Crystalline solids with intrinsically low lattice thermal conductivity are essential for advancing high-performance thermoelectric materials. Superionic conductor AgCuTe exhibits inherently low lattice thermal conductivity and exceptional tunability in both electronic and phononic transport, making it a promising candidate for medium-temperature thermoelectric applications. However, its practical deployment remains limited by suboptimal performance and insufficient optimization strategies. Here, we report a substantially enhanced dimensionless figure of merit (ZT) of ∼1.72 at 773 K in p-type polycrystalline AgCuTe through a systematic point defects engineering strategy. Guided by mass and strain field fluctuation criteria for suppressing lattice thermal conductivity, sulfur is identified as an effective dopant. Subsequent introduction of cation vacancies further synergizes electronic and thermal transport, yielding a high average ZT of 1.55 between 523-773 K, surpassing all previously reported values for AgCuTe. Moreover, a segmented single-leg thermoelectric module combining this material with commercial p-type (Bi, Sb)2Te3 achieves a high energy conversion efficiency of ∼13.7% under a temperature gradient of ∼467 K. These results underscore the efficacy of point defects engineering in optimizing superionic conductors and highlight the strong potential of AgCuTe for practical thermoelectric applications.
The p-type transistor is an indispensable component of semiconductor technology, enabling a complementary operation with n-channel transistors for computation, storage, and communication. Achieving both high robustness and high efficiency is highly desirable but challenging for p-type transistors due to the limited semiconductors with reliable hole transport and their high activation energies. Here, we achieved a robust yet efficient p-type transistor by heterogeneously integrating an ultrawide-bandgap semiconductor and a high-κ dielectric layer through van der Waals integration. The p-type transistor employs a two-dimensional hole channel on hydrogenated diamond (bandgap 5.6 eV) combined with a high-κ (30.5) SrTiO3 perovskite membrane. At room temperature, the transistor exhibits stable operation with a high on-current (∼200 mA/mm), low subthreshold swing (70 mV/dec), high hole mobility (566 cm2/(V·s) to 572 cm2/(V·s)), and high on-off ratio (∼109). Furthermore, tuning the annealing temperature allows operation in either enhancement or depletion mode. The robust p-type transistor with high efficiency holds great potential for future power electronics, ultraviolet (UV) optoelectronics, and harsh-environment electronic applications.
Phase-pure Ni x P y enables detailed investigations of Ni–P interactions across different phases, highlighting the P-site driven hydrogen evolution reaction mechanism in P-rich Ni x P y .
Correlated complex oxides feature tightly coupled charge, spin, orbital, and lattice degrees of freedom, which give rise to rich correlated behavior. Freestanding oxide membranes render these materials into tunable quasi-2D platforms that enable multifunctional and reconfigurable devices. This Review surveys recent advances in the research of freestanding oxide membranes, highlighting their coupled correlated properties. We focus on three development pathways: (i) strain-free membranes, (ii) strained membranes, and (iii) van der Waals-integrated heterostructures. This organization begins with the intrinsic properties of oxide membranes, then examines mechanical tuning, heterogeneous integration, and multiphysics coupling to provide a comprehensive account of the field's development. Finally, we evaluate practical challenges, including high-quality surfaces, robust multiphysics coupling, wafer-scale transfer, and silicon-compatible heterogeneous integration. Addressing these challenges will enable scalable, high-yield manufacturing and expand the design space for oxide-based architectures, thereby accelerating the transition from laboratory demonstrations to industry-ready systems.
The nonlinear Hall effect (NLHE) offers an efficient, ultrafast method for converting alternating-current (AC) signals into direct-current (DC) power without threshold voltages or complex fabrication, enabling compact next-generation rectifiers and ambient energy harvesters. NLHE arises from both the Berry curvature dipole (BCD) and scattering mechanisms; while BCD requires broken inversion symmetry, scattering-driven contributions can occur even in systems with 3-fold rotational symmetry, providing a more general pathway for nonlinear transport. However, the quantitative contributions of different scattering sources remain insufficiently understood, limiting material and device optimization. In this study, we systematically identify and quantify three distinct scattering channels—static disorder (impurities), dynamic disorder (phonons), and their hybridization—that govern the temperature-dependent NLHE in high-quality exfoliated Bi2Te3. The importance of each mechanism varies with temperature, and understanding their roles lays a foundation for designing high-performance NLHE-based devices.
The emergence of two-dimensional (2D) semiconductors, particularly transition metal dichalcogenides (TMDs), shows great potential in revolution of the development of electronics. However, challenges in contact engineering, such as Fermi-level pinning and metal-induced gap states (MIGS) and disorders greatly hinder the high-performance devices based on 2D materials. Here, we propose a novel strategy to establish quasi-one-dimensional tunneling contacts through locally modulating the electronic properties of monolayer MoS2 beneath the metal electrode by high-electron-affinity transition metal oxides (TMOs). MoO3 is introduced to induce strong charge-transfer anti-doping in the contact region, effectively depleting free carriers and rendering the underlying MoS2 electrically insulating and behaving as the tunneling layer. The Au/MoO3-contacted monolayer-MoS2 field-effect transistors exhibit near-ideal ohmic characteristics with an exceptionally low Schottky barrier height (SBH) of 1.6 meV, nearing the theoretical limit. The field effect mobility reaches 559.5 cm2/V∙s at 10 K. Moreover, we demonstrate that substitution of MoO3 with V2O5 provides a means to tune the SBH, underscoring the versatility of this device fabrication strategy. This study presents a promising pathway for achieving efficient tunneling contacts in 2D electronics, paving the way for the advancement of next-generation high-performance devices.
Van der Waals (vdW) magnetic materials offer a flexible platform for exploring low-dimensional spin-dependent transport. FePd2Te2 (FPT) is a layered ferromagnet with a Curie temperature of similar to 185 K, whose magnetic anisotropy and domain structure give rise to rich Hall responses. Here, by measuring the Hall effect as a function of the magnetic field rotation angle, we observe an unconventional anomalous Hall effect with two clear plateaus near the in-plane (IP) and out-of-plane (OOP) field directions, characteristic of an anisotropy-driven spin-reorientation process. Notably, within a narrow angular range close to the IP configuration, a pronounced hump-like Hall signal emerges. Temperature-dependent measurements at this optimal angle further uncover a distinct thermal window in which the hump amplitude is maximized. Remarkably, a similar angle- and temperature-selective hump is also observed in a much thicker FPT flake, showing that this effect is robust against a several-fold change in thickness and making extrinsic multi-domain or domain-wall mechanisms unlikely. Taken together with bulk magnetization data and tests of multi-channel anomalous Hall scenarios, these results are most consistently explained by a topological Hall effect arising from chiral or noncoplanar spin textures stabilized during the field-driven spin reorientation. Our findings identify FPT as a promising vdW platform exhibiting robust signatures of emergent topological transport and offer new possibilities for engineering spin-based functionalities in layered magnetic heterostructures.
A noble-metal-free Ni-NC@TiO2 core-shell photocatalyst was developed for efficient hydrogen production from ammonia photodecomposition under visible light without the use of sacrificial agents. In this architecture, Ni nanoparticles are anchored on the nitrogen-doped carbon shell through strong Ni-N interfacial coordination. The conductive NC shell promotes the separation and transport of photogenerated charge carriers, while the Ni sites provide favourable centres for NH3 adsorption and dehydrogenation. Under visible-light irradiation, Ni-NC@TiO2 exhibits a hydrogen evolution rate approximately 43 times higher than that of pristine TiO2. Combined experimental characterizations and DFT calculations reveal that the interfacial Ni-N coupling not only accelerates carrier migration, but also modulates the electronic structure of the Ni sites, thereby lowering the reaction barrier for NH3 decomposition. Meanwhile, the catalyst shows excellent durability, maintaining stable activity over 40 h without detectable deactivation.
Two-dimensional (2D) perovskites derived from phenethylammonium iodide (PEAI) and its halogenated derivatives are commonly employed as surface passivation layers in high performance perovskite solar cells. In contrast, their application as additives to the perovskite precursor, enabling a simpler, single-step incorporation, has been less extensively explored. Herein, we investigated three halide-substituted PEAI derivatives as spacer cations for 2D perovskite additives in the precursor solution. Owing to its favorable molecular size, dipole moment, and stronger adsorption to the 3D lattice, incorporation of (4-fluorophenethylammonium)2PbI4 ((4FPEA)2PbI4) modulated the perovskite crystallization kinetics, yielding films of improved quality characterized by enlarged grain sizes and reduced defect density, and produced beneficial CBM deepening (approximate to 0.15 eV), improving the energy alignment with PCBM. Devices fabricated with 0.5 mol% (4-FPEA)2PbI4 additive achieved a maximum power conversion efficiency (PCE) of 25.03 %, with an open-circuit voltage (VOC) of 1.17 V and a fill factor (FF) of 84.37 %, with improvement in thermal, humidity, light and N2 storage stability.
Two‐dimensional (2D) In 2 Se 3 is a polymorphic layered semiconductor offering switchable ferroic and electronic functionalities, but scalable and reproducible synthesis of phase‐pure, thickness‐uniform films remains challenging because growth conditions often trigger polymorph coexistence and uncontrolled multilayering. Here we develop an InI + Se chemical vapor deposition route enabled by a modified reactor geometry incorporating an inner quartz liner that stabilizes vapor transport and improves reproducibility. By systematically mapping growth temperature, InI loading, Se sublimation temperature, carrier‐gas flow, and dwell time, we establish clear process–morphology relationships spanning isolated monolayer domains and millimeter‐scale coalesced monolayer films, with second‐layer islands, multilayer stacks, and bulk‐like growth emerging beyond the optimal growth window, as resolved by optical microscopy and atomic force microscopy. Raman spectra acquired from multiple substrate regions retain the characteristic β′ ‐In 2 Se 3 fingerprint across all parameter series, with no features attributable to other In 2 Se 3 polymorphs. Electron diffraction collected over widely separated regions supports long‐range crystallographic coherence of the single crystalline β′ parent lattice while resolving symmetry‐related orientations of the nanostriped superstructure. Together, the modified reactor design and parameter maps identify an operating window for phase‐pure, continuous, thickness‐uniform 2D β′ ‐In 2 Se 3 films, providing a practical foundation for scalable synthesis and device‐oriented studies.
Two-dimensional (2D) In2Se3 is a polymorphic layered semiconductor offering switchable ferroic and electronic functionalities, but scalable and reproducible synthesis of phase-pure, thickness-uniform films remains challenging because growth conditions often trigger polymorph coexistence and uncontrolled multilayering. Here we develop an InI + Se chemical vapor deposition route enabled by a modified reactor geometry incorporating an inner quartz liner that stabilizes vapor transport and improves reproducibility. By systematically mapping growth temperature, InI loading, Se sublimation temperature, carrier-gas flow, and dwell time, we establish clear process-morphology relationships spanning isolated monolayer domains and millimeter-scale coalesced monolayer films, with second-layer islands, multilayer stacks, and bulk-like growth emerging beyond the optimal growth window, as resolved by optical microscopy and atomic force microscopy. Raman spectra acquired from multiple substrate regions retain the characteristic beta '-In2Se3 fingerprint across all parameter series, with no features attributable to other In2Se3 polymorphs. Electron diffraction collected over widely separated regions supports long-range crystallographic coherence of the single crystalline beta ' parent lattice while resolving symmetry-related orientations of the nanostriped superstructure. Together, the modified reactor design and parameter maps identify an operating window for phase-pure, continuous, thickness-uniform 2D beta '-In2Se3 films, providing a practical foundation for scalable synthesis and device-oriented studies.
Molybdenum oxides and sulfides are both promising anode materials for lithium-ion batteries due to their high theoretical capacities (over 600 mAh g1). However, their intrinsic structural and chemical limitations have hindered their widespread application in battery research. A core-sheath MoS2@MoO3 heterostructure can combine the advantages of both components, yet its practical fabrication remains challenging due to harsh synthesis conditions and high cost.In this study, a core-sheath MoS2@MoO3 heterostructure was successfully synthesized via a simple and scalable in-situ method. Notably, as an LIB anode, MoS2@MoO3 delivers a high specific capacity of 838.09 mAh g1 at 0.05 A g1 and retains over 80% of its capacity after 450 cycles at 1 A g1. The superior electrochemical performance is attributed to the vertically aligned MoS2 nanosheets on the MoO3 core, which maximize active edge exposure, enhance Li+diffusion, and improve structural stability. These results position MoS2@MoO3 as a strong candidate for next-generation high-performance LIB anodes.
Polar domains and their manipulation-particularly the creation and dynamic control-have garnered significant attention, owing to their rich physics and promising applications in digital memory devices. In this work, using density functional theory (DFT) and deep learning molecular dynamics (DLMD) simulations, it is demonstrated that polar domains can be created and manipulated in twisted bilayers of ferroelectric CuInP2S6, as a result of interfacial ferroelectric (antiferroelectric) coupling in AA (AB) stacked region. Unlike the topological polar vortex and skyrmions observed in superlattices of (PbTiO3)n/(SrTiO3)n and sliding bilayers of BN and MoS2, the underlying mechanism of polar domain formation in this system arises from stacking-dependent energy barriers for ferroelectric switching and variations in switching speeds under thermal perturbations. Notably, the thermal stability and polarization lifetimes are highly sensitive to twist angles and temperature, and can be further manipulated by external electric fields and strain. Through multi-scale simulations, this study provides a novel approach to exploring how twist angles influence domain evolution and underscores the potential for controlling local polarization in ferroelectric materials via rotational manipulation.
Lattice symmetry determines the manifestations of the spin-orbit coupling (SOC) effect in crystals, e.g. spin polarizations in hidden-spin Rashba systems are concealed by the sublattice inversion symmetry, making spintronic applications impractical with negligible spin lifetimes. Here, high performance planar Hall effect (PHE) devices based on van der Waals 1T-PtSe2 thin films with hidden-Rashba spins are reported. By temperature- and layer-dependent magneto-transport, the quantum signature of the hidden-Rashba PHE is unveiled, which exhibits suppressed backscattering for parallelled electric and magnetic fields, and thus, produces an opposite sign to the conventional Rashba-rooted PHE signals. The inherent strong hidden-spin SOC allows high performance magnetic device operations from 0.3 K to room temperature (RT), exhibiting an ultralow working heat load of 1 nW below 80 K and retaining a superior RT signal-to-noise ratio exceeding 18 000. It is demonstrated that, by eliminating defects and via optimizing device structure, the sensitivity of hidden-Rashba PHE devices can be efficiently improved to exceed the commercial Hall sensors, making 2D hidden-spin Rashba systems a promising material platform for spintronics.
Rechargeable aqueous Zinc‐ion batteries (AZIBs) hold great promise for sustainable storage, yet their practical deployment is impeded by dendrite growth and hydrogen evolution reaction (HER). Hydrogel electrolytes offer a potential solution to stabilization but suffer from a trade‐off in ionic conductivity and mechanical robustness. Herein, by leveraging the Hofmeister effect, the way ions influence the solubility, stability, and structure of polymers in aqueous solutions, a concentration gradient hydrogel electrolyte (CGHE) is designed to reconcile these challenges. By integrating two hydrogels with high (1.5 m OAc − ) and low (0.3 m ) acetate concentrations, the CGHE achieves a high Zn 2 ⁺ transference number ( = 0.88) and excellent mechanical strength ( σ = 1.7 MPa, ɛ max = 310%). The quasi‐solid gradient architecture regulates Zn 2+ transport and cation selectivity, promoting uniform Zn (002) deposition while suppressing HER through reduced water activity in the networks. Consequently, symmetric Zn//Zn cells exhibit ultrastable cycling over 2,500 h at 1 mA cm −2 , and Zn//Cu asymmetric cells deliver a coulombic efficiency of 99.1%. The Zn//hydrogel//V 2 O 5 full batteries retain 91% of capacity after 500 cycles at 2 A g −1 , while the quasi‐solid electrolyte offers flexibility and flame resistance, enabling potential safe operation in wearable devices. The gradient electrolyte design provides a general strategy for constructing advanced electrolytes in metal‐based energy systems.
The fabrication of glasses, including silicate glasses, polymers, and amorphous metals, typically relies on the melting‐quenching technique. However, this approach faces significant challenges when applied to recently emerging molecular glasses due to the inherent thermal instability of small molecules. Herein, the discovery of a new supramolecular glass (BGG) is presented, formed by a unique melting‐quenching method that leverages unusual chemistry pathways. By manipulating the heating of a small molecule (benzoguanamine, BG), catalyst‐free self‐condensation reactions occur and produce multiple oligomers in a liquid state. The resulting high compositional and conformational entropy suppresses crystallization, allowing solidification into a rigid supramolecular glass under robust conditions. Despite being composed of low‐weight molecules, the extensive intermolecular interactions endow BGG with distinct aggregation‐induced emission (AIE, quantum yield up to 60%), polymer‐like Young's modulus (7.95 GPa), and superior glass transition temperature (100.1 °C). BGG's excellent processability is exemplified by the fabrication of thin films and fibers, showcasing potential applications in photovoltaics and photonic waveguides. BGG also serves as a platform for synthesizing diverse donor‐acceptor hybrids with > 95% energy transfer efficiency, enabling the creation of advanced materials with customizable functionalities.
High-entropy oxides (HEOs) offer exceptional compositional flexibility and structural stability, making them promising materials for energy and catalytic applications. Here, we investigate Sr doping effects on B-site cation oxidation states, local composition, and structure in epitaxial La1-xSrx(Cr0.2Mn0.2Fe0.2Co0.2Ni0.2)O3 thin films. X-ray spectroscopies reveal that Sr doping preferentially promotes Cr oxidation from Cr3+ to Cr6+, partially oxidizes Co and Ni, while leaving Mn4+ and Fe3+ unchanged. Atomic-resolution scanning transmission electron microscopy with energy-dispersive X-ray spectroscopy shows pronounced Cr segregation, with depletion at the interface and enrichment at the surface, along with partial amorphization in heavily Sr-doped samples. This segregation is likely driven by oxidation-induced migration of smaller, high-valence Cr cations during growth. These findings highlight the critical interplay between charge compensation, local strain, and compositional fluctuations in HEOs, indicating that precise control over growth conditions is critical for tuning their surface composition and electronic structure toward more robust electrocatalyst design.