Free-space-addressable optical resonators with high quality factors () and wavelength-to-subwavelength mode volumes () enhance light-matter interactions in sensing, nonlinear optics, and quantum photonics. However, exper...Free-space-addressable optical resonators with high quality factors () and wavelength-to-subwavelength mode volumes () enhance light-matter interactions in sensing, nonlinear optics, and quantum photonics. However, experimental factors in this mode volume regime remain limited to ∼10 because existing asymmetry-driven designs couple geometric and optical perturbation components, constraining access to high- regimes. Here, we show that independently tuning these two asymmetry axes unlocks a biaxial radiative landscape with iso- contours connecting geometrically and optically distinct perturbations of equivalent . We demonstrate this framework in very-large-scale-integrated Si nanoantenna pixel (VINPix) resonators with 35-150 nm out-of-plane perturbations of amorphous Si, SiN, and SiO. Experimentally, we achieve up to 76 000 at of ∼1.7 λ across arrays of >80 resonators in water. Computationally, slotted VINPix resonators reach of >10 at of ∼0.2 λ. This biaxial framework establishes a generalizable design strategy for ultrahigh- free-space nanophotonic resonators.
We address the connection between negative electronic friction and non-Markovian effects in the nonadiabatic vibrational dynamics of molecules interacting with metal surfaces under nonequilibrium conditions. We show that...We address the connection between negative electronic friction and non-Markovian effects in the nonadiabatic vibrational dynamics of molecules interacting with metal surfaces under nonequilibrium conditions. We show that a generic nonequilibrium mechanism leading to negative Markovian electronic friction, where molecular vibrations couple directly to inelastic electronic transitions, also introduces significant non-Markovian contributions to the electronic friction. To demonstrate these ideas, we investigate nonequilibrium charge transport through a molecular nanojunction containing a vibrationally coupled donor-acceptor model, where negative electronic friction reflects driving of the vibrational mode beyond standard Joule heating. By comparison to numerically exact, fully quantum hierarchical equations of motion simulations, we verify that these non-Markovian effects have a significant impact on the nonequilibrium dynamics and even on the stability of the resulting Langevin equation.
Lithium metal batteries (LMBs) are one of the most promising candidates for next-generation energy storage due to their high energy density. However, their practical use is limited by a major performance drop at low temp...Lithium metal batteries (LMBs) are one of the most promising candidates for next-generation energy storage due to their high energy density. However, their practical use is limited by a major performance drop at low temperatures, because of high desolvation energy barriers and the uncontrolled growth of lithium dendrites, which eventually leads to the formation of "dead lithium". This review aims to explain, from a mechanistic perspective, how electrolyte additives address these challenges at low temperatures. A clear mechanistic understanding is achieved by classifying modern additives into four behavioral types: decomposition, sustained-release, suspension, and adsorption. We also focus on how advanced tools are utilized to see these hidden interfacial processes in their native state. Finally, we propose a multidimensional design framework that combines orbital engineering, entropy regulation, and mechanical toughness. Translating these molecular-level insights into macroscopic interfacial stability gives way to accelerating the realization of reliable, extreme-condition lithium metal batteries.
Conductive polymer thermoelectric fibers, featuring inherent flexibility and weavability, hold great promise for wearable generation in smart clothing. However, balancing their thermoelectric and mechanical properties re...Conductive polymer thermoelectric fibers, featuring inherent flexibility and weavability, hold great promise for wearable generation in smart clothing. However, balancing their thermoelectric and mechanical properties remains a critical challenge, restricting operational stability under mechanical deformation in wearable scenarios. Herein, we propose a novel wet-spinning strategy involving Ca-induced rapid gelation to fabricate high-performance PEDOT:PSS thermoelectric fibers. Ca-induced structural regulation optimized carrier transport, elevating the otherwise low Seebeck coefficient of PEDOT:PSS to 47.82 ± 1.04 μV·K while retaining high electrical conductivity of 197.71 ± 7.83 S·cm. More importantly, Ca can electrostatically anchor polymer chains, increasing cross-linking to form a tough network structure that improves both mechanical strength (140.37 ± 3.82 MPa) and fracture strain (29.14 ± 0.68%). The optimized fibers achieved synergistic thermoelectric-mechanical properties and a 0.05 K high temperature sensitivity. Integrated into smart gloves, these fibers enable temperature monitoring and heat-prevention warning, demonstrating significant potential for safeguarding the health and safety of disabled persons.
We present a tunable microfabrication pipeline for creating robust, reflective inserts that adapt conventional commercial imaging chambers for single-objective light sheet (LS) illumination. This system reduces the compl...We present a tunable microfabrication pipeline for creating robust, reflective inserts that adapt conventional commercial imaging chambers for single-objective light sheet (LS) illumination. This system reduces the complexity associated with dual-objective LS setups and specialized LS chambers while retaining the native functionality and biocompatibility of the original chambers. The fabricated insert features a metalized, 3D nanoprinted micromirror with an angled reflective surface, enabling alignment of a thin LS for sectioning and imaging throughout mammalian cells. Using this pipeline, we demonstrate that single-objective LS illumination achieves an over 4X improvement in the signal-to-background ratio compared with conventional widefield epi-illumination in both fixed and live cell samples. Furthermore, we show substantial resolution enhancement for single-molecule localization microscopy compared to epi-illumination for improved imaging at the nanoscale. The versatile and scalable design offers an easily implemented approach to bring the benefits of single-objective LS microscopy to a wide array of biological studies.
Given the limited efficiency of geometric optimization in enhancing formic acid dehydrogenation (FAD), advancing Pd-based catalysts requires deeper insight into electronic structural regulation. Here, we developed a cata...Given the limited efficiency of geometric optimization in enhancing formic acid dehydrogenation (FAD), advancing Pd-based catalysts requires deeper insight into electronic structural regulation. Here, we developed a catalytic system confined within metal-nitrogen-doped carbon supports (Pd@MNC) and applied machine learning to innovatively establish a multiparameter correlation model integrating intrinsic kinetic barriers () with diverse descriptors. Unlike traditional single-factor analyses, our findings unravel the central role of electronic structure engineering (48% relative importance) over geometric tunability (12%) in regulating catalytic kinetics, with the d-band center offset (, 30%) and Pd(II) proportion (, 18%) accounting for the electronic contribution. Validated experimentally via Co and Cr doping, this theory-based machine learning framework offers a predictive paradigm for rational catalyst design and activity trend. Ultimately, this multidimensional electronic regulation strategy elevates FAD performance while providing broad applicability for accelerating other critical Pd-catalyzed processes, such as Suzuki coupling and CO reduction reactions.
Selector-only memory (SOM) based on ovonic threshold switches is a promising candidate for dense cross-point memory by integrating selector and memory functions in a single two-terminal device. However, the physical orig...Selector-only memory (SOM) based on ovonic threshold switches is a promising candidate for dense cross-point memory by integrating selector and memory functions in a single two-terminal device. However, the physical origins of off-state conduction and threshold voltage () modulation remain unclear. Here, we investigate these mechanisms in a Te-rich Ge-Sb-Se-Te:Sn SOM by correlating DC transport, low-frequency noise (LFN), and materials analyses. DC - characteristics analyzed using Poole-Frenkel (PF) emission and trap-assisted tunneling (TAT) models reveal identical trap energy levels across prefirst firing, low-, and high- states, indicating a common trap species with state-dependent spatial redistribution. LFN measurements distinguish PF- and TAT-dominated regimes and show consistent state-dependent noise behavior. Cross-sectional energy-dispersive X-ray spectroscopy reveals electric-field-polarity-dependent Te redistribution near the top electrode, while ab initio calculations identify Te-Te dimer defects as acceptor-like deep traps governing off-state conduction. These results provide a unified mechanism for modulation in Te-based SOM devices.
Aqueous conversion-type batteries hold great promise for safe, low-cost, and high-energy storage, yet selenium (Se) cathodes are limited by the mismatch between their high redox potential and the narrow electrochemical s...Aqueous conversion-type batteries hold great promise for safe, low-cost, and high-energy storage, yet selenium (Se) cathodes are limited by the mismatch between their high redox potential and the narrow electrochemical stability window of aqueous electrolytes. Here, we report the first aqueous manganese-selenium battery that overcomes this limitation via the intrinsic hydrolysis acidity of Mn-based cations, eliminating the need for organic additives. This enables a highly reversible dual-phase conversion between Se, MnSe, and MnSe, effectively unlocking multi-electron reactions. Electrolyte anions critically regulate the reaction pathway: Cl induces soluble species and shuttle effects, while OTf stabilizes the interface. Consequently, The Mn-Se battery delivers a high initial capacity of 621 mAh g, retaining 501 mAh g after 1200 cycles and achieving a record-high energy density of 414 Wh kg, surpassing all previously reported aqueous manganese-metal batteries. This work provides valuable insights into the rational design of high-reversibility conversion-type cathode materials.
Materials with a Kagome lattice are intensely studied because they host exotic states that combine strong correlations and topology. Recently, critical current oscillations were observed in an unstructured flake of CsVSb...Materials with a Kagome lattice are intensely studied because they host exotic states that combine strong correlations and topology. Recently, critical current oscillations were observed in an unstructured flake of CsVSb. In this work, we show that the origin of these oscillations is a network of Josephson junctions intrinsic to the flake that emerges below its critical temperature. Under radio frequency radiation, we observe quantized Shapiro steps. The sensitivity of the step height to the contact placement indicates a complex network of junctions. By performing interference studies along multiple field directions, we demonstrate that the interference effects are a result of small junctions and filamentary supercurrent flow. Upon nanostructuring the flake, prominent features of the interference pattern are preserved, illustrating the localized nature of these junctions and their stability to thermal cycles. These results pave the way for determining the exact nature of superconductivity in the AVSb family.
High-resolution computed tomography (CT) is indispensable for noninvasive diagnostics. However, X-/γ-ray scintillators are fragile and easily damaged during the complex pixelation required to achieve maximum light output...High-resolution computed tomography (CT) is indispensable for noninvasive diagnostics. However, X-/γ-ray scintillators are fragile and easily damaged during the complex pixelation required to achieve maximum light output. Here, we report a large-area (43 × 30 cm) composite elastomer scintillator fabricated via low-cost solution processes for durable CT imagers. Synergistic dynamic covalent and noncovalent bonds enable efficient, thermally assisted self-healing of the composite film from diverse forms of damage (e.g., frost cracking, charring, scratching, and solvent swelling), thereby restoring >94% of its initial radioluminescence. Remarkably, this recovery is highly sustainable, with negligible radioluminescence degradation even after multiple damage-healing cycles. Furthermore, the composite film achieves ultrahigh spatial resolutions of 188.7 lp/cm (MTF = 0.2) and 235.2 lp/cm (MTF = 0.1) at a low effective dose of 0.33 mSv. This combination of robustness and high resolution contributes to processing fault tolerance, cost control, and enhancing imaging clarity.
Anode-free lithium metal batteries (ALMBs) are promising candidates for next-generation high-energy-density storage devices. However, conventional Cu current collectors (Cu-CC) suffer from nonuniform Li plating/stripping...Anode-free lithium metal batteries (ALMBs) are promising candidates for next-generation high-energy-density storage devices. However, conventional Cu current collectors (Cu-CC) suffer from nonuniform Li plating/stripping because of their poor lithiophilicity. Here, we report mechanochemical synthesis of diboron carbon (BC) for the first time, a material previously predicted only theoretically, and tune its electrical conductivity from as-grown ∼0.01-0.05 S cm to C-rich BC ∼0.23-0.28 S cm, enabling its application as a functional current-collector in ALMBs. Pristine BC exhibits anode-like electrochemical behavior, whereas increasing the carbon content (B:C from 64.3:35.7 to 47.4:52.6 weight%) shifts its function toward a current-collector-like electrode that supports reversible Li plating/stripping while minimizing Li loss. Anode-free full cells using C-rich BC deliver ∼500 stable cycles with an average Coulombic efficiency of ∼94%, markedly outperforming Cu-based cells. These findings identify C-rich BC as an effective alternative to conventional Cu-CC in ALMBs.
Controlling the epitaxial state in quasi-van der Waals heterostructures remains challenging because weak interfacial guidance often favors free epitaxy. Here, we show that light irradiation during sputtering drives FeN/m...Controlling the epitaxial state in quasi-van der Waals heterostructures remains challenging because weak interfacial guidance often favors free epitaxy. Here, we show that light irradiation during sputtering drives FeN/mica from a free-epitaxy state to a locked-epitaxy state. Under dark growth, the film adopts the FeN(001) with a bulk-like lattice constant and rotationally degenerate in-plane alignment, characteristic of free-epitaxy. Under illumination, the system follows a locked-epitaxy pathway and forms FeN(111)/mica with a specific in-plane registry and finite in-plane strain. Timing-, wavelength-, and intensity-dependent experiments show that this transition is established during the earliest stage of growth. Density functional theory calculations further reveal that the FeN(001)/mica interface is mainly vdW-dominated, whereas the FeN(111)/mica interface is stabilized by a much stronger non-vdW contribution, dominated by chemically specific interaction. These results establish optical modulation of interfacial coupling as a practical route toward free-to-locked epitaxy in quasi-vdW heterostructures.
Antisymmetric longitudinal resistance (ALR) is a striking transport anomaly in perpendicularly magnetized multilayers, but its microscopic origin remains under debate. Here, we demonstrate that ALR originates from an ano...Antisymmetric longitudinal resistance (ALR) is a striking transport anomaly in perpendicularly magnetized multilayers, but its microscopic origin remains under debate. Here, we demonstrate that ALR originates from an anomalous Hall effect-induced local potential difference created by the asymmetric distribution of magnetic domains in the current-voltage intersection region. Combining multiprobe transport measurements with in situ magneto-optical Kerr imaging, we establish a direct correlation between ALR and the domain distribution in Pt/Co multilayers. We use a femtosecond laser to precisely write magnetic domains with different area fractions, thereby demonstrating that the ALR amplitude is determined by the area fraction of reversed domains within the current-voltage intersection region. Moreover, by suppressing interlayer spin-coherent transport in a spin-valve structure, we achieve a layer-resolved ALR response. Our findings clarify the microscopic origin of ALR and reveal its potential for multilevel memory and three-dimensional spintronic architectures.
In poly(ethylene oxide) (PEO)-based solid-state Li-S batteries (SSLSBs), the stepwise sulfur redox reaction enables smooth energy delivery. However, concentrated polysulfides severely hinder Li transport and induce rapid...In poly(ethylene oxide) (PEO)-based solid-state Li-S batteries (SSLSBs), the stepwise sulfur redox reaction enables smooth energy delivery. However, concentrated polysulfides severely hinder Li transport and induce rapid performance degradation during cycling. Herein, we report a spatially decoupling strategy for sulfur redox and Li transport by introducing poly(vinylidene fluoride) (PVDF) into the PEO matrix. Due to the intrinsic low affinity of PVDF toward sulfur species, polysulfides dissolution is effectively suppressed within the PVDF phase, enabling continuous Li transport when the PEO phase is clogged by accumulated polysulfides. By regulation of phase separation and Li coordination in the PEO-PVDF hybrid, a Li conductive network is established within the PVDF phase, while the PEO phase preserves stepwise sulfur redox. As a result, the SSLSBs deliver a high initial capacity of 1402 mAh g at 0.08 C. Even at 0.2 C, a stable capacity of ∼560 mAh g is maintained over 90 cycles.
The emergence of multiferroic order in perovskite thin films is governed by symmetry-broken coupling between polar domains and magnetic order parameters; however, currently prevailing theoretical frameworks, due to a con...The emergence of multiferroic order in perovskite thin films is governed by symmetry-broken coupling between polar domains and magnetic order parameters; however, currently prevailing theoretical frameworks, due to a constraint of reduced-dimensional approximations, fail to capture the inherent three-dimensional (3D) complexity of domain-mediated cross-correlations. Here, performing atomic-resolution HAADF/iDPC-STEM on BiFeO (BFO), we discover a "pseudo-ferroelectric domain wall" bridging (1)/(0) planes of BFO, in which two-dimensional (2D) projection indicates a domain-wall angle of 54.37°, but the actual 3D orientation remains 70.17°. When the (1) plane is rotated 90° about the [2] axis, it reveals the atomic arrangement of the (0) plane, with polarization along [00]. These noncanonical 3D walls arise from oxygen-rearrangement-induced structural deviations and asymmetric Fe-O lattice coupling, which generate chiral polarization stabilized by a potent tripartite interaction between ferroelectric, shear, and spin degrees of freedom. This work provides a design principle for reconfigurable domain wall nanoelectronics.
The formation of epitaxial heterostructures between ionic halide perovskite and covalent chalcogenide semiconductor nanocrystals critically depends on interfacial coordination environments. Heteronucleation of chalcogeni...The formation of epitaxial heterostructures between ionic halide perovskite and covalent chalcogenide semiconductor nanocrystals critically depends on interfacial coordination environments. Heteronucleation of chalcogenides on perovskite facets therefore requires precise control over reaction parameters, and most reported such systems rely on a shared Pb-based sublattice. Here, we report epitaxial plasmonic-semiconductor perovskite-chalcogenide CsPbBr-CuSe nanocrystal heterostructures which do not share any common ions and are obtained with nucleation of CuSe on preferred facets of CsPbBr nanocrystals. This integration quenches the host photoluminescence but induces the plasmonic features yielding near-infrared absorption around ∼1000 nm. A cation-dominated synthetic pathway, in which copper precursor incorporation precedes selenium injection, suppresses undesired PbSe nucleation. High-resolution electron microscopy confirms favorable lattice matching and epitaxial growth at the interface. These results demonstrate that reaction chemistry can be engineered to access hybrid nanostructures of ionic and covalent interfaces and result in functional nanocrystal heterostructures.
Zinc-based sulfides are promising anodes for sodium-ion batteries (SIBs) due to their high theoretical capacities and low costs. However, inferior structural stability under high current densities leads to severe volume...Zinc-based sulfides are promising anodes for sodium-ion batteries (SIBs) due to their high theoretical capacities and low costs. However, inferior structural stability under high current densities leads to severe volume expansion and rapid capacity fading. Herein, a series of Se-doped, carbon-coated ZnS (ZnSSe@C) anodes with various vacancy levels are designed. Se doping and vacancy engineering modulate the band structure of ZnS and lift the p-band center of sulfur, thereby weakening Zn-S bonds, strengthening Na-S interactions, and accelerating reaction kinetics. The optimized ZnSSe@C anode delivers an exceptional rate capability of 328.7 mAh g at 30 A g and maintains a remarkable capacity of 372.4 mAh g over 2200 cycles at 10 A g. Particularly, the sodium-ion full cell exhibits superior rate capacity and long-term cycling stability. These findings provide new insights into enhancing sodium-ion storage performance through controlled doping and vacancy engineering to regulate the p-band center of sulfur.
Solid oxide electrolysis cells (SOECs) enable efficient high-temperature electrochemical CO conversion, yet cathode performance is limited by insufficient surface reactivity and bulk transport. Herein, we report a couple...Solid oxide electrolysis cells (SOECs) enable efficient high-temperature electrochemical CO conversion, yet cathode performance is limited by insufficient surface reactivity and bulk transport. Herein, we report a coupled engineering strategy to enhance surface reactivity and bulk transport of Ce-based cathodes via rational dual-metal (Co, Fe) incorporation. The resulting CoFe-incorporated Gd-doped ceria (CoFe-GDC) exhibits enriched surface Ce-oxygen vacancy (Ce-) motifs and improved bulk transport. A single cell with the CoFe-GDC cathode achieves a current density of 1.88 A cm (2.20 A cm with a thinner 250 μm electrolyte) at 800 °C under 1.6 V and demonstrates stable operation for 580 h. Mechanistic studies reveal that Fe promotes CO adsorption, activation, and dissociation via enriched Ce- motifs and active Fe sites, whereas Co lowers the oxygen migration barrier and narrows the bandgap, overcoming bulk transport limitations. This work provides a cost-effective design for high-performance ceria-based cathodes by coupling surface reactivity with bulk transport.
Electrons in high-mobility graphene devices have demonstrated great potential in establishing an electronic analogue of relativistic quantum fluid in solid-state systems. Over the past decade, complex device geometries h...Electrons in high-mobility graphene devices have demonstrated great potential in establishing an electronic analogue of relativistic quantum fluid in solid-state systems. Over the past decade, complex device geometries have been employed to enable experimental detection of viscous electronic flow; however, the observations have been found to be sensitive to the device architecture and fabrication process, raising questions about the signature of electron hydrodynamics itself. Here, we present a study on multiple ultraclean graphene field-effect transistors (FETs) in a rectangular four-terminal device architecture. Using electrical transport measurements, we have examined variation of the electrical resistance of FETs in the doped regime as a function of the carrier density and temperature. Our results reveal strong device-dependent variability, attributed to competing momentum-conserving and momentum-relaxing scattering mechanisms. Further, we have proposed a phenomenological method for analyzing the results, yielding transport parameters consistent with recent theory and experiments.
Graphene/metal oxide heterointerfaces are widely used in electrochemical and optoelectronic devices, yet their stability in electrolyte environments remains poorly understood. Here, we show that phosphate is not a passiv...Graphene/metal oxide heterointerfaces are widely used in electrochemical and optoelectronic devices, yet their stability in electrolyte environments remains poorly understood. Here, we show that phosphate is not a passive background species at the graphene-ITO interface. Low-angle rotational interferometric scattering microscopy directly visualizes spontaneous delamination of graphene from ITO in acidic phosphate electrolytes, whereas chloride, sulfate, and nitrate do not induce comparable behavior. The delamination kinetics depend strongly on phosphate concentration and pH and are quantitatively described by a modified extended-area model with Poisson correction. Spectroscopy, contact angle, ion-dissolution, and density functional theory analyses support a mechanism in which phosphate associates with surface In sites, promotes selective indium dissolution, and weakens graphene-ITO adhesion. These results identify an anion-specific interfacial failure pathway in a graphene/oxide heterointerface.