

Surface Template Realizing Oriented Perovskites for Highly Efficient Solar Cells
A surface quasi-2D template is introduced in the two-step fabrication technology to induce an ordered crystallization, enhancing photovoltaic device stability and efficiency. This resulted in 25.79% power conversion efficiency and a 1.188V open-circuit voltage, retaining 90.38% efficiency after 500 h.
Abstract
Formamidinium lead iodide (FAPbI3) perovskite films, ensuring optically active phase purity with uniform crystal orientation, are ideal for photovoltaic applications. However, the optically active α-FAPbI3 phase is easy to degrade into δ-phase due to numerous defects within randomly oriented films. Here, a “quasi-2D” perovskite template is pre-deposited on the film surface within the crystallization process based on the two-step preparation technology, which directly induced pure and highly orientated crystallization of α-FAPbI3 across the downward growth process. Furthermore, the enlarged interaction between 2D components with colloidal properties and lead iodide delayed the crystallization process effectively, yielding high crystallinity with low trap state density. The resulting perovskite photovoltaic devices exhibited a champion efficiency as high as 25.79% with comprehensively improved device stability. This work provides new insights into the utilization of 2D components and the formation mechanism behind 2D perovskites.
Designing Robust Quasi‐2D Perovskites Thin Films for Stable Light‐Emitting Applications
Quasi-2D perovskites are bright light emitter, but are thermodynamically unstable. In this work, it is found that 2D phase are re-distributed upon thermal stress that degrades the emission. To stabilize the 2D phases, a di-amine linker is introduced that can hold the 2D structure strongly that maintains the high emission.
Abstract
Quasi-2D perovskite made with organic spacers co-crystallized with inorganic cesium lead bromide inorganics is demonstrated for near unity photoluminescence quantum yield at room temperature. However, light emitting diodes made with quasi-2D perovskites rapidly degrade which remains a major bottleneck in this field. In this work, It is shown that the bright emission originates from finely tuned multi-component 2D nano-crystalline phases that are thermodynamically unstable. The bright emission is extremely sensitive to external stimuli and the emission quickly dims away upon heating. After a detailed analysis of their optical and morphological properties, the degradation is attributed to 2D phase redistribution associated with the dissociation of the organic spacers departing from the inorganic lattice. To circumvent the instability problem, a diamine is investigated spacer that has both sides attached to the inorganic lattice. The diamine spacer incorporated perovskite film shows significantly improved thermal tolerance over maintaining a high photoluminescence quantum yield of over 50%, which will be a more robust material for lighting applications. This study guides designing quasi-2D perovskites to stabilize the emission properties.
Advancing Room‐Temperature Magnetic Semiconductors with Organic Radical Charge Transfer Cocrystals
Pure organic room-temperature ferromagnetic semiconductors are constructed in organic radical cocrystals by a simple solution-process method. It is suggested that the primary sources of the boosting in magnetic and electrical properties are the enhancement of charge-transfer interactions induced by radicals.
Abstract
Developing purely organic room-temperature magnetic semiconductors has been a long-sought goal in the material community toward the simultaneous control of spin and charge. Organic cocrystals, known for their structural versatility and multifunctionality, are ideal candidates for these magnetoelectric coupling applications. However, organic room-temperature magnetic semiconductor cocrystals have rarely been reported, and their mechanisms remain poorly understood due to the complexity of cocrystal structures. Here, doping organic cocrystals with radicals offers a promising strategy for boosting their magnetism and conductivity while maintaining their cocrystal structures. The fluoranthene-7,7,8,8-tetracyanoquinodimethane radical (FA-HTCNQ•) is constructed through a simple, rapid, and eco-friendly solution-processing approach. The conductive FA-HTCNQ• exhibits excellent room-temperature ferromagnetism with the coercive fields of 96 Oe and the Curie temperature near 400 K, superior to its structural-identical undoped counterpart. Meanwhile, the room-temperature magnetoelectric coupling is demonstrated in the conductive FA-HTCNQ•. The stronger ferromagnetism and conductivity in organic cocrystals are attributed to the enhanced charge-transfer (CT) interactions induced by radicals, rather than the spin exchange interactions between these radicals alone. The research manifests the origin of ferromagnetism in organic cocrystals and provides a simple strategy to fabricate pure organic room-temperature magnetic semiconductor materials for future integrated magnetoelectric devices.
Size‐Controllable High‐Entropy Alloys Toward Stable Hydrogen Production at Industrial‐Scale Current Densities
A high-entropy alloy catalyst capable of stable hydrogen precipitation at current densities of −500 and −1000 mA·cm−2 is successfully developed with negligible activity loss over 100 h. This work offers new insights and approaches for designing HEAs that reliably produce hydrogen at high current densities.
Abstract
Efficient and stable electrocatalytic hydrogen evolution reaction (HER) at high current densities is highly desirable for industrial-scale hydrogen production, which is yet challenging, because of the electrocatalyst with short lifespans during the acidic HER process. Here, a controllable preparation technique is successfully developed to synthesize PdPtRuRhAu high-entropy alloys (HEAs) of various sizes, within the 3.14 nm particles (HEA-3.14) demonstrating exceptional catalytic performance and stable hydrogen production at current densities of −500 and −1000 mA·cm−2 with negligible activity loss over 100 h. Theoretical calculations indicate that the bridge adsorption site of Pd–Au serves as an ideal location for HER, with HEA-3.14 possessing the highest proportion of such sites, reaching 18.97%. To further analyze the thermodynamic stability of HEAs, an element-encoding machine learning model is developed from over 300 000 preprocessed dataset of HEAs that achieving an impressively low RMSE of 58.6 °C and a high R2 value of 0.98. By integrating thermodynamic modeling with machine learning methods, the melting point of the PdPtRuRhAu HEAs at 3.14 nm (366 °C) is predicted, which aligns well with the results obtained from differential scanning calorimetry tests. This work offers new insights and approaches for designing HEAs that reliably produce hydrogen at high current densities.
Woven Cement Slurry
A particle-polymer coalescence strategy is proposed to build balanced particle cohesion, successfully realizing the bending, knotting, coiling, winding, and interlacing of cement slurry for weaving. Beyond the state-of-the-art formwork casting, grouting, and 3D-printing, this cement weaving technology may invoke the construction technology revolution and new material and structure design.
Abstract
Weaving, a pivotal technique in human construction activities since the Neolithic era, remains unattainable in modern concrete construction. Here, a novel particle-polymer coalescence strategy is proposed, which involves electrostatic, bridging, coordinating, and hydrogen bonding interactions, to establish balanced particle cohesion, enabling the fabrication of stretchable cement slurry. The bending, knotting, coiling, winding, and interlacing of cement filaments for structural textiles is successfully realized beyond traditional formwork casting, grouting, and 3D-printing, and fabricate the first-ever Chinese knot woven with cement. Weaving construction builds a triaxially cross-penetrating structure that greatly promotes interlayer strength and toughness by ≈208.5% and 676.5% compared to the state-of-the-art layer-by-layer 3D printed structure. These findings not only make a breakthrough in concrete construction technology but also provide solutions for fabricating multi-directional woven structures with great engineering-application potentials.
Close‐to‐Equilibrium Crystallization for Large‐Scale and High‐Quality Perovskite Single Crystals
A close-to-equilibrium crystallization method that enables the growth of large, high-quality single crystals is proposed. This approach uses independent units for solute supply, crystal growth, and solute recycling, ensuring the system operates at an optimized, steady-state growth point within the solubility phase diagram, maintaining consistent crystal growth even with varying perovskite growth window widths.
Abstract
The growth of large semiconductor crystals is crucial for advancing modern electronics and optoelectronics. While various crystal growth techniques have been developed for lead halide perovskites, a significant challenge remains: as crystal size increases, performance tends to deteriorate dramatically. This study addresses the inherent limitations of perovskite crystal growth by designing a novel strategy for near-equilibrium growth system to maintain optimal conditions throughout the process. The system consists of three independent units: a solution supply unit, a crystal growth unit, and a solution recycling unit, which together ensure a constant solution concentration and temperature. By systematically optimizing temperature control and solution feeding rates, large and high-quality FAPbBr3 single crystals, including a notable crystal measuring 51 × 45 × 10 mm3 are successfully produced. This crystal demonstrates a mobility-lifetime product of 2.83 × 10⁻2 cm2 V⁻¹ and an ultralow detection limit of 319.22 pGyair, significantly surpassing existing perovskite crystals of similar size. The approach can serve as a universal platform for the controlled synthesis of all kinds of perovskite single crystals, laying the foundations for their use in various optoelectronic applications.
Ultrathin Rare‐Earth Oxyhalides as High‐κ van der Waals Layered Dielectrics
A class of ultrathin GdOX with a high dielectric constant and breakdown field strength is synthesized via van der Waals epitaxy. The fabricated MoS2 transistor gated by monocrystalline dielectric exhibits an on/off current ratio exceeding 109 and a near-Boltzmann-limit SS, indicating their tangible applications in 2D electronics.
Abstract
Van der Waals (vdW) dielectrics are extensively employed to enhance the performance of 2D electronic devices. However, current vdW dielectric materials still encounter challenges such as low dielectric constant (κ) and difficulties in synthesizing high-quality single crystals. 2D rare-earth oxyhalides (REOXs) with exceptional electrical properties present an opportunity for the exploration of novel high-κ dielectrics. In this study, for the first time, the synthesis of a series of van der Waals layered gadolinium oxyhalides with thicknesses down to monolayer through a space-confined vdW epitaxy approach and demonstrating their application as a single-crystalline gate dielectric is reported. It exhibits a remarkable relative dielectric constant exceeding 17 and an impressive breakdown field strength of 13.5 MV cm−1. The 2D transistors directly gated by the REOXs layer exhibit enhanced electron mobility and a low interface trap density. An ultrahigh on/off current ratio of 109 and a near-Boltzmann-limit subthreshold swing is achieved. The superior dielectric properties, combined with the universality and scalability of the production method (e.g., millimeter-scale films are achieved), demonstrate that 2D REOXs can serve as promising gate dielectrics for 2D electronics, thereby expanding the study of high-κ vdW materials and potentially providing new opportunities for the development of low-power electronic devices.
Lighting the Path to Precision Healthcare: Advances and Applications of Wearable Photonic Sensors
Wearable photonic sensors offer non-invasive, real-time monitoring of diverse physiological stimuli, revolutionizing personalized healthcare. This review highlights recent advancements in photonic sensing principles, key elements that enhance wearable performance, and their applications in detecting physical signals and monitoring chemical signals in alternative biofluids such as sweat, interstitial fluid, and tears. By exploring these developments, the aim is to provide valuable insights and inspire future innovations in wearable photonic sensor technologies.
Abstract
Recent advancements in wearable photonic sensors have marked a transformative era in healthcare, enabling non-invasive, real-time, portable, and personalized medical monitoring. These sensors leverage the unique properties of light toward high-performance sensing in form factors optimized for real-world use. Their ability to offer solutions to a broad spectrum of medical challenges – from routine health monitoring to managing chronic conditions, inspires a rapidly growing translational market. This review explores the design and development of wearable photonic sensors toward various healthcare applications. The photonic sensing strategies that power these technologies are first presented, alongside a discussion of the factors that define optimal use-cases for each approach. The means by which these mechanisms are integrated into wearable formats are then discussed, with considerations toward material selection for comfort and functionality, component fabrication, and power management. Recent developments in the space are detailed, accounting for both physical and chemical stimuli detection through various non-invasive biofluids. Finally, a comprehensive situational overview identifies critical challenges toward translation, alongside promising solutions. Associated future outlooks detail emerging trends and mechanisms that stand to enable the integration of these technologies into mainstream healthcare practice, toward advancing personalized medicine and improving patient outcomes.
Crystal Structural Editing: Novel Biaxial MgTe2O5 Crystal as Zero‐Order Waveplates
MgTe2O5 with 0D structure has been successfully selected and grown as a waveplate crystal. The MgTe2O5 crystal shows tiny birefringence of 0.0028 in the range from 0.4 to 5 µm with a high laser damage threshold of up to 2.7 GW cm−2. This work provides a novel waveplate crystal and excellent waveplate devices.
Abstract
Waveplates are important optical components to control the polarization of light. Currently, they are often fabricated from uniaxial crystals, and there is no report about waveplates based on the biaxial crystals. In this work, a novel biaxial crystal MgTe2O5 with a structure constructed by 0D Te2O5 groups is designed and grown as waveplate materials for the first time. The exciting result is that the birefringence in the (001)-plane is smaller than 0.0028 in the range from 0.4 to 5 µm, which is significantly smaller than that of the current waveplate materials. The polarization modulations of the MgTe2O5 devices working at 532 nm indicate that excellent zero-order half and quarter waveplates have been successfully prepared. In addition, achromatic waveplates used in the visible, near-infrared, and mid-infrared ranges have also been calculated. The MgTe2O5 crystal not only exhibits a high laser damage threshold of up to 2.7 GW cm−2 but also shows a wide transmission range from 0.37 to 6.3 µm. These results provide an excellent waveplate crystal and explore the applications of biaxial crystals.
Local Structure Distortion in Mn, Zn Doped Cu₂V₂O₇: Supercapacitor Performance and Emergent Spin‐Phonon Coupling
Mn/Zn co-doping in α-Cu₂V₂O₇ induces local structure distortions, enhancing supercapacitor performance (Specific capacitance-1950.95 Fg⁻¹; Energy density-97.54 Whkg⁻¹) and cycling stability. Spin-phonon coupling and superior magnetic properties enable thermo-magnetic applications. A prototype device powers LED bulbs, demonstrating real-world energy storage potential. This work integrates energy storage and spintronics, offering a transformative approach for advanced multifunctional materials.
Abstract
Supercapacitors are rapidly gaining attention as next-generation energy storage devices due to their superior power and energy densities. This study pioneers the investigation of Mn/Zn co-doping in α-Cu₂V₂O₇ (CVO) to enhance its performance as a supercapacitor electrode material. Structural and local Structural properties of Mn/Zn co-doped CVO have been investigated through X-ray Diffraction (XRD), Scanning Electron Microscopy (SEM), Transmission Electron Microscopy (TEM), X-ray Photoelectron Spectroscopy (XPS), and X-ray Absorption Spectroscopy (XAS), revealing significant distortions that enhance supercapacitor performance. The optimized sample demonstrates a remarkable specific capacitance of 1950.95 Fg−1, energy density of 97.54 Whkg−1, and enhanced capacitive retention, attributed to the unique Cu coordination environment and improved charge transfer kinetics. Temperature-dependent Raman spectroscopy unveils spin-phonon coupling (SPC), particularly in VO₄ stretching modes, supported by magnetic measurements that shows a reduction in the Néel temperature and the emergence of zero field-cooled (ZFC) exchange bias (EB). This work is the first to report the impact of local structure distortion on both supercapacitor performance and SPC in CVO, offering a novel strategy for developing high-performance energy storage materials with spintronics potential. In addition, the assembled symmetric optimized supercapacitor shows a high energy density of 93.32 Whkg−1 and excellent cycling stability. A prototype device incorporating the optimized CVO successfully powers eight commercial LED bulbs, demonstrating its practical application potential.
Constructing Anion Solvation Microenvironment Toward Durable High‐Voltage Sodium‐Based Batteries
The anion solvation structure is regulated by constructing a high-salt concentration microenvironment, which maintains highly oxidation-resistant contact ion pairs and ion aggregation. The tailored solvation structure assists in the formation of robust electrode-electrolyte interphase, restraining the electrolyte oxidation and solvent co-intercalation at high voltage, which promotes the rate capability and cycling stability of SDIBs over 10 000 cycles.
Abstract
Sodium-based rechargeable batteries are some of the most promising candidates for electric energy storage with abundant sodium reserves, particularly, sodium-based dual-ion batteries (SDIBs) perform advantages in high work voltage (≈5.0 V), high-power density, and potentially low cost. However, irreversible electrolyte decomposition and co-intercalation of solvent molecules at the electrode interface under a high charge state are blocking their development. Herein, a high-salt concentration microenvironment is created and proposed by tailoring the solvation structures of charge carriers including both cations and anions, which maintains highly oxidation-resistant contact ion pairs and ion aggregates and provides a high ion conductivity. The tailored solvation structure makes a great contribution to protecting the graphite cathode from electrolyte oxidation, solvent co-intercalation, and structural degradation by constructing a robust cathode-electrolyte interphase with standout electrochemical stability. Based on this, the SDIBs achieved an excellent high-voltage cycling stability with 81% capacity retention after 10 000 cycles and the battery showed an improved rate performance with 97.4 mAh g−1 maintained at 100 C. It is identified that regulating anion solvation structure is responsible for the stable interface chemistry and enhanced reaction kinetics, which provides deep insight into the compatibility design between the electrolyte and specialized charge storage in electrodes.
Electroactive Dressing with Selective Sorption of Exudate Enables Treatment of Complicated Wound
Electroactive dressing (cMO/PVA) designed via a facile bilayer composite approach and charging procedure integrates selective sorption, long-term electrical stimulation therapy, and antibacterial properties simultaneously, showing an appealing application prospect for complicated wound repair.
Abstract
Exudate management and cell activity enhancement are vital to complicated wound healing. However, current exudate management dressings indiscriminately remove exudate, which is detrimental to cell activity enhancement. Herein, a novel class of electroactive bilayer (cMO/PVA) dressing is developed by constructing manganese oxide nanoneedle-clusters decorated commercial carbon cloth (MO), in situ casting polyvinyl alcohol (PVA) hydrogel, and finally charging. Benefitting from the hierarchical nanoneedle-cluster structure of MO, abundant active sites are sufficiently exposed to achieve high area-specific capacitances (e.g., 1881.3 mF cm−2), thereby establishing the long-lasting electric field for cMO/PVA dressing. Such a unique cMO/PVA dressing can realize extraordinary selective sorption toward noxious substances over nutrient substances during exudate management. Meanwhile, its long-term electrical stimulation therapy can promote cell proliferation and migration and enhance antibacterial property. As a result, our multifunctional cMO/PVA dressing can rapidly repair full-thickness wounds in type II diabetic rats, offering an advanced strategy for the treatment of complicated wounds.
Observation of Real‐Time Spin‐Orbit Torque Driven Dynamics in Antiferromagnetic Thin Film
Antiferromagnetic dynamics in nanometer-thick LaFeO₃ films is unveiled using time-resolved Kerr effect, demonstrating ultra-low damping and spin-orbit torque manipulation. This study provides an experimental validation of theoretical predictions, offering new insights into nanoscale spintronic systems. The exceptional material quality enables precise probing of dynamics, bridging the gap between antiferromagnetic materials and practical applications in ultrafast spintronics.
Abstract
In the burgeoning field of spintronics, antiferromagnetic materials (AFMs) are attracting significant attention for their potential to enable ultra-fast, energy-efficient devices. Thin films of AFMs are particularly promising for practical applications due to their compatibility with spin-orbit torque (SOT) mechanisms. However, studying these thin films presents challenges, primarily due to the weak signals they produce and the rapid dynamics driven by SOT, that are too fast for conventional electric transport or microwave techniques to capture. The time-resolved magneto-optical Kerr effect (TR-MOKE) has been a successful tool for probing antiferromagnetic dynamics in bulk materials, thanks to its sub-picosecond (sub-ps) time resolution. Yet, its application to nanometer-scale thin films has been limited by the difficulty of detecting weak signals in such small volumes. In this study, the first successful observation of antiferromagnetic dynamics are presented in nanometer-thick orthoferrite films using the pump-probe technique to detect TR-MOKE signal. This paper report an exceptionally low damping constant of 1.5 × 10−4 and confirms the AFM magnonic nature of these dynamics through angular-dependent measurements. Furthermore, it is observed that electrical currents can potentially modulate these dynamics via SOT. The findings lay the groundwork for developing tunable, energy-efficient spintronic devices, paving the way for advancements in next-generation spintronic applications.
Cation‐Vacancy Engineering in Cobalt Selenide Boosts Electrocatalytic Upcycling of Polyester Thermoplastics at Industrial‐Level Current Density
Cation vacancies-vacancies-rich cobalt selenide as electrocatalyst to convert polybutylene terephthalate into succinic acid is crafted, which functions well at industrial-level current density (1.5 A cm−2 @1.477 V vs. RHE). The catalytic mechanism of catalyst and related generality of electrocatalytic upcycling of other polyester thermoplastics are investigated. This work contributes to propel current research frontier of utilization of low-value carbon resources.
Abstract
The past decades have witnessed the increasing accumulation of plastics, posing a daunting environmental crisis. Among various solutions, converting plastics into value-added products presents a significant endeavor. Here, an electrocatalytic upcycling route that efficiently converts waste poly(butylene terephthalate) plastics into high-value succinic acid with high Faradaic efficiency of 94.0% over cation vacancies-rich cobalt selenide catalyst is reported, showcasing unprecedented activity (1.477 V vs. RHE) to achieve an industrial-level current density of 1.5 A cm−2, and featuring a robust operating durability (≈170 h). In particular, when combining butane-1,4-diol monomer oxidation (BOR) with hydrogen evolution using the cation vacancy-engineered cobalt selenide as bifunctional catalyst, a relatively low cell voltage of 1.681 V is required to reach 400 mA cm−2, manifesting an energy-saving efficiency of ≈15% compared to pure water splitting. The mechanism and reaction pathways of BOR over the vacancies-rich catalyst are first revealed through theoretical calculations and in-situ spectroscopic investigations. The generality of this catalyst is evidenced by its powerful electrocatalytic activity to other polyester thermoplastics such as poly(butylene succinate) and poly(ethylene terephthalate). These electrocatalytic upcycling strategies can be coupled with the reduction of small molecules (e.g., H2O, CO2, and NO3 −), shedding light on energy-saving production of value-added chemicals.
Lattice‐Strain Engineering of High‐Entropy‐Oxide Nanoparticles: Regulation by Flame Spray Pyrolysis with Ultrafast Quenching
This study introduces a continuous-flow flame spray pyrolysis method for tuning lattice strain in high-entropy-oxide nanoparticles. By varying the cooling rates of quenching, tensile strain increases by 2.75%, enhancing oxygen evolution reaction performance with a 25 mV reduction in overpotential at a current density of 10 mA cm−2. This approach facilitates efficient mass production and precise control of lattice strain.
Abstract
The lattice-strain engineering of high-entropy-oxide nanoparticles (HEO-NPs) is considered an effective strategy for achieving outstanding performance in various applications. However, lattice-strain engineering independent of the composition variation still confronts significant challenges, with existing modulation techniques difficult to achieve mass production. Herein, a novel continuous-flow synthesis strategy by flame spray pyrolysis (FSP) is proposed, which air varying flow rates is introduced for fast quenching to alter the cooling rate and control the lattice strain of HEO-NPs. Experimental results demonstrate that as the flow rate of air increases from 0 L to 24 L min−1, the cooling rate has increased by more than ten times, and the tensile strain of the HEO-NPs increases by 2.75%. Utilizing the oxygen evolution reaction (OER) activity as an indicator, it is observed that the overpotential to achieve a current density of 10 mA cm−2 is reduced by 25 mV. Importantly, this approach enables the simple and efficient regulation of lattice strain in HEO-NPs (110 mg min−1). Thus, this study provides a new approach for both the mass production and regulation of lattice strain in HEO-NPs.
Coaxial Direct Ink Writing of Cholesteric Liquid Crystal Elastomers in 3D Architectures
A low-viscosity cholesteric liquid crystal (CLC) ink and a silicone ink are prepared for coaxial direct ink writing of 3D strain sensors. The silicone shell supports the CLC core to enable layer-by-layer printing in addition to enhancing the mechanical properties of the core. Monostable and bistable thin-shell domes are printed to demonstrate the 3D printing capabilities and mechanochromic behaviors.
Abstract
Cholesteric liquid crystal elastomers (CLCEs) hold great promise for mechanochromic applications in anti-counterfeiting, smart textiles, and soft robotics, thanks to the structural color and elasticity. While CLCEs are printed via direct ink writing (DIW) to fabricate free-standing films, complex 3D structures are not fabricated due to the opposing rheological properties necessary for cholesteric alignment and multilayer stacking. Here, 3D CLCE structures are realized by utilizing coaxial DIW to print a CLC ink within a silicone ink. By tailoring the ink compositions, and thus, the rheological properties, the cholesteric phase rapidly forms without an annealing step, while the silicone shell provides encapsulation and support to the CLCE core, allowing for layer-by-layer printing of self-supported 3D structures. As a demonstration, free-standing bistable thin-shell domes are printed. Color changes due to compressive and tensile stresses can be witnessed from the top and bottom of the inverted domes, respectively. When the domes are arranged in an array and inverted, they can snap back to their base state by uniaxial stretching, thereby functioning as mechanical sensors with memory. The additive manufacturing platform enables the rapid fabrication of 3D mechanochromic sensors thereby expanding the realm of potential applications for CLCEs.
Nucleation‐Controlled Crystallization of Chiral 2D Perovskite Single Crystal Thin Films for High‐Sensitivity Circularly Polarized Light Detection
A nucleation-controlled strategy is developed, to grow Dion−Jacobson phase 2D chiral perovskite single crystal thin films (SCTFs), from water-air interface, with a novel chiral ligand, (R/S)-3-Aminopyrrolidine. The obtained ultrathin SCTFs, with shortened spacing between inorganic layers, exhibit reduced exciton binding energy and enhanced carrier transport. In results, photodetectors based on the SCTFs show superior sensitivity to the circularly polarized light.
Abstract
2D Dion−Jacobson (DJ) chiral perovskite materials exhibit significant promise for developing high-performance circularly polarized light (CPL) photodetectors. However, the inherently thick nature of DJ-phase 2D perovskite single crystal limits their ability to differentiate CPL photons with the two opposite polarization states. In addition, the growth of DJ-phase perovskite single crystal thin films (SCTFs) has proven challenging due to the strong interlayer electronic coupling. Here, a nucleation-controlled strategy is employed to grow a novel DJ-phase perovskite [(R/S)-3APr]PbI4 [(R/S)-3APr = (R/S)-3-Aminopyrrolidine] SCTFs with large area, low thickness and hence high aspect ratios. Structural and photoluminescence analyses reveal that introducing the divalent organic cations into the perovskite framework reduce the interlayer distance, resulting in low exciton binding energy. This facilitates charge separation and transport. The resulting SCTF photodetector showcases excellent detection performance with anisotropy factor for photocurrent as high as 0.65, responsivity of 1.97 A W−1, detectivity of 5.3 × 1013 Jones, and 3-dB frequency of 2940 Hz, demonstrating its potential as a promising candidate for CPL-sensitive photodetectors. This novel approach, therefore, provides a framework for the growth of DJ-phase perovskite SCTFs and advances their applications in sensitive CPL photodetection.
Influence of Free Space on Lithium Growth Behavior at Open Surfaces and Internal Cracks of Sulfide‐Based Solid Electrolyte
Lithium growth follows two modes within the crack of argyrodite sulfide solid electrolyte: 1) Diffusion creep enabled infiltration along the crack side-wall surface toward the counter electrode, allowing the deposited lithium to cause short circuit without fully filling the crack; 2) Columnar growth perpendicular to the crack side-wall surface toward the free space inside the crack.
Abstract
Lithium dendrite penetration through solid electrolyte has been the major obstacle for practical sulfide-based all-solid-state lithium metal batteries (ASSLMBs). Herein, a series of tailored model solid cells are designed to investigate the intrinsic lithium growth behavior at open surfaces and internal cracks of sulfide solid electrolyte. It is shown that when plating lithium on the open surface of electrolyte (free space), the lithium exhibits an intrinsic columnar growth behavior perpendicular to the electrolyte surface, preferentially along the (110) crystal axis. When plating lithium within the internal cracks (confined free space), the growth of lithium follows two major modes: 1) Diffusion creep enabled infiltration along the crack side-wall surface toward the counter electrode, allowing the deposited lithium to cause short circuit without fully filling the crack; 2) Columnar growth perpendicular to the crack side-wall surface toward the confined free space inside the crack. The extent of lithium ingress into electrolyte under external pressure in the initial state is found to determine the rate of lithium infiltration after applying the current. As a further validation, intact sintered electrolytes with 99% relative density minimize initial lithium ingress, enabling lithium plating at 6.37 mA cm−2 with an areal capacity exceeding 76 mAh cm−2 without short circuit.
Nanomagnetism Triggering Carriers Double‐Resistance Conduction and Excellent Flexible Thermoelectrics
Nanomagnetism-triggered double-resistance conduction greatly enhances thermoelectric performance of Bi0.5Sb1.5Te3/epoxy films with a maximum zT of 1.44 at 320 K, providing insights into magnetism-enhanced thermoelectrics.
Abstract
Nanomagnetism may enable electrical conductivity and Seebeck coefficient to be decoupled and can potentially lead to remarkable enhancements in thermoelectric (TE) performance, however, their physical mechanisms have not been explored. Herein, it is shown that the nanomagnetism from Fe and Fe3O4 nanoparticles embedded in Bi0.5Sb1.5Te3/epoxy flexible films can lead to the carriers splitting into spin-up and spin-down conductive branches with different resistances and mobilities due to the exchange interaction between the spin of carriers and the nanomagnetism. The double-resistance conduction of carriers may well explain the decoupling of electrical conductivity and Seebeck coefficient and their simultaneous enhancements in the thermo-electro-magnetic flexible films. It is further shown that the maximum dimensionless figure of merit of the thermo-electro-magnetic flexible films reaches between 1.2 and 1.4 at room temperature, and their five-level cascaded device based on the films achieves a temperature drop of 3.1 K through in-plane heat dissipation, making a new record for printing flexible TE films and devices. The double-resistance conduction of carriers also reveals a deep physical mechanism for magneto-enhanced TE performance of bulk thermoelectrics.
PerC B‐Cells Activation via Thermogenetics‐Based CXCL12 Generator for Intraperitoneal Immunity Against Metastatic Disseminated Tumor Cells
An isotropic-porous, cell-fitting, thermogenetics-based chemokine CXCL12 generator is described as a B-cell-dependent intraperitoneal immunotherapy that can trigger intraperitoneal anti-tumor immunity against metastatic disseminated tumor cell to assuage peritoneal effusion and peritoneal metastasis. Unexpectedly, the peritoneal cavity B cell subset is identified as playing a key role in exogenous antigen presentation and presenting a unique transcriptional signature.
Abstract
During cancer peritoneal metastasis (PM), conventional antigen-presenting cells (dendritic cells, macrophages) promote tumorigenesis and immunosuppression in peritoneal cavity. While intraperitoneal immunotherapy (IPIT) has been used in clinical investigations to relieve PM, the limited knowledge of peritoneal immunocytes has hindered the development of therapeutic IPIT. Here, a dendritic cell-independent, next-generation IPIT is described that activates peritoneal cavity B (PerC B) cell subsets for intraperitoneal anti-tumor immunity via exogenous antigen presentation. The PerC B-cell-involved IPIT framework consists of an isotropic-porous, cell-fitting, thermogenetics-based CXCL12 generator. Such nanoscale thermal-confined generator can programmatically fine-tune the expression of CXCL12 to recruit disseminated tumor cells (DTCs) through CXCL12-CXCR4 axis while avoiding cytokine storm, subsequently release DTC-derived antigen to trigger PerC B-cell-involved immunity. Notably, antigen-presenting B-cell cluster, expressing the regulatory signaling molecules Ptpn6, Ms4a1, and Cd52, is identified playing the key role in the IPIT via single-cell RNA sequencing. Moreover, such IPIT availably assuages peritoneal effusion and PM in an orthotopic gastric cancer and metastatic model. Overall, this work offers a perspective on PerC B-cell-involved antigen-presenting in intraperitoneal immunity and provides a configurable strategy for activating anti-DTC immunity for next-generation IPIT.