Single-crystal Ni-rich cathodes are a promising candidate for high-energy lithium-ion batteries due to their higher structural and cycling stability than polycrystalline materials.However,the phase evolution and capac...Single-crystal Ni-rich cathodes are a promising candidate for high-energy lithium-ion batteries due to their higher structural and cycling stability than polycrystalline materials.However,the phase evolution and capacity degradation of these single-crystal cathodes during continuous lithation/delithation cycling remains unclear.Understanding the mapping relationship between the macroscopic electrochemical properties and the material physicochemical properties is crucial.Here,we investigate the correlation between the physical-chemical characteristics,phase transition,and capacity decay using capacity differential curve feature identification and in-situ X-ray spectroscopic imaging.We systematically clarify the dominant mechanism of phase evolution in aging cycling.Appropriately high cut-off voltages can mitigate the slow kinetic and electrochemical properties of single-crystal cathodes.We also find that second-order differential capacity discharge characteristic curves can be used to identify the crystal structure disorder of Ni-rich cathodes.These findings constitute a step forward in elucidating the correlation between the electrochemical extrinsic properties and the physicochemical intrinsic properties and provide new perspectives for failure analysis of layered electrode materials.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
The poor electrochemical performance of all-solid-state batteries(ASSBs),which is assemblied by Ni-rich cathode and poly(ethylene oxide)(PEO)-based electrolytes,can be attributed to unstable cathodic interface and poo...The poor electrochemical performance of all-solid-state batteries(ASSBs),which is assemblied by Ni-rich cathode and poly(ethylene oxide)(PEO)-based electrolytes,can be attributed to unstable cathodic interface and poor crystal structure stability of Ni-rich cathode.Several coating strategies are previously employed to enhance the stability of the cathodic interface and crystal structure for Ni-rich cathode.However,these methods can hardly achieve simplicity and high efficiency simultaneously.In this work,polyacrylic acid(PAA)replaced traditional PVDF as a binder for cathode,which can achieve a uniform PAA-Li(LixPAA(0<x≤1))coating layer on the surface of single-crystal LiNi_(0.83)Co_(0.12)Mn_(0.05)O_(2)(SC-NCM83)due to H^(+)/Li^(+)exchange reaction during the initial charging-discharging process.The formation of PAA-Li coating layer on cathode can promote interfacial Li^(+)transport and enhance the stability of the cathodic interface.Furthermore,the partially-protonated surface of SC-NCM83 casued by H^(+)/Li^(+)exchange reaction can restrict Ni ions transport to enhance the crystal structure stability.The proposed SC-NCM83-PAA exhibits superior cycling performance with a retention of 92%compared with that(57.3%)of SC-NCM83-polyvinylidene difluoride(PVDF)after 200 cycles.This work provides a practical strategy to construct high-performance cathodes for ASSBs.展开更多
LiNi_(0.5)Co_(0.2)Mn_(0.3)O_(2) is extensively researched as one of the most widely used commercially materials for Li-ion batteries at present.However,the poor high-voltage performance(≥4.3 V)with low reversible cap...LiNi_(0.5)Co_(0.2)Mn_(0.3)O_(2) is extensively researched as one of the most widely used commercially materials for Li-ion batteries at present.However,the poor high-voltage performance(≥4.3 V)with low reversible capacity limits its replacement for LiCoO_(2) in high-end digital field.Herein,three-in-one modification,Na-doping and Al_(2)O_(3)@Li_(3)BO_(3) dual-coating simultaneously,is explored for single-crystalline LiNi_(0.5)Co_(0.2)Mn_(0.3)O_(2)(N-NCM@AB),which exhibits excellent high-voltage performance.N-NCM@AB displays a discharge-specific capacity of 201.8 mAh g^(−1) at 0.2 C with a high upper voltage of 4.6 V and maintains 158.9 mAh g^(−1) discharge capacity at 1 C over 200 cycles with the corresponding capacity retention of 87.8%.Remarkably,the N-NCM@AB||graphite pouch-type full cell retains 81.2% of its initial capacity with high working voltage of 4.4 V over 1600 cycles.More importantly,the fundamental understandings of three-in-one modification on surface morphology,crystal structure,and phase transformation of N-NCM@AB are clearly revealed.The Na+doped into the Li–O slab can enhance the bond energy,stabilize the crystal structure,and facilitate Li+transport.Additionally,the interior surface layer of Li^(+)-ions conductor Li_(3)BO_(3) relieves the charge transfer resistance with surface coating,whereas the outer surface Al_(2)O_(3) coating layer is beneficial for reducing the active materials loss and alleviating the electrode/electrolyte parasite reaction.This three-in-one strategy provides a reference for the further research on the performance attenuation mechanism of NCM,paving a new avenue to boost the high-voltage performance of NCM cathode in Li-ion batteries.展开更多
The process of thermal stress damage during 1080 nm laser ablation of single-crystal germanium was recorded in real time using a high-speed charge-coupled device.A three-dimensional finite element numerical model base...The process of thermal stress damage during 1080 nm laser ablation of single-crystal germanium was recorded in real time using a high-speed charge-coupled device.A three-dimensional finite element numerical model based on Fourier's heat conduction equation,Hooke's law and the Alexander–Hasson equation was developed to analyze the thermal stress damage mechanism involved.The damage morphology of the ablated samples was observed using an optical microscope.The results show that the cooling process has an important influence on fracture in the laser-irradiated region of single-crystal germanium.Fracture is the result of a combination of thermal stress and reduction in local yield strength.展开更多
A single-crystal diamond detector is fabricated to diagnose 14.1 MeV deuterium-tritium(D-T)fusion neutrons.The size of its diamond film is 4.5 mm×4.5 mm×500μm.This film is sandwiched by a flat,strip-pattern...A single-crystal diamond detector is fabricated to diagnose 14.1 MeV deuterium-tritium(D-T)fusion neutrons.The size of its diamond film is 4.5 mm×4.5 mm×500μm.This film is sandwiched by a flat,strip-patterned gold electrode.The dark current of this detector is experimentally measured to be lower than 0.1 nA under an electric field of 30 kV cm^(-1).This diamond detector is used to measure D-T fusion neutrons with a flux of about 7.5×10^(5) s^(-1)cm^(-2).The pronounced peak with a central energy of 8.28 MeV characterizing the^(12)C(n,α)~9Be reaction in the neutron energy spectrum is experimentally diagnosed,and the energy resolution is better than 1.69%,which is the best result reported so far using a diamond detector.A clear peak with a central energy of 6.52 MeV characterizing the^(12)C(n,n')3αreaction is also identified with an energy resolution of better than 7.67%.展开更多
Lead halide perovskites have attracted considerable attention as potential candidates for high-performance nano/microlasers,owing to their outstanding optical properties.However,the further development of perovskite m...Lead halide perovskites have attracted considerable attention as potential candidates for high-performance nano/microlasers,owing to their outstanding optical properties.However,the further development of perovskite microlaser arrays(especially based on polycrystalline thin films)produced by the conventional processing techniques is hindered by the chemical instability and surface roughness of the perovskite structures.Herein,we demonstrate a laser patterning of large-scale,highly crystalline perovskite single-crystal films to fabricate reproducible perovskite single-crystal-based microlaser arrays.Perovskite thin films were directly ablated by femtosecond-laser in multiple low-power cycles at a minimum machining line width of approximately 300 nm to realize high-precision,chemically clean,and repeatable fabrication of microdisk arrays.The surface impurities generated during the process can be washed away to avoid external optical loss due to the robustness of the single-crystal film.Moreover,the high-quality,large-sized perovskite single-crystal films can significantly improve the quality of microcavities,thereby realizing a perovskite microdisk laser with narrow linewidth(0.09 nm)and low threshold(5.1µJ/cm2).Benefiting from the novel laser patterning method and the large-sized perovskite single-crystal films,a high power and high color purity laser display with single-mode microlasers as pixels was successfully fabricated.Thus,this study may offer a potential platform for mass-scale and reproducible fabrication of microlaser arrays,and further facilitate the development of highly integrated applications based on perovskite materials.展开更多
Within the framework of the density functional theory and the pseudopotential method,the electronic structure calculations of the“metal-Si(100)”systems with Li,Be and Al as metal coverings of one to four monolayers(...Within the framework of the density functional theory and the pseudopotential method,the electronic structure calculations of the“metal-Si(100)”systems with Li,Be and Al as metal coverings of one to four monolayers(ML)thickness,were carried out.Calculations showed that band gaps of 1.02 eV,0.98 eV and 0.5 eV,respectively,appear in the densities of electronic states when the thickness of Li,Be and Al coverings is one ML.These gaps disappear with increasing thickness of the metal layers:first in the Li-Si system(for two ML),then in the Al-Si system(for three ML)and then in the Be-Si system(for four ML).This behavior of the band gap can be explained by the passivation of the substrate surface states and the peculiarities of the electronic structure of the adsorbed metals.In common the results can be interpreted as describing the possibility of the formation of a two-dimensional silicide with semiconducting properties in Li-Si(100),Be-Si(100)and Al-Si(100)systems.展开更多
The microstructure of the RE silicide alloy was studied by SEM. The feature of the phase and the distribution of Ca, P, Al were analyzed, especially the distribution of micro-cracks and its composition were determined...The microstructure of the RE silicide alloy was studied by SEM. The feature of the phase and the distribution of Ca, P, Al were analyzed, especially the distribution of micro-cracks and its composition were determined. The result demonstrates that only a few phosphides contribute to the spontaneous crumbling of the RE silicide alloy by reacting with water and forming oxide or phosphorus oxide. The phosphorus content is not the critical factor of disintegration in the alloy studied.展开更多
The fracture behavior of fully lamellar binaryγ-TiAl alloys is extremely anisotropic with respect to the lamellar orientation.For the fully lamellar Ti-46Al-0.5W-0.5Si alloy,the existence of silicide clusters plays a...The fracture behavior of fully lamellar binaryγ-TiAl alloys is extremely anisotropic with respect to the lamellar orientation.For the fully lamellar Ti-46Al-0.5W-0.5Si alloy,the existence of silicide clusters plays a critical role on the fracture behavior.In the present study,tensile test and three point bending test were performed at room temperature with the loading axis parallel and perpendicular to the lamellar orientation,respectively.To investigate the influence of silicide clusters on the initiation and propagation of cracks,the fracture surface and the cracks adjacent to the fracture zone of the specimens have been analyzed.Results show that the fracture process is related to the morphology and distribution of the silicide clusters.Crack preferentially initiates at and propagates along the interface of silicide andα 2 /γlamellar with the loading axis perpendicular to the length direction of silicide.While the silicide can prevent the propagation of cracks from running across with the crack growth direction perpendicular to the length direction of silicide.展开更多
To investigate the interdiffusion behavior of Ge-modified silicide coatings on an Nb–Si-based alloy substrate,the coating was oxidized at 1250°C for 5,10,20,50,or 100 h.The interfacial diffusion between the(Nb,X...To investigate the interdiffusion behavior of Ge-modified silicide coatings on an Nb–Si-based alloy substrate,the coating was oxidized at 1250°C for 5,10,20,50,or 100 h.The interfacial diffusion between the(Nb,X)(Si,Ge)_2(X = Ti,Cr,Hf) coating and the Nb–Si based alloy was also examined.The transitional layer is composed of(Ti,Nb)_5(Si,Ge)_4 and a small amount of(Nb,X)_5(Si,Ge)_3.With increasing oxidation time,the thickness of the transitional layer increases because of the diffusion of Si from the outer layer to the substrate,which obeys a parabolic rate law.The parabolic growth rate constant of the transitional layer under oxidation conditions is 2.018 μm×h^(-1/2).Moreover,the interdiffusion coefficients of Si in the transitional layer were determined from the interdiffusion fluxes calculated directly from experimental concentration profiles.展开更多
Manganese silicide MnSi_(2-x) thin films have been prepared on n-type siliconsubstrates through solid phase reaction. The heterostructures were analyzed by X-ray diffraction,Rutherford backscattering spectroscopy, Fou...Manganese silicide MnSi_(2-x) thin films have been prepared on n-type siliconsubstrates through solid phase reaction. The heterostructures were analyzed by X-ray diffraction,Rutherford backscattering spectroscopy, Fourier transform infrared transmittance spectroscopy andthe four-point probe technique. The results show that two manganese silicides have been formedsequentially via the reaction of thin layer Mn with Si substrate at different irradiation annealingstages, i.e., MnSi at 450 deg C and MnSi_(1.73) at 550 deg C. MnSi_(1.73) phase exhibits preferredgrowth after irradiation with infrared. In situ four-point probe measurements of sheet resistanceduring infrared irradiation annealing show that nucleation of MnSi and phase transformation of MnSito MaSi_(1.73) occur at 410 deg C and 530 deg C, respectively; the MnSi phase shows metallicbehavior, while MnSi_(1.73) exhibits semiconducting behavior. Characteristic phonon bands ofMnSi_(2-x) silicides, which can be used for phase identification along with conventional XRDtechniques, have been observed by FTIR spectroscopy.展开更多
Chemical vapor deposition(CVD)-grown diamond films have been developed as irradiation-resistant materials to replace or upgrade current detectors for use in extreme radiation environments. However, their sensitivity i...Chemical vapor deposition(CVD)-grown diamond films have been developed as irradiation-resistant materials to replace or upgrade current detectors for use in extreme radiation environments. However, their sensitivity in practical applications has been inhibited by space charge stability issues caused by defects and impurities in pure diamond crystal materials. In this study, two high-quality CVD-grown single-crystal diamond(SCD) detectors with low content of nitrogen impurities were fabricated and characterized. The intrinsic properties of the SCD samples were characterized using Raman spectroscopy, stereomicroscopy, and X-ray diffraction with the rocking curve mode, cathode luminescence(CL), and infrared and ultraviolet-visible-near infrared spectroscopies. After packaging the detectors, the dark current and energy resolution under α particle irradiation were investigated. Dark currents of less than 5 pA at 100 V were obtained after annealing the electrodes, which is comparable with the optimal value previously reported. The detector that uses a diamond film with higher nitrogen content showed poor energy resolution, whereas the detector with more dislocations showed poor charge collection efficiency(CCE). This demonstrates that the nitrogen content in diamond has a significant effect on the energy resolution of detectors, while the dislocations in diamond largely contribute to the poor CCE of detectors.展开更多
This paper reports that the nickel silicide ohmic contacts to n-type 6H-SiC have been fabricated. Transfer length method test patterns with NiSi/SiC and NiSi2/SiC structure axe formed on N-wells created by N^+ ion im...This paper reports that the nickel silicide ohmic contacts to n-type 6H-SiC have been fabricated. Transfer length method test patterns with NiSi/SiC and NiSi2/SiC structure axe formed on N-wells created by N^+ ion implantation into Si-faced p-type 6H-SiC epilayer respectively. NiSi and NiSi2 films are prepared by annealing the Ni and Si films separately deposited. A two-step annealing technology is performed for decreasing of oxidation problems occurred during high temperature processes. The specific contact resistance Pc of NiSi contact to n-type 6H-SiC as low as 1.78× 10^-6Ωcm^2 is achieved after a two-step annealing at 350 ℃for 20 min and 950℃ for 3 min in N2. And 3.84×10-6Ωcm^2 for NiSi2 contact is achieved. The result for sheet resistance Rsh of the N+ implanted layers is about 1210Ω/□. X-ray diffraction analysis shows the formation of nickel silicide phases at the metal/n-SiC interface after thermal annealing. The surfaces of the nickel silicide after thermal annealing are analysed by scanning electron microscope.展开更多
The structural, elastic, and electronic properties of the very recently discovered ternary silicide superconductor, Li2IrSi3, are calculated using an ab-initio technique. We adopt the plane-wave pseudopotential approa...The structural, elastic, and electronic properties of the very recently discovered ternary silicide superconductor, Li2IrSi3, are calculated using an ab-initio technique. We adopt the plane-wave pseudopotential approach within the frame- work of the first-principles density functional theory (DFT) implemented by the CASTEP code. The calculated structural parameters show reasonable agreement with the experimental results. The elastic moduli of this interesting material are calculated for the first time. The electronic band structure and electronic energy density of states indicate the strong cova- lent Ir-Si and Si-Si bonding, which leads to the formation of the rigid structure of Li2IrSi3. Strong covalency gives rise to a high Debye temperature in this system. We discuss the theoretical results in detail in this paper.展开更多
We developed an apparatus for producing high-density hydrogen plasma. The atomic hydrogen density was 3.1 × 1021 m<sup>?3</sup> at a pressure of 30 Pa, a microwave power of 1000 W, and a hydrogen gas ...We developed an apparatus for producing high-density hydrogen plasma. The atomic hydrogen density was 3.1 × 1021 m<sup>?3</sup> at a pressure of 30 Pa, a microwave power of 1000 W, and a hydrogen gas flow rate of 10 sccm. We confirmed that the temperatures of transition-metal films increased to above 800<sup>。</sup>C within 5 s when they were exposed to hydrogen plasma formed using the apparatus. We applied this phenomenon to the selective heat treatment of nickel films deposited on silicon wafers and formed nickel silicide electrodes. We found that this heat phenomenon automatically stopped after the nickel slicidation reaction finished. To utilize this method, we can perform the nickel silicidation process without heating the other areas such as channel regions and improve the reliability of silicon ultralarge-scale integration devices.展开更多
The self-assembled silicon substrate. The resultant contact angle meter and atomic method was introduced to successfully obtain film was characterized by means of X-ray rare earth(RE) nanofilm on a single-crystal ph...The self-assembled silicon substrate. The resultant contact angle meter and atomic method was introduced to successfully obtain film was characterized by means of X-ray rare earth(RE) nanofilm on a single-crystal photoelectron spectroscopy (XPS), ellipsometer, force microscopy (AFM). The scratch experiment was performed for interfacial adhesion measurement of the RE film. The friction and wear behavior of RE nanofilm was examined on a DF-PM reciprocating friction and wear tester. The results indicate the RE nanofilm is of low coefficient of friction (COF) and high wear resistance. These desirable characteristics of RE nanofilm together with its nanometer thickness, strong bonding to the substrate and low surface energy make it a promising choice as a solid lubricant film in micro electromechanical system (MEMS) devices.展开更多
Epitaxial high-crystallization film semiconductor heterostructures has been proved to be an effective method to prepare single-crystal films for different functional devices in modern microelectronics,electro-optics,a...Epitaxial high-crystallization film semiconductor heterostructures has been proved to be an effective method to prepare single-crystal films for different functional devices in modern microelectronics,electro-optics,and optoelectronics.With superior semiconducting properties,halide perovskite materials are rising as building blocks for heterostructures.Here,the conformal vapor phase epitaxy of CsPbBr3 on PbS single-crystal films is realized to form the CsPbBr3/PbS heterostructures via a two-step vapor deposition process.The structural characterization reveals that PbS substrates and the epilayer CsPbBr3 have clear relationships:CsPbBr3(110)//PbS(100),CsPbBr3[001]//PbS[001]and CsPbBr3[001]//PbS[010].The absorption and photoluminescence(PL)characteristics of CsPbBr3/PbS heterostructures show the broadband light absorption and efficient photogenerated carrier transfer.Photodetectors based on the heterostructures show superior photoresponsivity of 15 A/W,high detectivity of 2.65×10^(11) Jones,fast response speed of 96 ms and obvious rectification behavior.Our study offers a convenient method for establishing the high-quality CsPbBr3/PbS single-crystal film heterostructures and providing an effective way for their application in optoelectronic devices.展开更多
A novel star-like single-crystal ZnO structure was synthesized by a simple solvothermal method. The as-prepared products were characterized by XRD, SEM and TEM. The star-like ZnO, which shows sixfold symmetry, was con...A novel star-like single-crystal ZnO structure was synthesized by a simple solvothermal method. The as-prepared products were characterized by XRD, SEM and TEM. The star-like ZnO, which shows sixfold symmetry, was constructed by six uniform arms distributing symmetrically around the [0001] zone axis. It is also found that the arms are not perpendicular to the [0001] zone axis and each arm is grown at a certain angle with the [0001] direction. CBED pattern and corresponding simulation demonstrate that the convex part of the star-like ZnO is O-terminated (000-1) plane and the concave part is Zn-terminated (0001) plane. H2S plays a crucial role in the synthesis process. The anisotropic growth habit along [0001] and [000-1] results in the formation of star-like structure.展开更多
The relationship between the spatial position of the diamond seed and growth mode is investigated with an enclosedtype holder for single-crystal diamond growth using the microwave plasma chemical vapor deposition epit...The relationship between the spatial position of the diamond seed and growth mode is investigated with an enclosedtype holder for single-crystal diamond growth using the microwave plasma chemical vapor deposition epitaxial method.The results demonstrate that there are three main regions by varying the spatial position of the seed.Due to the plasma concentration occurring at the seed edge,a larger depth is beneficial to transfer the plasma to the holder surface and suppress the polycrystalline diamond rim around the seed edge.However,the plasma density at the edge decreases drastically when the depth is too large,resulting in the growth of a vicinal grain plane and the reduction of surface area.By adopting an appropriate spatial location,the size of single-crystal diamond can be increased from 7 mm×7 mm×0.35 mm to8.6 mm×8.6 mm×2.8 mm without the polycrystalline diamond rim.展开更多
文摘Single-crystal Ni-rich cathodes are a promising candidate for high-energy lithium-ion batteries due to their higher structural and cycling stability than polycrystalline materials.However,the phase evolution and capacity degradation of these single-crystal cathodes during continuous lithation/delithation cycling remains unclear.Understanding the mapping relationship between the macroscopic electrochemical properties and the material physicochemical properties is crucial.Here,we investigate the correlation between the physical-chemical characteristics,phase transition,and capacity decay using capacity differential curve feature identification and in-situ X-ray spectroscopic imaging.We systematically clarify the dominant mechanism of phase evolution in aging cycling.Appropriately high cut-off voltages can mitigate the slow kinetic and electrochemical properties of single-crystal cathodes.We also find that second-order differential capacity discharge characteristic curves can be used to identify the crystal structure disorder of Ni-rich cathodes.These findings constitute a step forward in elucidating the correlation between the electrochemical extrinsic properties and the physicochemical intrinsic properties and provide new perspectives for failure analysis of layered electrode materials.
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the financial support from the National Natural Science Foundation of China(Nos.52034011 and 52204328)the Science and Technology Innovation Program of Hunan Province(2023RC305)the Changsha Municipal Natural Science Foundation(kq2202085)。
文摘The poor electrochemical performance of all-solid-state batteries(ASSBs),which is assemblied by Ni-rich cathode and poly(ethylene oxide)(PEO)-based electrolytes,can be attributed to unstable cathodic interface and poor crystal structure stability of Ni-rich cathode.Several coating strategies are previously employed to enhance the stability of the cathodic interface and crystal structure for Ni-rich cathode.However,these methods can hardly achieve simplicity and high efficiency simultaneously.In this work,polyacrylic acid(PAA)replaced traditional PVDF as a binder for cathode,which can achieve a uniform PAA-Li(LixPAA(0<x≤1))coating layer on the surface of single-crystal LiNi_(0.83)Co_(0.12)Mn_(0.05)O_(2)(SC-NCM83)due to H^(+)/Li^(+)exchange reaction during the initial charging-discharging process.The formation of PAA-Li coating layer on cathode can promote interfacial Li^(+)transport and enhance the stability of the cathodic interface.Furthermore,the partially-protonated surface of SC-NCM83 casued by H^(+)/Li^(+)exchange reaction can restrict Ni ions transport to enhance the crystal structure stability.The proposed SC-NCM83-PAA exhibits superior cycling performance with a retention of 92%compared with that(57.3%)of SC-NCM83-polyvinylidene difluoride(PVDF)after 200 cycles.This work provides a practical strategy to construct high-performance cathodes for ASSBs.
基金We gratefully acknowledge the financial support from the National Natural Science Foundation of China(52070194,51902347,51908555,and 51822812)Natural Science Foundation of Hunan Province(2020JJ5741)the Graduate Innovation Project of Central South University(2020zzts093).
文摘LiNi_(0.5)Co_(0.2)Mn_(0.3)O_(2) is extensively researched as one of the most widely used commercially materials for Li-ion batteries at present.However,the poor high-voltage performance(≥4.3 V)with low reversible capacity limits its replacement for LiCoO_(2) in high-end digital field.Herein,three-in-one modification,Na-doping and Al_(2)O_(3)@Li_(3)BO_(3) dual-coating simultaneously,is explored for single-crystalline LiNi_(0.5)Co_(0.2)Mn_(0.3)O_(2)(N-NCM@AB),which exhibits excellent high-voltage performance.N-NCM@AB displays a discharge-specific capacity of 201.8 mAh g^(−1) at 0.2 C with a high upper voltage of 4.6 V and maintains 158.9 mAh g^(−1) discharge capacity at 1 C over 200 cycles with the corresponding capacity retention of 87.8%.Remarkably,the N-NCM@AB||graphite pouch-type full cell retains 81.2% of its initial capacity with high working voltage of 4.4 V over 1600 cycles.More importantly,the fundamental understandings of three-in-one modification on surface morphology,crystal structure,and phase transformation of N-NCM@AB are clearly revealed.The Na+doped into the Li–O slab can enhance the bond energy,stabilize the crystal structure,and facilitate Li+transport.Additionally,the interior surface layer of Li^(+)-ions conductor Li_(3)BO_(3) relieves the charge transfer resistance with surface coating,whereas the outer surface Al_(2)O_(3) coating layer is beneficial for reducing the active materials loss and alleviating the electrode/electrolyte parasite reaction.This three-in-one strategy provides a reference for the further research on the performance attenuation mechanism of NCM,paving a new avenue to boost the high-voltage performance of NCM cathode in Li-ion batteries.
文摘The process of thermal stress damage during 1080 nm laser ablation of single-crystal germanium was recorded in real time using a high-speed charge-coupled device.A three-dimensional finite element numerical model based on Fourier's heat conduction equation,Hooke's law and the Alexander–Hasson equation was developed to analyze the thermal stress damage mechanism involved.The damage morphology of the ablated samples was observed using an optical microscope.The results show that the cooling process has an important influence on fracture in the laser-irradiated region of single-crystal germanium.Fracture is the result of a combination of thermal stress and reduction in local yield strength.
基金supported by National Natural Science Foundation of China(No.12075241)。
文摘A single-crystal diamond detector is fabricated to diagnose 14.1 MeV deuterium-tritium(D-T)fusion neutrons.The size of its diamond film is 4.5 mm×4.5 mm×500μm.This film is sandwiched by a flat,strip-patterned gold electrode.The dark current of this detector is experimentally measured to be lower than 0.1 nA under an electric field of 30 kV cm^(-1).This diamond detector is used to measure D-T fusion neutrons with a flux of about 7.5×10^(5) s^(-1)cm^(-2).The pronounced peak with a central energy of 8.28 MeV characterizing the^(12)C(n,α)~9Be reaction in the neutron energy spectrum is experimentally diagnosed,and the energy resolution is better than 1.69%,which is the best result reported so far using a diamond detector.A clear peak with a central energy of 6.52 MeV characterizing the^(12)C(n,n')3αreaction is also identified with an energy resolution of better than 7.67%.
基金the support from the National Natural Science Foundation of China (No. 61925506)the Natural Science Foundation of Shanghai (No. 20JC1414605)+1 种基金Hangzhou Science and Technology Bureau of Zhejiang Province (No. TD2020002)the Academic/Technology Research Leader Program of Shanghai (23XD1404500)
文摘Lead halide perovskites have attracted considerable attention as potential candidates for high-performance nano/microlasers,owing to their outstanding optical properties.However,the further development of perovskite microlaser arrays(especially based on polycrystalline thin films)produced by the conventional processing techniques is hindered by the chemical instability and surface roughness of the perovskite structures.Herein,we demonstrate a laser patterning of large-scale,highly crystalline perovskite single-crystal films to fabricate reproducible perovskite single-crystal-based microlaser arrays.Perovskite thin films were directly ablated by femtosecond-laser in multiple low-power cycles at a minimum machining line width of approximately 300 nm to realize high-precision,chemically clean,and repeatable fabrication of microdisk arrays.The surface impurities generated during the process can be washed away to avoid external optical loss due to the robustness of the single-crystal film.Moreover,the high-quality,large-sized perovskite single-crystal films can significantly improve the quality of microcavities,thereby realizing a perovskite microdisk laser with narrow linewidth(0.09 nm)and low threshold(5.1µJ/cm2).Benefiting from the novel laser patterning method and the large-sized perovskite single-crystal films,a high power and high color purity laser display with single-mode microlasers as pixels was successfully fabricated.Thus,this study may offer a potential platform for mass-scale and reproducible fabrication of microlaser arrays,and further facilitate the development of highly integrated applications based on perovskite materials.
文摘Within the framework of the density functional theory and the pseudopotential method,the electronic structure calculations of the“metal-Si(100)”systems with Li,Be and Al as metal coverings of one to four monolayers(ML)thickness,were carried out.Calculations showed that band gaps of 1.02 eV,0.98 eV and 0.5 eV,respectively,appear in the densities of electronic states when the thickness of Li,Be and Al coverings is one ML.These gaps disappear with increasing thickness of the metal layers:first in the Li-Si system(for two ML),then in the Al-Si system(for three ML)and then in the Be-Si system(for four ML).This behavior of the band gap can be explained by the passivation of the substrate surface states and the peculiarities of the electronic structure of the adsorbed metals.In common the results can be interpreted as describing the possibility of the formation of a two-dimensional silicide with semiconducting properties in Li-Si(100),Be-Si(100)and Al-Si(100)systems.
文摘The microstructure of the RE silicide alloy was studied by SEM. The feature of the phase and the distribution of Ca, P, Al were analyzed, especially the distribution of micro-cracks and its composition were determined. The result demonstrates that only a few phosphides contribute to the spontaneous crumbling of the RE silicide alloy by reacting with water and forming oxide or phosphorus oxide. The phosphorus content is not the critical factor of disintegration in the alloy studied.
基金supported by National Natural Science Foundation of China(Grant Nos.50975060,50901025)the National Basic Research Program of China(Grant No.2011CB610406)+2 种基金the China Postdoctoral Science Foundation(Grant Nos.201104420,20090450840)the Fundamental Research Funds for the Central Universities(Grant No.HIT.BRET1.2010008)Scientific and Technological Project in Heilongjiang Province(Grant No.GZ09A206)
文摘The fracture behavior of fully lamellar binaryγ-TiAl alloys is extremely anisotropic with respect to the lamellar orientation.For the fully lamellar Ti-46Al-0.5W-0.5Si alloy,the existence of silicide clusters plays a critical role on the fracture behavior.In the present study,tensile test and three point bending test were performed at room temperature with the loading axis parallel and perpendicular to the lamellar orientation,respectively.To investigate the influence of silicide clusters on the initiation and propagation of cracks,the fracture surface and the cracks adjacent to the fracture zone of the specimens have been analyzed.Results show that the fracture process is related to the morphology and distribution of the silicide clusters.Crack preferentially initiates at and propagates along the interface of silicide andα 2 /γlamellar with the loading axis perpendicular to the length direction of silicide.While the silicide can prevent the propagation of cracks from running across with the crack growth direction perpendicular to the length direction of silicide.
基金financially supported by the National Natural Science Foundation of China(No.51431003)the Joint Funds of the National Natural Science Foundation of China(No.U1435201)
文摘To investigate the interdiffusion behavior of Ge-modified silicide coatings on an Nb–Si-based alloy substrate,the coating was oxidized at 1250°C for 5,10,20,50,or 100 h.The interfacial diffusion between the(Nb,X)(Si,Ge)_2(X = Ti,Cr,Hf) coating and the Nb–Si based alloy was also examined.The transitional layer is composed of(Ti,Nb)_5(Si,Ge)_4 and a small amount of(Nb,X)_5(Si,Ge)_3.With increasing oxidation time,the thickness of the transitional layer increases because of the diffusion of Si from the outer layer to the substrate,which obeys a parabolic rate law.The parabolic growth rate constant of the transitional layer under oxidation conditions is 2.018 μm×h^(-1/2).Moreover,the interdiffusion coefficients of Si in the transitional layer were determined from the interdiffusion fluxes calculated directly from experimental concentration profiles.
基金This work has been supported jointly by the National Natural Science Foundation ofChina (Crant No. 69806005)the Natural Scie
文摘Manganese silicide MnSi_(2-x) thin films have been prepared on n-type siliconsubstrates through solid phase reaction. The heterostructures were analyzed by X-ray diffraction,Rutherford backscattering spectroscopy, Fourier transform infrared transmittance spectroscopy andthe four-point probe technique. The results show that two manganese silicides have been formedsequentially via the reaction of thin layer Mn with Si substrate at different irradiation annealingstages, i.e., MnSi at 450 deg C and MnSi_(1.73) at 550 deg C. MnSi_(1.73) phase exhibits preferredgrowth after irradiation with infrared. In situ four-point probe measurements of sheet resistanceduring infrared irradiation annealing show that nucleation of MnSi and phase transformation of MnSito MaSi_(1.73) occur at 410 deg C and 530 deg C, respectively; the MnSi phase shows metallicbehavior, while MnSi_(1.73) exhibits semiconducting behavior. Characteristic phonon bands ofMnSi_(2-x) silicides, which can be used for phase identification along with conventional XRDtechniques, have been observed by FTIR spectroscopy.
基金This work was financially supported by the Natural Science Foundation of Beijing,China(No.4192038)National Key Research and Development Program of China(Nos.2016YFE0133200 and 2018YFB0406501)European Union’s Horizon 2020 Research and Innovation Staff Exchange Scheme(No.734578).
文摘Chemical vapor deposition(CVD)-grown diamond films have been developed as irradiation-resistant materials to replace or upgrade current detectors for use in extreme radiation environments. However, their sensitivity in practical applications has been inhibited by space charge stability issues caused by defects and impurities in pure diamond crystal materials. In this study, two high-quality CVD-grown single-crystal diamond(SCD) detectors with low content of nitrogen impurities were fabricated and characterized. The intrinsic properties of the SCD samples were characterized using Raman spectroscopy, stereomicroscopy, and X-ray diffraction with the rocking curve mode, cathode luminescence(CL), and infrared and ultraviolet-visible-near infrared spectroscopies. After packaging the detectors, the dark current and energy resolution under α particle irradiation were investigated. Dark currents of less than 5 pA at 100 V were obtained after annealing the electrodes, which is comparable with the optimal value previously reported. The detector that uses a diamond film with higher nitrogen content showed poor energy resolution, whereas the detector with more dislocations showed poor charge collection efficiency(CCE). This demonstrates that the nitrogen content in diamond has a significant effect on the energy resolution of detectors, while the dislocations in diamond largely contribute to the poor CCE of detectors.
基金Project supported by the National Basic Research Program of China (Grant No 2002CB311904), the National Defense Basic Research Program of China (Grant No 51327010101) and the National Natural Science Foundation of China (Grant No 60376001).
文摘This paper reports that the nickel silicide ohmic contacts to n-type 6H-SiC have been fabricated. Transfer length method test patterns with NiSi/SiC and NiSi2/SiC structure axe formed on N-wells created by N^+ ion implantation into Si-faced p-type 6H-SiC epilayer respectively. NiSi and NiSi2 films are prepared by annealing the Ni and Si films separately deposited. A two-step annealing technology is performed for decreasing of oxidation problems occurred during high temperature processes. The specific contact resistance Pc of NiSi contact to n-type 6H-SiC as low as 1.78× 10^-6Ωcm^2 is achieved after a two-step annealing at 350 ℃for 20 min and 950℃ for 3 min in N2. And 3.84×10-6Ωcm^2 for NiSi2 contact is achieved. The result for sheet resistance Rsh of the N+ implanted layers is about 1210Ω/□. X-ray diffraction analysis shows the formation of nickel silicide phases at the metal/n-SiC interface after thermal annealing. The surfaces of the nickel silicide after thermal annealing are analysed by scanning electron microscope.
文摘The structural, elastic, and electronic properties of the very recently discovered ternary silicide superconductor, Li2IrSi3, are calculated using an ab-initio technique. We adopt the plane-wave pseudopotential approach within the frame- work of the first-principles density functional theory (DFT) implemented by the CASTEP code. The calculated structural parameters show reasonable agreement with the experimental results. The elastic moduli of this interesting material are calculated for the first time. The electronic band structure and electronic energy density of states indicate the strong cova- lent Ir-Si and Si-Si bonding, which leads to the formation of the rigid structure of Li2IrSi3. Strong covalency gives rise to a high Debye temperature in this system. We discuss the theoretical results in detail in this paper.
文摘We developed an apparatus for producing high-density hydrogen plasma. The atomic hydrogen density was 3.1 × 1021 m<sup>?3</sup> at a pressure of 30 Pa, a microwave power of 1000 W, and a hydrogen gas flow rate of 10 sccm. We confirmed that the temperatures of transition-metal films increased to above 800<sup>。</sup>C within 5 s when they were exposed to hydrogen plasma formed using the apparatus. We applied this phenomenon to the selective heat treatment of nickel films deposited on silicon wafers and formed nickel silicide electrodes. We found that this heat phenomenon automatically stopped after the nickel slicidation reaction finished. To utilize this method, we can perform the nickel silicidation process without heating the other areas such as channel regions and improve the reliability of silicon ultralarge-scale integration devices.
文摘The self-assembled silicon substrate. The resultant contact angle meter and atomic method was introduced to successfully obtain film was characterized by means of X-ray rare earth(RE) nanofilm on a single-crystal photoelectron spectroscopy (XPS), ellipsometer, force microscopy (AFM). The scratch experiment was performed for interfacial adhesion measurement of the RE film. The friction and wear behavior of RE nanofilm was examined on a DF-PM reciprocating friction and wear tester. The results indicate the RE nanofilm is of low coefficient of friction (COF) and high wear resistance. These desirable characteristics of RE nanofilm together with its nanometer thickness, strong bonding to the substrate and low surface energy make it a promising choice as a solid lubricant film in micro electromechanical system (MEMS) devices.
基金This work was supported by the Natural Science Foundation of China(Grant No.11704389)Scientific Equipment Development Project and Youth Innovation Promotion Association Project of Chinese Academy of Sciences.
文摘Epitaxial high-crystallization film semiconductor heterostructures has been proved to be an effective method to prepare single-crystal films for different functional devices in modern microelectronics,electro-optics,and optoelectronics.With superior semiconducting properties,halide perovskite materials are rising as building blocks for heterostructures.Here,the conformal vapor phase epitaxy of CsPbBr3 on PbS single-crystal films is realized to form the CsPbBr3/PbS heterostructures via a two-step vapor deposition process.The structural characterization reveals that PbS substrates and the epilayer CsPbBr3 have clear relationships:CsPbBr3(110)//PbS(100),CsPbBr3[001]//PbS[001]and CsPbBr3[001]//PbS[010].The absorption and photoluminescence(PL)characteristics of CsPbBr3/PbS heterostructures show the broadband light absorption and efficient photogenerated carrier transfer.Photodetectors based on the heterostructures show superior photoresponsivity of 15 A/W,high detectivity of 2.65×10^(11) Jones,fast response speed of 96 ms and obvious rectification behavior.Our study offers a convenient method for establishing the high-quality CsPbBr3/PbS single-crystal film heterostructures and providing an effective way for their application in optoelectronic devices.
文摘A novel star-like single-crystal ZnO structure was synthesized by a simple solvothermal method. The as-prepared products were characterized by XRD, SEM and TEM. The star-like ZnO, which shows sixfold symmetry, was constructed by six uniform arms distributing symmetrically around the [0001] zone axis. It is also found that the arms are not perpendicular to the [0001] zone axis and each arm is grown at a certain angle with the [0001] direction. CBED pattern and corresponding simulation demonstrate that the convex part of the star-like ZnO is O-terminated (000-1) plane and the concave part is Zn-terminated (0001) plane. H2S plays a crucial role in the synthesis process. The anisotropic growth habit along [0001] and [000-1] results in the formation of star-like structure.
基金Project supported by the Key-Area Research and Development Program of Guangdong Province,China(Grant No.2020B0101690001)。
文摘The relationship between the spatial position of the diamond seed and growth mode is investigated with an enclosedtype holder for single-crystal diamond growth using the microwave plasma chemical vapor deposition epitaxial method.The results demonstrate that there are three main regions by varying the spatial position of the seed.Due to the plasma concentration occurring at the seed edge,a larger depth is beneficial to transfer the plasma to the holder surface and suppress the polycrystalline diamond rim around the seed edge.However,the plasma density at the edge decreases drastically when the depth is too large,resulting in the growth of a vicinal grain plane and the reduction of surface area.By adopting an appropriate spatial location,the size of single-crystal diamond can be increased from 7 mm×7 mm×0.35 mm to8.6 mm×8.6 mm×2.8 mm without the polycrystalline diamond rim.