Solar wind charge exchange produces emissions in the soft X-ray energy range which can enable the study of near-Earth space regions such as the magnetopause,the magnetosheath and the polar cusps by remote sensing tech...Solar wind charge exchange produces emissions in the soft X-ray energy range which can enable the study of near-Earth space regions such as the magnetopause,the magnetosheath and the polar cusps by remote sensing techniques.The Solar wind Magnetosphere Ionosphere Link Explorer(SMILE)and Lunar Environment heliospheric X-ray Imager(LEXI)missions aim to obtain soft Xray images of near-Earth space thanks to their Soft X-ray Imager(SXI)instruments.While earlier modeling works have already simulated soft X-ray images as might be obtained by SMILE SXI during its mission,the numerical models used so far are all based on the magnetohydrodynamics description of the space plasma.To investigate the possible signatures of ion-kinetic-scale processes in soft Xray images,we use for the first time a global hybrid-Vlasov simulation of the geospace from the Vlasiator model.The simulation is driven by fast and tenuous solar wind conditions and purely southward interplanetary magnetic field.We first produce global X-ray images of the dayside near-Earth space by placing a virtual imaging satellite at two different locations,providing meridional and equatorial views.We then analyze regional features present in the images and show that they correspond to signatures in soft X-ray emissions of mirrormode wave structures in the magnetosheath and flux transfer events(FTEs)at the magnetopause.Our results suggest that,although the time scales associated with the motion of those transient phenomena will likely be significantly smaller than the integration time of the SMILE and LEXI imagers,mirror-mode structures and FTEs can cumulatively produce detectable signatures in the soft X-ray images.For instance,a local increase by 30%in the proton density at the dayside magnetopause resulting from the transit of multiple FTEs leads to a 12%enhancement in the line-of-sight-and time-integrated soft X-ray emissivity originating from this region.Likewise,a proton density increase by 14%in the magnetosheath associated with mirror-mode structures can result in an enhancement in the soft X-ray signal by 4%.These are likely conservative estimates,given that the solar wind conditions used in the Vlasiator run can be expected to generate weaker soft X-ray emissions than the more common denser solar wind.These results will contribute to the preparatory work for the SMILE and LEXI missions by providing the community with quantitative estimates of the effects of small-scale,transient phenomena occurring on the dayside.展开更多
Thermal diffusion of Si atoms at the interface in Mo/Si multilayers was observed with an imaging type soft X ray emission microscope developed by us. It was possible to observe the diffusion with 0.2nm depth resolutio...Thermal diffusion of Si atoms at the interface in Mo/Si multilayers was observed with an imaging type soft X ray emission microscope developed by us. It was possible to observe the diffusion with 0.2nm depth resolution in the direction normal to the interface by comparing the emission intensity for exactly the same position. The diffusion coefficient of Si atoms in Mo at 600℃ was roughly estimated to be 6.0×10 17 cm 2/s.展开更多
Burners of metal halide lamps used for illumination are generally made of polycrystalline alumina ceramic (PCA) which is translucent to visible light. We show that the difficulty of selecting a line of sight through...Burners of metal halide lamps used for illumination are generally made of polycrystalline alumina ceramic (PCA) which is translucent to visible light. We show that the difficulty of selecting a line of sight through the lamp prevents the use of optical emission diagnostic. X-rays photons are mainly absorbed and not scattered by PCA. Absorption by mercury atoms contributing to the discharge allowed us to determine the density of mercury in the lamp. By comparing diagnostic methods, we put in evidence the difficulty of taking into account the scattering of light mathematically.展开更多
By using soft X-ray spectroscopy, we investigate the inner-shell excitation and relaxation processes in atomic and ionic neon targets. Resonant X-ray emission spectroscopy was applied to neutral neon atom in the regio...By using soft X-ray spectroscopy, we investigate the inner-shell excitation and relaxation processes in atomic and ionic neon targets. Resonant X-ray emission spectroscopy was applied to neutral neon atom in the regions of the [1s]np (n = 3, 4,…, ε) excited states and [1s2p]3pmp (m = 3,4) doubly excited states to obtain the spectroscopic information on the [2p]np and [2p^2]3prnp final electronic states, where square brackets indicate hole states. The energy levels of the [2p^2]3prnp (m = 3,4) electronic states were spectroscopically measured for the first time. As for the ionic neon target, on the other hand, the photoion yield spectroscopy was adopted to survey the 1s→ np (n = 2, 3) resonant excitation and subsequent Auger decay processes for Ne^+ target-ions. The observed Ne^2+ photoion yield spectrum is successflllly explained by the theoretical calculations based on the nmlticonfiguration Dirac-Fock method展开更多
Based on the synchrotron soft X-ray absorption spectroscopy experiments,the fundamental electronic structures of layered Li NixCoyMnzO_(2)(NCM)are investigated systematically and the data of transitionmetal(TM)L-and O...Based on the synchrotron soft X-ray absorption spectroscopy experiments,the fundamental electronic structures of layered Li NixCoyMnzO_(2)(NCM)are investigated systematically and the data of transitionmetal(TM)L-and O K-edges spectra are collected.Distribution of Ni ions under different oxidation states is evaluated according to linear combination fit.It is found that the ratio of Ni^(4+)expands with the increase of Ni since it dominates in charge compensation during charging,and that the existence of Ni^(3+)is nearly negligible in delithiated NCM.The valence state of Co also strongly depends on Ni content,the perceptible position shift of Co L_(3)-edge absorption peak towards higher energy in Ni-rich material agrees well with the small voltage plateau at around 4.2 V.The stability of Mn is verified as no obvious spectral change with the Mn L-edge is observed.Moreover,as Ni content rises,the O 2p holes near the Femi level increases with higher oxidation state of Ni,indicating the enhanced hybridization of O 2p-TM 3 d.Delithiated NCMs with higher Ni content are prior to lose electron existing in highly hybridized Ni3 dO 2 p bands upon heating,which accounts for the pronounced O_(2)release in phase transitions and the deterioration in thermal stability.These detailed observation of the electronic structure evolution is one of the key ingredients to improving the electrochemical and thermal performance of NCM.展开更多
Understanding electronic structure is crucial to enhance the battery performance. Soft X-ray spectroscopy(SXS) is one of the most effective methods to provide direct probe of electronic states. Here, spectroscopic mea...Understanding electronic structure is crucial to enhance the battery performance. Soft X-ray spectroscopy(SXS) is one of the most effective methods to provide direct probe of electronic states. Here, spectroscopic measurements of transition metal 3 d and oxygen 2 p states are simply reviewed. Then, we mainly focus on the perspective of the development direction of modern SXS techniques. Although the true power of recently developed high efficiency mapping of resonant inelastic X-ray scattering(m RIXS) has been apparent for materials and chemistry studies, great challenges remain for mRIXS spectroscopic interpretation, and the understanding of the battery materials on novel redox activities remains elusive.展开更多
The lightweight,rechargeable lithium-ion battery is one of the dominant energy storage devices globally in portable electronics due to its high energy density,no memory effect,wide operating voltage,lightweight,and go...The lightweight,rechargeable lithium-ion battery is one of the dominant energy storage devices globally in portable electronics due to its high energy density,no memory effect,wide operating voltage,lightweight,and good charge efficiency.However,due to safety concerns,the depletion of lithium reserves,and the corresponding increase of cost,an alternative battery system becomes more and more desirable.To develop alternative battery systems with low cost and high material abundance,for example,sodium,magnesium,zinc,and calcium,it is important to understand the chemical and electronic structure of materials.Soft X-ray spectroscopy,for example,X-ray absorption spectroscopy(XAS),X-ray emission spectroscopy(XES),and resonant inelastic soft X-ray scattering(RIXS),is an element-specific technique with sensitivity to the local chemical environment and structural order of the element of interest.Modern soft X-ray systems enable operando experiments that can be applied to amorphous and crystalline samples,making it a powerful tool for studying the electronic and structural changes in electrode and electrolyte species.In this article,the application of in situ/operando(soft)X-ray spectroscopy in beyond lithium-ion batteries is reviewed to demonstrate how such spectroscopic characterizations could facilitate the interpretation of interfacial phenomena under in situ/operando condition and subsequent development of the beyond lithium-ion batteries.展开更多
The formidable challenge of developing high-performance battery system stems from the complication of battery operations, both mechanically and electronically. In the electrodes and at the electrode-electrolyte interf...The formidable challenge of developing high-performance battery system stems from the complication of battery operations, both mechanically and electronically. In the electrodes and at the electrode-electrolyte interfaces, chemical reactions take place with evolving electron states. In addition to the extensive studies of material synthesis, electrochem- ical, structural, and mechanical properties, soft x-ray spectroscopy provides unique opportunities for revealing the critical electron states in batteries. This review discusses some of the recent soft x-ray spectroscopic results on battery binder, transition-metal based positive electrodes, and the solid-electrolyte-interphase. By virtue of soft x-ray's sensitivity to electron states, the electronic property, the redox during electrochemical operations, and the chemical species of the interphases could be fingerprinted by soft x-ray spectroscopy. Understanding and innovating battery technologies need a multimodal approach, and soft x-ray spectroscopy is one of the incisive tools to probe the chemical and physical evolutions in batteries.展开更多
The oxidation of aluminium was studied using optical emission spectroscopy (OES) during the evaporation of aluminium in traces of oxygen in a thermal plasma reactor. The ratio of the measured line intensities of Al-...The oxidation of aluminium was studied using optical emission spectroscopy (OES) during the evaporation of aluminium in traces of oxygen in a thermal plasma reactor. The ratio of the measured line intensities of Al-O with that of Al follows the exact trend as of that obtained from the corresponding line intensities in X-ray diffraction spectra of the synthesized samples. In this paper the inherent capacity of emission spectroscopy in evaluating the growth processes under plasma induced reactions is presented.展开更多
The visualization and data mining of tumor multidimensional information may play a major role in the analysis of the growth,metastasis,and microenvironmental changes of tumors while challenging traditional imaging and...The visualization and data mining of tumor multidimensional information may play a major role in the analysis of the growth,metastasis,and microenvironmental changes of tumors while challenging traditional imaging and data processing techniques.In this study,a general trans-scale and multi-modality measurement method was developed for the quantitative diagnosis of hepatocellular carcinoma(HCC)using a combination of propagation-based phase-contrast computed tomography(PPCT),scanning transmission soft X-ray microscopy(STXM),and Fourier transform infrared micro-spectroscopy(FTIR).Our experimental results reveal the trans-scale micro-morpho-logical HCC pathology and facilitate quantitative data analysis and comprehensive assessment.These results include some visualization features of PPCT-based tissue microenvironments,STXM-based cellular fine structures,and FTIR-based bio-macromolecular spectral characteris-tics during HCC tumor differentiation and proliferation.The proposed method provides multidimensional feature data support for constructing a high-accuracy machine learning algorithm based on a gray-level histogram,gray-gradient co-occurrence matrix,gray-level co-occurrence matrix,and back-propagation neural network model.Multi-dimensional information analysis and diagnosis revealed the morphological pathways of HCC pathological evolution and we explored the relationships between HCC-related feature changes in inflammatory microenviron-ments,cellular metabolism,and the stretching vibration peaks of biomolecules of lipids,proteins,and nucleic acids.Therefore,the proposed methodology has strong potential for the visualization of complex tumors and assessing the risks of tumor differentiation and metastasis.展开更多
The pointed observations of NGC3077 are analyzed by position sensitive proportional counter (PSPC) on board the ROSAT satellite on 1991-04-18, 1991, finding out that the X-ray emission range of M81 galaxy has, in the ...The pointed observations of NGC3077 are analyzed by position sensitive proportional counter (PSPC) on board the ROSAT satellite on 1991-04-18, 1991, finding out that the X-ray emission range of M81 galaxy has, in the softer and more sensitive ROSAT PSPC band (0. 2-2. 4 keV), extended by 40% larger than ever observed by image proportional counter (IPC) on board the Einstein satellite, which shows that M81 galaxy has a larger X-ray corona. And by the aid of the timing analysis, it is concluded that M81 nucleus has no variabilities on time scale of a few minutes; hence the possibility of M81 nucleus having the marginal variability over time scale of about 2 min that Fabbiano (1988) found from the Einstein IPC observation is ruled out.展开更多
Breakthroughs in energy storage and conversion devices depend heavily on the exploration of low-cost and high-performance materials.Carbon-supported electrocatalysts with dimensional varieties have recently attracted ...Breakthroughs in energy storage and conversion devices depend heavily on the exploration of low-cost and high-performance materials.Carbon-supported electrocatalysts with dimensional varieties have recently attracted significant attention due to their strong structural flexibility and easy accessibility.Nevertheless,understanding the connection between their electronic,structural properties,and catalytic performance must remain a top priority.Synchrotron radiation(SR)X-ray absorption spectroscopy(XAS)techniques,including hard XAS and soft XAS,are recognized as efficient and comprehensive platforms for probing the surface,interface,and bulk electronic structure of elements of interest in the materials community.In the past decade,the flourishing development of materials science and advanced characterization technologies have led to a deeper understanding at different temporal,longitudinal,and spatial scales.In this review,we briefly describe the concept of XAS techniques and summarize their recent progress in addressing scientific questions on carbon-supported electrocatalysts through the development of advanced instruments and experimental methods.We then discuss the remaining challenges and potential research directions in nextgeneration materials frontiers,and suggest challenges and perspectives for shedding light on the structure–activity relationship.展开更多
Spectral analysis was a method of identifying substances, determining their chemical composition and calculating their content based on their spectral characteristics. This paper mainly discussed the application of va...Spectral analysis was a method of identifying substances, determining their chemical composition and calculating their content based on their spectral characteristics. This paper mainly discussed the application of various spectroscopic techniques, mainly including atomic absorption spectrometry (AAS) inductively coupled plasma emission spectrometry (ICP-AES) X-ray fluorescence spectroscopy (XRF) atomic fluorescence spectroscopy (AFS) direct reading spectroscopy (OES) glow discharge emission spectroscopy (GD-OSE) laser-induced breakdown spectroscopy (LIBS), in the formulation of non-ferrous metal standards in China. The AAS method was the most widely used single-element microanalysis method among the non-ferrous metal standards. The ICP-AES method was good at significant advantages in the simultaneous detection of multiple elements. The XRF method was increasingly used in the determination of primary and secondary trace elements due to its simple sample preparation and high efficiency. The AFS was mostly detected by single-element trace analysis. OES GD-OES and LIBS were playing an increasingly important role in the new demand area for non-ferrous metals. This paper discussed matrix elimination, sample digestion, sample preparation, instrument categories and other aspects of some standards, and summarized the advantages of spectral analysis and traditional chemical analysis methods. The new methods of future spectroscopic technology had been illustrated in the process of developing non-ferrous metal standards.展开更多
Nickel based magnetic nanocrystals have been widely applied in magnetic and catalytic facilities.Tunable magnetic properties of nickel can be easily obtained via non-magnetic doping or phase transformation.However,pha...Nickel based magnetic nanocrystals have been widely applied in magnetic and catalytic facilities.Tunable magnetic properties of nickel can be easily obtained via non-magnetic doping or phase transformation.However,phase transformation from face centered cubic(fcc)to hexagonal close packed(hcp)induced magnetism adjustment of Ni are always confused with nickel carbide(Ni_(3)C),due to the similar atomic structures of hcp-Ni and Ni3C.Here,we present series of Au@Ni-carbide magnetic materials achieved from the controlled carbonation of Au@Ni core-shell structures,whose magnetism is tunable by adjusting the amount of carbon in the Ni layer.Ex-situ hard X-ray absorption spectroscopy(XAS)at the metal K edge and soft XAS at both metal L edge and carbon K edge provide solid evidence for the carbonation process from fcc-Ni to Ni_(x)C,rather than phase transformation to hcp-Ni.Further investigation reveals that the magnetism of the hybrids is mainly contributed from the residual fcc-Ni.The result represents an accurate and effective way to distinguish hexagonal Ni_(3)C from hcp-Ni,and provides the pathway to control magnetism of Ni-based materials for applications.展开更多
By virtue of the crucial effect of the crystal structure and transition metal(TM)redox evolution on the performance of LiNi_(x)Co_(y)Mn_(z)O_(2)(NCM)cathode,systematical investigation is carried out to better understa...By virtue of the crucial effect of the crystal structure and transition metal(TM)redox evolution on the performance of LiNi_(x)Co_(y)Mn_(z)O_(2)(NCM)cathode,systematical investigation is carried out to better understand the charge mechanism upon deep charging.Based on the results of X-ray diffraction and highresolution transmission electron microscope,phase transformations existing on particle surface are promoted by high potential because of the deeper lithium vacancies,accompanied by more substantial structure instability.Soft X-ray absorption spectroscopy indicates that Ni acts as the major contributor to charge compensation while Co displays a remarkable redox activity over the deep charge range.The elevated integrated intensity of pre-edge in O K-edge spectra reveals the extensive amount of holes formed in O 2 p orbitals and the enhanced hybridization of TM 3 d-O 2 p orbitals.Considering the close relationship between thermal behavior and structural evolution,the tendency of phase transitions and O_(2) release upon heating is accelerated by voltage rise,demonstrating the aggravated instability due to deeper Li utilization.Remaining Li contents in NCM are employed to estimate the amount of oxygen released in structural transformation and its detrimental effect on stability declares Li contentdependent characteristics.Furthermore,the extended Li vacancies,higher proportion of Ni4+and stronger orbital hybridization are considered as three factors impeding the thermal stability of the highlydelithiated NCM.展开更多
Dry etching of 6H silicon carbide (6H-SiC) wafers in a C4Fs/Ar dual-frequency capacitively coupled plasma (DF-CCP) was investigated. Atomic force microscopy (AFM) and X-ray photoelectron spectroscopy (XPS) wer...Dry etching of 6H silicon carbide (6H-SiC) wafers in a C4Fs/Ar dual-frequency capacitively coupled plasma (DF-CCP) was investigated. Atomic force microscopy (AFM) and X-ray photoelectron spectroscopy (XPS) were used to measure the SiC surface structure and compositions, respectively. Optical emission spectroscopy (OES) was used to measure the relative concentration of F radicals in the plasma. It was found that the roughness of the etched SiC surface and the etching rate are directly related to the power of low-frequency (LF) source. At lower LF power, a smaller surface roughness and a lower etching rate are obtained due to weak bombardment of low energy ions on the SiC wafers. At higher LF power the etching rate can be efficiently increased, but the surface roughness increases too. Compared with other plasma dry etching methods, the DF-CCP can effectively inhibit CχFγ films' deposition, and reduce surface residues.展开更多
The study of soft X-ray amplification is important and interesting. Pierre Jaeglé et al. have done some work in this field about soft X-ray amplification by Li-like Al ions and have got promising results. In this...The study of soft X-ray amplification is important and interesting. Pierre Jaeglé et al. have done some work in this field about soft X-ray amplification by Li-like Al ions and have got promising results. In this note, we report our recent result about it.展开更多
This paper describes the behaviour of impurity transport in HL-2A ohmic discharges. In 2005, small quantities of metallic impurities (A1, Ni and Ti) were successfully injected into HL-2A plasmas by laser blow-off te...This paper describes the behaviour of impurity transport in HL-2A ohmic discharges. In 2005, small quantities of metallic impurities (A1, Ni and Ti) were successfully injected into HL-2A plasmas by laser blow-off technique, and their progression was followed by the soft x-ray cameras with good spatial and temporal resolutions. The impurity confinement time is estimated from the characteristic decay time of the soft x-ray signal of the injected impurities, and it is about 30-60 ms. The transport coefficients of impurities (including diffusion coefficient and convection velocity) in radial different region have been derived by using a one-dimenslonal impurity transport code, the results present that diffusion coefficient is much smaller in the central region of plasmas than the outside of it, and it is much larger than that of neoclassical theory predictions; namely, it is anomalous.展开更多
Nitrogen ion was implanted into the nano-TiO2 film surfaces by electron cyclotron resonance (ECR) plasma modification to improve the optical reactivity in visible-light region for nano-TiO2. Diagnosing the N2 plasma...Nitrogen ion was implanted into the nano-TiO2 film surfaces by electron cyclotron resonance (ECR) plasma modification to improve the optical reactivity in visible-light region for nano-TiO2. Diagnosing the N2 plasma by optical emission spectroscopy (OES) was applied to the process of plasma modification. X-ray photoelectron spectroscopy (XPS) was used for analysis of the binding of element after plasma modification. It is shown that the surface modification was caused by excitated N. The injecting of N2 and N+ leads to the increase in the dissociative interstitial state N in the films. The doped N makes for TiO2-xNx appearing in the TiO2 films. TiO2-xNx forms the impurity energy state in the TiO2 energy band gap and reduces the energy band gap. This is the main reason leading to the red shift of absorption edge.展开更多
基金the European Research Council for starting grant 200141-QuESpace,with which the Vlasiator model was developedconsolidator grant 682068-PRESTISSIMO awarded for further development of Vlasiator and its use in scientific investigations+4 种基金Academy of Finland grant numbers 338629-AERGELC’H,339756-KIMCHI,336805-FORESAIL,and 335554-ICT-SUNVACThe Academy of Finland also supported this work through the PROFI4 grant(grant number 3189131)support from the NASA grants,80NSSC20K1670 and 80MSFC20C0019the NASA GSFC FY23 IRADHIF funds。
文摘Solar wind charge exchange produces emissions in the soft X-ray energy range which can enable the study of near-Earth space regions such as the magnetopause,the magnetosheath and the polar cusps by remote sensing techniques.The Solar wind Magnetosphere Ionosphere Link Explorer(SMILE)and Lunar Environment heliospheric X-ray Imager(LEXI)missions aim to obtain soft Xray images of near-Earth space thanks to their Soft X-ray Imager(SXI)instruments.While earlier modeling works have already simulated soft X-ray images as might be obtained by SMILE SXI during its mission,the numerical models used so far are all based on the magnetohydrodynamics description of the space plasma.To investigate the possible signatures of ion-kinetic-scale processes in soft Xray images,we use for the first time a global hybrid-Vlasov simulation of the geospace from the Vlasiator model.The simulation is driven by fast and tenuous solar wind conditions and purely southward interplanetary magnetic field.We first produce global X-ray images of the dayside near-Earth space by placing a virtual imaging satellite at two different locations,providing meridional and equatorial views.We then analyze regional features present in the images and show that they correspond to signatures in soft X-ray emissions of mirrormode wave structures in the magnetosheath and flux transfer events(FTEs)at the magnetopause.Our results suggest that,although the time scales associated with the motion of those transient phenomena will likely be significantly smaller than the integration time of the SMILE and LEXI imagers,mirror-mode structures and FTEs can cumulatively produce detectable signatures in the soft X-ray images.For instance,a local increase by 30%in the proton density at the dayside magnetopause resulting from the transit of multiple FTEs leads to a 12%enhancement in the line-of-sight-and time-integrated soft X-ray emissivity originating from this region.Likewise,a proton density increase by 14%in the magnetosheath associated with mirror-mode structures can result in an enhancement in the soft X-ray signal by 4%.These are likely conservative estimates,given that the solar wind conditions used in the Vlasiator run can be expected to generate weaker soft X-ray emissions than the more common denser solar wind.These results will contribute to the preparatory work for the SMILE and LEXI missions by providing the community with quantitative estimates of the effects of small-scale,transient phenomena occurring on the dayside.
文摘Thermal diffusion of Si atoms at the interface in Mo/Si multilayers was observed with an imaging type soft X ray emission microscope developed by us. It was possible to observe the diffusion with 0.2nm depth resolution in the direction normal to the interface by comparing the emission intensity for exactly the same position. The diffusion coefficient of Si atoms in Mo at 600℃ was roughly estimated to be 6.0×10 17 cm 2/s.
文摘Burners of metal halide lamps used for illumination are generally made of polycrystalline alumina ceramic (PCA) which is translucent to visible light. We show that the difficulty of selecting a line of sight through the lamp prevents the use of optical emission diagnostic. X-rays photons are mainly absorbed and not scattered by PCA. Absorption by mercury atoms contributing to the discharge allowed us to determine the density of mercury in the lamp. By comparing diagnostic methods, we put in evidence the difficulty of taking into account the scattering of light mathematically.
文摘By using soft X-ray spectroscopy, we investigate the inner-shell excitation and relaxation processes in atomic and ionic neon targets. Resonant X-ray emission spectroscopy was applied to neutral neon atom in the regions of the [1s]np (n = 3, 4,…, ε) excited states and [1s2p]3pmp (m = 3,4) doubly excited states to obtain the spectroscopic information on the [2p]np and [2p^2]3prnp final electronic states, where square brackets indicate hole states. The energy levels of the [2p^2]3prnp (m = 3,4) electronic states were spectroscopically measured for the first time. As for the ionic neon target, on the other hand, the photoion yield spectroscopy was adopted to survey the 1s→ np (n = 2, 3) resonant excitation and subsequent Auger decay processes for Ne^+ target-ions. The observed Ne^2+ photoion yield spectrum is successflllly explained by the theoretical calculations based on the nmlticonfiguration Dirac-Fock method
基金supported by the National Natural Science Foundation of China(No.51976209)the Fundamental Research Funds for the Central Universities(No.WK2320000040)supported by the Youth Innovation Promotion Association CAS(No.Y201768)。
文摘Based on the synchrotron soft X-ray absorption spectroscopy experiments,the fundamental electronic structures of layered Li NixCoyMnzO_(2)(NCM)are investigated systematically and the data of transitionmetal(TM)L-and O K-edges spectra are collected.Distribution of Ni ions under different oxidation states is evaluated according to linear combination fit.It is found that the ratio of Ni^(4+)expands with the increase of Ni since it dominates in charge compensation during charging,and that the existence of Ni^(3+)is nearly negligible in delithiated NCM.The valence state of Co also strongly depends on Ni content,the perceptible position shift of Co L_(3)-edge absorption peak towards higher energy in Ni-rich material agrees well with the small voltage plateau at around 4.2 V.The stability of Mn is verified as no obvious spectral change with the Mn L-edge is observed.Moreover,as Ni content rises,the O 2p holes near the Femi level increases with higher oxidation state of Ni,indicating the enhanced hybridization of O 2p-TM 3 d.Delithiated NCMs with higher Ni content are prior to lose electron existing in highly hybridized Ni3 dO 2 p bands upon heating,which accounts for the pronounced O_(2)release in phase transitions and the deterioration in thermal stability.These detailed observation of the electronic structure evolution is one of the key ingredients to improving the electrochemical and thermal performance of NCM.
文摘Understanding electronic structure is crucial to enhance the battery performance. Soft X-ray spectroscopy(SXS) is one of the most effective methods to provide direct probe of electronic states. Here, spectroscopic measurements of transition metal 3 d and oxygen 2 p states are simply reviewed. Then, we mainly focus on the perspective of the development direction of modern SXS techniques. Although the true power of recently developed high efficiency mapping of resonant inelastic X-ray scattering(m RIXS) has been apparent for materials and chemistry studies, great challenges remain for mRIXS spectroscopic interpretation, and the understanding of the battery materials on novel redox activities remains elusive.
基金supported as part of the Joint Center for Energy Storage Research(JCESR)an Energy Innovation Hub funded by the U.S.Department of Energy(DOE),Office of Science,Basic Energy Sciences
文摘The lightweight,rechargeable lithium-ion battery is one of the dominant energy storage devices globally in portable electronics due to its high energy density,no memory effect,wide operating voltage,lightweight,and good charge efficiency.However,due to safety concerns,the depletion of lithium reserves,and the corresponding increase of cost,an alternative battery system becomes more and more desirable.To develop alternative battery systems with low cost and high material abundance,for example,sodium,magnesium,zinc,and calcium,it is important to understand the chemical and electronic structure of materials.Soft X-ray spectroscopy,for example,X-ray absorption spectroscopy(XAS),X-ray emission spectroscopy(XES),and resonant inelastic soft X-ray scattering(RIXS),is an element-specific technique with sensitivity to the local chemical environment and structural order of the element of interest.Modern soft X-ray systems enable operando experiments that can be applied to amorphous and crystalline samples,making it a powerful tool for studying the electronic and structural changes in electrode and electrolyte species.In this article,the application of in situ/operando(soft)X-ray spectroscopy in beyond lithium-ion batteries is reviewed to demonstrate how such spectroscopic characterizations could facilitate the interpretation of interfacial phenomena under in situ/operando condition and subsequent development of the beyond lithium-ion batteries.
基金supported by the Director,Office of Science,Office of Basic Energy Sciences,of the U.S.Department of Energy under Contract No.DE-AC02-05CH11231supported by the LDRD program at the Lawrence Berkeley National Laboratory
文摘The formidable challenge of developing high-performance battery system stems from the complication of battery operations, both mechanically and electronically. In the electrodes and at the electrode-electrolyte interfaces, chemical reactions take place with evolving electron states. In addition to the extensive studies of material synthesis, electrochem- ical, structural, and mechanical properties, soft x-ray spectroscopy provides unique opportunities for revealing the critical electron states in batteries. This review discusses some of the recent soft x-ray spectroscopic results on battery binder, transition-metal based positive electrodes, and the solid-electrolyte-interphase. By virtue of soft x-ray's sensitivity to electron states, the electronic property, the redox during electrochemical operations, and the chemical species of the interphases could be fingerprinted by soft x-ray spectroscopy. Understanding and innovating battery technologies need a multimodal approach, and soft x-ray spectroscopy is one of the incisive tools to probe the chemical and physical evolutions in batteries.
基金support rendered by BRNS (DAE, India) for the project
文摘The oxidation of aluminium was studied using optical emission spectroscopy (OES) during the evaporation of aluminium in traces of oxygen in a thermal plasma reactor. The ratio of the measured line intensities of Al-O with that of Al follows the exact trend as of that obtained from the corresponding line intensities in X-ray diffraction spectra of the synthesized samples. In this paper the inherent capacity of emission spectroscopy in evaluating the growth processes under plasma induced reactions is presented.
基金supported by the Natural Science Foundation of Shandong Province,China(No.ZR2020MA088)Natural Science Foundation of Xinjiang Uygur Autonomous Region,China(No.2019D01C188)+1 种基金National Key Research and Development Program of China(No.2018YFC1200204)National Natural Science Foundation of China(No.12175127).
文摘The visualization and data mining of tumor multidimensional information may play a major role in the analysis of the growth,metastasis,and microenvironmental changes of tumors while challenging traditional imaging and data processing techniques.In this study,a general trans-scale and multi-modality measurement method was developed for the quantitative diagnosis of hepatocellular carcinoma(HCC)using a combination of propagation-based phase-contrast computed tomography(PPCT),scanning transmission soft X-ray microscopy(STXM),and Fourier transform infrared micro-spectroscopy(FTIR).Our experimental results reveal the trans-scale micro-morpho-logical HCC pathology and facilitate quantitative data analysis and comprehensive assessment.These results include some visualization features of PPCT-based tissue microenvironments,STXM-based cellular fine structures,and FTIR-based bio-macromolecular spectral characteris-tics during HCC tumor differentiation and proliferation.The proposed method provides multidimensional feature data support for constructing a high-accuracy machine learning algorithm based on a gray-level histogram,gray-gradient co-occurrence matrix,gray-level co-occurrence matrix,and back-propagation neural network model.Multi-dimensional information analysis and diagnosis revealed the morphological pathways of HCC pathological evolution and we explored the relationships between HCC-related feature changes in inflammatory microenviron-ments,cellular metabolism,and the stretching vibration peaks of biomolecules of lipids,proteins,and nucleic acids.Therefore,the proposed methodology has strong potential for the visualization of complex tumors and assessing the risks of tumor differentiation and metastasis.
文摘The pointed observations of NGC3077 are analyzed by position sensitive proportional counter (PSPC) on board the ROSAT satellite on 1991-04-18, 1991, finding out that the X-ray emission range of M81 galaxy has, in the softer and more sensitive ROSAT PSPC band (0. 2-2. 4 keV), extended by 40% larger than ever observed by image proportional counter (IPC) on board the Einstein satellite, which shows that M81 galaxy has a larger X-ray corona. And by the aid of the timing analysis, it is concluded that M81 nucleus has no variabilities on time scale of a few minutes; hence the possibility of M81 nucleus having the marginal variability over time scale of about 2 min that Fabbiano (1988) found from the Einstein IPC observation is ruled out.
基金supported in part by the National Key R&D Program of China(Nos.2020YFA0405800,2022YFA1504104,and 2022YFA1605400)the National Natural Science Foundation of China(Nos.12225508,12322515,U1932201,U2032113,and 22075264)+5 种基金the Youth Innovation Promotion Association of CAS(No.2022457)the Institute of Energy,Hefei Comprehensive National Science Center,University Synergy Innovation Program of Anhui Province(No.GXXT-2020-002)and the CAS Iterdisciplinary Innovation Team.We thank the Shanghai Synchrotron Radiation Facility(BL14W1,BL14B1,and SSRF)the Beijing Synchrotron Radiation Facility(1W1B,4B7A,and BSRF)the Hefei Synchrotron Radiation Facility(Infrared Spectroscopy and Microspectroscopy,MCD-A and MCD-B Soochow Beamline for Energy Materials at NSRL)and the USTC Center for Micro and Nanoscale Research and Fabrication for helps in characterizations.
文摘Breakthroughs in energy storage and conversion devices depend heavily on the exploration of low-cost and high-performance materials.Carbon-supported electrocatalysts with dimensional varieties have recently attracted significant attention due to their strong structural flexibility and easy accessibility.Nevertheless,understanding the connection between their electronic,structural properties,and catalytic performance must remain a top priority.Synchrotron radiation(SR)X-ray absorption spectroscopy(XAS)techniques,including hard XAS and soft XAS,are recognized as efficient and comprehensive platforms for probing the surface,interface,and bulk electronic structure of elements of interest in the materials community.In the past decade,the flourishing development of materials science and advanced characterization technologies have led to a deeper understanding at different temporal,longitudinal,and spatial scales.In this review,we briefly describe the concept of XAS techniques and summarize their recent progress in addressing scientific questions on carbon-supported electrocatalysts through the development of advanced instruments and experimental methods.We then discuss the remaining challenges and potential research directions in nextgeneration materials frontiers,and suggest challenges and perspectives for shedding light on the structure–activity relationship.
文摘Spectral analysis was a method of identifying substances, determining their chemical composition and calculating their content based on their spectral characteristics. This paper mainly discussed the application of various spectroscopic techniques, mainly including atomic absorption spectrometry (AAS) inductively coupled plasma emission spectrometry (ICP-AES) X-ray fluorescence spectroscopy (XRF) atomic fluorescence spectroscopy (AFS) direct reading spectroscopy (OES) glow discharge emission spectroscopy (GD-OSE) laser-induced breakdown spectroscopy (LIBS), in the formulation of non-ferrous metal standards in China. The AAS method was the most widely used single-element microanalysis method among the non-ferrous metal standards. The ICP-AES method was good at significant advantages in the simultaneous detection of multiple elements. The XRF method was increasingly used in the determination of primary and secondary trace elements due to its simple sample preparation and high efficiency. The AFS was mostly detected by single-element trace analysis. OES GD-OES and LIBS were playing an increasingly important role in the new demand area for non-ferrous metals. This paper discussed matrix elimination, sample digestion, sample preparation, instrument categories and other aspects of some standards, and summarized the advantages of spectral analysis and traditional chemical analysis methods. The new methods of future spectroscopic technology had been illustrated in the process of developing non-ferrous metal standards.
基金This work was supported by the National Natural Science Foundation of China(NSFC,Nos.21801140,51532001,51667009,21771014,and 52002010)。
文摘Nickel based magnetic nanocrystals have been widely applied in magnetic and catalytic facilities.Tunable magnetic properties of nickel can be easily obtained via non-magnetic doping or phase transformation.However,phase transformation from face centered cubic(fcc)to hexagonal close packed(hcp)induced magnetism adjustment of Ni are always confused with nickel carbide(Ni_(3)C),due to the similar atomic structures of hcp-Ni and Ni3C.Here,we present series of Au@Ni-carbide magnetic materials achieved from the controlled carbonation of Au@Ni core-shell structures,whose magnetism is tunable by adjusting the amount of carbon in the Ni layer.Ex-situ hard X-ray absorption spectroscopy(XAS)at the metal K edge and soft XAS at both metal L edge and carbon K edge provide solid evidence for the carbonation process from fcc-Ni to Ni_(x)C,rather than phase transformation to hcp-Ni.Further investigation reveals that the magnetism of the hybrids is mainly contributed from the residual fcc-Ni.The result represents an accurate and effective way to distinguish hexagonal Ni_(3)C from hcp-Ni,and provides the pathway to control magnetism of Ni-based materials for applications.
基金supported by the National Natural Science Foundation of China(No.51976209)the Fundamental Research Funds for the Central Universities(No.WK2320000040)+1 种基金the Synchrotron Radiation Joint Fund of University of Science and Technology of Chinasupported by Youth Innovation Promotion Association CAS(No.Y201768)。
文摘By virtue of the crucial effect of the crystal structure and transition metal(TM)redox evolution on the performance of LiNi_(x)Co_(y)Mn_(z)O_(2)(NCM)cathode,systematical investigation is carried out to better understand the charge mechanism upon deep charging.Based on the results of X-ray diffraction and highresolution transmission electron microscope,phase transformations existing on particle surface are promoted by high potential because of the deeper lithium vacancies,accompanied by more substantial structure instability.Soft X-ray absorption spectroscopy indicates that Ni acts as the major contributor to charge compensation while Co displays a remarkable redox activity over the deep charge range.The elevated integrated intensity of pre-edge in O K-edge spectra reveals the extensive amount of holes formed in O 2 p orbitals and the enhanced hybridization of TM 3 d-O 2 p orbitals.Considering the close relationship between thermal behavior and structural evolution,the tendency of phase transitions and O_(2) release upon heating is accelerated by voltage rise,demonstrating the aggravated instability due to deeper Li utilization.Remaining Li contents in NCM are employed to estimate the amount of oxygen released in structural transformation and its detrimental effect on stability declares Li contentdependent characteristics.Furthermore,the extended Li vacancies,higher proportion of Ni4+and stronger orbital hybridization are considered as three factors impeding the thermal stability of the highlydelithiated NCM.
基金supported by National Natural Science Foundation of China (Nos. 10975105, 11275136, 10975106, 11175126, 11204266 and 11075114) the National Magnetic Confinement Fusion Science Program of China (Nos. 2010GB106000, 2010GB106009), the Open Project of State Key Laboratory of Functional Materials for Information and Qing Lan Project, a Project Funded by the Priority Academic Program Development of Jiangsu Higher Education Institutions and the Program for graduates Research & Innovation in University of Jiangsu Province, China (No. CX10B-031Z)
文摘Dry etching of 6H silicon carbide (6H-SiC) wafers in a C4Fs/Ar dual-frequency capacitively coupled plasma (DF-CCP) was investigated. Atomic force microscopy (AFM) and X-ray photoelectron spectroscopy (XPS) were used to measure the SiC surface structure and compositions, respectively. Optical emission spectroscopy (OES) was used to measure the relative concentration of F radicals in the plasma. It was found that the roughness of the etched SiC surface and the etching rate are directly related to the power of low-frequency (LF) source. At lower LF power, a smaller surface roughness and a lower etching rate are obtained due to weak bombardment of low energy ions on the SiC wafers. At higher LF power the etching rate can be efficiently increased, but the surface roughness increases too. Compared with other plasma dry etching methods, the DF-CCP can effectively inhibit CχFγ films' deposition, and reduce surface residues.
基金Project supported by the National High Technology Program, the National Natural Science Foundation of China, and the Signification Scientific Project of the Chinese Academy of Sciences
文摘The study of soft X-ray amplification is important and interesting. Pierre Jaeglé et al. have done some work in this field about soft X-ray amplification by Li-like Al ions and have got promising results. In this note, we report our recent result about it.
基金Project supported by the National Natural Science Foundation of China (Grant No 10475022).
文摘This paper describes the behaviour of impurity transport in HL-2A ohmic discharges. In 2005, small quantities of metallic impurities (A1, Ni and Ti) were successfully injected into HL-2A plasmas by laser blow-off technique, and their progression was followed by the soft x-ray cameras with good spatial and temporal resolutions. The impurity confinement time is estimated from the characteristic decay time of the soft x-ray signal of the injected impurities, and it is about 30-60 ms. The transport coefficients of impurities (including diffusion coefficient and convection velocity) in radial different region have been derived by using a one-dimenslonal impurity transport code, the results present that diffusion coefficient is much smaller in the central region of plasmas than the outside of it, and it is much larger than that of neoclassical theory predictions; namely, it is anomalous.
基金the Guangdong Provincial Natural Science Foundation under grant No. 031502.
文摘Nitrogen ion was implanted into the nano-TiO2 film surfaces by electron cyclotron resonance (ECR) plasma modification to improve the optical reactivity in visible-light region for nano-TiO2. Diagnosing the N2 plasma by optical emission spectroscopy (OES) was applied to the process of plasma modification. X-ray photoelectron spectroscopy (XPS) was used for analysis of the binding of element after plasma modification. It is shown that the surface modification was caused by excitated N. The injecting of N2 and N+ leads to the increase in the dissociative interstitial state N in the films. The doped N makes for TiO2-xNx appearing in the TiO2 films. TiO2-xNx forms the impurity energy state in the TiO2 energy band gap and reduces the energy band gap. This is the main reason leading to the red shift of absorption edge.