An in-depth understanding of the structure-activity relationship between the surface structure,chemical composition,adsorption and desorption of molecules,and their reaction activity and selectivity is necessary for t...An in-depth understanding of the structure-activity relationship between the surface structure,chemical composition,adsorption and desorption of molecules,and their reaction activity and selectivity is necessary for the rational design of high-performance catalysts.Herein,we present a method for studying catalytic mechanisms using a combination of in situ reaction cells and surface science techniques.The proposed system consists of four parts:preparation chamber,temperatureprogrammed desorption(TPD)chamber,quick load-lock chamber,and in situ reaction cell.The preparation chamber was equipped with setups based on the surface science techniques used for standard sample preparation and characterization,including an Ar+sputter gun,Auger electron spectrometer,and a low-energy electron diffractometer.After a well-defined model catalyst was prepared,the sample was transferred to a TPD chamber to investigate the adsorption and desorption of the probe molecule,or to the reaction cell,to measure the catalytic activity.A thermal desorption experiment for methanol on a clean Cu(111)surface was conducted to demonstrate the functionality of the preparation and TPD chambers.Moreover,the repeatability of the in situ reaction cell experiment was verified by CO_(2) hydrogenation on the Ni(110)surface.At a reaction pressure of 800 Torr at 673 K,turnover frequencies for the methanation reaction and reverse water-gas shift reaction were 0.15 and 7.55 Ni atom^(-1) s^(-1),respectively.展开更多
X-ray photon correlation spectroscopy(XPCS)has emerged as a powerful tool for probing the nanoscale dynamics of soft condensed matter and strongly correlated materials owing to its high spatial resolution and penetrat...X-ray photon correlation spectroscopy(XPCS)has emerged as a powerful tool for probing the nanoscale dynamics of soft condensed matter and strongly correlated materials owing to its high spatial resolution and penetration capabilities.This technique requires high brilliance and beam coherence,which are not directly available at modern synchrotron beamlines in China.To facilitate future XPCS experiments,we modified the optical setup of the newly commissioned BL10U1 USAXS beamline at the Shanghai Synchrotron Radiation Facility(SSRF).Subsequently,we performed XPCS measurements on silica suspensions in glycerol,which were opaque owing to their high concentrations.Images were collected using a high frame rate area detector.A comprehensive analysis was performed,yielding correlation functions and several key dynamic parameters.All the results were consistent with the theory of Brownian motion and demonstrated the feasibility of XPCS at SSRF.Finally,by carefully optimizing the setup and analyzing the algorithms,we achieved a time resolution of 2 ms,which enabled the characterization of millisecond dynamics in opaque systems.展开更多
Fewest-switches surfacing hopping(FSSH) simulations have been performed with the high-level multi-reference electronic structure method to explore the coupled electronic and nuclear dynamics upon photoexcitation of cy...Fewest-switches surfacing hopping(FSSH) simulations have been performed with the high-level multi-reference electronic structure method to explore the coupled electronic and nuclear dynamics upon photoexcitation of cyanogen bromide(BrCN). The potential energy surfaces(PES) of BrCN are charted as functions of the Jacobi coordinates(R, θ). An indepth examination of the FSSH trajectories reveals the temporal dynamics of the molecule and the population changes of the lowest twelve states during BrCN's photodissociation process, which presents a rich tapestry of dynamical information.Furthermore, the carbon K-edge x-ray absorption spectroscopy(XAS) is calculated with multi-reference inner-shell spectral simulations. The rotation of the CN fragment and the elongation of the C–Br bond are found to be the reason for the peak shifting in the XAS. Our findings offer a nuanced interpretation for inner-shell probe investigations of BrCN, setting the stage for a deeper understanding of the photodissociation process of cyanogen halides molecules.展开更多
With the integration of ultrafast reflectivity and polarimetry probes,we observed carrier relaxation and spin dynamics induced by ultrafast laser excitation of Ni(111)single crystals.The carrier relaxation time within...With the integration of ultrafast reflectivity and polarimetry probes,we observed carrier relaxation and spin dynamics induced by ultrafast laser excitation of Ni(111)single crystals.The carrier relaxation time within the linear excitation range reveals that electron-phonon coupling and dissipation of photon energy into the bulk of the crystal take tens of picoseconds.On the other hand,the observed spin dynamics indicate a longer time of about 120 ps.To further understand how the lattice degree of freedom is coupled with these dynamics may require the integration of an ultrafast diffraction probe.展开更多
Magnetic topological semimetals have been at the forefront of condensed matter physics due to their ability to exhibit exotic transport phenomena.Investigating the interplay between magnetic and topological orders in ...Magnetic topological semimetals have been at the forefront of condensed matter physics due to their ability to exhibit exotic transport phenomena.Investigating the interplay between magnetic and topological orders in systems with broken time-reversal symmetry is crucial for realizing non-trivial quantum effects.We delve into the electronic structure of the rare-earth-based antiferromagnetic Dirac semimetal EuMg_(2)Bi_(2) using first-principles calculations and angle-resolved photoemission spectroscopy.Our calculations reveal that the spin-orbit coupling(SOC)in EuMg_(2)Bi_(2) prompts an insulator to topological semimetal transition,with the Dirac bands protected by crystal symmetries.The linearly dispersive states near the Fermi level,primarily originating from Bi 6p orbitals,are observed on both the(001)and(100)surfaces,confirming that EuMg_(2)Bi_(2) is a three-dimensional topological Dirac semimetal.This research offers pivotal insights into the interplay between magnetism,SOC and topological phase transitions in spintronics applications.展开更多
We report on experimental measurements of the transition dipole moments(TDMs)between the intermediate state 5s5p^(3)P_(1)and the triplet Rydberg series 5sns^(3)S_(1)in an ultracold strontium gas.Here n is the principa...We report on experimental measurements of the transition dipole moments(TDMs)between the intermediate state 5s5p^(3)P_(1)and the triplet Rydberg series 5sns^(3)S_(1)in an ultracold strontium gas.Here n is the principal quantum number ranging from 19 to 40.The transition 5s5p^(3)P_(1)–5sns^(3)S_(1)is coupled via an ultraviolet(UV)beam,inducing Autler–Townes splitting of both states.Such a splitting of the intermediate state is spectroscopically measured by using absorption imaging on a narrow transition 5s^(21)S_(0)–5s5p^(3)P_(1)in an ultracold gas of strontium atoms.The power and size of the UV beam are carefully determined,with which the TDMs are extracted from the measured Autler–Townes splitting.The experimentally obtained TDMs are compared to the calculations based on a parametric core potential,on a Coulomb potential with quantum defect,and on the open-source library Alkali Ryderg calculator,finding good agreement with the former two models and significant deviation with the latter.展开更多
The accurate analysis of the elemental composition plays a crucial role in the research of functional materials.The emitting characteristic x-ray fluorescence(XRF)photons can be used for precisely discriminating the s...The accurate analysis of the elemental composition plays a crucial role in the research of functional materials.The emitting characteristic x-ray fluorescence(XRF)photons can be used for precisely discriminating the specified element.The detection accuracy of conventional XRF methodology using semiconductor detector is limited by the energy resolution,thus posing a challenge in accurately scaling the actual energy of each XRF photon.We adopt a novel high-resolution x-ray spectrometer based on the superconducting transition-edge sensor(TES)for the XRF spectroscopy measurement of different elements.Properties including high energy resolution,high detection efficiency and precise linearity of the new spectrometer will bring significant benefits in analyzing elemental composition via XRF.In this paper,we study the Ledge emission line profiles of three adjacent rare earth elements with the evenly mixed sample of their oxide components:terbium,dysprosium and holmium.Two orders of magnitude better energy resolution are obtained compared to a commercial silicon drift detector.With this TES-based spectrometer,the spectral lines overlapped or interfered by background can be clearly distinguished,thus making the chemical component analysis more accurate and quantitative.A database of coefficient values for the line strength of the spectrum can then be constructed thereafter.Equipped with the novel XRF spectrometer and an established coefficient database,a direct analysis of the composition proportion of a certain element in an unknown sample can be achieved with high accuracy.展开更多
Fe_(3)GaTe_(2),a recently discovered van der Waals ferromagnetic crystal with the highest Curie temperature and strong perpendicular magnetic anisotropy among two-dimensional(2D)magnetic materials,has attracted signif...Fe_(3)GaTe_(2),a recently discovered van der Waals ferromagnetic crystal with the highest Curie temperature and strong perpendicular magnetic anisotropy among two-dimensional(2D)magnetic materials,has attracted significant attention and makes it a promising candidate for next-generation spintronic applications.Compared with Fe_(3)GeTe_(2),which has the similar crystal structure,the mechanism of the enhanced ferromagnetic properties in Fe_(3)GaTe_(2)is still unclear and needs to be investigated.Here,by using x-ray magnetic circular dichroism measurements,we find that both Ga and Te atoms contribute to the total magnetic moment of the system with antiferromagnetic coupling to Fe atoms.Our first-principles calculations reveal that Fe_(3)GaTe_(2)has van Hove singularities at the Fermi level in nonmagnetic state,resulting in the magnetic instability of the system and susceptibility to magnetic phase transitions.In addition,the calculation results about the density of states in ferromagnetic states of two materials suggest that the exchange interaction between Fe atoms is strengthened by replacing Ge atoms with Ga atoms.These findings indicate the increase of both the itinerate and local moments in Fe_(3)GaTe_(2)in view of Stoner and exchange interaction models,which results in the enhancement of the overall magnetism and a higher Curie temperature.Our work provides insight into the underlying mechanism of Fe_(3)GaTe_(2)’s remarkable magnetic properties and has important implications for searching 2D materials with expected magnetic properties in the future.展开更多
The migration of protons during the oxygen evolution reaction(OER)is a key factor that affects the performance of OER catalysts.To enhance proton transportation,we designed a catalyst based on nickel/iron-pyromellitic...The migration of protons during the oxygen evolution reaction(OER)is a key factor that affects the performance of OER catalysts.To enhance proton transportation,we designed a catalyst based on nickel/iron-pyromellitic acid(NiFe-PMA)prepared by the electrochemical deposition method.This catalyst exhibited a low overpotential of 188 mV at a current density of 10 mA·cm^(-2),a Tafel slope of 28.2 mV·dec^(-1),and long-term stability for 30 days with a current of 50 mA·cm^(-2).We characterized the NiFe-PMA catalyst using various techniques,including Fourier transform infrared(FTIR)spectroscopy,Raman spectroscopy,X-ray photoelectron spectroscopy(XPS),X-ray absorption spectroscopy(XAS),transmission electron microscopy(TEM),scanning electron microscopy(SEM),and inductively coupled plasma-optical emission spectrometry(ICP-OES).Our results showed that NiFe-PMA contains nickel,iron atoms,and both coordinated and uncoordinated carboxylate groups.Additionally,XPS data confirmed that carboxylate ligands could adjust the outer electronic structure of metal ions,resulting in the high valence state of Ni in NiFe-PMA.The result of XAS indicated that the nickel atoms present in the catalyst might be easier to maintain a higher chemical state.Further investigations using kinetic isotope effects(KIEs)and proton inventory revealed that the uncoordinated carboxylic protons played a crucial role in receiving protons during the OER,which promoted the proton transfer of the rate-determining step of the OER.Our novel electrocatalysts provide a new strategy for designing more active and cost-effective catalysts for the OER.展开更多
The Shanghai soft X-ray free-electron laser(SXFEL)user facility project started in 2016 and is expected to be open to users by 2022.It aims to deliver ultra-intense coherent femtosecond X-ray pulses to five endstation...The Shanghai soft X-ray free-electron laser(SXFEL)user facility project started in 2016 and is expected to be open to users by 2022.It aims to deliver ultra-intense coherent femtosecond X-ray pulses to five endstations covering a range of 100–620 eV for ultrafast X-ray science.Two undulator lines are designed and constructed,based on different lasing modes:self-amplified spontaneous emission and echo-enabled harmonic generation.The coherent scattering and imaging(CSI)endstation is the first of five endstations to be commissioned online.It focuses on high-resolution single-shot imaging and the study of ultrafast dynamic processes using coherent forward scattering techniques.Both the single-shot holograms and coherent diffraction patterns were recorded and reconstructed for nanoscale imaging,indicating the excellent coherence and high peak power of the SXFEL and the possibility of‘‘diffraction before destruction’’experiments at the CSI endstation.In this study,we report the first commissioning results of the CSI endstation.展开更多
Based on the first-principles method,we predict two new stable BN allotropes:C12-BN and O16-BN,which belong to cubic and orthorhombic crystal systems,respectively.It is confirmed that both the phases are thermally and...Based on the first-principles method,we predict two new stable BN allotropes:C12-BN and O16-BN,which belong to cubic and orthorhombic crystal systems,respectively.It is confirmed that both the phases are thermally and dynamically stable.The results of molecular dynamics simulations suggest that both the BN phases are highly stable even at high temperatures of 1000 K.In the case of mechanical properties,C12-BN has a bulk modulus of 359 GPa and a hardness of 43.4 GPa,making it a novel superhard material with potential technological and industrial applications.Electronic band calculations reveal that both C12-BN and O16-BN are insulators with direct band gaps of 3.02 e V and 3.54 e V,respectively.The XRD spectra of C12-BN and O16-BN are also simulated to provide more information for possible experimental observation.Our findings enrich the BN allotrope family and are expected to stimulate further experimental interest.展开更多
Photoelectron diffraction is an effective tool to probe the structures of molecules.The higher the photoelectron kinetic energy is,the higher order the diffraction pattern is disclosed in.Up to date,either the multi-a...Photoelectron diffraction is an effective tool to probe the structures of molecules.The higher the photoelectron kinetic energy is,the higher order the diffraction pattern is disclosed in.Up to date,either the multi-atomic molecule with the photoelectron kinetic energy below 150 e V or the diatomic molecule with 735 eV photoelectron has been experimentally reported.In this study,we measured the diffraction pattern of C 1 s and O 1 s photoelectrons in CO_(2)with 319.7 and 433.5 eV kinetic energies,respectively.The extracted C–O bond lengths are longer than the C–O bond length at the ground state,which is attributed to the asymmetric fragmentation that preferentially occurs at the longer chemical bond side during the zero-energy asymmetric vibration.展开更多
We investigate the dissociation dynamics of core-excited O_(2)molecules using a high-resolution energy-resolved electron-ion coincidence experimental setup.The excited cationic states with two valence holes and one Ry...We investigate the dissociation dynamics of core-excited O_(2)molecules using a high-resolution energy-resolved electron-ion coincidence experimental setup.The excited cationic states with two valence holes and one Rydberg electron are created after spectator Auger decay induced by O 1s→(^(4)Σ_(u)^(-))3sσcore excitation in O_(2).From the energy correlation between the kinetic energy of the Auger electron and the ion kinetic energy release,we distinguish several dissociation channels.Rather complex dissociation channels of the spectator Auger final states are disclosed,which can be explained by the increased number of the crossing point due to the existence of Rydberg electron.The quantum system will evolve into different dissociation limits at each crossing point between the potential energy curves.展开更多
A transition edge sensor(TES)is extremely sensitive to changes in temperature,and combined with a high-Z metal of a certain thickness,it can realize high-energy resolution measurements of particles such as X-rays.X-ra...A transition edge sensor(TES)is extremely sensitive to changes in temperature,and combined with a high-Z metal of a certain thickness,it can realize high-energy resolution measurements of particles such as X-rays.X-rays with energies below 10 keV have a weak penetrating ability,hence,only gold or bismuth of a few micrometers in thickness can guarantee a quantum efficiency higher than 70%.Therefore,the entire structure of the TES X-ray detector in this energy range can be realized using a microfabrication process.However,for X-rays or γ-rays from 10 keV to 200 keV,submillimeter absorber layers are required,which cannot be realized using the microfabrication process.This paper first briefly introduces a set of TES X-ray detectors and their auxiliary systems,and then focuses on the introduction of the TES γ-ray detector with an absorber based on a submillimeter lead-tin alloy sphere.The detector achieved a quantum efficiency above 70% near 100 keV and an energy resolution of approximately 161.5 eV at 59.5 keV.展开更多
Noninvasive X-ray imaging of nanoscale three-dimensional objects,such as integrated circuits(ICs),generally requires two types of scanning:ptychographic,which is translational and returns estimates of the complex elec...Noninvasive X-ray imaging of nanoscale three-dimensional objects,such as integrated circuits(ICs),generally requires two types of scanning:ptychographic,which is translational and returns estimates of the complex electromagnetic field through the IC;combined with a tomographic scan,which collects these complex field projections from multiple angles.Here,we present Attentional Ptycho-Tomography(APT),an approach to drastically reduce the amount of angular scanning,and thus the total acquisition time.APT is machine learning-based,utilizing axial self-Attention for Ptycho-Tomographic reconstruction.APT is trained to obtain accurate reconstructions of the ICs,despite the incompleteness of the measurements.The training process includes regularizing priors in the form of typical patterns found in IC interiors,and the physics of X-ray propagation through the IC.We show that APT with×12 reduced angles achieves fidelity comparable to the gold standard Simultaneous Algebraic Reconstruction Technique(SART)with the original set of angles.When using the same set of reduced angles,then APT also outperforms Filtered Back Projection(FBP),Simultaneous Iterative Reconstruction Technique(SIRT)and SART.The time needed to compute the reconstruction is also reduced,because the trained neural network is a forward operation,unlike the iterative nature of these alternatives.Our experiments show that,without loss in quality,for a 4.48×93.2×3.92µm^(3) IC(≃6×10^(8) voxels),APT reduces the total data acquisition and computation time from 67.96 h to 38 min.We expect our physics-assisted and attention-utilizing machine learning framework to be applicable to other branches of nanoscale imaging,including materials science and biological imaging.展开更多
The chemical stoichiometry on the surface of superconducting δ-NbN thin films is of great importance for their application.Here,we fabricated the δ-NbN thin films on SiO2/Si substrate by DC sputtering method.The fil...The chemical stoichiometry on the surface of superconducting δ-NbN thin films is of great importance for their application.Here,we fabricated the δ-NbN thin films on SiO2/Si substrate by DC sputtering method.The film was characterized using X-ray diffraction(XRD) and atomic force microscopy(AFM).Transport properties were measured to reveal the field dependent superconducting transition temperature.Both XRD and electrical measurement show high crystallinity of δ-NbN phase.A homogeneous and smooth surface morphology was measured by AFM.Auger electron spectroscopy(AES) was applied to analyze the composition along the depth of the film.The evolution of Auger peak profile,heights and nitride stoichiometry at the film surface is discussed.The current study provides a more thorough understanding of complex chemical compositions of δ-NbN thin films.展开更多
Ultrafast extreme ultraviolet (XUV) transient absorption spectroscopy measures the time- and frequencydependent light losses after light–matter interactions. In the linear region, the matter response to an XUV light ...Ultrafast extreme ultraviolet (XUV) transient absorption spectroscopy measures the time- and frequencydependent light losses after light–matter interactions. In the linear region, the matter response to an XUV light field is usually determined by the complex refractive index ̃n. The absorption signal is directly related to the imaginary part of ̃n, namely, the absorption index. The real part of ̃n refers to the real refractive index, which describes the chromatic dispersion of an optical material. However, the real refractive index information is usually not available in conventional absorption experiments. Here, we investigate the refractive index line shape in ultrafast XUV transient absorption spectroscopy by using a scheme that the XUV pulse traverses the target gas jet off-center. The jet has a density gradient in the direction perpendicular to the gas injection direction, which induces deflection on the XUV radiation. Our experimental and theoretical results show that the shape of the frequency-dependent XUV deflection spectra reproduces the refractive index line profile. A typical dispersive refractive index line shape is measured for a single-peak absorption;an additional shoulder structure appears for a doublet absorption.Moreover, the refractive index line shape is controlled by introducing a later-arrived near-infrared pulse to modify the phase of the XUV free induction decay, resulting in different XUV deflection spectra. The results promote our understanding of matter-induced absorption and deflection in ultrafast XUV spectroscopy.展开更多
In this paper,a simple theoretical model combining Monte Carlo simulation with the enthalpy method is provided to simulate the damage resistance of B4C/Si-sub mirror under X-ray free-electron laser irradiation.Two dif...In this paper,a simple theoretical model combining Monte Carlo simulation with the enthalpy method is provided to simulate the damage resistance of B4C/Si-sub mirror under X-ray free-electron laser irradiation.Two different damage mechanisms are found,dependent on the photon energy.The optimum B4C film thickness is determined by studying the dependence of the damage resistance on the film thickness.Based on the optimized film thickness,the damage thresholds are simulated at photon energy of 0.4-25 keV and a grazing incidence angle of 2 mrad.It is recommended that the energy range around the Si K-edge should be avoided for safety reasons.展开更多
Organic-inorganic layered perovskites are two-dimensional quantum well layers in which the layers of lead halide octahedra are stacked between the organic cation layers.The packing geometry of the soft organic molecul...Organic-inorganic layered perovskites are two-dimensional quantum well layers in which the layers of lead halide octahedra are stacked between the organic cation layers.The packing geometry of the soft organic molecules and the stiff ionic crystals induce structural deformation of the inorganic octahedra,generating complex lattice dynamics.Especially,the dielectric confinement and ionic sublattice lead to strong coupling between the photogenerated excitons and the phonons from the polar lattice which intensively affects the properties for device applications.The anharmonicity and dynamic disorder from the organic cations participate in the relaxation dynamics coupled with excitations.However,a detailed understanding of this underlying mechanism remains obscure.This work investigates the electron–optical phonon coupling dynamics by employing ultrafast pump-probe transient absorption spectroscopy.The activated different optical phonon modes are observed via systematic studies of(PEA)_(2)PbBr_(4) perovskite films on the ultrafast lattice vibrational dynamics.The experimental results indicate that solvent engineering has a significant influence on lattice vibrational modes and coherent phonon dynamics.This work provides fresh insights into electron-optical phonon coupling for emergent optoelectronics development based on layered perovskites.展开更多
We demonstrate via first-principle calculations based on the density functional theory that the magnetic moment of a helium atom under a given magnetic field has a positive correlation with the electric dipole moment ...We demonstrate via first-principle calculations based on the density functional theory that the magnetic moment of a helium atom under a given magnetic field has a positive correlation with the electric dipole moment when an external electric field is applied to the system.Our calculation shows that the enhancement of the magnetic moment is significant due to the reduction of the triplet-singlet splitting.We argue that this finding can be generalized to organic molecules,especially to macromolecules where the structure induced an electric dipole moment which may give rise to significantly enhanced responses to the external magnetic field.These results suggest that considerable magnetic responses prevail,particularly in bio-molecules without an inversion center.展开更多
基金supported by the National Natural Science Foundation of China (Nos.21802096,21832004,21902179,21991152,and 21991150)the Shanghai XFEL Beamline Project (SBP) (31011505505885920161A2101001)the support of the Shanghai Sailing Program (19YF1455600)。
文摘An in-depth understanding of the structure-activity relationship between the surface structure,chemical composition,adsorption and desorption of molecules,and their reaction activity and selectivity is necessary for the rational design of high-performance catalysts.Herein,we present a method for studying catalytic mechanisms using a combination of in situ reaction cells and surface science techniques.The proposed system consists of four parts:preparation chamber,temperatureprogrammed desorption(TPD)chamber,quick load-lock chamber,and in situ reaction cell.The preparation chamber was equipped with setups based on the surface science techniques used for standard sample preparation and characterization,including an Ar+sputter gun,Auger electron spectrometer,and a low-energy electron diffractometer.After a well-defined model catalyst was prepared,the sample was transferred to a TPD chamber to investigate the adsorption and desorption of the probe molecule,or to the reaction cell,to measure the catalytic activity.A thermal desorption experiment for methanol on a clean Cu(111)surface was conducted to demonstrate the functionality of the preparation and TPD chambers.Moreover,the repeatability of the in situ reaction cell experiment was verified by CO_(2) hydrogenation on the Ni(110)surface.At a reaction pressure of 800 Torr at 673 K,turnover frequencies for the methanation reaction and reverse water-gas shift reaction were 0.15 and 7.55 Ni atom^(-1) s^(-1),respectively.
基金This work was supported by National Natural Science Foundation of China(No.12075304)Natural Science Foundation of Shanghai(No.22ZR1442100)National Key Research and Development Program of China(No.2022YFB3503904).
文摘X-ray photon correlation spectroscopy(XPCS)has emerged as a powerful tool for probing the nanoscale dynamics of soft condensed matter and strongly correlated materials owing to its high spatial resolution and penetration capabilities.This technique requires high brilliance and beam coherence,which are not directly available at modern synchrotron beamlines in China.To facilitate future XPCS experiments,we modified the optical setup of the newly commissioned BL10U1 USAXS beamline at the Shanghai Synchrotron Radiation Facility(SSRF).Subsequently,we performed XPCS measurements on silica suspensions in glycerol,which were opaque owing to their high concentrations.Images were collected using a high frame rate area detector.A comprehensive analysis was performed,yielding correlation functions and several key dynamic parameters.All the results were consistent with the theory of Brownian motion and demonstrated the feasibility of XPCS at SSRF.Finally,by carefully optimizing the setup and analyzing the algorithms,we achieved a time resolution of 2 ms,which enabled the characterization of millisecond dynamics in opaque systems.
基金supported by the start-up funding of ShanghaiTech University in Chinasupported by a user project at the Molecular Foundry (LBNL) and its computing resources administered by the High-Performance Computing Services Group at LBNL+2 种基金supported by the Office of Science and Office of Basic Energy Sciences of the U.S.Department of Energy (Grant No.DE-AC02-05CH11231)the National Energy Research Scientific Computing Center (NERSC),a U.S.Department of Energy Office of Science User Facility located at Lawrence Berkeley National Laboratory (Grant No.DE-AC02-05CH11231)supported by the High-Performance Computing (HPC) Platform of ShanghaiTech University。
文摘Fewest-switches surfacing hopping(FSSH) simulations have been performed with the high-level multi-reference electronic structure method to explore the coupled electronic and nuclear dynamics upon photoexcitation of cyanogen bromide(BrCN). The potential energy surfaces(PES) of BrCN are charted as functions of the Jacobi coordinates(R, θ). An indepth examination of the FSSH trajectories reveals the temporal dynamics of the molecule and the population changes of the lowest twelve states during BrCN's photodissociation process, which presents a rich tapestry of dynamical information.Furthermore, the carbon K-edge x-ray absorption spectroscopy(XAS) is calculated with multi-reference inner-shell spectral simulations. The rotation of the CN fragment and the elongation of the C–Br bond are found to be the reason for the peak shifting in the XAS. Our findings offer a nuanced interpretation for inner-shell probe investigations of BrCN, setting the stage for a deeper understanding of the photodissociation process of cyanogen halides molecules.
基金Project supported by the National Key R&D Program of China (Grant Nos. 2022YFA1604402 and 2022YFA1604403)the National Natural Science Foundation of China (NSFC) (Grant No. 11721404)+3 种基金the Shanghai Rising-Star Program (Grant No. 21QA1406100)the Technology Innovation Action Plan of the Science and Technology Commission of Shanghai Municipality (Grant No. 20JC1416000)support by the Air Force Office of Scientific Research (AFOSR) (Grant No. FA9550-20-10139)the Texas A&M Engineering Experimental Station (TEES)
文摘With the integration of ultrafast reflectivity and polarimetry probes,we observed carrier relaxation and spin dynamics induced by ultrafast laser excitation of Ni(111)single crystals.The carrier relaxation time within the linear excitation range reveals that electron-phonon coupling and dissipation of photon energy into the bulk of the crystal take tens of picoseconds.On the other hand,the observed spin dynamics indicate a longer time of about 120 ps.To further understand how the lattice degree of freedom is coupled with these dynamics may require the integration of an ultrafast diffraction probe.
基金supported by the National Key R&D Program of China(Grant No.2022YFA1604302)the National Natural Science Foundation of China(Grant Nos.U1632266,11927807,and U2032207)the approval of the Proposal Assessing Committee of SiP.ME^(2) platform project(Proposal No.11227902)supported by the National Science Foundation of China。
文摘Magnetic topological semimetals have been at the forefront of condensed matter physics due to their ability to exhibit exotic transport phenomena.Investigating the interplay between magnetic and topological orders in systems with broken time-reversal symmetry is crucial for realizing non-trivial quantum effects.We delve into the electronic structure of the rare-earth-based antiferromagnetic Dirac semimetal EuMg_(2)Bi_(2) using first-principles calculations and angle-resolved photoemission spectroscopy.Our calculations reveal that the spin-orbit coupling(SOC)in EuMg_(2)Bi_(2) prompts an insulator to topological semimetal transition,with the Dirac bands protected by crystal symmetries.The linearly dispersive states near the Fermi level,primarily originating from Bi 6p orbitals,are observed on both the(001)and(100)surfaces,confirming that EuMg_(2)Bi_(2) is a three-dimensional topological Dirac semimetal.This research offers pivotal insights into the interplay between magnetism,SOC and topological phase transitions in spintronics applications.
基金supported by the Anhui Initiative in Quantum Information Technologiessupport from the National Natural Science Foundation of China(Grant No.11827806)。
文摘We report on experimental measurements of the transition dipole moments(TDMs)between the intermediate state 5s5p^(3)P_(1)and the triplet Rydberg series 5sns^(3)S_(1)in an ultracold strontium gas.Here n is the principal quantum number ranging from 19 to 40.The transition 5s5p^(3)P_(1)–5sns^(3)S_(1)is coupled via an ultraviolet(UV)beam,inducing Autler–Townes splitting of both states.Such a splitting of the intermediate state is spectroscopically measured by using absorption imaging on a narrow transition 5s^(21)S_(0)–5s5p^(3)P_(1)in an ultracold gas of strontium atoms.The power and size of the UV beam are carefully determined,with which the TDMs are extracted from the measured Autler–Townes splitting.The experimentally obtained TDMs are compared to the calculations based on a parametric core potential,on a Coulomb potential with quantum defect,and on the open-source library Alkali Ryderg calculator,finding good agreement with the former two models and significant deviation with the latter.
基金the National Major Scientific Research Instrument Development Project(Grant No.11927805)the National Key Research and Development Program of China(Grant No.2022YFF0608303)+2 种基金the NSFC Young Scientists Fund(Grant No.12005134)the Shanghai-XFEL Beamline Project(SBP)(Grant No.31011505505885920161A2101001)the Shanghai Municipal Science and Technology Major Project(Grant No.2017SHZDZX02)。
文摘The accurate analysis of the elemental composition plays a crucial role in the research of functional materials.The emitting characteristic x-ray fluorescence(XRF)photons can be used for precisely discriminating the specified element.The detection accuracy of conventional XRF methodology using semiconductor detector is limited by the energy resolution,thus posing a challenge in accurately scaling the actual energy of each XRF photon.We adopt a novel high-resolution x-ray spectrometer based on the superconducting transition-edge sensor(TES)for the XRF spectroscopy measurement of different elements.Properties including high energy resolution,high detection efficiency and precise linearity of the new spectrometer will bring significant benefits in analyzing elemental composition via XRF.In this paper,we study the Ledge emission line profiles of three adjacent rare earth elements with the evenly mixed sample of their oxide components:terbium,dysprosium and holmium.Two orders of magnitude better energy resolution are obtained compared to a commercial silicon drift detector.With this TES-based spectrometer,the spectral lines overlapped or interfered by background can be clearly distinguished,thus making the chemical component analysis more accurate and quantitative.A database of coefficient values for the line strength of the spectrum can then be constructed thereafter.Equipped with the novel XRF spectrometer and an established coefficient database,a direct analysis of the composition proportion of a certain element in an unknown sample can be achieved with high accuracy.
基金supported by the National Key R&D Program of China(Grant Nos.2022YFB3608000,2022YFE0134600)the National Natural Science Foundation of China(Grant Nos.U1632266,11927807,U2032207,52272152)performed with the approval of the Proposal Assessing Committee of SiP·ME2 platform project(Proposal No.11227902)。
文摘Fe_(3)GaTe_(2),a recently discovered van der Waals ferromagnetic crystal with the highest Curie temperature and strong perpendicular magnetic anisotropy among two-dimensional(2D)magnetic materials,has attracted significant attention and makes it a promising candidate for next-generation spintronic applications.Compared with Fe_(3)GeTe_(2),which has the similar crystal structure,the mechanism of the enhanced ferromagnetic properties in Fe_(3)GaTe_(2)is still unclear and needs to be investigated.Here,by using x-ray magnetic circular dichroism measurements,we find that both Ga and Te atoms contribute to the total magnetic moment of the system with antiferromagnetic coupling to Fe atoms.Our first-principles calculations reveal that Fe_(3)GaTe_(2)has van Hove singularities at the Fermi level in nonmagnetic state,resulting in the magnetic instability of the system and susceptibility to magnetic phase transitions.In addition,the calculation results about the density of states in ferromagnetic states of two materials suggest that the exchange interaction between Fe atoms is strengthened by replacing Ge atoms with Ga atoms.These findings indicate the increase of both the itinerate and local moments in Fe_(3)GaTe_(2)in view of Stoner and exchange interaction models,which results in the enhancement of the overall magnetism and a higher Curie temperature.Our work provides insight into the underlying mechanism of Fe_(3)GaTe_(2)’s remarkable magnetic properties and has important implications for searching 2D materials with expected magnetic properties in the future.
基金supported by the National Key Research and Development Program of Ministry of Science and Technology of China(No.2021YFA1500604)ShanghaiTech University start-up funding.We would like to thank the Analytical Instrumentation Center(#SPST-AIC 10112914)at the School of Physical Science and Technology(SPST)+1 种基金ShanghaiTech University,for their generous support.We are grateful to Peihong Cheng at ShanghaiTech University for assisting with XPS measurements and Siyuan Du for assisting us in the XAS test at Shanghai Synchrotron Radiation Facility(SSRF)We appreciate the Centre for High-Resolution Electron Microscopy(CћEM),which is supported by SPST of ShanghaiTech University under contract No.EM02161943.
文摘The migration of protons during the oxygen evolution reaction(OER)is a key factor that affects the performance of OER catalysts.To enhance proton transportation,we designed a catalyst based on nickel/iron-pyromellitic acid(NiFe-PMA)prepared by the electrochemical deposition method.This catalyst exhibited a low overpotential of 188 mV at a current density of 10 mA·cm^(-2),a Tafel slope of 28.2 mV·dec^(-1),and long-term stability for 30 days with a current of 50 mA·cm^(-2).We characterized the NiFe-PMA catalyst using various techniques,including Fourier transform infrared(FTIR)spectroscopy,Raman spectroscopy,X-ray photoelectron spectroscopy(XPS),X-ray absorption spectroscopy(XAS),transmission electron microscopy(TEM),scanning electron microscopy(SEM),and inductively coupled plasma-optical emission spectrometry(ICP-OES).Our results showed that NiFe-PMA contains nickel,iron atoms,and both coordinated and uncoordinated carboxylate groups.Additionally,XPS data confirmed that carboxylate ligands could adjust the outer electronic structure of metal ions,resulting in the high valence state of Ni in NiFe-PMA.The result of XAS indicated that the nickel atoms present in the catalyst might be easier to maintain a higher chemical state.Further investigations using kinetic isotope effects(KIEs)and proton inventory revealed that the uncoordinated carboxylic protons played a crucial role in receiving protons during the OER,which promoted the proton transfer of the rate-determining step of the OER.Our novel electrocatalysts provide a new strategy for designing more active and cost-effective catalysts for the OER.
基金the Shanghai Soft X-ray Free-Electron Laser Facility beamline projectionfunded by the Major State Basic Research Development Program of China(No.2017YFA0504802)+1 种基金Strategic Priority Research Program of the Chinese Academy of Sciences(No.XDB 37040303)National Natural Science Foundation of China(No.21727817).
文摘The Shanghai soft X-ray free-electron laser(SXFEL)user facility project started in 2016 and is expected to be open to users by 2022.It aims to deliver ultra-intense coherent femtosecond X-ray pulses to five endstations covering a range of 100–620 eV for ultrafast X-ray science.Two undulator lines are designed and constructed,based on different lasing modes:self-amplified spontaneous emission and echo-enabled harmonic generation.The coherent scattering and imaging(CSI)endstation is the first of five endstations to be commissioned online.It focuses on high-resolution single-shot imaging and the study of ultrafast dynamic processes using coherent forward scattering techniques.Both the single-shot holograms and coherent diffraction patterns were recorded and reconstructed for nanoscale imaging,indicating the excellent coherence and high peak power of the SXFEL and the possibility of‘‘diffraction before destruction’’experiments at the CSI endstation.In this study,we report the first commissioning results of the CSI endstation.
基金supported by PhD research startup foundation of Civil Aviation University of China(Grant No.2020KYQD94)。
文摘Based on the first-principles method,we predict two new stable BN allotropes:C12-BN and O16-BN,which belong to cubic and orthorhombic crystal systems,respectively.It is confirmed that both the phases are thermally and dynamically stable.The results of molecular dynamics simulations suggest that both the BN phases are highly stable even at high temperatures of 1000 K.In the case of mechanical properties,C12-BN has a bulk modulus of 359 GPa and a hardness of 43.4 GPa,making it a novel superhard material with potential technological and industrial applications.Electronic band calculations reveal that both C12-BN and O16-BN are insulators with direct band gaps of 3.02 e V and 3.54 e V,respectively.The XRD spectra of C12-BN and O16-BN are also simulated to provide more information for possible experimental observation.Our findings enrich the BN allotrope family and are expected to stimulate further experimental interest.
基金Supported by the National Natural Science Foundation of China(Grant No.11574020)The experiment was performed at the PLEIADES beamline at the SOLEIL Synchrotron,France(Grant No.20130821)。
文摘Photoelectron diffraction is an effective tool to probe the structures of molecules.The higher the photoelectron kinetic energy is,the higher order the diffraction pattern is disclosed in.Up to date,either the multi-atomic molecule with the photoelectron kinetic energy below 150 e V or the diatomic molecule with 735 eV photoelectron has been experimentally reported.In this study,we measured the diffraction pattern of C 1 s and O 1 s photoelectrons in CO_(2)with 319.7 and 433.5 eV kinetic energies,respectively.The extracted C–O bond lengths are longer than the C–O bond length at the ground state,which is attributed to the asymmetric fragmentation that preferentially occurs at the longer chemical bond side during the zero-energy asymmetric vibration.
基金Project supported by the National Natural Science Foundation of China(Grant No.11574020)the Project of Thousand Youth Talents in Chinathe Starting Grant of ShanghaiTech University。
文摘We investigate the dissociation dynamics of core-excited O_(2)molecules using a high-resolution energy-resolved electron-ion coincidence experimental setup.The excited cationic states with two valence holes and one Rydberg electron are created after spectator Auger decay induced by O 1s→(^(4)Σ_(u)^(-))3sσcore excitation in O_(2).From the energy correlation between the kinetic energy of the Auger electron and the ion kinetic energy release,we distinguish several dissociation channels.Rather complex dissociation channels of the spectator Auger final states are disclosed,which can be explained by the increased number of the crossing point due to the existence of Rydberg electron.The quantum system will evolve into different dissociation limits at each crossing point between the potential energy curves.
基金supported by the National major scientific research instrument development project(No.11927805)National Natural Science Foundation of China Young Scientists Fund(No.12005134)+2 种基金Shanghai-XFEL Beamline Project(SBP)(No.31011505505885920161A2101001)Shanghai Municipal Science and Technology Major Project(No.2017SHZDZX02)Shanghai Pujiang Program(No.20PJ1410900).
文摘A transition edge sensor(TES)is extremely sensitive to changes in temperature,and combined with a high-Z metal of a certain thickness,it can realize high-energy resolution measurements of particles such as X-rays.X-rays with energies below 10 keV have a weak penetrating ability,hence,only gold or bismuth of a few micrometers in thickness can guarantee a quantum efficiency higher than 70%.Therefore,the entire structure of the TES X-ray detector in this energy range can be realized using a microfabrication process.However,for X-rays or γ-rays from 10 keV to 200 keV,submillimeter absorber layers are required,which cannot be realized using the microfabrication process.This paper first briefly introduces a set of TES X-ray detectors and their auxiliary systems,and then focuses on the introduction of the TES γ-ray detector with an absorber based on a submillimeter lead-tin alloy sphere.The detector achieved a quantum efficiency above 70% near 100 keV and an energy resolution of approximately 161.5 eV at 59.5 keV.
基金We are grateful to Jung Ki Song,Mo Deng,Baoliang Ge,William Harrod,Ed Cole,Zachary Levine,Bradley Alpert,Nina Weisse-Bernstein,Lee Oesterling,and Antonio Orozco for helpful discussions and comments.Funding from the Intelligence Advanced Research Projects Activity,Office of the Director of National Intelligence(IARPA-ODNI),contract FA8650-17-C-9113 is gratefully acknowledged.The MIT SuperCloud and Lincoln Laboratory Supercomputing Center provided resources(high performance computing,database,consultation)that have contributed to the research results reported within this paperI.Kang acknowledges support from Korea Foundation for Advanced Studies(KFAS).This research used resources of the Advanced Photon Source,a U.S.Department of Energy(DOE)Office of Science User Facility,operated for the DOE Office of Science by Argonne National Laboratory under Contract No.DE-AC02-06CH11357.The views and conclusions contained herein are those of the authors and should not be interpreted as necessarily representing the official policies or endorsements,either expressed or implied,of the ODNI,IARPA,or the US Government.
文摘Noninvasive X-ray imaging of nanoscale three-dimensional objects,such as integrated circuits(ICs),generally requires two types of scanning:ptychographic,which is translational and returns estimates of the complex electromagnetic field through the IC;combined with a tomographic scan,which collects these complex field projections from multiple angles.Here,we present Attentional Ptycho-Tomography(APT),an approach to drastically reduce the amount of angular scanning,and thus the total acquisition time.APT is machine learning-based,utilizing axial self-Attention for Ptycho-Tomographic reconstruction.APT is trained to obtain accurate reconstructions of the ICs,despite the incompleteness of the measurements.The training process includes regularizing priors in the form of typical patterns found in IC interiors,and the physics of X-ray propagation through the IC.We show that APT with×12 reduced angles achieves fidelity comparable to the gold standard Simultaneous Algebraic Reconstruction Technique(SART)with the original set of angles.When using the same set of reduced angles,then APT also outperforms Filtered Back Projection(FBP),Simultaneous Iterative Reconstruction Technique(SIRT)and SART.The time needed to compute the reconstruction is also reduced,because the trained neural network is a forward operation,unlike the iterative nature of these alternatives.Our experiments show that,without loss in quality,for a 4.48×93.2×3.92µm^(3) IC(≃6×10^(8) voxels),APT reduces the total data acquisition and computation time from 67.96 h to 38 min.We expect our physics-assisted and attention-utilizing machine learning framework to be applicable to other branches of nanoscale imaging,including materials science and biological imaging.
基金supported in part by the Ministry of Science and Technology (MOST) of China (No. 2018YFE0202700)the National Natural Science Foundation of China (Grants No.12004251,12104302,12104303)+3 种基金the Natural Science Foundation of Shanghai (Grant No.20ZR1436100)the Science and Technology Commission of Shanghai Municipality,the start-up funding from ShanghaiTech UniversityBeijing National Laboratory for Condensed Matter Physicsthe Interdisciplinary Program of Wuhan National High Magnetic Field Center (WHMFC202124)。
文摘The chemical stoichiometry on the surface of superconducting δ-NbN thin films is of great importance for their application.Here,we fabricated the δ-NbN thin films on SiO2/Si substrate by DC sputtering method.The film was characterized using X-ray diffraction(XRD) and atomic force microscopy(AFM).Transport properties were measured to reveal the field dependent superconducting transition temperature.Both XRD and electrical measurement show high crystallinity of δ-NbN phase.A homogeneous and smooth surface morphology was measured by AFM.Auger electron spectroscopy(AES) was applied to analyze the composition along the depth of the film.The evolution of Auger peak profile,heights and nitride stoichiometry at the film surface is discussed.The current study provides a more thorough understanding of complex chemical compositions of δ-NbN thin films.
基金support of the Joint Centre for Extreme Photonics.Funding:This work is supported by the start-up grant of ShanghaiTech University,Double First-Class Initiative Fund of ShanghaiTech University,Shanghai Rising-Star Program(22QA1406200)National Natural Science Foundation of China(12274297,92250303)+7 种基金Shanghai Science and Technology Program(21511105000)NSERC Discovery Grant program(RGPIN-327147-2012)by the U.S.Army Research Office through Award W911NF-14-1-0383Part of this research used Beamline 03U of the Shanghai Synchrotron Radiation Facilitysupported by the ME2 project under contract no.11227902the National Natural Science Foundation of China.Y.F.and C.J.are supported by the National Natural Science Foundation of China(12274230,91950102,and 11834004)Funding of NJUST(TSXK2022D005)H.X.is supported by the National Natural Science Foundation of China(12074063 and 12264003)。
文摘Ultrafast extreme ultraviolet (XUV) transient absorption spectroscopy measures the time- and frequencydependent light losses after light–matter interactions. In the linear region, the matter response to an XUV light field is usually determined by the complex refractive index ̃n. The absorption signal is directly related to the imaginary part of ̃n, namely, the absorption index. The real part of ̃n refers to the real refractive index, which describes the chromatic dispersion of an optical material. However, the real refractive index information is usually not available in conventional absorption experiments. Here, we investigate the refractive index line shape in ultrafast XUV transient absorption spectroscopy by using a scheme that the XUV pulse traverses the target gas jet off-center. The jet has a density gradient in the direction perpendicular to the gas injection direction, which induces deflection on the XUV radiation. Our experimental and theoretical results show that the shape of the frequency-dependent XUV deflection spectra reproduces the refractive index line profile. A typical dispersive refractive index line shape is measured for a single-peak absorption;an additional shoulder structure appears for a doublet absorption.Moreover, the refractive index line shape is controlled by introducing a later-arrived near-infrared pulse to modify the phase of the XUV free induction decay, resulting in different XUV deflection spectra. The results promote our understanding of matter-induced absorption and deflection in ultrafast XUV spectroscopy.
基金supported by the National Natural Science Foundation of China(NSFC)(No.11875203)。
文摘In this paper,a simple theoretical model combining Monte Carlo simulation with the enthalpy method is provided to simulate the damage resistance of B4C/Si-sub mirror under X-ray free-electron laser irradiation.Two different damage mechanisms are found,dependent on the photon energy.The optimum B4C film thickness is determined by studying the dependence of the damage resistance on the film thickness.Based on the optimized film thickness,the damage thresholds are simulated at photon energy of 0.4-25 keV and a grazing incidence angle of 2 mrad.It is recommended that the energy range around the Si K-edge should be avoided for safety reasons.
基金supported by the National Natural Science Foundation of China(Nos.U1804261,61627818,12074104,11804084,62075058,and 11827806)Natural Science Foundation of Henan Province(No.222300420057)+1 种基金the Outstanding Youth Foundation of Henan Normal University(No.20200171)the Young Backbone Teacher Training Program in Higher Education of Henan Province(No.2019GGJS065).
文摘Organic-inorganic layered perovskites are two-dimensional quantum well layers in which the layers of lead halide octahedra are stacked between the organic cation layers.The packing geometry of the soft organic molecules and the stiff ionic crystals induce structural deformation of the inorganic octahedra,generating complex lattice dynamics.Especially,the dielectric confinement and ionic sublattice lead to strong coupling between the photogenerated excitons and the phonons from the polar lattice which intensively affects the properties for device applications.The anharmonicity and dynamic disorder from the organic cations participate in the relaxation dynamics coupled with excitations.However,a detailed understanding of this underlying mechanism remains obscure.This work investigates the electron–optical phonon coupling dynamics by employing ultrafast pump-probe transient absorption spectroscopy.The activated different optical phonon modes are observed via systematic studies of(PEA)_(2)PbBr_(4) perovskite films on the ultrafast lattice vibrational dynamics.The experimental results indicate that solvent engineering has a significant influence on lattice vibrational modes and coherent phonon dynamics.This work provides fresh insights into electron-optical phonon coupling for emergent optoelectronics development based on layered perovskites.
基金supported by the National Natural Science Foundation of China(11974366)the Fundamental Research Funds for the Central Universities.
文摘We demonstrate via first-principle calculations based on the density functional theory that the magnetic moment of a helium atom under a given magnetic field has a positive correlation with the electric dipole moment when an external electric field is applied to the system.Our calculation shows that the enhancement of the magnetic moment is significant due to the reduction of the triplet-singlet splitting.We argue that this finding can be generalized to organic molecules,especially to macromolecules where the structure induced an electric dipole moment which may give rise to significantly enhanced responses to the external magnetic field.These results suggest that considerable magnetic responses prevail,particularly in bio-molecules without an inversion center.
