calculations covering a range of electrode work functions. Our results reveal volcano-type relationships between ferroelectric-electrode binding affinity and work function, which are further unified by a quadratic scaling between the binding energy and the transferred interfacial charge. At the monolayer limit, the charge transfer dictates the ferroelectric stability and switching properties. This is a general characteristic confirmed in various 2D ferroelectrics including $\alpha$-In$_2$Se$_3$, CuInP$_2$S$_6$, and SnTe. As the ferroelectric layer's thickness increases, the stability of the capacitor evolves from a charge transfer-dominated to a screening-dominated state. The delicate interplay between these two effects will have important implications for the applications of 2D ferroelectric capacitors.

cond-mat.mtrl-sci↗

arXiv2023

Intrinsic ferroelectric switching in two-dimension $\alpha$-In$_2$Se$_3$

Two-dimensional (2D) ferroelectric semiconductors present opportunities for integrating ferroelectrics into high-density ultrathin nanoelectronics. Among the few synthesized 2D ferroelectrics, $\alpha$-In$_2$Se$_3$, known for its electrically addressable vertical polarization has attracted significant interest. However, the understanding of many fundamental characteristics of this material, such as the existence of spontaneous in-plane polarization and switching mechanisms, remains controversial, marked by conflicting experimental and theoretical results. Here, our combined experimental characterizations with piezoresponse force microscope and symmetry analysis conclusively dismiss previous claims of in-plane ferroelectricity in $\alpha$-In$_2$Se$_3$. The processes of vertical polarization switching in monolayer $\alpha$-In$_2$Se$_3$ are explored with deep-learning-assisted large-scale molecular dynamics simulations, revealing atomistic mechanisms fundamentally different from those of bulk ferroelectrics. Despite lacking in-plane effective polarization, 1D domain walls can be moved by both out-of-plane and in-plane fields, exhibiting unusual avalanche dynamics characterized by abrupt, intermittent moving patterns. The propagating velocity at various temperatures, field orientations, and strengths can be statistically described with a universal creep equation, featuring a dynamical exponent of 2 that is distinct from all known values for elastic interfaces moving in disordered media. This work rectifies a long-held misunderstanding regarding the in-plane ferroelectricity of $\alpha$-In$_2$Se$_3$, and the quantitative characterizations of domain wall velocity will hold broad implications for both the fundamental understanding and technological applications of 2D ferroelectrics.

cond-mat.mtrl-sci↗

arXiv2023

Semiconducting nonperovskite ferroelectric oxynitride designed ab initio

Recent discovery of HfO2-based and nitride-based ferroelectrics that are compatible to the semiconductor manufacturing process have revitalized the field of ferroelectric-based nanoelectronics. Guided by a simple design principle of charge compensation and density functional theory calculations, we discover HfO2-like mixed-anion materials, TaON and NbON, can crystallize in the polar Pca21 phase with a strong thermodynamic driving force to adopt anion ordering spontaneously. Both oxynitrides possess large remnant polarization, low switching barriers, and unconventional negative piezoelectric effect, making them promising piezoelectrics and ferroelectrics. Distinct from HfO2 that has a wide band gap, both TaON and NbON can absorb visible light and have high charge carrier mobilities, suitable for ferroelectric photovoltaic and photocatalytic applications. This new class of multifunctional nonperovskite oxynitride containing economical and environmentally benign elements offer a platform to design and optimize high-performing ferroelectric semiconductors for integrated systems.

cond-mat.mtrl-sci↗

arXiv2023

Depolarization Induced III-V Triatomic Layers with Tristable Polarization States

The integration of ferroelectrics that exhibit high dielectric, piezoelectric, and thermal susceptibilities with the mainstream semiconductor industry will enable novel device types for widespread applications, and yet there are few silicon-compatible ferroelectrics suitable for device downscaling. We demonstrate with first-principles calculations that the enhanced depolarization field at the nanoscale can be utilized to soften unswitchable wurtzite III-V semiconductors, resulting in ultrathin two-dimensional (2D) sheets possessing reversible polarization states. A 2D sheet of AlSb consisting of three atomic planes is identified to host both ferroelectricity and antiferroelectricity, and the tristate switching is accompanied by a metal-semiconductor transition. The thermodynamics stability and potential synthesizability of the triatomic layer are corroborated with phonon spectrum calculations, ab initio molecular dynamics, and variable-composition evolutionary structure search. We propose a 2D AlSb-based homojunction field effect transistor that supports three distinct and nonvolatile resistance states. This new class of III-V semiconductor-derived 2D materials with dual ferroelectricity and antiferroelectricity opens up the possibility for nonvolatile multibit-based integrated nanoelectronics.

cond-mat.mtrl-sci↗

arXiv2022

One Dimensional Ferroelectric Nanothreads with Axial and Radial Polarization

Long-range ferroelectric crystalline order usually fades away as the spatial dimension decreases, hence there are few two-dimensional (2D) ferroelectrics and far fewer one-dimensional (1D) ferroelectrics. Due to the depolarization field, low-dimensional ferroelectrics rarely possess the polarization along the direction of reduced dimensionality. Here, using first-principles density functional theory, we explore the structural evolution of nanoribbons of varying widths constructed by cutting the 2D sheet of ferroelectric $\alpha$-III$_2$IV$_3$ (III=Al, Ga, In; VI=S, Se, Te). We discover a one-dimensional ferroelectric nanothread (1DFENT) of ultrasmall diameter with both axial and radial polarization, potentially enabling ultra-dense data storage with a 1D domain of just three unit cells being the functional unit. The polarization in 1DFENT of Ga$_2$Se$_3$ exhibits an unusual piezoelectric response: a stretching stress along the axial direction will increase both axial and radial polarization, referred to as auxetic piezoelectric effect. Utilizing the intrinsically flat electronic bands, we demonstrate the coexistence of ferroelectricity and ferromagnetism in 1DFENT and a counterintuitive charge-doping-induced metal-to-insulator transition. The 1DFENT with both axial and radial polarization offers a counterexample to the Mermin--Wagner theorem in 1D and suggests a new platform for the design of ultrahigh-density memory and the exploration of exotic states of matter.

cond-mat.mtrl-sci↗

arXiv2022

Three Dimensional Activity Volcano Plot under External Electric Field

An external electric field (EEF) can impact a broad range of catalytic processes beyond redox systems. Computational design of catalysts under EEFs targeting specific operation conditions essentially requires accurate predictions of the response of a complex physicochemical system to collective parameters such as EEF strength/direction and temperature. Here, we develop a first-principles-based multiscale approach that enables efficient EEF-dependent kinetic modeling of heterogeneous catalysis. Taking steam reforming of methanol as an example, we find that the methanol conversion rate exhibits strong nonlinear response to temperature and EEF, and the optimal field line and constant carbon concentration line defined in the temperature--EEF parameter space serve as powerful metrics for catalyst design. Assisted with a deep neural network, we establish a three-dimensional activity volcano plot under EEFs for thousands of metallic alloys.

cond-mat.mtrl-sci↗

arXiv2021

Two-dimensional ferroelectric metal for electrocatalysis

The coexistence of metallicity and ferroelectricity has been an intriguing and controversial phenomenon as these two material properties are considered incompatible in bulk. We clarify the concept of ferroelectric metal by revisiting the original definitions for ferroelectric and metal. Two-dimensional (2D) ferroelectrics with out-of-plane polarization can be engineered via layer stacking to a genuine ferroelectric metal characterized by switchable polarization and non-zero density of states at the Fermi level. We demonstrate that 2D ferroelectric metals can serve as electrically-tunable, high-quality electrocatalysts.

cond-mat.mtrl-sci↗