Intrinsic magnetic topological insulators have been reported to exhibit novel physical phenomena such as the quantum anomalous Hall effect and axion insulator states,demonstrating potential for applications in spintro...Intrinsic magnetic topological insulators have been reported to exhibit novel physical phenomena such as the quantum anomalous Hall effect and axion insulator states,demonstrating potential for applications in spintronics and topological quantum computing.Here we perform low-temperature scanning tunneling microscopy(STM)investigations of the antiferromagnetic ground state of MnSb_(2)Te_(4),a predicted magnetic topological insulator isostructural with MnBi_(2)Te_(4).We visualize the hexagonal Te-terminated surface of MnSb_(2)Te_(4)and identify two distinct defects originating from different antisite substitutions.Notably,we identify an in-gap state above the Fermi energy where the tunneling spectrum exhibits a negative differential conductance behavior.This electronic state can be modulated by external electric and magnetic fields,suggesting effective pathways for electronic state manipulation.Spin-resolved STM measurements further reveal additional magnetic resonance peaks associated with Mn antisite defects.Our results provide novel insights into the investigation of magnetic topological insulators and demonstrate a promising approach to modulate the localized electronic states.展开更多
Developing transition metal oxides(TMOs)with high energy,power,and long cycle lifetime for elec-tric energy storage devices remains a critical challenge to date.Herein,we demonstrate a facile method that enables in-si...Developing transition metal oxides(TMOs)with high energy,power,and long cycle lifetime for elec-tric energy storage devices remains a critical challenge to date.Herein,we demonstrate a facile method that enables in-situ transformation of nickel cobalt oxide nanowire arrays(NiCoO NWA)into hierarchical nanowire-nanosheet arrays(ac-NiCoO NWSA)for enhanced energy storage properties.More specifically,the method leads to formation of atomically thin nanosheets(only 2.0 nm)and creates abundant an-tisite defects and oxygen vacancies.Owing to these merits,the as-prepared ac-NiCoO NWSA electrode exhibits over five-fold higher specific capacity,superior rate capability(up to 100 A/g),and excellent cy-cling stability of 10,000 cycles at 50 A/g in alkaline electrolyte compared to pristine NiCoO NWA.Density functional theory(DFT)simulations elucidate the electrochemical activity enhancement mechanism of the TMOs.Moreover,our method triggers similar structural reconstruction phenomenon on other TMOs including ZnCo-,CoMn-and ZnNiCo-oxides,proving the universality of the method.Our findings provide a general method towards simultaneously manipulating the micro-morphologies and defects of TMOs for advanced energy storage devices.展开更多
A half-metallic full-Heusler Mn_(2)VAl alloy is a potential p-type thermoelectric material that can directly generate electricity from waste heat via the Seebeck effect.For practical use,the Seebeck coefficient S of M...A half-metallic full-Heusler Mn_(2)VAl alloy is a potential p-type thermoelectric material that can directly generate electricity from waste heat via the Seebeck effect.For practical use,the Seebeck coefficient S of Mn_(2)VAl should be increased while maintaining a high electrical conductivity s from its half-metallic character.Herein,we achieved this objective through antisite defect engineering.Theoretically,it was predicted that the S was maximized by regulating partial density of states of majority-spin sp-electrons through the control of the fraction of antisite defect,f_(AD),between V and Al atoms in Mn_(2)VAl.Experi-mentally,a significant increase in S and a slight decrease in s were observed for an Mn_(2)VAl sample with an optimal fAD=33%,enhancing the thermoelectric power factor PF by 2.7 times from an Mn_(2)VAl sample with fAD=14%.Furthermore,we combined the antisite defect engineering with a partial substitution method.An Mn_(2)V(Al_(0.96)Si_(0.04))sample with fAD=33%exhibited the highest PF=4.5×10^(-4)W·m^(-1)·K^(-2)at 767 K among the samples.The maximum dimensionless figure-of-merit zT of the Mn_(2)V(Al_(0.96)Si_(0.04))sample with f_(AD)=33%was measured to be 3.4×10^(-2)at 767 K,which is the highest among the p-type half-metallic full-Heusler alloys.展开更多
From the UV?Vis absorption spectra,the FT-IR absorption spectra and the Raman spectra,it is deduced that Co ionsprimarily occupy the tetrahedral(A)site,with a minor number of them entering into the octahedral(B)site i...From the UV?Vis absorption spectra,the FT-IR absorption spectra and the Raman spectra,it is deduced that Co ionsprimarily occupy the tetrahedral(A)site,with a minor number of them entering into the octahedral(B)site in the Ni1?xCoxCr2O4compounds.The origin of the position disorder of the Co ions is consistent with the similar ionic radii of the Co ion(0.65?)and theCr ion(0.62?)at B site.The FT-IR peak at about510cm?1shifts towards high frequency side with the increasing cobalt content.Itis resulted from the reduction of the cation?oxygen distance in the octahedron by the replacement of the Ni2+with the Co2+ions.Themagnetic measurement shows that Curie temperatures(TC)are75and90K for the compounds with x=0.2and0.8,respectively.展开更多
Equilibrium equation of point defects in Ll_2 type intermetallic compounds was established to calculate the relations of the concentration of antisite defects and vacancies and bulk composi- tion in Ni_3Al.The examina...Equilibrium equation of point defects in Ll_2 type intermetallic compounds was established to calculate the relations of the concentration of antisite defects and vacancies and bulk composi- tion in Ni_3Al.The examination of temperature effects on the point defects cleared up the mis. understanding of the properties of the“constitutional point defects”in Ni_3Al.展开更多
Low temperature(77 K)photoluminescence measurements have been performed on different GaAs substrates to evaluate the GaAs crystal quality.Several defect-related luminescence peaks have been observed,including 1.452 eV...Low temperature(77 K)photoluminescence measurements have been performed on different GaAs substrates to evaluate the GaAs crystal quality.Several defect-related luminescence peaks have been observed,including 1.452 eV,1.476 eV,1.326 eV peaks deriving from 78 meV GaAs antisite defects,and 1.372 eV,1.289 eV peaks resulting from As vacancy related defects.Changes in photoluminescence emission intensity and emission energy as a function of temperature and excitation power lead to the identification of the defect states.The luminescence mechanisms of the defect states were studied by photoluminescence spectroscopy and the growth quality of GaAs crystal was evaluated.展开更多
Benefited from its high process feasibility and controllable costs,binary-metal layered structured LiNi_(0.8)Mn_(0.2)O_(2)(NM)can effectively alleviate the cobalt supply crisis under the surge of global electric vehic...Benefited from its high process feasibility and controllable costs,binary-metal layered structured LiNi_(0.8)Mn_(0.2)O_(2)(NM)can effectively alleviate the cobalt supply crisis under the surge of global electric vehicles(EVs)sales,which is considered as the most promising nextgeneration cathode material for lithium-ion batteries(LIBs).However,the lack of deep understanding on the failure mechanism of NM has seriously hindered its application,especially under the harsh condition of high-voltage without sacrifices of reversible capacity.Herein,singlecrystal LiNi_(0.8)Mn_(0.2)O_(2) is selected and compared with traditional LiNi_(0.8)Co_(0.1)Mn_(0.1)O_(2)(NCM),mainly focusing on the failure mechanism of Cofree cathode and illuminating the significant effect of Co element on the Li/Ni antisite defect and dynamic characteristic.Specifically,the presence of high Li/Ni antisite defect in NM cathode easily results in the extremely dramatic H2/H3 phase transition,which exacerbates the distortion of the lattice,mechanical strain changes and exhibits poor electrochemical performance,especially under the high cutoff voltage.Furthermore,the reaction kinetic of NM is impaired due to the absence of Co element,especially at the single-crystal architecture.Whereas,the negative influence of Li/Ni antisite defect is controllable at low current densities,owing to the attenuated polarization.Notably,Co-free NM can exhibit better safety performance than that of NCM cathode.These findings are beneficial for understanding the fundamental reaction mechanism of single-crystal Ni-rich Co-free cathode materials,providing new insights and great encouragements to design and develop the next generation of LIBs with low-cost and high-safety performances.展开更多
We investigate the evolution of magnetic properties as well as the content and distribution of Mn for Mn(Sb_(1-x)Bi_(x))_(2)Te_(4) single crystals grown by large-temperature-gradient chemical vapor transport method.It...We investigate the evolution of magnetic properties as well as the content and distribution of Mn for Mn(Sb_(1-x)Bi_(x))_(2)Te_(4) single crystals grown by large-temperature-gradient chemical vapor transport method.It is found that the ferromagnetic MnSb_(2)Te_(4) changes to antiferromagnetism with Bi doping when x≥0.25.Further analysis implies that the occupations of Mn ions at Sb/Bi site Mn_(Sb/Bi) and Mn site Mn_(Mn) have a strong influence on the magnetic ground states of these systems.With the decrease of Mn_(Mn) increase of Mn_(Sb/Bi),the system will favor the ferromagnetic ground state.In addition,the rapid decrease of T_(C/N) with increasing Bi content when x ≤0.25 and the insensitivity of T_(N) to x when x> 0.25 suggest that the main magnetic interaction may change from the Ruderman-Kittel-Kasuya-Yosida type at low Bi doping region to the van-Vleck type in high Bi doped samples.展开更多
Based on the microscopic phase-field model, the correlation between site occupation evolution of alloying elements in Ni3V-DO22 phase and growth of Ni3Al-L12 phase was studied during the phase transformation of Ni75Al...Based on the microscopic phase-field model, the correlation between site occupation evolution of alloying elements in Ni3V-DO22 phase and growth of Ni3Al-L12 phase was studied during the phase transformation of Ni75Al4.2V20.8. The results demonstrate that the growth of L12 phase can be divided into two stages： at the early stage, the composition of alloying elements in DO22 phase almost remains unchanged; at the late stage, the compositions of Ni and Al decrease while V increases in DO22 phase. Part of alloying elements for L12 phase growth are supplied from the site occupation evolution of alloying elements on three kinds of sublattices in DO22 phase. Ni is mainly supplied from V sublattice, and part of Al is supplied from NiⅠ and V sites at the centre of DO22 phase. The excessive V from the decreasing DO22 phase migrates into the centre of DO22 phase and mainly occupies V and NiII sites. It is the site occupation evolution of antisite atoms and ternary additions in DO22 phase that controls the growth rate of L12 phase at the late stage.展开更多
Correlation between site occupation evolution of alloying elements in L12 phase and growth of DO22 phase in Ni75Al7.5V17.5 was studied using microscopic phase field model. The results demonstrate that the growing proc...Correlation between site occupation evolution of alloying elements in L12 phase and growth of DO22 phase in Ni75Al7.5V17.5 was studied using microscopic phase field model. The results demonstrate that the growing process of DO22 phase can be divided into two stages. At the early stage, composition in the centre part of L12 phase almost remains unchanged, and the nucleation and growth of DO22 phase is controlled by the decrease of interface between L12 phases. At the late stage, part of V for growth of DO22 phase is supplied from the centre part of L12 phase and mainly comes from Al sublattice, the excess Ni spared from the decreasing L12 phase migrates into the centre part of L12 phase and occupies the Ni sublattices exclusively, while the excess Al mainly occupies the Al sublattice. At the late stage, the growth of DO22 phase is controlled by the evolution of antisite atoms and ternary additions in the centre part of L12 phase.展开更多
Magnesium aluminate spinel(MgAl2O4)is widely used in steel metallurgy industry.Thermal conductivity at high temperature signifcantly infuences the cooling process of blast furnace and the heat preservation of steel co...Magnesium aluminate spinel(MgAl2O4)is widely used in steel metallurgy industry.Thermal conductivity at high temperature signifcantly infuences the cooling process of blast furnace and the heat preservation of steel converter.The efect of external(temperature)and internal(antisite defect and grain boundary)factors on the thermal conductivity of MgAl2O4 was studied with non-equilibrium molecular dynamics.The main factors afecting the thermal conductivity of MgAl2O4 were summarized.In the temperature range of 100-2000 K,the results showed that the thermal conductivity of MgAl2O4 changed from 11.54 to 4.95 W/(m K)with the increase in temperature and was relatively stable at the temperature above 1000 K.The thermal conductivity of MgAl2O4 declined frst and then rose with the increase in the antisite defects,and the minimum value was 6.95 W/(m K)at the inversion parameter i=0.35.In addition,grain boundaries reduced the thermal conductivity of MgAl2O4 by 20%-30%at temperature below 1000 K comparing with the non-grain boundary system.The grain boundary rotation angle at temperature above 1000 K had less efect on the thermal conductivity than that below 1000 K.Present simulation scheme for thermal conductivity of MgAl2O4 can also be applied to the study of other nonmetallic ceramics.展开更多
Transparent Ce:lutetium aluminum garnet(Ce:Lu_(3)A_(l5)O_(12),Ce:LuAG)ceramics have been regarded as potential scintillator materials due to their relatively high density and atomic number(Zeff).However,the current Ce...Transparent Ce:lutetium aluminum garnet(Ce:Lu_(3)A_(l5)O_(12),Ce:LuAG)ceramics have been regarded as potential scintillator materials due to their relatively high density and atomic number(Zeff).However,the current Ce:LuAG ceramics exhibit a light yield much lower than the expected theoretical value due to the inevitable presence of LuAl antisite defects at high sintering temperatures.This work demonstrates a low-temperature(1100℃)synthetic strategy for elaborating transparent LuAG–Al_(2)O_(3) nanoceramics through the crystallization of 72 mol%Al_(2)O_(3)–28 mol%Lu_(2)O_(3)(ALu28)bulk glass.The biphasic nanostructure composed of LuAG and Al_(2)O_(3) nanocrystals makes up the whole ceramic materials.Most of Al_(2)O_(3) is distributed among LuAG grains,and the rest is present inside the LuAG grains.Fully dense biphasic LuAG–Al_(2)O_(3) nanoceramics are highly transparent from the visible region to mid-infrared(MIR)region,and particularly the transmittance reaches 82%at 780 nm.Moreover,LuAl antisite defect-related centers are completely undetectable in X-ray excited luminescence(XEL)spectra of Ce:LuAG–Al_(2)O_(3) nanoceramics with 0.3–1.0 at%Ce.The light yield of 0.3 at%Ce:LuAG–Al_(2)O_(3) nanoceramics is estimated to be 20,000 ph/MeV with short 1μs shaping time,which is far superior to that of commercial Bi_(4)Ge_(3)O_(12)(BGO)single crystals.These results show that a low-temperature glass crystallization route provides an alternative approach for eliminating the antisite defects in LuAG-based ceramics,and is promising to produce garnet-based ceramic materials with excellent properties,thereby meeting the demands of advanced scintillation applications.展开更多
Twin boundaries have been exploited to stabilize ultrafine grains and improve mechanical properties of nanomaterials.The production of the twin boundaries and nanotwins is however prohibitively challenging in carbide ...Twin boundaries have been exploited to stabilize ultrafine grains and improve mechanical properties of nanomaterials.The production of the twin boundaries and nanotwins is however prohibitively challenging in carbide ceramics.Using a scanning transmission electron microscope as a unique platform for atomic-scale structure engineering,we demonstrate that twin platelets could be produced in carbides by engineering antisite defects.The antisite defects at metal sites in various layered ternary carbides are collectively and controllably generated,and the metal elements are homogenized by electron irradiation,which transforms a twin-like lamellae into nanotwin platelets.Accompanying chemical homogenization,α-Ti_(3)AlC_(2) transforms to unconventionalβ-Ti_(3)AiC_(2).The chemical homogeneity and the width of the twin platelets can be tuned by dose and energy of bombarding electrons.Chemically homogenized nanotwins can boost hardness by~45%.Our results provide a new way to produce ultrathin(<5 nm)nanotwin platelets in scientifically and technologically important carbide materials and showcase feasibility of defect engineering by an angstrom-sized electron probe.展开更多
Identification of atomic disorders and their subsequent control has proven to be a key issue in predicting, understanding, and enhancing the properties of newly emerging topological insulator materials. Here, we demon...Identification of atomic disorders and their subsequent control has proven to be a key issue in predicting, understanding, and enhancing the properties of newly emerging topological insulator materials. Here, we demonstrate direct evidence of the cation antisites in single-crystal SnBi2Te4 nanoplates grown by chemical vapor deposition, through a combination of sub-angstr6m-resolution imaging, quantitative image simulations, and density functional theory calculations. The results of these combined techniques revealed a recognizable amount of cation antisites between Bi and Sn, and energetic calculations revealed that such cation antisites have a low formation energy. The impact of the cation antisites was also investigated by electronic structure calculations together with transport measurement. The topological surface properties of the nanoplates were further probed by angle-dependent magnetotransport, and from the results, we observed a two-dimensional weak antilocalization effect associated with surface carriers. Our approach provides a pathway to identify the antisite defects in ternary chalcogenides and the application potential of SnBi2Te4 nanostructures in next-generation electronic and spintronic devices.展开更多
基金Project supported by the National Key R&D Program of China(Grant Nos.2022YFA1403800 and 2023YFA1406500)the National Natural Science Foundation of China(Grant No.12274459)。
文摘Intrinsic magnetic topological insulators have been reported to exhibit novel physical phenomena such as the quantum anomalous Hall effect and axion insulator states,demonstrating potential for applications in spintronics and topological quantum computing.Here we perform low-temperature scanning tunneling microscopy(STM)investigations of the antiferromagnetic ground state of MnSb_(2)Te_(4),a predicted magnetic topological insulator isostructural with MnBi_(2)Te_(4).We visualize the hexagonal Te-terminated surface of MnSb_(2)Te_(4)and identify two distinct defects originating from different antisite substitutions.Notably,we identify an in-gap state above the Fermi energy where the tunneling spectrum exhibits a negative differential conductance behavior.This electronic state can be modulated by external electric and magnetic fields,suggesting effective pathways for electronic state manipulation.Spin-resolved STM measurements further reveal additional magnetic resonance peaks associated with Mn antisite defects.Our results provide novel insights into the investigation of magnetic topological insulators and demonstrate a promising approach to modulate the localized electronic states.
基金supported by National Natural Science Foundation of China (Nos. 21905229, 22071195 and 21805227)China Postdoctoral Science Foundation (No. 2020M683557)+2 种基金Fundamental Research Funds for the Central Universities (No. 3102017jc01001)the postgraduate research scholarship at Queensland University of Technology (QUT-PRA scholarship)the Youth Innovation Team of Shaanxi Universities
文摘Developing transition metal oxides(TMOs)with high energy,power,and long cycle lifetime for elec-tric energy storage devices remains a critical challenge to date.Herein,we demonstrate a facile method that enables in-situ transformation of nickel cobalt oxide nanowire arrays(NiCoO NWA)into hierarchical nanowire-nanosheet arrays(ac-NiCoO NWSA)for enhanced energy storage properties.More specifically,the method leads to formation of atomically thin nanosheets(only 2.0 nm)and creates abundant an-tisite defects and oxygen vacancies.Owing to these merits,the as-prepared ac-NiCoO NWSA electrode exhibits over five-fold higher specific capacity,superior rate capability(up to 100 A/g),and excellent cy-cling stability of 10,000 cycles at 50 A/g in alkaline electrolyte compared to pristine NiCoO NWA.Density functional theory(DFT)simulations elucidate the electrochemical activity enhancement mechanism of the TMOs.Moreover,our method triggers similar structural reconstruction phenomenon on other TMOs including ZnCo-,CoMn-and ZnNiCo-oxides,proving the universality of the method.Our findings provide a general method towards simultaneously manipulating the micro-morphologies and defects of TMOs for advanced energy storage devices.
基金supported by Grant-in-Aid for JSPS Fellows(no.20J11073)from the Japan Society for the Promotion of Science and by the Tsinghua-Tohoku Collaborative Research Fund from Tsinghua University and Tohoku Universitysupported by the Grant-in-Aid for Scientific Research(B)(nos.20H01841,22H02161)from the Japan Society for the Promotion of Science.
文摘A half-metallic full-Heusler Mn_(2)VAl alloy is a potential p-type thermoelectric material that can directly generate electricity from waste heat via the Seebeck effect.For practical use,the Seebeck coefficient S of Mn_(2)VAl should be increased while maintaining a high electrical conductivity s from its half-metallic character.Herein,we achieved this objective through antisite defect engineering.Theoretically,it was predicted that the S was maximized by regulating partial density of states of majority-spin sp-electrons through the control of the fraction of antisite defect,f_(AD),between V and Al atoms in Mn_(2)VAl.Experi-mentally,a significant increase in S and a slight decrease in s were observed for an Mn_(2)VAl sample with an optimal fAD=33%,enhancing the thermoelectric power factor PF by 2.7 times from an Mn_(2)VAl sample with fAD=14%.Furthermore,we combined the antisite defect engineering with a partial substitution method.An Mn_(2)V(Al_(0.96)Si_(0.04))sample with fAD=33%exhibited the highest PF=4.5×10^(-4)W·m^(-1)·K^(-2)at 767 K among the samples.The maximum dimensionless figure-of-merit zT of the Mn_(2)V(Al_(0.96)Si_(0.04))sample with f_(AD)=33%was measured to be 3.4×10^(-2)at 767 K,which is the highest among the p-type half-metallic full-Heusler alloys.
基金Project(11264024)supported by the National Natural Science Foundation of ChinaProjects(2015MS0102,2015MS0524)supported by Natural Science Foundation of Inner Mongolia,China
文摘From the UV?Vis absorption spectra,the FT-IR absorption spectra and the Raman spectra,it is deduced that Co ionsprimarily occupy the tetrahedral(A)site,with a minor number of them entering into the octahedral(B)site in the Ni1?xCoxCr2O4compounds.The origin of the position disorder of the Co ions is consistent with the similar ionic radii of the Co ion(0.65?)and theCr ion(0.62?)at B site.The FT-IR peak at about510cm?1shifts towards high frequency side with the increasing cobalt content.Itis resulted from the reduction of the cation?oxygen distance in the octahedron by the replacement of the Ni2+with the Co2+ions.Themagnetic measurement shows that Curie temperatures(TC)are75and90K for the compounds with x=0.2and0.8,respectively.
文摘Equilibrium equation of point defects in Ll_2 type intermetallic compounds was established to calculate the relations of the concentration of antisite defects and vacancies and bulk composi- tion in Ni_3Al.The examination of temperature effects on the point defects cleared up the mis. understanding of the properties of the“constitutional point defects”in Ni_3Al.
基金Project supported by the National Natural Science Foundation of China(Grant No.21972103)the National Key Research and Development Program of China(Grant No.2016YFB040183)Research and Development Program of Shanxi Province,China(Grant No.201703D111026)
文摘Low temperature(77 K)photoluminescence measurements have been performed on different GaAs substrates to evaluate the GaAs crystal quality.Several defect-related luminescence peaks have been observed,including 1.452 eV,1.476 eV,1.326 eV peaks deriving from 78 meV GaAs antisite defects,and 1.372 eV,1.289 eV peaks resulting from As vacancy related defects.Changes in photoluminescence emission intensity and emission energy as a function of temperature and excitation power lead to the identification of the defect states.The luminescence mechanisms of the defect states were studied by photoluminescence spectroscopy and the growth quality of GaAs crystal was evaluated.
基金the National Natural Science Foundation of China(52070194,52073309,51902347,51908555)Natural Science Foundation of Hunan Province(2022JJ20069,2020JJ5741).
文摘Benefited from its high process feasibility and controllable costs,binary-metal layered structured LiNi_(0.8)Mn_(0.2)O_(2)(NM)can effectively alleviate the cobalt supply crisis under the surge of global electric vehicles(EVs)sales,which is considered as the most promising nextgeneration cathode material for lithium-ion batteries(LIBs).However,the lack of deep understanding on the failure mechanism of NM has seriously hindered its application,especially under the harsh condition of high-voltage without sacrifices of reversible capacity.Herein,singlecrystal LiNi_(0.8)Mn_(0.2)O_(2) is selected and compared with traditional LiNi_(0.8)Co_(0.1)Mn_(0.1)O_(2)(NCM),mainly focusing on the failure mechanism of Cofree cathode and illuminating the significant effect of Co element on the Li/Ni antisite defect and dynamic characteristic.Specifically,the presence of high Li/Ni antisite defect in NM cathode easily results in the extremely dramatic H2/H3 phase transition,which exacerbates the distortion of the lattice,mechanical strain changes and exhibits poor electrochemical performance,especially under the high cutoff voltage.Furthermore,the reaction kinetic of NM is impaired due to the absence of Co element,especially at the single-crystal architecture.Whereas,the negative influence of Li/Ni antisite defect is controllable at low current densities,owing to the attenuated polarization.Notably,Co-free NM can exhibit better safety performance than that of NCM cathode.These findings are beneficial for understanding the fundamental reaction mechanism of single-crystal Ni-rich Co-free cathode materials,providing new insights and great encouragements to design and develop the next generation of LIBs with low-cost and high-safety performances.
基金Project supported by the Beijing Natural Science Foundation (Grant No. Z200005)the National Key R&D Program of China (Grant Nos. 2022YFA1403800 and 2023YFA1406500)+1 种基金the National Natural Science Foundation of China (Grant No. 12274459)Collaborative Research Project of Laboratory for Materials and Structures, Institute of Innovative Research, Tokyo Institute of Technology。
文摘We investigate the evolution of magnetic properties as well as the content and distribution of Mn for Mn(Sb_(1-x)Bi_(x))_(2)Te_(4) single crystals grown by large-temperature-gradient chemical vapor transport method.It is found that the ferromagnetic MnSb_(2)Te_(4) changes to antiferromagnetism with Bi doping when x≥0.25.Further analysis implies that the occupations of Mn ions at Sb/Bi site Mn_(Sb/Bi) and Mn site Mn_(Mn) have a strong influence on the magnetic ground states of these systems.With the decrease of Mn_(Mn) increase of Mn_(Sb/Bi),the system will favor the ferromagnetic ground state.In addition,the rapid decrease of T_(C/N) with increasing Bi content when x ≤0.25 and the insensitivity of T_(N) to x when x> 0.25 suggest that the main magnetic interaction may change from the Ruderman-Kittel-Kasuya-Yosida type at low Bi doping region to the van-Vleck type in high Bi doped samples.
基金Projects(51174168,51274167)supported by the National Natural Science Foundation of ChinaProject(2013M532082)supported by Postdoctoral Science Foundation of ChinaProjects(13R21421700,13R21421800)supported by the Postdoctoral Science Foundation of Shanghai,China
文摘Based on the microscopic phase-field model, the correlation between site occupation evolution of alloying elements in Ni3V-DO22 phase and growth of Ni3Al-L12 phase was studied during the phase transformation of Ni75Al4.2V20.8. The results demonstrate that the growth of L12 phase can be divided into two stages： at the early stage, the composition of alloying elements in DO22 phase almost remains unchanged; at the late stage, the compositions of Ni and Al decrease while V increases in DO22 phase. Part of alloying elements for L12 phase growth are supplied from the site occupation evolution of alloying elements on three kinds of sublattices in DO22 phase. Ni is mainly supplied from V sublattice, and part of Al is supplied from NiⅠ and V sites at the centre of DO22 phase. The excessive V from the decreasing DO22 phase migrates into the centre of DO22 phase and mainly occupies V and NiII sites. It is the site occupation evolution of antisite atoms and ternary additions in DO22 phase that controls the growth rate of L12 phase at the late stage.
基金Projects (50941020, 10902086, 50875217, 20903075) supported by the National Natural Science Foundation of ChinaProjects (SJ08-ZT05, SJ08-B14) supported by the Natural Science Foundation of Shaanxi Province, China
文摘Correlation between site occupation evolution of alloying elements in L12 phase and growth of DO22 phase in Ni75Al7.5V17.5 was studied using microscopic phase field model. The results demonstrate that the growing process of DO22 phase can be divided into two stages. At the early stage, composition in the centre part of L12 phase almost remains unchanged, and the nucleation and growth of DO22 phase is controlled by the decrease of interface between L12 phases. At the late stage, part of V for growth of DO22 phase is supplied from the centre part of L12 phase and mainly comes from Al sublattice, the excess Ni spared from the decreasing L12 phase migrates into the centre part of L12 phase and occupies the Ni sublattices exclusively, while the excess Al mainly occupies the Al sublattice. At the late stage, the growth of DO22 phase is controlled by the evolution of antisite atoms and ternary additions in the centre part of L12 phase.
基金This work is sponsored by the National Natural Science Foundation of China(Grant Nos.21233010 and 51474047).
文摘Magnesium aluminate spinel(MgAl2O4)is widely used in steel metallurgy industry.Thermal conductivity at high temperature signifcantly infuences the cooling process of blast furnace and the heat preservation of steel converter.The efect of external(temperature)and internal(antisite defect and grain boundary)factors on the thermal conductivity of MgAl2O4 was studied with non-equilibrium molecular dynamics.The main factors afecting the thermal conductivity of MgAl2O4 were summarized.In the temperature range of 100-2000 K,the results showed that the thermal conductivity of MgAl2O4 changed from 11.54 to 4.95 W/(m K)with the increase in temperature and was relatively stable at the temperature above 1000 K.The thermal conductivity of MgAl2O4 declined frst and then rose with the increase in the antisite defects,and the minimum value was 6.95 W/(m K)at the inversion parameter i=0.35.In addition,grain boundaries reduced the thermal conductivity of MgAl2O4 by 20%-30%at temperature below 1000 K comparing with the non-grain boundary system.The grain boundary rotation angle at temperature above 1000 K had less efect on the thermal conductivity than that below 1000 K.Present simulation scheme for thermal conductivity of MgAl2O4 can also be applied to the study of other nonmetallic ceramics.
基金supported by the National Natural Science Foundation of China (No.51972304)Beijing Municipal Science&Technology Commission,Administrative Commission of Zhongguancun Science Park (No.Z221100006722022)+1 种基金the Project of Scientific Experiment on Chinese Manned Space Station,Chinese Academy of Sciences President’s International Fellowship Initiative for 2021 (No.2021VEA0012)the Fundamental Research Funds for the Central Universities.
文摘Transparent Ce:lutetium aluminum garnet(Ce:Lu_(3)A_(l5)O_(12),Ce:LuAG)ceramics have been regarded as potential scintillator materials due to their relatively high density and atomic number(Zeff).However,the current Ce:LuAG ceramics exhibit a light yield much lower than the expected theoretical value due to the inevitable presence of LuAl antisite defects at high sintering temperatures.This work demonstrates a low-temperature(1100℃)synthetic strategy for elaborating transparent LuAG–Al_(2)O_(3) nanoceramics through the crystallization of 72 mol%Al_(2)O_(3)–28 mol%Lu_(2)O_(3)(ALu28)bulk glass.The biphasic nanostructure composed of LuAG and Al_(2)O_(3) nanocrystals makes up the whole ceramic materials.Most of Al_(2)O_(3) is distributed among LuAG grains,and the rest is present inside the LuAG grains.Fully dense biphasic LuAG–Al_(2)O_(3) nanoceramics are highly transparent from the visible region to mid-infrared(MIR)region,and particularly the transmittance reaches 82%at 780 nm.Moreover,LuAl antisite defect-related centers are completely undetectable in X-ray excited luminescence(XEL)spectra of Ce:LuAG–Al_(2)O_(3) nanoceramics with 0.3–1.0 at%Ce.The light yield of 0.3 at%Ce:LuAG–Al_(2)O_(3) nanoceramics is estimated to be 20,000 ph/MeV with short 1μs shaping time,which is far superior to that of commercial Bi_(4)Ge_(3)O_(12)(BGO)single crystals.These results show that a low-temperature glass crystallization route provides an alternative approach for eliminating the antisite defects in LuAG-based ceramics,and is promising to produce garnet-based ceramic materials with excellent properties,thereby meeting the demands of advanced scintillation applications.
文摘Twin boundaries have been exploited to stabilize ultrafine grains and improve mechanical properties of nanomaterials.The production of the twin boundaries and nanotwins is however prohibitively challenging in carbide ceramics.Using a scanning transmission electron microscope as a unique platform for atomic-scale structure engineering,we demonstrate that twin platelets could be produced in carbides by engineering antisite defects.The antisite defects at metal sites in various layered ternary carbides are collectively and controllably generated,and the metal elements are homogenized by electron irradiation,which transforms a twin-like lamellae into nanotwin platelets.Accompanying chemical homogenization,α-Ti_(3)AlC_(2) transforms to unconventionalβ-Ti_(3)AiC_(2).The chemical homogeneity and the width of the twin platelets can be tuned by dose and energy of bombarding electrons.Chemically homogenized nanotwins can boost hardness by~45%.Our results provide a new way to produce ultrathin(<5 nm)nanotwin platelets in scientifically and technologically important carbide materials and showcase feasibility of defect engineering by an angstrom-sized electron probe.
文摘Identification of atomic disorders and their subsequent control has proven to be a key issue in predicting, understanding, and enhancing the properties of newly emerging topological insulator materials. Here, we demonstrate direct evidence of the cation antisites in single-crystal SnBi2Te4 nanoplates grown by chemical vapor deposition, through a combination of sub-angstr6m-resolution imaging, quantitative image simulations, and density functional theory calculations. The results of these combined techniques revealed a recognizable amount of cation antisites between Bi and Sn, and energetic calculations revealed that such cation antisites have a low formation energy. The impact of the cation antisites was also investigated by electronic structure calculations together with transport measurement. The topological surface properties of the nanoplates were further probed by angle-dependent magnetotransport, and from the results, we observed a two-dimensional weak antilocalization effect associated with surface carriers. Our approach provides a pathway to identify the antisite defects in ternary chalcogenides and the application potential of SnBi2Te4 nanostructures in next-generation electronic and spintronic devices.
