Pressure-Tuned Intrinsic Anomalous Hall Conductivity in Kagome Magnets RV_(6)Sn_(6)(R=Gd,Tb)

Exploration of exotic phenomena in magnetic topological systems is at the frontier of condensed matter physics,holding a significant promise for applications in topological spintronics.However,complex magnetic structures carrying nontrivial topological properties hinder its progresses.Here,we investigate the pressure effect on the novel topological kagome magnets GdV_(6)Sn_(6) and TbV_(6)Sn_(6) to dig out the interplay between magnetic Gd/Tb layers and nonmagnetic V-based kagome sublattice.The pressure-tuned magnetic transition temperature Tm in both the compounds exhibit a turning point at the critical pressure P_(c),accompanied with a sign reversal in anomalous Hall effect(AHE).The separation of intrinsic and extrinsic contributions using the Tian-Ye-Jin scaling model suggests that the intrinsic mechanism originating from the electronic Berry curvature holds the priority in the competition with extrinsic mechanism in AHE.The above-mentioned findings can be attributed to the combined effect of pressure-tuned band topology and magnetic interaction in segregated layers.Our results provide a practical route to design and manipulate the intrinsic AHE in magnetic topological materials.

Pressure-Tunable Large Anomalous Hall Effect in Ferromagnetic Metal LiMn_(6)Sn_(6)

Recently, giant intrinsic anomalous Hall effect(AHE) has been observed in the materials with kagome lattice.Here, we systematically investigate the influence of high pressure on the AHE in the ferromagnet LiMn_(6)Sn_(6) with clean Mn kagome lattice. Our in situ high-pressure Raman spectroscopy indicates that the crystal structure of LiMn_(6)Sn_(6) maintains a hexagonal phase under high pressures up to 8.51 GPa. The anomalous Hall conductivity(AHC) σ_(xy)^(A) remains around 150 Ω^(-1)·cm^(-1), dominated by the intrinsic mechanism. Combined with theoretical calculations, our results indicate that the stable AHE under pressure in Li Mn_(6)Sn_(6) originates from the robust electronic and magnetic structure.

Ultrafast Carbonized Wood of Electrode-Scaled Aligned-Porous Structure for High-Performance Lithium Batteries

The use of carbonized wood in various functional devices is attracting considerable attention due to its low cost,vertical channels,and high electrical conduction.However,the conventional carbonization method requires a long processing time and an inert atmosphere.Here,a microwave-assisted ultrafast carbonization technique was developed that carbonizes natural wood in seconds without the need for an inert atmosphere,and the obtained aligned-porous carbonized wood provided an excellent electrochemical performance as an anode material for lithium-ion batteries.This ultrafast carbonization technique simultaneously produced ZnO nanoparticles during the carbonization process that were uniformly distributed on the alignedporous carbon.The hierarchical structure of carbonized wood functionalized with ZnO nanoparticles was used as a host for achieving high-performance lithium-sulfur batteries:the highly conductive carbonized wood framework with vertical channels provided good electron transport pathways,and the homogeneously dispersed ZnO nanoparticles effectively adsorbed lithium polysulfide and catalyzed its conversion reactions.In summary,a new method was developed to realize the ultrafast carbonization of biomass materials with decorated metal oxide nanoparticles.

Pressure-Induced Superconductivity in the Charge-Density-Wave Compound LaTe_(2-x)Sb_(x)(x=0 and 0.4)

Magnetic CeTe_(2)achieving superconductivity under external pressure has received considerable attention.The intermingling of 4f and 5d electrons from Ce raised the speculation of an unconventional pairing mechanism arising from magnetic fluctuations.Here,we address this speculation using a nonmagnetic 4f-electron-free LaTe_(2)as an example.No structural phase transition can be observed up to 35 GPa in the in situ synchrotron diffraction patterns.Subsequent high-pressure electrical measurements show that LaTe_(2)exhibits superconductivity at20 Gpa with its T_(c)(4.5 K)being two times higher than its Ce-counterpart.Detailed theoretical calculations reveal that charge transfer from the 4p orbitals of the planar square Te-Te network to the 5d orbitals of La is responsible for the emergence of superconductivity in LaTe_(2),as confirmed by Hall experiments.Furthermore,we study the modulation of q_(CDW)by Sb substitution and find a record high T_(c)^(onset)~6.5 K in LaTe_(1.6)Sb_(0.4).Our work provides an informative clue to comprehend the role of 5d-4p hybridization in the relationship between charge density wave(CDW)and superconductivity in these RETe_(2)(RE=rare-earth elements)compounds.

Quantum Oscillations in Noncentrosymmetric Weyl Semimetal SmAlSi

As a new type of quantum state of matter hosting low energy relativistic quasiparticles,Weyl semimetals(WSMs)have attracted significant attention for scientific community and potential quantum device applications.In this study,we present a comprehensive investigation of the structural,magnetic,and transport properties of noncentrosymmetric RAl Si(R=Sm,Ce),which have been predicted to be new magnetic WSM candidates.Both samples exhibit nonsaturated magnetoresistance,with about 900%and 80%for Sm Al Si and Ce Al Si,respectively,at temperature of 1.8 K and magnetic field of 9 T.The carrier densities of Sm Al Si and Ce Al Si exhibit remarkable change around magnetic transition temperatures,signifying that the electronic states are sensitive to the magnetic ordering of rare-earth elements.At low temperatures,Sm Al Si reveals prominent Shubnikov–de Haas oscillations associated with the nontrivial Berry phase.High-pressure experiments demonstrate that the magnetic order is robust and survival under high pressure.Our results would yield valuable insights into WSM physics and potentials in applications to next-generation spintronic devices in the RAl Si(R=Sm,Ce)family.

Pressure-induced reemergence of superconductivity in BaIr_(2)Ge_(7)and Ba_(3)Ir_(4)Ge_(16)with cage structures

Clathrate-like or caged compounds have attracted great interest owing to their structural flexibility,as well as their fertile physical properties.Here,we report the pressure-induced reemergence of superconductivity in BaIr2Ge7 and Ba3Ir4Ge16,two new caged superconductors with two-dimensional building blocks of cage structures.After suppression of the ambient-pressure superconducting(SC-I)states,new superconducting(SC-II)states emerge unexpectedly,with Tc increased to a maximum of 4.4 and 4.0 K for BaIr2Ge7 and Ba3Ir4Ge16,respectively.Combined with high-pressure synchrotron x-ray diffraction and Raman measurements,we propose that the reemergence of superconductivity in these caged superconductors can be ascribed to a pressure-induced phonon softening linked to cage shrinkage.

Application of Auger electron spectroscopy in lithium-ion conducting oxide solid electrolytes

Garnet-type oxide solid electrolytes are the critical materials for all-solid-state lithium ion batteries.Nanoscale spectroscopic analysis on solid electrolytes plays a key role in bridging the gap between microstructure and properties.In this work,Auger electron spectroscopy(AES),which can directly detect lithium element and distinguish its valence state,was applied to characterize the garnet-type Li_(6.4)La_(3)Zr_(1.4)Ta_(0.6O12)(LLZTO).Different spectroscopy parameters were evaluated and optimal acquisition conditions were provided.Electron induced precipitation of lithium metal from LLZTO was observed.By exploring the influence factors of precipitation and combining transmission electron microscopy(TEM)and focused ion beam(FIB)experiments,the underlying mechanism of the phenomenon was revealed and previous controversy was resolved.The analysis method was also extended to other types of solid electrolytes,and this work provides a reference for future in-depth research on the structure-property relationship of solid electrolytes using AES.

Cu/Mo2C synthesized through Anderson-type polyoxometalates modulate interfacial water structure to achieve hydrogen evolution at high current density

The development of efficient non-precious metal catalysts is important for the large-scale application of alkaline hydrogen evolution reaction(HER).Here,we synthesized a composite catalyst of Cu and Mo_(2)C(Cu/Mo_(2)C)using Anderson-type polyoxometalates(POMs)synthesized by the facile soaking method as precursors.The electronic interaction between Cu and Mo_(2)C drives the positive charge of Cu,alleviating the strong adsorption of hydrogen at the Mo site by modulating the d-band center of Mo_(2)C.By studying the interfacial water structure using in situ attenuated total reflection surface-enhanced infrared absorption spectroscopy(ATR-SEIRAS),we determined that the positively charged Cu crystals have the function of activating water molecules and optimizing the interfacial water structure.The interfacial water of Cu/Mo_(2)C contains a large amount of free water,which could facilitate the transport of reaction intermediates.Due to activated water molecules and optimized interfacial water structure and hydrogen adsorption energy,the overpotential of Cu/Mo_(2)C is 24 mV at a current density of 10 mA·cm^(-2) and 178 mV at a current density of 1000 mA·cm^(-2).This work improves catalyst performance in terms of interfacial water structure optimization and deepens the understanding of water-mediated catalysis.

Post-synthesis and structural evolution of hollow titanium silicalite-1 with solvent-free method

Generating hollow structure inside titanium silicalite-1(TS-1)is a widely used method to improve its liquid-phase oxidation catalytic performance in industry.However,traditional dissolution-recrystallization method usually required a large amount of aqueous solution of organic template,leading to unfavorable polluted waste,low production efficiency,and high manufacture cost.Here,a facile and environmental friendly strategy was proposed for the post-synthesis of hollow TS-1 zeolite with a solventfree method utilizing NH4HCO3 and tetrapropylammounium bromide as selective etching agents,which reduced the usage of organic template and avoided the liquid waste.The high crystallinity,the microporous structure,and the active Ti sites were preserved at a high product yield(>93%).The formation mechanism of hollow structure was also investigated by exploring effects of different reactants and experimental parameters.Meanwhile,the obtained hollow TS-1 showed an outstanding performance in the epoxidation of 1-hexene in comparison to the parent zeolite.

In-situ growth of low-dimensional perovskite-based insular nanocrystals for highly efficient light emitting diodes

Regulation of perovskite growth plays a critical role in the development of high-performance optoelectronic devices.However,judicious control of the grain growth for perovskite light emitting diodes is elusive due to its multiple requirements in terms of morphology,composition,and defect.Herein,we demonstrate a supramolecular dynamic coordination strategy to regulate perovskite crystallization.The combined use of crown ether and sodium trifluoroacetate can coordinate with A site and B site cations in ABX_(3) perovskite,respectively.The formation of supramolecular structure retard perovskite nucleation,while the transformation of supramolecular intermediate structure enables the release of components for slow perovskite growth.This judicious control enables a segmented growth,inducing the growth of insular nanocrystal consist of low-dimensional structure.Light emitting diode based on this perovskite film eventually brings a peak external quantum efficiency up to 23.9%,ranking among the highest efficiency achieved.The homogeneous nano-island structure also enables high-efficiency large area(1 cm^(2))device up to 21.6%,and a record high value of 13.6%for highly semi-transparent ones.

通过热愈合方法回收被锂枝晶刺穿的石榴石型固态电解质

固态锂金属电池(SSLMBs)因其高安全性和潜在的高能量密度引起了广泛的兴趣.然而,锂枝晶在固态电解质中的生长严重阻碍了SSLMBs的实际应用.在本文中,我们开发了一种简单的方法,通过热处理修复和回收被锂枝晶刺穿的石榴石氧化物电解质.与初始对照样相比,回收后的石榴石电解质表现出更高的相对密度、离子电导率和临界电流密度.热愈合是基于树突状锂枝晶和空气间的反应产物,其有助于在热处理过程中石榴石电解质的进一步致密化.这项工作为石榴石型固态电解质的回收利用开辟了一条新的途径.

Microwave heating as a universal method to transform confined molecules into armchair graphene nanoribbons

Armchair graphene nanoribbons(AGNRs)with sub-nanometer width are potential materials for the fabrication of novel nanodevices thanks to their moderate direct band gaps.AGNRs are usually synthesized by polymerizing precursor molecules on substrate surface.However,it is time-consuming and not suitable for large-scale production.AGNRs can also be grown by transforming precursor molecules inside single-walled carbon nanotubes(SWCNTs)via furnace annealing,but the obtained AGNRs are normally twisted.In this work,microwave heating is applied for transforming precursor molecules into AGNRs.The fast heating process allows synthesizing the AGNRs in seconds.Several different molecules were successfully transformed into AGNRs,suggesting that it is a universal method.More importantly,as demonstrated by Raman spectroscopy,aberrationcorrected high-resolution transmission electron microscopy and theoretical calculations,less twisted AGNRs are synthesized by the microwave heating than the furnace annealing.Our results reveal a route for rapid production of AGNRs in large scale,which would benefit future applications in novel AGNRs-based semiconductor devices.

Pressure-Induced Intermetallic Charge Transfer and Semiconductor- Metal Transition in Two-Dimensional AgRuO_(3)

The intricate correlation between charge degrees of freedom and physical properties is a fascinating area of research in solid state chemistry and condensed matter physics.Herein,we report on the pressureinduced successive charge transfer and accompanied resistive evolution in honeycomb layered ruthenate AgRuO_(3).Structural revisiting and spectroscopic analyses affirm the ilmenite type R-3 structure with mixed valence cations as Ag^(+1/+2)Ru^(+4/+5)O_(3) at ambient pressure.In-situ pressure-and temperature-dependent resistance variation reveals a successive insulatormetal-insulator transition upon pressing,accompanied by unprecedented charge transfer between Ag and Ru under applied pressure,and a further structural phase transition in the insulator region at higher pressure.These phenomena are also corroborated by in-situ pressure-dependent Raman spectra,synchrotron X-ray diffraction,bond valence sums,and electronic structure calculations,emphasizing the dominated rare Ag2+,and near zero thermal expansion in the ab-plane in the metallic zone mostly due to the Jahn-Teller effect of d9-Ag2+.The multiple electronic instabilities in AgRuO_(3) may offer new possibilities toward novel and unconventionally physical and chemical behaviors in strongly correlated honeycomb lattices.

Absolute Structure Determination of Chiral Organic Nanocrystals Using Zone-Axis Electron Diffraction

Enantiomorphic identification of chiral molecules is essential in organic chemistry and the pharmaceutical industry,as two enantiomorphic structures can show distinctively different properties.Here,we illustrate the absolute structural determination of organic nanocrystals using zone-axis electron diffraction by taking advantage of electron multiple scattering.Two enantiomorphs are distinguished by comparing the reflection intensities of Friedel pairs in the zone-axis electron diffraction pattern,after confirming the absolute indices of reflections by locating relative positions of diffraction spots from two patterns that deviate from a certain angle.We demonstrate the protocol with successful applications in two chiral drug nanocrystals.

High-performance Ta-doped Li_(7)La_(3)Zr_(2)O_(12) garnet oxides with AlN additive

Garnet-type oxide is one of the most promising solid-state electrolytes(SSEs)for solid-state lithium-metal batteries(SSLMBs).However,the Li dendrite formation in garnet oxides obstructs the further development of the SSLMBs seriously.Here,we report a high-performance garnet oxide by using AlN as a sintering additive and Li as an anode interface layer.AlN with high thermal conductivity can promote the sintering activity of the garnet oxides,resulting in larger particle size and higher relative density.Moreover,Li3N with high ionic conductivity formed at grain boundaries and interface can also improve Li-ion transport kinetics.As a result,the garnet oxide electrolytes with AlN show enhanced thermal conductivity,improved ionic conductivity,reduced electronic conductivity,and increased critical current density(CCD),compared with the counterpart using Al_(2)O_(3) sintering aid.In addition,Li symmetric cells and Li|LiFePO_(4)(Li|LFP)half cells using the garnet electrolyte with the AlN additive exhibit good electrochemical performances.This work provides a simple and effective strategy for high-performance SSEs.

金属-有机框架吸附剂走向工业化碳捕集应用

Combustion of fossil fuels in industrial settings,such as coalfired power plants,steel-smelting furnaces,and cement kilns accounts for more than 70%of CO_(2) emission.Although liquid amine scrubbing processes that are based on 30 wt%monoethanolamine aqueous solutions are feasible in capturing CO_(2)on a large scale,significant drawbacks remain concerning the energy penalty for regeneration and environmental pollution upon their disposal after degradation[1].

Distinct superconducting behaviors of pressurized WB2 and ReB2 with different local B layers

The recent discovery of superconductivity up to 32 K in the pressurized MoBreignites the interest in exploring high-Tc superconductors in transition-metal diborides. Inspired by that work, we turn our attention to the 5 d transition-metal diborides.Here we systematically investigate the responses of both structural and physical properties of WBand ReBto external pressure,which possess different types of boron layers. Similar to MoB, the pressure-induced superconductivity was also observed in WBabove 60 GPa with a maximum Tcof 15 K at 100 GPa, while no superconductivity was detected in ReBin this pressure range. Interestingly, the structures at ambient pressure for both WBand ReBpersist to high pressure without structural phase transitions. Theoretical calculations suggest that the ratio of flat boron layers in this class of transition-metal diborides may be crucial for the appearance of high Tc. The combined theoretical and experimental results highlight the effect of the geometry of boron layers on superconductivity and shed light on the exploration of novel high-Tcsuperconductors in borides.