Topological spin texture in the pseudogap phase of a high-Tc superconductor.

An outstanding challenge in condensed-matter-physics research over the past three decades has been to understand the pseudogap (PG) phenomenon of the high-transition-temperature (high-Tc) copper oxides. A variety of experiments have indicated a symmetry-broken state below the characteristic temperature T* (refs. 1-8). Among them, although the optical study5 indicated the mesoscopic domains to be small, all these experiments lack nanometre-scale spatial resolution, and the microscopic order parameter has so far remained elusive. Here we report, to our knowledge, the first direct observation of topological spin texture in an underdoped cuprate, YBa2Cu3O6.5, in the PG state, using Lorentz transmission electron microscopy (LTEM). The spin texture features vortex-like magnetization density in the CuO2 sheets, with a relatively large length scale of about 100 nm. We identify the phase-diagram region in which the topological spin texture exists and demonstrate the ortho-II oxygen order and suitable sample thickness to be crucial for its observation by our technique. We also discuss an intriguing interplay observed among the topological spin texture, PG state, charge order and superconductivity.

Transformation of 2D Flakes to 3D Hollow Bowls: Matthew Effect Enables Defects to Prevail in Electromagnetic Wave Absorption of Hollow rGO Bowls.

High-efficiency electromagnetic (EM) wave (EMW)-absorbing materials have attracted extensive scientific and technical interest. Although identifying the dominant EM loss mechanism in dielectric-loss materials is indispensable, it is challenging due to a complex synergism between dipole/interfacial polarization and conduction loss. Modulation of defects and microstructures can be a possible approach to determine the dominant EM loss mechanism and realize high-efficiency absorption. Herein, 2D reduced graphene oxide (rGO) flakes are integrated into a 3D hollow bowl-like structure, which increases defect sites (i.e., oxygen vacancy and lattice defect) and reduces the stacked thickness of rGO. Despite their lower stacked thicknesses, the hollow rGO bowls with more defects exhibit lower conductivities but higher permittivities. Accompanied by the transformation from 2D flakes to 3D hollow bowls, the dominant EM loss mechanism of rGO transforms from conduction loss to defect-induced polarization. Furthermore, the defect engineering and structural design endow rGO with well-matched impedance and strong EMW-absorbing capacity. A minimum reflection loss of -41.6 dB (1.3 mm) and an effective absorption bandwidth of 4.8 GHz (1.5 mm) is achieved at a filler loading of 5 wt%. This study will provide meaningful insights into the development of materials with superior EMW-absorbing performances via defect engineering and structural design.

Integrating Sulfur Doping with a Multi-Heterointerface Fe7S8/NiS@C Composite for Wideband Microwave Absorption.

Heterointerface engineering is presently considered a valuable strategy for enhancing the microwave absorption (MA) properties of materials via compositional modification and structural design. In this study, a sulfur-doped multi-interfacial composite (Fe7S8/NiS@C) coated with NiFe-layered double hydroxides (LDHs) is successfully prepared using a hydrothermal method and post-high-temperature vulcanization. When assembled into twisted surfaces, the NiFe-LDH nanosheets exhibit porous morphologies, improving impedance matching, and microwave scattering. Sulfur doping in composites generates heterointerfaces, numerous sulfur vacancies, and lattice defects, which facilitate the polarization process to enhance MA. Owing to the controllable heterointerface design, the unique porous structure induced multiple heterointerfaces, numerous vacancies, and defects, endowing the Fe7S8/NiS@C composite with an enhanced MA capability. In particular, the minimum reflection loss (RLmin) value reached -58.1 dB at 15.8 GHz at a thickness of 2.1 mm, and a broad effective absorption bandwidth (EAB) value of 7.3 GHz is achieved at 2.5 mm. Therefore, the Fe7S8/NiS@C composite exhibits remarkable potential as a high-efficiency MA material owing to the synergistic effects of the polarization processes, multiple scatterings, porous structures, and impedance matching.

Fixed-Point Atomic Regulation Engineered Low-Thickness Wideband Microwave Absorption.

Atomic doping is widely employed to fine-tune crystal structures, energy band structures, and the corresponding electrical properties. However, due to the difficulty in precisely regulating doping sites and concentrations, establishing a relationship between electricity properties and doping becomes a huge challenge. In this work, a modulation strategy on A-site cation dopant into spinel-phase metal sulfide Co9S8 lattice via Fe and Ni elements is developed to improve the microwave absorption (MA) properties. At the atomic scale, accurately controlling doped sites can introduce local lattice distortions and strain concentration. Tunned electron energy redistribution of the doped Co9S8 strengthens electron interactions, ultimately enhancing the high-frequency dielectric polarization (ɛ' from 10.5 to 12.5 at 12 GHz). For the Fe-doped Co9S8, the effective absorption bandwidth (EAB) at 1.7 mm increases by 5%, and the minimum reflection loss (RLmin) improves by 26% (EAB = 5.8 GHz, RLmin = -46 dB). The methodology of atomic-scale fixed-point doping presents a promising avenue for customizing the dielectric properties of nanomaterials, imparting invaluable insights for the design of cutting-edge high-performance microwave absorption materials.

Controllable Synthesis of Highly Symmetrical Streamlined Structure for Wideband Microwave Absorption.

Highly symmetrical and streamlined nanostructures possessing unique electron scattering, electron-phonon coupling, and electron confinement characteristics have attracted a lot of attention. However, the controllable synthesis of such a nanostructure with regulated shapes and sizes remains a huge challenge. In this work, a peanut-like MnO@C structure, assembled by two core-shell nanosphere is developed via a facile hydrogen ion concentration regulation strategy. Off-axis electron holography technique, charge reconstruction, and COMSOL Multiphysics simulation jointly reveal the unique electronic distribution and confirm its higher dielectric sensitive ability, which can be used as microwave absorption to deal with currently electromagnetic pollution. The results reveal that the peanut-like core-shell MnO@C exhibits great wideband properties with effective absorption bandwidth of 6.6 GHz, covering 10.8-17.2 GHz band. Inspired by this structure-induced sensitively dielectric behavior, promoting the development of symmetrical and streamlined nanostructure would be attractive for many other promising applications in the future, such as piezoelectric material and supercapacitor and electromagnetic shielding.

Wrinkle Structure Regulating Electromagnetic Parameters in Constructed Core-shell ZnFe2O4@PPy Microspheres as Absorption Materials.

Structure engineering of magnetic-dielectric multi-components is emerging as an effective approach for presuming high-performance electromagnetic (EM) absorption, but still faces bottlenecks due to the ambiguous regulation mechanism of surface morphology. Here, a novel wrinkled surface structure is tailored on the ZnFe2O4 microsphere via a spray-pyrolysis induced Kirkendall diffusion effect, the conductivity of the sample is affected, and a better impedance matching is adjusted by modulating the concentration of metal nitrate precursors. Driven by a vapor phase polymerization, conductive polypyrrole (PPy) shell are in situ decorated on the ZnFe2O4 microsphere surfaces, ingeniously constructing a core-shell ZnFe2O4@PPy composites. Moreover, a systematic investigation reveals that this unique wrinkled surface structure is highly dependent on the metal salt concentration. Optimized wrinkle ZnFe2O4@PPy composite exhibits a minimum reflection loss (RLmin) reached -41.0 dB and the effective absorption bandwidth (EAB) can cover as wide as 4.1 GHz. The enhanced interfacial polarization originated from high-density ZnFe2O4-PPy heterostructure, and the conduction loss of PPy contributes to the boosted dielectric loss capability. This study gives a significant guidance for preparing high-performance EM composites by tailoring the surface wrinkle structure.

Metal Valence State Modulation Strategy to Design Core@shell Hollow Carbon Microspheres@MoSe2/MoOx Multicomponent Composites for Anti-Corrosion and Microwave Absorption.

The exploitation of multicomponent composites (MCCs) has become the main pathway for obtaining advanced microwave absorption materials (MAMs). Herein, a metal valence state modulation strategy is proposed to tune the electromagnetic (EM) parameters and improve microwave absorption performances. Core@shell hollow carbon microspheres@MoSe2 and hollow carbon microspheres@MoSe2/MoOx MCCs with various mixed-valence states content are well-designed and produced by a simple hydrothermal reaction or/and heat treatment process. The results reveal that the thermal treatment of hollow carbon microspheres@MoSe2 in Ar and Ar/H2 leads to the in situ formation of MoOx and multivalence state, respectively, and the enhanced content of Mo4+ in the designed MCCs greatly boosts their impedance matching characteristics, polarization, and conduction loss capacities, which lead to their evidently improved EM wave absorption properties. Amongst, the as-prepared hollow carbon microspheres@MoSe2/MoOx MCCs achieve an effective absorption bandwidth of 5.80 GHz under a matching thickness of 1.97 mm and minimum reflection loss of -21.49 dB. Therefore, this work offers a simple and universal method to fabricate core@shell hollow carbon microspheres@MoSe2/MoOx MCCs, and a novel and feasible metal valence state modulation strategy is proposed to develop high-efficiency MAMs.

Porous Co3O4/NiO@C Chains Assembled from Nanosheets with Excellent Lithium Storage Performance.

Carbon layers-coated porous Co3O4/NiO (denoted as PCNO@C) chains are synthesized by the facile solvothermal method and subsequently annealing treatment under an Ar atmosphere, which are assembled from numerous Co3O4/NiO nanosheets. Benefiting from the unique porous chain structure, the volume change of the electrode is greatly relieved during the long-term cycling processes, and then an excellent cycling stability is obtained (the reversible specific capacity of the 1000th cycle can reach 637.3 mA h g-1 at 5000 mA g-1). Besides, a continuous conductive network is constructed by the coated carbon layers and long chains, the movement rate of electrons is effectively accelerated, and the high rate capability is obtained (the high reversible specific capacity of 480.6 mA h g-1 is retained at 10,000 mA g-1). This work contributes a new idea to construct porous chain structure anode materials.

Insight into Surface Electronic Effects on Pd Nanostructures as Efficient Electrocatalysts.

Although the unique properties of nanomaterials have endowed enzyme-mimic catalysts with broad applications, the development of catalysts still relies on trial-and-error strategies without predictive indicators. Surface electronic structures have rarely been studied in enzyme-mimic catalysts. Herein, we present a platform for understanding the impact of surface electronic structures on electrocatalysis toward H2O2 decomposition, using the Pd icosahedra (Pd ico), Pd octahedra (Pd oct) and Pd cubic nanocrystals as electrocatalysts. The electronic properties on Pd were modulated with a correlation of surface orientation. We revealed the relationship between the electronic properties and electrocatalytic performance, in which the surface electron accumulation can boost the electrocatalytic activity of the enzyme-mimic catalysts. As a result, the Pd icodimer exhibits the highest electrocatalytic and sensing efficiency. This work offers new perspectives for the investigation of structure-activity relationships and provides an effective knob for utilizing the surface electronic structures to boost the catalytic performance for enzyme-mimics.

Functional Tailoring of Multi-Dimensional Pure MXene Nanostructures for Significantly Accelerated Electromagnetic Wave Absorption.

Transition metal carbide (Ti3 C2 Tx MXene), with a large specific surface area and abundant surface functional groups, is a promising candidate in the family of electromagnetic wave (EMW) absorption. However, the high conductivity of MXene limits its EMW absorption ability, so it remains a challenge to obtain outstanding EMW attenuation ability in pure MXene. Herein, by integrating HF etching, KOH shearing, and high-temperature molten salt strategies, layered MXene (L-MXene), network-like MXene nanoribbons (N-MXene NRs), porous MXene monolayer (P-MXene ML), and porous MXene layer (P-MXene L) are rationally constructed with favorable microstructures and surface states for EMW absorption. HF, KOH, and KCl/LiCl are used to functionalize MXene to tune its microstructure and surface state (F- , OH- , and Cl- terminals), thereby improving the EMW absorption capacity of MXene-based nanostructures. Impressively, with the unique structure, proper electrical conductivity, large specific surface area, and abundant porous defects, MXene-based nanostructures achieve good impedance matching, dipole polarization, and conduction loss, thus inheriting excellent EMW absorption performance. Consequently, L-MXene, N-MXene NRs, P-MXene ML, and P-MXene L enable a reflection loss (RL ) value of -43.14, -63.01, -60.45, and -56.50 dB with a matching thickness of 0.95, 1.51, 3.83, and 4.65 mm, respectively.

Phase Transition Induced via the Template Enabling Cocoon-like MoS2 an Exceptionally Electromagnetic Absorber.

Structural engineering via the template method is efficient for micro-nano assembling. However, only structural design and lack of composition control restrict their advanced application. To overcome this issue, applying a template to simultaneously realize the structural design and fine component control is highly desired, which has been ignored. In this study, a spinel-shaped MoS2 heterostructure with controlled phase ratios of 1H and 2H phase is developed using the AlOOH template method. This work demonstrates that the MoS2 phase transition mechanism from 2H to 1T is substantially attributed to the close exposed crystal's surface and approximately accordant surface energy. The superiority and additional proof are provided based on density-functional theory simulation, transmission electron microscope holography, etc. With an effective absorptance region of 6.3 GHz under a thickness of 1.4 mm, the reported samples present outstanding microwave absorption capacity. This is attributed to the beneficial coupled effect between the well-designed structure and phase regulation. This work offers valuable insights into structural engineering and component regulation template methods.

An Ion-Engineering Strategy to Design Hollow FeCo/CoFe2 O4 Microspheres for High-Performance Microwave Absorption.

Although assembled hollow architectures have received considerable attention as lightweight functional materials, their uncontrollable self-aggregation and tedious synthetic methods hinder precise construction and modulation. Therefore, this study proposes a bi-ion synergistic regulation strategy to design assembled hollow-shaped cobalt spinel oxide microspheres. Dominated by the coordination-etching effects of F- and the hydrolysis-complex contributions of NH4 + , the unique construction is formed attributed to the dynamic cycles between metal complexes and precipitates. Meanwhile, their basic structures are perfectly retained after reduction treatment, enabling FeCo/CoFe2 O4 bimagnetic system to be obtained. Subsequently, in-depth analyses are conducted. Investigations reveal that multiscale magnetic coupling networks and enriched air-material heterointerfaces contribute to the remarkable magnetic-dielectric behavior, supported by the advanced off-axis electron holography technique. Consequently, the obtained FeCo/CoFe2 O4 composites exhibit excellent microwave absorption performances with minimal reflection losses (RLmin ) as high as -51.6 dB, an effective absorption bandwidth (EAB) of 4.7 GHz, and a matched thickness of 1.4 mm. Thus, this work provides an informative guide for rationally assembling building blocks into hollow architectures as advanced microwave absorbers through bi-ion and even multi-ion synergistic engineering mechanisms.

Exceptionally Bifunctional ORR/OER Performance via Synergistic Atom-Cluster Interaction.

The single-atom sites (SAs) have achieved enhanced performance toward oxygen reduction reaction (ORR) with the effective utilization of the active sites. However, the excess adsorption of the intermediates and the limited stability hinders performance improvement. Metal clusters with promising stability and weak adsorption can be used as potential substitutions, but the lack of active sites is considered undesirable for catalytic reactions. Herein, a framework of Fe nanoclusters combined with SAs on One dimensional (1D) carbon nanotubes (Fe3 C-NCNTs 90 min CC-1 ) is synthesized to confirm the synergistic atom-cluster interaction. The composite exhibits strong polarization and electron redistribution between nanocluster and SAs. The electron redistribution will significantly boost the electron transport and the desorption of the intermediates, which is confirmed by off-axis holography and DFT calculation. The electrocatalytic performance is significantly enhanced as the half-wave potential of ORR increased 75 mV and the potential of OER increased 133 mV compared with the sample without nanoclusters. Furthermore, such a bifunctional catalyst endows homemade Zn-air batteries (ZABs) with high power density and long-term stability. This work paves a facile route to design bifunctional ORR/OER electrocatalysts consisting of 0D composite structures.

Temperature Effects on Electrochemical Energy-Storage Materials: A Case Study of Yttrium Niobate Porous Microspheres.

Lithium-ion batteries (LIBs) are very popular electrochemical energy-storage devices. However, their applications in extreme environments are hindered because their low- and high-temperature electrochemical performance is currently unsatisfactory. In order to build all-climate LIBs, it is highly desirable to fully understand the underlying temperature effects on electrode materials. Here, based on a novel porous-microspherical yttrium niobate (Y0.5 Nb24.5 O62 ) model material, this work demonstrates that the operation temperature plays vital roles in electrolyte decomposition on electrode-material surfaces, electrochemical kinetics, and crystal-structure evolution. When the operation temperature increases, the reaction between the electrolyte and the electrode material become more intensive, causing the formation of thicker solid electrolyte interface (SEI) films, which decreases the initial Coulombic efficiency. Meanwhile, the electrochemical kinetics becomes faster, leading to the larger reversible capacity, higher rate capability, and more suitable working potential (i.e., lower working potential for anodes and higher working potential for cathodes). Additionally, the maximum unit-cell-volume change becomes larger, resulting in poorer cyclic stability. The insight gains here can provide a universal guide for the exploration of all-climate electrode materials and their modification methods.

Engineering Phase to Reinforce Dielectric Polarization in Nickel Sulfide Heterostructure for Electromagnetic Wave Absorption.

Engineering phase transition in micro-nanomaterials to optimize the dielectric properties and further enhance the electromagnetic microwave absorption (EMA) performance is highly desirable. However, the severe synthesis conditions restrict the design of EMA materials featuring controllable phases, which hinders the tunability of effective absorption bandwidth (EAB) and leads to an unclear loss mechanism. Herein, a seed phase decomposition-controlled strategy is proposed to induct nickel sulfide (NiSx ) absorbers with controllable phases and hollow sphere nature. Transmission electron microscopy holography and theoretical calculations evidence that the reconstruction of atoms in phase transition induces numerous heterogeneous interfaces and lattice defects/sulfur vacancies to cause varied work functions and local electronic redistribution, which contributes to reinforced dielectric polarization. As a result, the optimized NiS2 /NiS heterostructure enables enhanced EM attenuation capability with a wide EAB of 5.04 GHz at only 1.6 mm, compared to that of NiS2 and NiS. Moreover, the correlation between EAB and NiS phase content is demonstrated as the "volcano" feature. This study on the concept of phase transition of micro-nanomaterials can offer a novel approach to constructing highly efficient absorbers for EMA and other functionalities.

Graphene Oxide-Wrapped Porous Hollow Co3O4 Microspheres with Enhanced Lithium Storage Performance.

Porous hollow Co3O4 microspheres wrapped with graphene oxide were synthesized by a step solvothermal method and subsequent heat treatment. Benefiting from the design of special porous hollow microspheres, the effective specific surface area was greatly increased, the sufficient contact between the porous hollow Co3O4 microspheres and electrolyte was achieved, and then a charge specific capacity of 888.59 mA h g-1 was gained. Meanwhile, partial stress from the charging/discharging process was greatly relieved due to the abundant pores and hollow structure, excellent cycling stability was realized, and the charge specific capacity of the 1000th cycle was 465.75 mA h g-1 at 5 C (1 C = 890 mA g-1). In addition, the conductivity of Co3O4 microspheres was effectively improved due to the tight package of graphene oxide to Co3O4 microspheres, and superior rate performance was attained (280.99 mA h g-1 at 10 C).

Graphene Oxide-Wrapped Co3O4/NiO Micron Flowers as an Anode of Lithium-Ion Batteries with Enhanced Rate Performance and Cycling Stability.

A graphene oxide-wrapped Co3O4/NiO (denoted as CNO/GO) micron flower is successfully synthesized by a rapid solvothermal method, which is formed through interpenetrating nanosheets. Nanosheets with a large specific surface area expose a large number of active sites for an electrochemical reaction. Moreover, abundant pores formed during the interpenetration of nanosheets are instrumental in providing enough buffer space to relieve the large volume expansion from the repeated lithium insertion/delithiation processes, and the tightly wrapped GO can effectively sustain the stability of the CNO micron flower structure during the long-term cycle processes. The reversible specific capacity as high as 602.9 mA h g-1 is maintained after 800 cycles at 5000 mA g-1. In addition, GO with good conductivity can greatly enhance the conductivity of CNO micron flowers, accelerate the transfer of electrons, and then achieve a high rate performance (the reversible specific capacity is 570.2 mA h g-1 at 10 000 mA g-1). This work provides a viable method for synthesizing the CNO micron flowers as a promising high-performance transition metal oxide anode for lithium-ion batteries.

Current-Induced Magnetic Skyrmions with Controllable Polarities in the Helical Phase.

We report the current-induced creation of magnetic skyrmions in a chiral magnet FeGe nanostructure by using in situ Lorentz transmission electron microscopy. We show that magnetic skyrmions with controllable polarity can be transferred from the helical ground state simply by controlling the direction of the current flow at zero magnetic fields. The force analysis and symmetry consideration, backed up by micromagnetic simulations, well explain the experimental results, where magnetic skyrmions are created because of the edge instability of the helical state in the presence of spin-transfer torque. The on-demand generation of skyrmions and control of their polarity by electric current without the need for a magnetic field will enable novel purely electric-controlled skyrmion devices.

Anisotropic Self-Assembly of Asymmetric Mesoporous Hemispheres with Tunable Pore Structures at Liquid-Liquid Interfaces.

Asymmetric materials have attracted tremendous interest because of their intriguing physicochemical properties and promising applications, but endowing them with precisely controlled morphologies and porous structures remains a formidable challenge. Herein, a facile micelle anisotropic self-assembly approach on a droplet surface is demonstrated to fabricate asymmetric carbon hemispheres with a jellyfish-like shape and radial multilocular mesostructure. This facile synthesis follows an interface-energy-mediated nucleation and growth mechanism, which allows easy control of the micellar self-assembly behaviors from isotropic to anisotropic modes. Furthermore, the micelle structure can also be systematically manipulated by selecting different amphiphilic triblock copolymers as a template, resulting in diverse novel asymmetric nanostructures, including eggshell, lotus, jellyfish, and mushroom-shaped architectures. The unique jellyfish-like hemispheres possess large open mesopores (∼14 nm), a high surface area (∼684 m2 g-1), abundant nitrogen dopants (∼6.3 wt %), a core-shell mesostructure and, as a result, manifest excellent sodium-storage performance in both half and full-cell configurations. Overall, our approach provides new insights and inspirations for exploring sophisticated asymmetric nanostructures for many potential applications.

Constructing Unique Mesoporous Carbon Superstructures via Monomicelle Interface Confined Assembly.

Constructing hierarchical three-dimensional (3D) mesostructures with unique pore structure, controllable morphology, highly accessible surface area, and appealing functionality remains a great challenge in materials science. Here, we report a monomicelle interface confined assembly approach to fabricate an unprecedented type of 3D mesoporous N-doped carbon superstructure for the first time. In this hierarchical structure, a large hollow locates in the center (∼300 nm in diameter), and an ultrathin monolayer of spherical mesopores (∼22 nm) uniformly distributes on the hollow shells. Meanwhile, a small hole (4.0-4.5 nm) is also created on the interior surface of each small spherical mesopore, enabling the superstructure to be totally interconnected. Vitally, such interconnected porous supraparticles exhibit ultrahigh accessible surface area (685 m2 g-1) and good underwater aerophilicity due to the abundant spherical mesopores. Additionally, the number (70-150) of spherical mesopores, particle size (22 and 42 nm), and shell thickness (4.0-26 nm) of the supraparticles can all be accurately manipulated. Besides this spherical morphology, other configurations involving 3D hollow nanovesicles and 2D nanosheets were also obtained. Finally, we manifest the mesoporous carbon superstructure as an advanced electrocatalytic material with a half-wave potential of 0.82 V (vs RHE), equivalent to the value of the commercial Pt/C electrode, and notable durability for oxygen reduction reaction (ORR).