Bulk metallic glass (BMG) composites with the austenite B2 phase as reinforcement macroscopically showed strain hardening behavior due to the plasticity induced by martensitic transformation during deformation. Relati...Bulk metallic glass (BMG) composites with the austenite B2 phase as reinforcement macroscopically showed strain hardening behavior due to the plasticity induced by martensitic transformation during deformation. Relationship between characteristics of the B2-CuZr reinforcing phase and uniaxial compressive properties of CuZr-based BMG composites was studied. Mechanical properties of these BMG composites were found to depend on not only the reinforced phases but also the amorphous matrix,and the yield and fracture strength can be roughly estimated by the rule of mixture principle. Distribution of the reinforced B2-CuZr phase has an important impact on the compressive plasticity even for the composites with a similar volume fraction of the crystalline phase.展开更多
We put forward a method of fabricating Aluminum(Al)/carbon fibers(CFs) composite sheets by the accumulative roll bonding(ARB) method. The finished Al/CFs composite sheet has CFs and pure Al sheets as sandwich and surf...We put forward a method of fabricating Aluminum(Al)/carbon fibers(CFs) composite sheets by the accumulative roll bonding(ARB) method. The finished Al/CFs composite sheet has CFs and pure Al sheets as sandwich and surface layers. After cross-section observation of the Al/CFs composite sheet, we found that the CFs discretely distributed within the sandwich layer. Besides, the tensile test showed that the contribution of the sandwich CFs layer to tensile strength was less than 11% compared with annealed pure Al sheet. With ex-situ observation of the CFs breakage evolution with-16%,-32%, and-45% rolling reduction during the ARB process, the plastic instability of the Al layer was found to bring shear damages to the CFs. At last, the bridging strengthening mechanism introduced by CFs was sacrificed. We provide new insight into and instruction on Al/CFs composite sheet preparation method and processing parameters.展开更多
Coal measure source rocks, located in the Xihu Sag of the East China Sea Shelf Basin, were analyzed to define the hydrocarbon generation potential, organic geochemistry/petrology characteristics, and coal preservation...Coal measure source rocks, located in the Xihu Sag of the East China Sea Shelf Basin, were analyzed to define the hydrocarbon generation potential, organic geochemistry/petrology characteristics, and coal preservation conditions. The Pinghu source rocks in the Xihu Sag are mainly gas-prone accompany with condensate oil generation. The coals and shales of the Pinghu Formation are classified from "fair" to "excellent" source rocks with total organic carbon(TOC) contents ranging from 25.2% to 77.2% and 1.29% to 20.9%, respectively. The coals are richer in TOC and S1+S2 than the shales, indicating that the coals have more generation potential per unit mass. Moreover, the kerogen type of the organic matter consists of types Ⅱ-Ⅲ and Ⅲ, which the maturity Ro ranges from 0.59% to 0.83%. Petrographically, the coals and shales are dominated by vitrinite macerals(69.1%–96.8%) with minor proportions of liptinite(2.5%–17.55%) and inertinite(0.2%–6.2%). The correlation between maceral composition and S1+S2 indicates that the main contributor to the generation potential is vitrinite. Therefore, the coals and shales of the Pinghu Formation has good hydrocarbon generation potential, which provided a good foundation for coal measure gas accumulation. Furthermore, coal facies models indicates that the Pinghu coal was deposited in limno-telmatic environment under high water levels, with low tree density(mainly herbaceous) and with low-moderate nutrient supply. Fluctuating water levels and intermittent flooding during the deposition of peat resulted in the inter-layering of coal, shale and sandstone, which potentially providing favorable preservation conditions for coal measure gas.展开更多
CONSPECTUS:Hydrogen-bonded organic frameworks(HOFs)are a class of porous molecular materials that rely on the assembly of organic building blocks by means of hydrogen-bonding interactions to form two-dimensional(2D)an...CONSPECTUS:Hydrogen-bonded organic frameworks(HOFs)are a class of porous molecular materials that rely on the assembly of organic building blocks by means of hydrogen-bonding interactions to form two-dimensional(2D)and three-dimensional(3D)crystalline networks.The reversible nature of the hydrogenbond formation endows HOFs with the attributes of solution processability and simple regeneration.High-quality single crystals of HOFs can be grown easily for unambiguous superstructure determination by single-crystal X-ray diffraction,which is crucial for the elucidation of superstructure−property relationships.During the past decade,considerable progress has been achieved in realizing stable HOFs with permanent porosities by focusing on the design of molecular building blocks in order to introduce rigidity,auxiliary[π···π]interactions,and interpenetration of their frameworks to sustain the extended networks.The applications of HOFs are far-reaching,spanning catalysis,energy,and biomedical products as well as the storage and separation of fine chemicals.In this Account,we,first of all,provide an overview of the chronological development of HOFs,starting from the seminal work by Marsh and Duchamp in 1969 on the crystal superstructure of the hydrogen-bonded networks of trimesic acid.We identify the development of novel hydrogen-bonding motifs such as diaminotriazine(DTA),the introduction of the concept of molecular tectonics,and the establishment of permanent porosity in HOFs as being some of the milestones,which incentivized the current burgeoning research endeavors on developing HOFs as multifunctional materials.This Account is focused primarily on surveying the strategies for constructing porous 3D HOFs based on organic building blocks with peripheral carboxyl groups.These strategies are presented in the following categories:(1)the polycatenation of 2D networks by trigonal building blocks to form global 3D frameworks,(2)the utilization of building blocks with 3D geometriestetrahedral and trigonal prismatic展开更多
Shear-banding behavior in metallic glasses plays a key role in the operation of plastic deformation,which is associated with yield strength.In a micro-scale,the shear-banding behavior must be affected by many factors ...Shear-banding behavior in metallic glasses plays a key role in the operation of plastic deformation,which is associated with yield strength.In a micro-scale,the shear-banding behavior must be affected by many factors from the test machine and the substrate.Therefore,in this study,comprehensively considering a machine compliance,a geometry imperfection of micro-pillar,and a substrate sink-in the machine-sample-substrate system,we developed a plastic-strength model at a micrometer scale in this study,which is evidenced by the microscale compressive properties of 18 kinds of metallic glasses.The the-oretical model provides a guidance for the elastic limits and shear-banding dynamics of metallic glasses at the micro-scale,which can be applicable to characterize the microscale deformation behavior of other amorphous materials.展开更多
Carbon and oxygen-rich corrosion barrier layer formed on Mg by a simple and scalable CO_(2) atmospheric plasma(CO_(2)-AP)process.The reactive CO_(2)-AP interacts with the Mg surface and forms a unique layered structur...Carbon and oxygen-rich corrosion barrier layer formed on Mg by a simple and scalable CO_(2) atmospheric plasma(CO_(2)-AP)process.The reactive CO_(2)-AP interacts with the Mg surface and forms a unique layered structure with the top MgCO_(3)/MgO-intermixed particulates pillars and the bottom dense layer.The surface features were simultaneously formed on the nano-/micro-structured MgO layer by carbonate molecules,plasma-active CO_(2) molecules,and/or other volatile organic compounds on the nano-/micro-structured MgO particle layer.The resulting surfaces after CO_(2)-AP were either hydrophobic or hydrophilic and exhibited lower anodic current or high resistance for Mg corrosion.For the hydrophobic surfaces of CO_(2)-AP treated Mg,molecular dynamic simulations were performed to understand the origin of hydrophobicity and identified that the amorphous carbon layers formed on the Mg surface are the source.The environmentally benign abundant-gas-based process enables the cost reduction associated with waste treatment,generation of by-product,and supply of raw material.展开更多
The glass-forming ability of Mg-Cu-Gd alloys could be significantly promoted with the addition of Ag.A calorimetric anomaly could be observed in the supercooled liquid region of the Mg-Cu-Ag-Gd metallic glass,indicati...The glass-forming ability of Mg-Cu-Gd alloys could be significantly promoted with the addition of Ag.A calorimetric anomaly could be observed in the supercooled liquid region of the Mg-Cu-Ag-Gd metallic glass,indicating the occurrence of a liquid-state phase transition driven by entropy.However,the underlying mechanism of the polyamorphous phase transition remains unsettled.In the paper,in situ scattering techniques were employed to reveal multiscale structure evidence in a Mg65Cu15Ag10Gd10metallic glass with an anomalous exothermic peak upon heating.Resistivity measurements indicate a reentrant behavior for the Mg-Cu-Ag-Gd metallic glass in the anomalous exothermic peak temperature region during heating.In situ synchrotron diffraction results revealed that the local atomic structure tends to be ordered and loosely packed first,followed by reentering into the initial state upon heating.Moreover,time-resolved small-angle synchrotron X-ray scattering(SAXS) results show an increase in nanoscale heterogeneity first followed by a reentrant supercooled liquid behavior.A core-shell structure model has been used to fit the SAXS profiles when polyamorphous phase transition occurs.In contrast,there is no structure anomaly for the reference Mg-Cu-Gd alloy system.The detailed multiscale structural evidence suggests the occurrence of a liquid-liquid phase transition followed by a reentrant behavior in the MgCu-Ag-Gd metallic glass.Our results deepen the understanding of the structural origin of the glass-forming ability and shed light on the possibility of tuning the physical and mechanical properties by heat-treatment in the supercooled liquid region of Mg-based metallic glasses.展开更多
Developing ductile bulk metallic glasses(BMGs)can benefit from an in-depth understanding of the structure-property relation during plastic deformation.However,endowing BMGs with tensile ductility in BMGs needs to reve...Developing ductile bulk metallic glasses(BMGs)can benefit from an in-depth understanding of the structure-property relation during plastic deformation.However,endowing BMGs with tensile ductility in BMGs needs to reveal the response of critical structure units during deformation.Here,we report the experimental results of an in-situ synchrotron high-energy X-ray study of a Zr-based BMG under uniaxial tension after preprocessing by canning compression of the three-dimensional compressive stress state.It is revealed that the canning-compressed BMG(CC-BMG)sample has better tensile ductility and higher ultimate strength than the as-cast sample,which possesses heterogeneous and loosely packed local struc-tures on medium-range scales.The experimental results revealed two stages of plastic deformation in the CC-BMGs compared with one stage of plastic deformation in the as-cast BMG.Moreover,the shift in the first sharp diffraction peak along the tension direction for the canning-compressed sample is substan-tially more pronounced than that of the as-cast sample.Furthermore,the real-space analysis illustrates a competition mechanism between the 2-atom and 3-atom connection modes on medium-range order during the plastic deformation of the CC-BMG.Additionally,the ordering on the medium-range scale de-creases in the first plastic deformation stage but increases in the second plastic deformation stage.There-fore,a structural crossover phenomenon occurs in the CC-BMG during plastic deformation.Our results demonstrate a structure-property correlation for the CC-BMGs of heterogeneous medium-range ordered structures,which may be beneficial for endowing BMGs with ductility based on medium-range order engineering techniques.展开更多
The discovery of new perovskite compounds under high pressure mainly focuses on the ABO_(3)compositions and the compositions highly deviated from ABO_(3)are less explored.Here we demonstrate that the La_(6)Sr_(3)Si_(6...The discovery of new perovskite compounds under high pressure mainly focuses on the ABO_(3)compositions and the compositions highly deviated from ABO_(3)are less explored.Here we demonstrate that the La_(6)Sr_(3)Si_(6)O_(24)silicate composition can be stabilized as a hexagonal perovskite-related structure with isolated tetrahedra anions under high pressure of 6 GPa.The compound adopts 9-layer shifted hexagonal perovskite-like structure with both B-cation and oxygen deficiencies and contains pseudo-cubic(c)(La/Sr)O_(2)layers and hexagonal(h)(La/Sr)O_(3)layers stacked according to(c hh)_(3)sequence.This structure features both B-cation vacancy ordering between the two consecutive hexagonal layers and oxygen vacancy ordering in c-(La/Sr)O_(2)layers,resulting in isolated tetrahedral Si O_(4)anions and ionic conduction behavior.This work demonstrates the practicability of accessing new perovskite-related functional materials from the compositions highly deviated from ABO_(3)under high pressure.展开更多
Zero thermal expansion(ZTE)alloys have unique aspects in the application of the engineering of precise dimensional control.However,the harsh conditions to realize ZTE,i.e.,appropriate coupling among spin,lattice,and c...Zero thermal expansion(ZTE)alloys have unique aspects in the application of the engineering of precise dimensional control.However,the harsh conditions to realize ZTE,i.e.,appropriate coupling among spin,lattice,and charge upon heating,have limited the ZTE alloys by very few numbers of species.In this work,we report a route to achieving twodimensional(2D)ZTE behavior by regulating crystallographic texture and magneto-volume effects(MVEs)in volumetric positive thermal expansion alloys.This is illustrated in a series of Mn_(x)Fe_(5-x)Si_(3)compounds by those earth-abundant elements.As a result,a 2D ZTE performance with a coefficient of thermal expansion α_(1)=0.45×10^(-7)K^(-1) over a broad temperature window of 10–310 K was observed in MnFe4Si3.The experimental results by synchrotron X-ray diffraction,neutron diffraction,microscopy,and magnetization measurements reveal that such a ZTE behavior is strongly coupled with fiber crystallographic texture and magnetic moment at the crystallographic 6g site that dominates MVEs in the a-b plane.The competition between ferromagnetic Fe_(4d)–Fe_(6g)(J_(FM))and antiferromagnetic Mn_(4d)–Mn_(6g)(J_(AFM))interactions makes the Mn_(1.5)Fe_(3.5)Si_(3) and Mn_(2)Fe_(3)Si_(3)compounds show mixed magnetism and negative thermal expansion(NTE).The integral approach presented here can be used to extend the scope of ZTE/NTE species in other magnetic or ferroelectric materials.展开更多
Phonons are quasi-particles,observed as lattice vibrations in periodic materials,that often dampen in the presence of structural perturbations.Nevertheless,phonon-like collective excitations exist in highly complex sy...Phonons are quasi-particles,observed as lattice vibrations in periodic materials,that often dampen in the presence of structural perturbations.Nevertheless,phonon-like collective excitations exist in highly complex systems,such as proteins,although the origin of such collective motions has remained elusive.Here we present a picture of temperature and hydration dependence of collective excitations in green fluorescent protein(GFP)obtained by inelastic neutron scattering.Our results provide evidence that such excitations can be used as a measure of flexibility/softness and are possibly associated with the protein’s activity.Moreover,we show that the hydration water in GFP interferes with the phonon propagation pathway,enhancing the structural rigidity and stability of GFP.展开更多
The challenge of growing rare-earth(RE)sesquioxide crystals can be overcome by tailoring their structural stability and melting point via composition engineering.This work contributes to the advancement of the field o...The challenge of growing rare-earth(RE)sesquioxide crystals can be overcome by tailoring their structural stability and melting point via composition engineering.This work contributes to the advancement of the field of crystal growth of high-entropy oxides.A compound with only small REs(Lu,Y,Ho,Yb,Er)_(2)O_(3)maintains a cubic C-type structure upon cooling from the melt,as observed via in-situ high-temperature neutron diffraction on aerodynamically levitated samples.On the other hand,a compound with a mixture of small and large REs(Lu,Y,Ho,Nd,La)_(2)O_(3)crystallizes as a mixture of a primary C-type phase with an unstable secondary phase.Crystals of compositions(Lu,Y,Ho,Nd,La)_(2)O_(3)and(Lu,Y,Gd,Nd,La)_(2)O_(3)were grown by the micro-pulling-down(mPD)method with a single monoclinic B-type phase,while a powder of(Lu,Y,Ho,Yb,Er)_(2)O_(3)did not melt at the maximum operating temperature of an iridium-rhenium crucible.The minimization of the melting point of the two grown crystals is attributed to the mismatch in cation sizes.The electron probe microanalysis reveals that the general element segregation behavior in the crystals depends on the composition.展开更多
Thermal stability and the crystallization kinetics of a phase-separated Zr-Cu-Fe-Al bulk metallic glass were investigated using in situ high-energy synchrotron X-ray and neutron diffraction,as well as small-angle sync...Thermal stability and the crystallization kinetics of a phase-separated Zr-Cu-Fe-Al bulk metallic glass were investigated using in situ high-energy synchrotron X-ray and neutron diffraction,as well as small-angle synchrotron X-ray scattering.It was revealed that this glass with excellent glass-forming ability possesses a two-step crystallization behavior.The crystalline products and their evolution sequence are more complicated than a homogeneous Zr-Cu-Al glass with average glass-forming ability.The experimental results indicate that a finely distributed nanometer-sized cubic Zr_(2)Cu phase forms first and then transforms to a tetragonal Zr_(2)Cu phase,while the matrix transforms to an orthorhombic Zr_(3)Fe phase.The strength of the Zr-Cu-Fe-Al composite containing cubic Zr_(2)Cu phase and glass matrix increases,and the plasticity also improves compared to the as-cast Zr-Cu-Fe-Al bulk metallic glass.Our results suggest that the formation of multiple and complex crystalline products would be the characteristics of the Zr-Cu-Fe-Al glass with better glass-forming ability.Our study may shed light on the synthesis of bulk-sized glass-nanocrystals composites of high strength and good plasticity.展开更多
Despite the long-established rocking-chair theory of lithium-ion batteries(LIBs),developing novel characterization methodology with higher spatiotemporal resolution facilitates a better understanding of the solid elec...Despite the long-established rocking-chair theory of lithium-ion batteries(LIBs),developing novel characterization methodology with higher spatiotemporal resolution facilitates a better understanding of the solid electrolyte interphase studies to shape the reaction mechanisms.In this work,we develop a Xenon ion plasma focused ion beam(Xe+PFIB)-based characterization technique to probe the cross-sectional interface of both ternary cathode and graphite anode electrodes,with the focus on revealing the chemical composition and distribution underneath the electrode surface by in-depth analysis of secondary ions.Particularly,the lithium fluoride is detected in the pristine cathode prior to contact with the electrolyte,reflecting that the electrode degradation is in the form of the loss of lithium inventory during electrode preparation.This degradation is related to the hydrolysis of the cathode material and the decomposition of the PVDF binder.Through the quantitative analysis of the transition-metal degradation products,manganese is found to be the dominant element in the newly formed inactive fluoride deposition on the cathode,while no transition metal signal can be found inside the anode electrode.These insights at high resolution implemented via a PFIB-based characterization technique not only enrich the understanding of the degradation mechanism in the LIBs but also identify and enable a high-sensitivity methodology to obtain the chemical survey at the subsurface,which will help remove the capacity-fade observed in most LIBs.展开更多
As phase separation between the small-molecule semiconductor and the polymer binder is the key enabler of blend-based organic field-effect transistors(OFETs)fabricated by low-cost solution processing,it is crucial to ...As phase separation between the small-molecule semiconductor and the polymer binder is the key enabler of blend-based organic field-effect transistors(OFETs)fabricated by low-cost solution processing,it is crucial to understand the underlying phase separation mechanisms that determine the phase morphology,which significantly impacts device performance.Beyond the parameter space investigated in previous work,here we investigate the formation of blends by varying the branch architecture of the polymer binder and by shortening the solvent dry time using ultrasonic spray casting.The phase morphologies of the resulting blend films have been thoroughly characterized with a variety of techniques in three dimensions over multiple length scales,including AFM,energy-filtered transmission electron microscope,and neutron reflectivity,and have been correlated with electrical transport performance.From the results,we have inferred that the phase morphology is kinetically determined,limited by the inherent slow movement of polymer macromolecules.The kinetic picture,supported by molecular dynamics modeling,not only consistently explains our observations but also resolves inconsistencies in previous works.The achieved mechanistic understanding will guide further optimization of blend-based organic electronics,such as OFETs and organic photovoltaics.展开更多
Oxide dispersion strengthened CoCrFeMnNi high-entropy alloys(ODS-HEAs)were prepared using two different powder preparation methods classified by yttrium addition strategy to investigate the effects of in-situ and ex-s...Oxide dispersion strengthened CoCrFeMnNi high-entropy alloys(ODS-HEAs)were prepared using two different powder preparation methods classified by yttrium addition strategy to investigate the effects of in-situ and ex-situ oxide dispersoid formation on the microstructure and mechanical properties.Systematic micro structural analysis was carried out by X-ray diffraction(XRD),electron backscattered diffraction(EBSD),high-resolution transmission electron microscopy(HRTEM),atom probe tomography(APT),and small-angle neutron scattering(SANS).Cryo-milled powder analysis,grain structure evolution after spark plasma sintering,dispersoid characteristics,and matrix/dispersoid interface structure analysis of the insitu and ex-situ dispersoids within the high-entropy alloy(HEA)matrix were performed.The in-situ dispersoid formation was dominantly observed in the Y-alloyed ODS-HEA through the construction of a coherent interface relationship with complex chemical composition,leading to an increase in the Zener pinning forces on the grain boundary movement.ODS-HEA with in-situ oxide dispersoids enhanced the formation of ultrafine-grained structures with an average diameter of 330 nm at a sintering temperature of 1173 K.This study shows that the Y pre-alloying method is efficient in achieving fine coherent dispersoids with an ultra fine-grained structure,resulting in an enhancement of the tensile strength of the CoCrFeMnNi HEA.展开更多
Magnetic susceptibility,specific heat,and neutron powder diffraction measurements have been performed on polycrystalline Li_(2)Co(WO_4)_(2)samples.Under zero magnetic field,two successive magnetic transitions at T_(N1...Magnetic susceptibility,specific heat,and neutron powder diffraction measurements have been performed on polycrystalline Li_(2)Co(WO_4)_(2)samples.Under zero magnetic field,two successive magnetic transitions at T_(N1)~9.4 K and T_(N2)~7.4 K are observed.The magnetic ordering temperatures gradually decrease as the magnetic field increases.Neutron diffraction reveals that Li_(2)Co(WO_4)_(2)enters an incommensurate magnetic state with a temperature dependent k between T_(N1)and T_(N2).The magnetic propagation vector locks-in to a commensurate value k=(1/2,1/4,1/4)below T_(N2).The antiferromagnetic structure is refined at 1.7 K with Co2+magnetic moment 2.8(1),μ_B,consistent with our first-principles calculations.展开更多
Antiferroelectrics have attracted increasing research interests in recent years due to both their great potential in energy storage applications and intriguing structural characteristics.However,the links between the ...Antiferroelectrics have attracted increasing research interests in recent years due to both their great potential in energy storage applications and intriguing structural characteristics.However,the links between the electrical properties and structural characteristics of distorted perovskite antiferroelectrics are yet to be fully deciphered.Here,we adopt local-structure methods to elucidate the nanoscale atomic structure of AgNbO,-based antiferroelectrics and their structural evolution upon La doping.The local structural features including interatomic distance distributions and atomic displacements have been analyzed using neutron small-box pair distribution function(PDF)refinement in conjunction with large-box Reverse Monte Carlo modelling.Our results highlight the correlation of cation displacements in AgNbo,and its disruption by the incorporation of La,apparently in corroboration with the observed anomalous dielectric properties.Spatial ordering of cation vacancies is observed in La-doped AgNbo,samples,which coordinates with oxygen octahedral tilting to relieve lattice strain.These results provide renewed insights into the atomic structure and antiferroelectric phase instabilities of AgNbO,and relevant perovskite materials,further lending versatile opportunities for enhancing their functionalities.展开更多
The energy materials performance is intrinsically determined by structures from the average lattice structure to the atom arrangement, valence, and distribution of the containing transition metal(TM) elements. Underst...The energy materials performance is intrinsically determined by structures from the average lattice structure to the atom arrangement, valence, and distribution of the containing transition metal(TM) elements. Understanding the mechanism of the structure transition and atom rearrangement via synthesis or processing is key to expediting the exploration of excellent energy materials. In this work, in situ neutron scattering is employed to reveal the real-time structure evolution, including the TM-O bonds, lattice,TM valence and the migration of the high-voltage spinel cathode LiNi_(0.5)Mn_(1.5)O_(4). The transition-metalmediated spinel destabilization under the annealing at the oxygen-deficient atmosphere is pinpointed.The formation of Mn^(3+) is correlated to the TM migration activation, TM disordered rearrangement in the spinel, and the transition to a layered-rocksalt phase. The further TM interdiffusion and Mn^(3+) reduction are also revealed with multi-stage thermodynamics and kinetics. The mechanisms of phase transition and atom migrations as functions of temperature, time and atmosphere present important guidance on the synthesis in various-valence element containing oxides.展开更多
From heavy fermion compounds and cuprates to iron pnictides and chalcogenides, a spin resonance at hΩ0 ∝ kBTc is a staple of nearly magnetic superconductors. Possible explanations include a two-particle bound state ...From heavy fermion compounds and cuprates to iron pnictides and chalcogenides, a spin resonance at hΩ0 ∝ kBTc is a staple of nearly magnetic superconductors. Possible explanations include a two-particle bound state or loss of magnon damping in the superconducting state. While both scenarios suggest a central role for magnetic fluctuations,distinguishing them is important to identify the right theoretical framework to understand these types of unconventional superconductors. Using an inelastic neutron scattering technique,we show that the spin resonance in the optimally doped Fe1.03 Se0.4 Te0.6 superconductor splits into three peaks in a high magnetic field,a signature of a two-particle S = 1 triplet bound state.展开更多
基金supported in part by the National Natural Science Foundation of China (50725104, 51010001 and 51001009)China Postdoctoral Science Foundation (20100470208) the Fundamental Research Funds for the Central Universities (FRF-BR-10-036B)
文摘Bulk metallic glass (BMG) composites with the austenite B2 phase as reinforcement macroscopically showed strain hardening behavior due to the plasticity induced by martensitic transformation during deformation. Relationship between characteristics of the B2-CuZr reinforcing phase and uniaxial compressive properties of CuZr-based BMG composites was studied. Mechanical properties of these BMG composites were found to depend on not only the reinforced phases but also the amorphous matrix,and the yield and fracture strength can be roughly estimated by the rule of mixture principle. Distribution of the reinforced B2-CuZr phase has an important impact on the compressive plasticity even for the composites with a similar volume fraction of the crystalline phase.
基金Supported by Innovation and Technology Fund (No.ITP/045/19AP)Commercial Research&Development (CRD) Funding Supported by Hong Kong Productivity Council (No.10008787)。
文摘We put forward a method of fabricating Aluminum(Al)/carbon fibers(CFs) composite sheets by the accumulative roll bonding(ARB) method. The finished Al/CFs composite sheet has CFs and pure Al sheets as sandwich and surface layers. After cross-section observation of the Al/CFs composite sheet, we found that the CFs discretely distributed within the sandwich layer. Besides, the tensile test showed that the contribution of the sandwich CFs layer to tensile strength was less than 11% compared with annealed pure Al sheet. With ex-situ observation of the CFs breakage evolution with-16%,-32%, and-45% rolling reduction during the ARB process, the plastic instability of the Al layer was found to bring shear damages to the CFs. At last, the bridging strengthening mechanism introduced by CFs was sacrificed. We provide new insight into and instruction on Al/CFs composite sheet preparation method and processing parameters.
基金National Science and Technology Major Project(2017ZX05035004-002)the National Natural Science Foundation of China(41802183)+1 种基金the National Postdoctoral Program for Innovative Talents(BX201700282)the China Postdoctoral Science Foundation(2017M621870),the project of investigation and evaluation of special coal resources(DD20I60187-1).
文摘Coal measure source rocks, located in the Xihu Sag of the East China Sea Shelf Basin, were analyzed to define the hydrocarbon generation potential, organic geochemistry/petrology characteristics, and coal preservation conditions. The Pinghu source rocks in the Xihu Sag are mainly gas-prone accompany with condensate oil generation. The coals and shales of the Pinghu Formation are classified from "fair" to "excellent" source rocks with total organic carbon(TOC) contents ranging from 25.2% to 77.2% and 1.29% to 20.9%, respectively. The coals are richer in TOC and S1+S2 than the shales, indicating that the coals have more generation potential per unit mass. Moreover, the kerogen type of the organic matter consists of types Ⅱ-Ⅲ and Ⅲ, which the maturity Ro ranges from 0.59% to 0.83%. Petrographically, the coals and shales are dominated by vitrinite macerals(69.1%–96.8%) with minor proportions of liptinite(2.5%–17.55%) and inertinite(0.2%–6.2%). The correlation between maceral composition and S1+S2 indicates that the main contributor to the generation potential is vitrinite. Therefore, the coals and shales of the Pinghu Formation has good hydrocarbon generation potential, which provided a good foundation for coal measure gas accumulation. Furthermore, coal facies models indicates that the Pinghu coal was deposited in limno-telmatic environment under high water levels, with low tree density(mainly herbaceous) and with low-moderate nutrient supply. Fluctuating water levels and intermittent flooding during the deposition of peat resulted in the inter-layering of coal, shale and sandstone, which potentially providing favorable preservation conditions for coal measure gas.
基金The authors thank Professor Gautam Desiraju(Indian Institute of Science,Bangalore)for helpful discussions.P.L.and J.F.S.thank Northwestern University(NU)for the support of the research.M.R.R.acknowledges the U.S.Department of Energy(DOE)Office of Science(Basic Energy Sciences)for research funding.
文摘CONSPECTUS:Hydrogen-bonded organic frameworks(HOFs)are a class of porous molecular materials that rely on the assembly of organic building blocks by means of hydrogen-bonding interactions to form two-dimensional(2D)and three-dimensional(3D)crystalline networks.The reversible nature of the hydrogenbond formation endows HOFs with the attributes of solution processability and simple regeneration.High-quality single crystals of HOFs can be grown easily for unambiguous superstructure determination by single-crystal X-ray diffraction,which is crucial for the elucidation of superstructure−property relationships.During the past decade,considerable progress has been achieved in realizing stable HOFs with permanent porosities by focusing on the design of molecular building blocks in order to introduce rigidity,auxiliary[π···π]interactions,and interpenetration of their frameworks to sustain the extended networks.The applications of HOFs are far-reaching,spanning catalysis,energy,and biomedical products as well as the storage and separation of fine chemicals.In this Account,we,first of all,provide an overview of the chronological development of HOFs,starting from the seminal work by Marsh and Duchamp in 1969 on the crystal superstructure of the hydrogen-bonded networks of trimesic acid.We identify the development of novel hydrogen-bonding motifs such as diaminotriazine(DTA),the introduction of the concept of molecular tectonics,and the establishment of permanent porosity in HOFs as being some of the milestones,which incentivized the current burgeoning research endeavors on developing HOFs as multifunctional materials.This Account is focused primarily on surveying the strategies for constructing porous 3D HOFs based on organic building blocks with peripheral carboxyl groups.These strategies are presented in the following categories:(1)the polycatenation of 2D networks by trigonal building blocks to form global 3D frameworks,(2)the utilization of building blocks with 3D geometriestetrahedral and trigonal prismatic
基金This work was financially supported by the National Natural Science Foundation of China(Nos.51925103,51801027)the program 173(No.2020-JCIQ-ZD-186-01)+1 种基金China Postdoctoral Science Foundation(No.2022M713334)the Research Grants Council of the Hong Kong Special Administrative Region,China(No.PolyU 15222017).
文摘Shear-banding behavior in metallic glasses plays a key role in the operation of plastic deformation,which is associated with yield strength.In a micro-scale,the shear-banding behavior must be affected by many factors from the test machine and the substrate.Therefore,in this study,comprehensively considering a machine compliance,a geometry imperfection of micro-pillar,and a substrate sink-in the machine-sample-substrate system,we developed a plastic-strength model at a micrometer scale in this study,which is evidenced by the microscale compressive properties of 18 kinds of metallic glasses.The the-oretical model provides a guidance for the elastic limits and shear-banding dynamics of metallic glasses at the micro-scale,which can be applicable to characterize the microscale deformation behavior of other amorphous materials.
基金the US Department of Energy’s(DOE’s)Office of Energy Efficiency and Renewable Energy,Vehicle Technology Office,Powertrain Materials Core and Light Metals Core ProgramsSample characterization is also partially supported by the Technology Commercialization Fund Fiscal Year 2020 of DOE’s Office of Technology Transitionsby the Creative Materials Discovery Program through the National Research Foundation of Korea,with computational modeling of amorphous carbons funded by the Ministry of Science,ICT and Future Planning(NRF-2016M3D1A1919181)。
文摘Carbon and oxygen-rich corrosion barrier layer formed on Mg by a simple and scalable CO_(2) atmospheric plasma(CO_(2)-AP)process.The reactive CO_(2)-AP interacts with the Mg surface and forms a unique layered structure with the top MgCO_(3)/MgO-intermixed particulates pillars and the bottom dense layer.The surface features were simultaneously formed on the nano-/micro-structured MgO layer by carbonate molecules,plasma-active CO_(2) molecules,and/or other volatile organic compounds on the nano-/micro-structured MgO particle layer.The resulting surfaces after CO_(2)-AP were either hydrophobic or hydrophilic and exhibited lower anodic current or high resistance for Mg corrosion.For the hydrophobic surfaces of CO_(2)-AP treated Mg,molecular dynamic simulations were performed to understand the origin of hydrophobicity and identified that the amorphous carbon layers formed on the Mg surface are the source.The environmentally benign abundant-gas-based process enables the cost reduction associated with waste treatment,generation of by-product,and supply of raw material.
基金financially supported by the National Natural Science Foundation of China(No.51871120)the Natural Science Foundation of Jiangsu Province(No.BK20200019)+4 种基金the Fundamental Research Funds for the Central Universities(Nos.30919011107 and 30919011404)support by Shenzhen Science and Technology Innovation Committee(No.JCYJ20170413140446951)the supports by Shenzhen Science and Technology Innovation Commission(No.JCYJ20180507181806316)the supports by Shenzhen Science and Technology Innovation Commission(No.JCYJ202000109105618137)the Ministry of Science and Technology of China(No.2016YFA0401501)。
文摘The glass-forming ability of Mg-Cu-Gd alloys could be significantly promoted with the addition of Ag.A calorimetric anomaly could be observed in the supercooled liquid region of the Mg-Cu-Ag-Gd metallic glass,indicating the occurrence of a liquid-state phase transition driven by entropy.However,the underlying mechanism of the polyamorphous phase transition remains unsettled.In the paper,in situ scattering techniques were employed to reveal multiscale structure evidence in a Mg65Cu15Ag10Gd10metallic glass with an anomalous exothermic peak upon heating.Resistivity measurements indicate a reentrant behavior for the Mg-Cu-Ag-Gd metallic glass in the anomalous exothermic peak temperature region during heating.In situ synchrotron diffraction results revealed that the local atomic structure tends to be ordered and loosely packed first,followed by reentering into the initial state upon heating.Moreover,time-resolved small-angle synchrotron X-ray scattering(SAXS) results show an increase in nanoscale heterogeneity first followed by a reentrant supercooled liquid behavior.A core-shell structure model has been used to fit the SAXS profiles when polyamorphous phase transition occurs.In contrast,there is no structure anomaly for the reference Mg-Cu-Gd alloy system.The detailed multiscale structural evidence suggests the occurrence of a liquid-liquid phase transition followed by a reentrant behavior in the MgCu-Ag-Gd metallic glass.Our results deepen the understanding of the structural origin of the glass-forming ability and shed light on the possibility of tuning the physical and mechanical properties by heat-treatment in the supercooled liquid region of Mg-based metallic glasses.
基金the National Key R&D Program of China(No.2021YFB3802800)the National Natural Sci-ence Foundation of China(Nos.52222104,12261160364,51871120 and 51520105001)+3 种基金the Natural Science Foundation of Jiangsu Province(No.BK20200019)Si Lan acknowledges the support by Guangdong-Hong Kong-Macao Joint Laboratory for Neutron Scat-tering Science and Technology and Shenzhen Science and Technol-ogy Innovation Commission(No.JCYJ20200109105618137)the resources of the China Spallation Neutron Source located in Dongguan,China,and the Advanced Photon Source,a US Department of Energy(DOE)Office of Science User Facility op-erated for the DOE Office of Science by Argonne National Labora-tory under Contract No.DE-AC02-06CH11357the US DOE Office of Science,Office of Basic Energy Sciences.The neutron scattering experiments carried out at the Spallation Neutron Source were sponsored by the Scientific User Facilities Di-vision,Office of Basic Energy Sciences,U.S.Department of Energy,under Contract No.DE-AC05-00OR22725 with Oak Ridge National Laboratory.
文摘Developing ductile bulk metallic glasses(BMGs)can benefit from an in-depth understanding of the structure-property relation during plastic deformation.However,endowing BMGs with tensile ductility in BMGs needs to reveal the response of critical structure units during deformation.Here,we report the experimental results of an in-situ synchrotron high-energy X-ray study of a Zr-based BMG under uniaxial tension after preprocessing by canning compression of the three-dimensional compressive stress state.It is revealed that the canning-compressed BMG(CC-BMG)sample has better tensile ductility and higher ultimate strength than the as-cast sample,which possesses heterogeneous and loosely packed local struc-tures on medium-range scales.The experimental results revealed two stages of plastic deformation in the CC-BMGs compared with one stage of plastic deformation in the as-cast BMG.Moreover,the shift in the first sharp diffraction peak along the tension direction for the canning-compressed sample is substan-tially more pronounced than that of the as-cast sample.Furthermore,the real-space analysis illustrates a competition mechanism between the 2-atom and 3-atom connection modes on medium-range order during the plastic deformation of the CC-BMG.Additionally,the ordering on the medium-range scale de-creases in the first plastic deformation stage but increases in the second plastic deformation stage.There-fore,a structural crossover phenomenon occurs in the CC-BMG during plastic deformation.Our results demonstrate a structure-property correlation for the CC-BMGs of heterogeneous medium-range ordered structures,which may be beneficial for endowing BMGs with ductility based on medium-range order engineering techniques.
基金the National Science Foundation of China(Nos.21875049,22090043 and 22161014)Guangxi Natural Science Foundation(Nos.2019GXNSFGA245006,AD19245097 and 2020GXNSFAA297220)the Foundation of Guilin University of Technology(No.GUTQDJJ2018115)for the financial support。
文摘The discovery of new perovskite compounds under high pressure mainly focuses on the ABO_(3)compositions and the compositions highly deviated from ABO_(3)are less explored.Here we demonstrate that the La_(6)Sr_(3)Si_(6)O_(24)silicate composition can be stabilized as a hexagonal perovskite-related structure with isolated tetrahedra anions under high pressure of 6 GPa.The compound adopts 9-layer shifted hexagonal perovskite-like structure with both B-cation and oxygen deficiencies and contains pseudo-cubic(c)(La/Sr)O_(2)layers and hexagonal(h)(La/Sr)O_(3)layers stacked according to(c hh)_(3)sequence.This structure features both B-cation vacancy ordering between the two consecutive hexagonal layers and oxygen vacancy ordering in c-(La/Sr)O_(2)layers,resulting in isolated tetrahedral Si O_(4)anions and ionic conduction behavior.This work demonstrates the practicability of accessing new perovskite-related functional materials from the compositions highly deviated from ABO_(3)under high pressure.
基金supported by the National Key R&D Program of China(2020YFA0406202)the National Natural Science Foundation of China(22090042,21971009 and 21731001)+1 种基金the Fundamental Research Funds for the Central Universities,China(FRF-IDRY-19-018 and FRF-BR-19-003B)Neutron texture analysis was carried out at the Spallation Neutron Source(SNS)(Proposal No.2020B26069)。
文摘Zero thermal expansion(ZTE)alloys have unique aspects in the application of the engineering of precise dimensional control.However,the harsh conditions to realize ZTE,i.e.,appropriate coupling among spin,lattice,and charge upon heating,have limited the ZTE alloys by very few numbers of species.In this work,we report a route to achieving twodimensional(2D)ZTE behavior by regulating crystallographic texture and magneto-volume effects(MVEs)in volumetric positive thermal expansion alloys.This is illustrated in a series of Mn_(x)Fe_(5-x)Si_(3)compounds by those earth-abundant elements.As a result,a 2D ZTE performance with a coefficient of thermal expansion α_(1)=0.45×10^(-7)K^(-1) over a broad temperature window of 10–310 K was observed in MnFe4Si3.The experimental results by synchrotron X-ray diffraction,neutron diffraction,microscopy,and magnetization measurements reveal that such a ZTE behavior is strongly coupled with fiber crystallographic texture and magnetic moment at the crystallographic 6g site that dominates MVEs in the a-b plane.The competition between ferromagnetic Fe_(4d)–Fe_(6g)(J_(FM))and antiferromagnetic Mn_(4d)–Mn_(6g)(J_(AFM))interactions makes the Mn_(1.5)Fe_(3.5)Si_(3) and Mn_(2)Fe_(3)Si_(3)compounds show mixed magnetism and negative thermal expansion(NTE).The integral approach presented here can be used to extend the scope of ZTE/NTE species in other magnetic or ferroelectric materials.
基金supported by NSF No.1616008the Department of Energy(DoE),Office of Basic Energy Sciences,and Wayne State University.X.C was supported by NSAF No.U1930403National Natural Science Foundation of China(NSFC)11875051.Neutron scattering measurements at ORNL’s Spallation Neutron Source were supported by the Scientific User Facilities Division,Office of Basic Energy Sciences,DoE.
文摘Phonons are quasi-particles,observed as lattice vibrations in periodic materials,that often dampen in the presence of structural perturbations.Nevertheless,phonon-like collective excitations exist in highly complex systems,such as proteins,although the origin of such collective motions has remained elusive.Here we present a picture of temperature and hydration dependence of collective excitations in green fluorescent protein(GFP)obtained by inelastic neutron scattering.Our results provide evidence that such excitations can be used as a measure of flexibility/softness and are possibly associated with the protein’s activity.Moreover,we show that the hydration water in GFP interferes with the phonon propagation pathway,enhancing the structural rigidity and stability of GFP.
基金This work was supported by the National Science Foundation(DMR 1846935)。
文摘The challenge of growing rare-earth(RE)sesquioxide crystals can be overcome by tailoring their structural stability and melting point via composition engineering.This work contributes to the advancement of the field of crystal growth of high-entropy oxides.A compound with only small REs(Lu,Y,Ho,Yb,Er)_(2)O_(3)maintains a cubic C-type structure upon cooling from the melt,as observed via in-situ high-temperature neutron diffraction on aerodynamically levitated samples.On the other hand,a compound with a mixture of small and large REs(Lu,Y,Ho,Nd,La)_(2)O_(3)crystallizes as a mixture of a primary C-type phase with an unstable secondary phase.Crystals of compositions(Lu,Y,Ho,Nd,La)_(2)O_(3)and(Lu,Y,Gd,Nd,La)_(2)O_(3)were grown by the micro-pulling-down(mPD)method with a single monoclinic B-type phase,while a powder of(Lu,Y,Ho,Yb,Er)_(2)O_(3)did not melt at the maximum operating temperature of an iridium-rhenium crucible.The minimization of the melting point of the two grown crystals is attributed to the mismatch in cation sizes.The electron probe microanalysis reveals that the general element segregation behavior in the crystals depends on the composition.
基金supported by the National Natural Science Foundation of China(Grant Nos.51871120,51571170)the Natural Science Foundation of Jiangsu Province(Grant No.BK20200019)+2 种基金the Fundamental Research Funds for the Central Universities(Grant Nos.30919011107 and 30919011404)the Shenzhen Key Project for Basic Research(Grant No.JCYJ20200109105618137)the Guangdong-Hong Kong-Macao Joint Laboratory for Neutron Scattering Science and Technology(Grant No.2019B121205003)。
文摘Thermal stability and the crystallization kinetics of a phase-separated Zr-Cu-Fe-Al bulk metallic glass were investigated using in situ high-energy synchrotron X-ray and neutron diffraction,as well as small-angle synchrotron X-ray scattering.It was revealed that this glass with excellent glass-forming ability possesses a two-step crystallization behavior.The crystalline products and their evolution sequence are more complicated than a homogeneous Zr-Cu-Al glass with average glass-forming ability.The experimental results indicate that a finely distributed nanometer-sized cubic Zr_(2)Cu phase forms first and then transforms to a tetragonal Zr_(2)Cu phase,while the matrix transforms to an orthorhombic Zr_(3)Fe phase.The strength of the Zr-Cu-Fe-Al composite containing cubic Zr_(2)Cu phase and glass matrix increases,and the plasticity also improves compared to the as-cast Zr-Cu-Fe-Al bulk metallic glass.Our results suggest that the formation of multiple and complex crystalline products would be the characteristics of the Zr-Cu-Fe-Al glass with better glass-forming ability.Our study may shed light on the synthesis of bulk-sized glass-nanocrystals composites of high strength and good plasticity.
基金The electrochemical part of the research done at Oak Ridge National Laboratory,managed by UT Battelle,LLC,for the U.S.Department of Energy(DOE)under contract DE-AC05-00OR22725,was sponsored by the Office of Energy Efficiency and Renewable Energy(EERE)Vehicle Technologies OfficeT.S.acknowledges the support from the EPSRC project(EP/P001521/1)“Integrated Plasma Source Focused Ion Beam with Scanning Electron Microscope.”Y.Z.acknowledges support from EPSRC project(EP/V002260/1),UK National Measurement System and ISCF Measurement Fellowship.
文摘Despite the long-established rocking-chair theory of lithium-ion batteries(LIBs),developing novel characterization methodology with higher spatiotemporal resolution facilitates a better understanding of the solid electrolyte interphase studies to shape the reaction mechanisms.In this work,we develop a Xenon ion plasma focused ion beam(Xe+PFIB)-based characterization technique to probe the cross-sectional interface of both ternary cathode and graphite anode electrodes,with the focus on revealing the chemical composition and distribution underneath the electrode surface by in-depth analysis of secondary ions.Particularly,the lithium fluoride is detected in the pristine cathode prior to contact with the electrolyte,reflecting that the electrode degradation is in the form of the loss of lithium inventory during electrode preparation.This degradation is related to the hydrolysis of the cathode material and the decomposition of the PVDF binder.Through the quantitative analysis of the transition-metal degradation products,manganese is found to be the dominant element in the newly formed inactive fluoride deposition on the cathode,while no transition metal signal can be found inside the anode electrode.These insights at high resolution implemented via a PFIB-based characterization technique not only enrich the understanding of the degradation mechanism in the LIBs but also identify and enable a high-sensitivity methodology to obtain the chemical survey at the subsurface,which will help remove the capacity-fade observed in most LIBs.
文摘As phase separation between the small-molecule semiconductor and the polymer binder is the key enabler of blend-based organic field-effect transistors(OFETs)fabricated by low-cost solution processing,it is crucial to understand the underlying phase separation mechanisms that determine the phase morphology,which significantly impacts device performance.Beyond the parameter space investigated in previous work,here we investigate the formation of blends by varying the branch architecture of the polymer binder and by shortening the solvent dry time using ultrasonic spray casting.The phase morphologies of the resulting blend films have been thoroughly characterized with a variety of techniques in three dimensions over multiple length scales,including AFM,energy-filtered transmission electron microscope,and neutron reflectivity,and have been correlated with electrical transport performance.From the results,we have inferred that the phase morphology is kinetically determined,limited by the inherent slow movement of polymer macromolecules.The kinetic picture,supported by molecular dynamics modeling,not only consistently explains our observations but also resolves inconsistencies in previous works.The achieved mechanistic understanding will guide further optimization of blend-based organic electronics,such as OFETs and organic photovoltaics.
基金supported by the Civil-Military Technology Cooperation Program under the Agency for Defence Development(ADD)of the Republic of Korea(No.1415156504)the National Research Foundation grant funded by the Korean government(Nos.NRF-2020R1A5A6017701 and 2017K1A3A7A09016308)。
文摘Oxide dispersion strengthened CoCrFeMnNi high-entropy alloys(ODS-HEAs)were prepared using two different powder preparation methods classified by yttrium addition strategy to investigate the effects of in-situ and ex-situ oxide dispersoid formation on the microstructure and mechanical properties.Systematic micro structural analysis was carried out by X-ray diffraction(XRD),electron backscattered diffraction(EBSD),high-resolution transmission electron microscopy(HRTEM),atom probe tomography(APT),and small-angle neutron scattering(SANS).Cryo-milled powder analysis,grain structure evolution after spark plasma sintering,dispersoid characteristics,and matrix/dispersoid interface structure analysis of the insitu and ex-situ dispersoids within the high-entropy alloy(HEA)matrix were performed.The in-situ dispersoid formation was dominantly observed in the Y-alloyed ODS-HEA through the construction of a coherent interface relationship with complex chemical composition,leading to an increase in the Zener pinning forces on the grain boundary movement.ODS-HEA with in-situ oxide dispersoids enhanced the formation of ultrafine-grained structures with an average diameter of 330 nm at a sintering temperature of 1173 K.This study shows that the Y pre-alloying method is efficient in achieving fine coherent dispersoids with an ultra fine-grained structure,resulting in an enhancement of the tensile strength of the CoCrFeMnNi HEA.
基金Project supported by the National Natural Science Foundation of China(Grant Nos.11834002,12074111,and 11704109)the National Key R&D Project of China(Grant No.2016YFA0300101)。
文摘Magnetic susceptibility,specific heat,and neutron powder diffraction measurements have been performed on polycrystalline Li_(2)Co(WO_4)_(2)samples.Under zero magnetic field,two successive magnetic transitions at T_(N1)~9.4 K and T_(N2)~7.4 K are observed.The magnetic ordering temperatures gradually decrease as the magnetic field increases.Neutron diffraction reveals that Li_(2)Co(WO_4)_(2)enters an incommensurate magnetic state with a temperature dependent k between T_(N1)and T_(N2).The magnetic propagation vector locks-in to a commensurate value k=(1/2,1/4,1/4)below T_(N2).The antiferromagnetic structure is refined at 1.7 K with Co2+magnetic moment 2.8(1),μ_B,consistent with our first-principles calculations.
基金supported by the Basic Science Center Project of NSFC under.Grant,No.51788104,NSFC under_Grant_No.52073155,and Tsinghua-Foshan Innovation Special Fund(TFISF)under Grant No.2020THFS0113Research conducted at the NOMAD beamlines at ORNL's Spallation Neutron Source was sponsored by the Scientific User Facilities Division,Office of Basic Sciences,U.S.Department of Energy.
文摘Antiferroelectrics have attracted increasing research interests in recent years due to both their great potential in energy storage applications and intriguing structural characteristics.However,the links between the electrical properties and structural characteristics of distorted perovskite antiferroelectrics are yet to be fully deciphered.Here,we adopt local-structure methods to elucidate the nanoscale atomic structure of AgNbO,-based antiferroelectrics and their structural evolution upon La doping.The local structural features including interatomic distance distributions and atomic displacements have been analyzed using neutron small-box pair distribution function(PDF)refinement in conjunction with large-box Reverse Monte Carlo modelling.Our results highlight the correlation of cation displacements in AgNbo,and its disruption by the incorporation of La,apparently in corroboration with the observed anomalous dielectric properties.Spatial ordering of cation vacancies is observed in La-doped AgNbo,samples,which coordinates with oxygen octahedral tilting to relieve lattice strain.These results provide renewed insights into the atomic structure and antiferroelectric phase instabilities of AgNbO,and relevant perovskite materials,further lending versatile opportunities for enhancing their functionalities.
基金supported by the Division of Materials Science and Engineering, Office of Basic Energy Sciences, U.S. Department of Energy (DOE)。
文摘The energy materials performance is intrinsically determined by structures from the average lattice structure to the atom arrangement, valence, and distribution of the containing transition metal(TM) elements. Understanding the mechanism of the structure transition and atom rearrangement via synthesis or processing is key to expediting the exploration of excellent energy materials. In this work, in situ neutron scattering is employed to reveal the real-time structure evolution, including the TM-O bonds, lattice,TM valence and the migration of the high-voltage spinel cathode LiNi_(0.5)Mn_(1.5)O_(4). The transition-metalmediated spinel destabilization under the annealing at the oxygen-deficient atmosphere is pinpointed.The formation of Mn^(3+) is correlated to the TM migration activation, TM disordered rearrangement in the spinel, and the transition to a layered-rocksalt phase. The further TM interdiffusion and Mn^(3+) reduction are also revealed with multi-stage thermodynamics and kinetics. The mechanisms of phase transition and atom migrations as functions of temperature, time and atmosphere present important guidance on the synthesis in various-valence element containing oxides.
基金Supported by the National Basic Research Program of China under Grant Nos 2012CB921700 and 2011CBA00112the National Natural Science Foundation of China under Grant Nos 11034012 and 11190024+1 种基金the National Science Foundation under Grant No DMR-0645305,the US DOE under Grant No DE-FG02-07ER46358the US Department of Energy,Office of Science,Office of Basic Energy Sciences under Grant No DE-AC05-00OR22725
文摘From heavy fermion compounds and cuprates to iron pnictides and chalcogenides, a spin resonance at hΩ0 ∝ kBTc is a staple of nearly magnetic superconductors. Possible explanations include a two-particle bound state or loss of magnon damping in the superconducting state. While both scenarios suggest a central role for magnetic fluctuations,distinguishing them is important to identify the right theoretical framework to understand these types of unconventional superconductors. Using an inelastic neutron scattering technique,we show that the spin resonance in the optimally doped Fe1.03 Se0.4 Te0.6 superconductor splits into three peaks in a high magnetic field,a signature of a two-particle S = 1 triplet bound state.
