Low-temperature catalytic oxidation of nitric oxide (NO) has drawn significant attention, underscoring the need for catalysts with enhanced activity in the low-temperature regime. Zeolites possess intrinsic advantages for NO oxidation, as their confined microporous frameworks can stabilize the transition state (TS) through enthalpic interactions while mitigating entropy loss, thereby enabling efficient catalysis at reduced temperatures. To achieve stronger confinement of the NO oxidation TS and consequently improve catalytic performance, a three-step zeolite optimization strategy was developed to simultaneously regulate spatial and electrostatic environments within the framework. First, a zeolite with appropriate void spaces was selected; second, its Si/Al ratio (SAR) was adjusted to fine-tune the framework properties; and third, ion exchange was conducted to further modulate spatial and electrostatic effects. The results indicate that both pore size and extra-framework cations play critical roles in governing the catalytic activity of zeolites for NO oxidation. Among the synthesized materials, potassium-exchanged SSZ-13 with an SAR of 8 (K-SSZ-13-8) exhibited the highest low-temperature NO oxidation activity, achieving 87.2% of NO conversion at 25 degrees C, along with relatively good tolerance to sulfur dioxide. This study provides a rational design strategy for developing high-performance zeolite catalysts for low-temperature NO oxidation.
The Yb2SiO5/(Yb2SiO5–Yb2Si2O7)/Si trilayer environmental barrier coating (EBC) has garnered significant attention in recent years for its excellent corrosion resistance and thermal compatibility with SiCf/SiC. Under thermal cycling, surface vertical cracks initiate and propagate downward, branch and coalesce within the interlayer, ultimately leading to coating delamination and failure. This study employs the finite element method to quantitatively elucidate the influence of interlayer composition and surface crack density on integrated crack propagation behavior. Three critical crack propagation mechanisms are systematically analyzed, including effect of inter-crack elastic shielding within Yb2SiO5 top coat on suppressing the downward propagation, the competition between deflection and penetration at the Yb2SiO5/(Yb2SiO5–Yb2Si2O7) interface, and composition-driving crack bifurcation geometry within the (Yb2SiO5–Yb2Si2O7) interlayer. Based on these insights, an optimal surface crack geometry and interlayer compositions are proposed enables stable crack arrest, controlled interfacial deflection, and moderate-energy-dissipative branching, thereby maximizing structural toughness and extending service lifetime.
Optical skyrmions offer a robust vectorial information degree of freedom for free-space communication, but practical deployment requires a compact platform capable of active topological reconfiguration. Here, we propose a silicon microring-resonator optical phased array that integrates spin-selective emission and programmable phase control on a single chip. Optimized inner- and outer-grating microring emitters provide decoupled LCP and RCP radiation bases with polarization fractions of 90.27
The high-entropy design strategy offers a route to control the spin order in rare-earth orthoferrites (RFeO3). In this work, a high-entropy perovskite single crystal of Y0.2Nd0.2Sm0.2Er0.2Tm0.2FeO3 (5RFeO) was grown using the optical floating zone method. Its high crystalline quality and precise orientation were confirmed by x-ray and Laue diffraction. The effects of temperature, magnetic field, and hydrostatic pressure on the spin reorientation (SR) behavior were systematically investigated. Our measurements reveal that under low magnetic fields, the crystal exhibits a Gamma(4) -> Gamma(4) + Gamma(2) -> Gamma(2) transition sequence within the temperature range of 125-160 K. The applied magnetic field suppresses the SR, broadening the transition temperature window. Furthermore, hydrostatic pressure above similar to 0.80 GPa reconstructs the transition pathway in a manner that points to a Gamma(1)-like intermediate state, leading to a complex and multi-step transition sequence. The magnetic moment along the b axis remains insensitive to both the magnetic field and pressure. This study demonstrates the tunability of spin reorientation to multiple physical stimuli in a chemically disordered high-entropy system, elucidates the underlying spin structure evolution mechanism, and highlights the application potential of such high-entropy orthoferrites in spin-based devices.
Colloidal perovskite nanocrystals (PeNCs) are rapidly advancing the frontier of next-generation display technologies, propelled by their superior properties such as near-unity photoluminescence quantum yield (PLQY), high color purity, and low-cost solution processability. Despite these advantages, the electroluminescence (EL) performance of PeNC-based light-emitting diodes (LEDs) is still constrained by a high density of surface defects during the film-forming process. To address this challenge, we propose a synergistic, one-step dynamic surface engineering strategy to simultaneously reconstruct the ligand environment and passivate surface defects. By introducing a triethylene glycol dimethacrylate (TEGDMA)/ethyl acetate (EtOAc) solution during the critical spin-coating stage, we achieved a synchronized "wash-and-passivate" effect. The EtOAc serves as a moderate-polarity mediator to strip away the disordered, loosely-bound ligands, thereby eliminating steric hindrance. Concurrently, the TEGDMA molecules, acting as potent Lewis bases, promptly anchor onto the newly exposed undercoordinated Pb²⁺ sites via robust C=O and -O- coordination, significantly suppressing non-radiative recombination. This instantaneous passivation effectively heals the nanocrystal surface, yielding a smoother film morphology and a markedly reduced trap-state density. Consequently, the resulting PeNC LEDs exhibited a remarkable performance boost, with the peak external quantum efficiency (EQE) increasing from 10.82% to 17.82%, and the maximum luminance rising from 10548 cd m⁻² to 35142 cd m⁻². This study offers a practical perspective on interfacial modulation, demonstrating the importance of synergistic ligand management and defect passivation in realizing high-performance PeNCs-based optoelectronic devices.
Molecular pre-aggregation behavior plays a critical role in the morphology of organic films and the device performance of organic solar cells (OSCs). In the high-boiling-point solvent system, the relatively slow drying crystallization kinetics impacted the solution-state molecular pre-aggregation control, complicating the films crystallization regulation. In this work, a novel approach to regulate the pre-aggregation characteristics of the thin films was developed by constructing a droplet-merging and dissolution-induced intermediate state during inkjet printing (IJP). During this process, three key parameters, the printing temperature, droplet space, and additives, were identified to be critical for the intermediate state formation. This method created an intermediate aggregation state that finally enhanced the crystallization and molecular orientations in films printed from ortho-dichlorobenzene, overcoming the slow kinetics challenge. Consequently, IJP OSCs achieved a record power conversion efficiency of 17.57% through this droplet-merging and dissolution-induced intermediate strategy.
Abstract Rational interface design is of paramount importance for advancing energy devices. However, molecular-scale interfacial engineering faces two fundamental challenges: first, the intrinsic nanoscale heterogeneity in interfacial morphology, structure, and composition impedes the seamless upscaling from molecular-level insights to macroscopic device behavior; second, static molecular characteristics alone are insufficient to capture the dynamic evolution of these nanoscale interfacial features under operating conditions. Atomic force microscopy (AFM), with its high spatial resolution, versatile functional imaging modes, and exceptional capability for dynamic characterization, provides an ideal platform for interrogating nanoscale interfacial phenomena and holds the potential to bridge molecular design with device performance. This review focuses on the application of functional AFM in the study of interfaces in thin-film solar cells and all-solid-state lithium batteries, tracing the development from in situ to in operando characterization. We discuss the associated challenges and corresponding strategies, highlight the critical role of nanoscale interfacial characterization under operando scenarios, and conclude with an outlook on future directions for the development of the in operando AFM fields.
Inkjet printing (IJP) is a non-contact digital technique for the industrialization of organic solar cells (OSC). It features high material utilization and roll-to-roll compatibility. Moreover, its droplet-to-droplet film formation makes it an ideal model to study the intrinsic morphology evolution of OSCs in high-boiling-point solvent systems. However, the slow evaporation of the high-boiling point solvents often induces premature acceptor aggregation and abnormal crystallization, resulting in inferior active layer morphology and compromised device performance. This work proposed a fullerene derivative-induced crystallization sequence regulation strategy in the inkjet-printed OSCs. It demonstrated that the fullerene derivatives strongly interacted with acceptors via synergistic electrostatic interactions, which inhibited the excessive acceptor aggregation and promoted the crystallization of the donor in a fiber morphology. In addition, this strategy showed good universality in a series of donor and acceptor systems. Due to the formation of a fiber morphology in the printed films, the efficiency of the inkjet-printed device improved from 15.28
Although Li-ion conductivity has been the primary focus during decades of solid-electrolyte research, the mechanical compliance is equally important. For most state-of-the-art solid electrolytes, the mechanical compliance is characterized by the hardness above 1 GPa and Young's modulus above 15 GPa. Here, we report a particularly compliant solid electrolyte, 1.4Li2O-0.75ZrCl4-0.25AlCl3, whose hardness and Young's modulus reach 0.22 and 1.41 GPa, respectively. Meanwhile, it shows an ionic conductivity of 2.55 mS cm-1 at 25 °C and an estimated cost of $43.70 L-1, considerably lower than that of the Li2ZrCl6 solid electrolyte known for cost-effectiveness ($140.01 L-1). The improved mechanical compliance and fast Li-ion transport in 1.4Li2O-0.75ZrCl4-0.25AlCl3 enable decent cell performance. With high positive electrode active material loading above 20 mg cm-2, these two types of cells achieve areal capacities of 3.62 mAh cm-2 (85.78% capacity retention) and 3.92 mAh cm-2 (90.11% capacity retention), respectively, after 100 cycles under 0.1 C at 25 °C. The simultaneous achievement of highly competitive mechanical compliance, Li-ion conductivity, and cost-effectiveness in 1.4Li2O-0.75ZrCl4-0.25AlCl3 have the potential to pave the way for the realization of commercial, practical all-solid-state Li batteries.
Silicon monoxide (SiO) is a promising anode material for next-generation lithium-ion batteries, yet the practical application remains hindered by drastic volume expansion, unstable solid electrolyte interphase (SEI), and sluggish reaction kinetics. Herein, we propose a rational interfacial engineering strategy to construct a robust O–Fe–C bridging architecture for SiO via high-energy ball-milling combined with in situ polymerization and carbonization. It has been demonstrated that the constructed O–Fe–C architecture establishes a highly efficient electron/ion transport network to significantly accelerate charge transfer kinetics. More importantly, such bridging structure could also function as an elastic buffer with a distinctive “spring effect” to accommodate the volume expansion of SiO over cycling, which effectively suppresses the interfacial rupture and regulates the electrolyte decomposition to foster a stable and LiF-rich SEI layer. Consequently, the SiO anode with the O–Fe–C bridging architecture delivers a superior reversible capacity of 1061.4 mA h g−1 after 100 cycles at 0.1 A g−1, and a high rate capability of 613.0 mA h g−1 at 3.0 A g−1. This work offers deeper insights into interfacial design for stable silicon-based anodes with enhanced reaction kinetics, providing a feasible strategy for the construction of next-generation energy storage systems.
Molecular pre-aggregation behavior plays a critical role in the morphology of organic films and the device performance of organic solar cells (OSCs). In the high-boiling-point solvent system, the relatively slow drying crystallization kinetics impacted the solution-state molecular pre-aggregation control, complicating the films crystallization regulation. In this work, a novel approach to regulate the pre-aggregation characteristics of the thin films was developed by constructing a droplet-merging and dissolution-induced intermediate state during inkjet printing (IJP). During this process, three key parameters, the printing temperature, droplet space, and additives, were identified to be critical for the intermediate state formation. This method created an intermediate aggregation state that finally enhanced the crystallization and molecular orientations in films printed from ortho-dichlorobenzene, overcoming the slow kinetics challenge. Consequently, IJP OSCs achieved a record power conversion efficiency of 17.57
This study systematically investigates the regulation of the spin reorientation behavior in YFe0.7Mn0.3O3 (YFMO) single crystal under electric, magnetic, and hydrostatic pressure fields. X-ray photoelectron spectroscopy analysis reveals a characteristic mixed-valence state dominated by Fe2+ along with a high concentration of oxygen vacancies. Magnetic measurements indicate that an electric field of 10 kV/cm does not alter the c axis magnetization, regardless of the field direction. The magnetic response shows clear anisotropy. A high field (>23 kOe) along the a axis induces the Gamma(2) (F-x) phase, while along the c axis it drives a reversible transition between the Gamma(1) (C-z) and Gamma(4) (F-z) phases. Hydrostatic pressure further exhibits versatile regulatory capabilities. It not only shifts the Gamma(4)->Gamma(1) transition temperature along the c axis but also induces an emergent Gamma(3) (F-y) phase along the b axis. Consequently, the phase transition pathway expands from a simple Gamma(4)->Gamma(1) sequence to a complex process involving mixed Gamma(3) phases. This work elucidates the anisotropic response of YFMO to external fields and reveals the potential of pressure for regulating spin order, providing valuable insights for developing room-temperature spintronic devices.
This work investigates spin reorientation in Nd0.6Y0.4FeO3 single crystals under temperature, magnetic field and hydrostatic pressure. High-quality crystals were grown by the optical floating zone method. Temperature-dependent magnetization reveals a continuous Γ4 → Γ4 + Γ2 → Γ2 transition upon cooling, with the transition region occurring at 50–150 K. Magnetic field manipulation exhibits strong anisotropy, wherein the field-induced Γ4 → Γ2 transition occurs along the a-axis above a temperature-dependent critical field, while the b-axis remains antiferromagnetic and the c-axis evolves from weak ferromagnetic to antiferromagnetic. Remarkably, hydrostatic pressure reconstructs the transition pathway. Above ∼0.63 GPa, the otherwise unstable Γ1 antiferromagnetic phase emerges as a thermodynamic intermediate state, transforming the simple Γ4 → Γ2 sequence into a multi-step process of Γ4 → Γ4 + Γ1 → Γ4 + Γ1 + Γ2 → Γ1 + Γ2 → Γ2. This pathway reconstruction is evidenced by decoupled a- and c-axis magnetic responses under pressure. A pressure-temperature magnetic phase diagram is established, visualizing this pressure-induced pathway evolution. This study demonstrates lattice-strain-spin coupling in manipulating spin reorientation, offering insights into magnetic interactions in rare-earth orthoferrites for spintronic applications.
The Rice-Mele (RM) model, as a paradigmatic extension of the Su-Schrieffer-Heeger (SSH) chain, plays a pivotal role in understanding topological phases and quantized adiabatic transport in one-dimensional systems. Its realization in acoustic systems, however, has been hindered by the need for simultaneous precise modulation of on-site potentials and couplings. In this work, we demonstrate a method to linearly tune on-site potentials and couplings, thus realizing an acoustic Rice-Mele model. During parameter evolution, the system exhibits a Thouless pump, with the acoustic field distribution adiabatically shifting from the left edge through the bulk to the right edge, fully consistent with tight-binding model predictions. Moreover, the strategy of leveraging geometric parameters to linearly and precisely control on-site potentials and couplings is highly effective and universal for designing acoustic metamaterials, and it can be extended to other classical wave systems.
Material property mismatches and interface morphology significantly influence the thermal stress distribution and failure behavior of environmental barrier coatings (EBCs). The finite element method is utilized to investigate the effects of material properties and interface morphologies on the thermal stress distribution in EBCs. The thermal stress behavior during cooling from 1623 K to 298 K is assessed using several rare earth silicates as potential top coat candidates. Three representative interface morphologies: convex, concave, and cosine were analyzed to assess their impact on stress concentration and distribution. Stress profiles were extracted along various paths to characterize the relationship between interface morphology and internal stress behavior. The findings provide critical insights for optimizing material selection and interface design, enabling enhanced durability and prolonged service life of coating systems under extreme thermal conditions.
This work presents a systematic investigation of magnetoelectric (ME) coupling in high-quality MnTiO3 single crystals, a prototypical geometrically frustrated antiferromagnet. X-ray diffraction confirms a pure hexagonal structure with excellent crystallinity. A paramagnetic to antiferromagnetic transition is observed at T-N similar to 64 K, exhibiting significant magnetic anisotropy. The key finding is the direct evidence of bidirectional magnetoelectric coupling: An applied magnetic field induces a sharp anomaly in the c-axis dielectric constant near T-N, while an electric field effectively modulates the magnetization. Specific heat and thermal strain measurements reveal a concomitant structural distortion (a-axis contraction and c-axis elongation) at T-N. Crucially, this distortion is field-independent, ruling out magnetostriction. Our results demonstrate that the magnetoelectric coupling is cooperatively driven by the antiferromagnetic order and the structural phase transition, consistent with spin-lattice coupling or exchange striction mechanisms. This work provides critical insights for the design of multiferroic materials.
Anode-free lithium batteries are limited by irreversible lithium loss and unstable lithium deposition on Cu current collectors. Herein, Cu foil was modified by a simple wet-chemical treatment using 2-mercaptobenzimidazole (MBI) to regulate the Cu/electrolyte interface. X-ray photoelectron spectroscopy suggests that MBI is anchored on the Cu surface through Cu-S and Cu-N interactions, while atomic force microscopy and Kelvin probe force microscopy show that the modification changes the surface roughness and surface potential of Cu foil. Electrochemical measurements show that MBI Cu exhibits a lower lithium nucleation overpotential (26.6 mV), a higher exchange current density (1.64 mA cm-2), and reduced interfacial kinetic barriers compared with Bare Cu. In Li∥Cu half cells, MBI Cu also shows improved plating/stripping reversibility, slower impedance growth, and more compact lithium deposits. In anode-free Cu∥LiFePO4 full cells, MBI Cu delivers an initial discharge capacity of 119.03 mAh g-1 and retains 49.15% of its capacity after 100 cycles, whereas the Bare Cu counterpart retains 20.71% under the same conditions. These results suggest that MBI modification is a simple molecular approach for improving interfacial stability and regulating lithium deposition on Cu current collectors in anode-free lithium batteries.
In this study, SmFe0.6Mn0.4O3 (SFMO) single crystals with orthorhombic perovskite structure were successfully grown using the optical floating zone method. X-ray diffraction combined with Laue back-reflection demonstrates their high crystallographic quality. Magnetic measurements reveal that at ambient pressure, SFMO undergoes a rapid spin-reorientation transition from Γ1 to Γ2 phase within the narrow temperature range of 255–258 K. Application of hydrostatic pressure induces a remarkably anisotropic response in the spin-reorientation behavior. When the applied hydrostatic pressure exceeds approximately 1.03 GPa, distinct weak ferromagnetic signals emerge along the a, b and c axes, unambiguously evidencing a pressure induced modification of the magnetic structure of SFMO, which can be well described by a superposition of the Γ2, Γ3 and Γ4 phases. The constructed pressure–temperature phase diagram further delineates the pressure dependent evolution of the magnetic phase configuration. Collectively, these findings offer essential experimental evidence for understanding spin lattice coupling and multi-phase magnetic competition in perovskite oxides.
The advent of two-dimensional (2D) ferroelectrics offers a new paradigm for device miniaturization and multifunctionality. Recently, 2D α-In2Se3 and related III–VI compound ferroelectrics manifest room-temperature ferroelectricity and exhibit reversible spontaneous polarization even at the monolayer limit. Here, we employ first-principles calculations to investigate group-III selenide van der Waals (vdW) heterojunctions built up by 2D α-In2Se3 and α-Ga2Se3 ferroelectric (FE) semiconductors, including structural stability, electrostatic potential, interfacial charge transfer, and electronic band structures. When the FE polarization directions of α-In2Se3 and α-Ga2Se3 are parallel, both the α-In2Se3/α-Ga2Se3 P↑↑ (UU) and α-In2Se3/α-Ga2Se3 P↓↓ (NN) configurations possess strong built-in electric fields and hence induce electron–hole separation, resulting in carrier depletion at the α-In2Se3/α-Ga2Se3 heterointerfaces. Conversely, when they are antiparallel, the α-In2Se3/α-Ga2Se3 P↓↑ (NU) and α-In2Se3/α-Ga2Se3 P↑↓ (UN) configurations demonstrate the switchable electron and hole accumulation at the 2D ferroelectric interfaces, respectively. The nonvolatile characteristic of ferroelectric polarization presents an innovative approach to achieving tunable n-type and p-type conductive channels for ferroelectric field-effect transistors (FeFETs). In addition, in-plane biaxial strain modulation has successfully modulated the band alignments of the α-In2Se3/α-Ga2Se3 ferroelectric heterostructures, inducing a type III–II–III transition in UU and NN, and a type I–II–I transition in UN and NU, respectively. Our findings highlight the great potential of 2D group-III selenides and ferroelectric vdW heterostructures to harness nonvolatile spontaneous polarization for next-generation electronics, nonvolatile optoelectronic memories, sensors, and neuromorphic computing.