As an advanced 4^(th) generation synchrotron radiation facility,the Shenzhen Innovation Light-source Facility(SILF)storage ring is based on multi-bend achromat(MBA)lattices,enabling one to two orders of magnitude redu...As an advanced 4^(th) generation synchrotron radiation facility,the Shenzhen Innovation Light-source Facility(SILF)storage ring is based on multi-bend achromat(MBA)lattices,enabling one to two orders of magnitude reduction in beam emittance compared to the 3^(rd) generation storage ring.This significantly enhance the radiation brightness and coherence.The multipole magnets of many types for SILF storage ring are under preliminary design,which require high integral field homogeneity.As a result,a dedicated pole tip optimization procedure with high efficiency is developed for quadrupole and sextupole magnets with Opera-2D^(■)python script.The procedure considers also the 3D field effect which makes the optimization more straightforward.In this paper,the design of the quadrupole and sextupole magnets for SILF storage ring is first presented,followed by a detailed description of the implemented pole shape optimization method.展开更多
The partitioning of membrane proteins into lipid domains in cellular membranes is closely associated with the realization of the protein functions and it is influenced by various factors such as the post-translational...The partitioning of membrane proteins into lipid domains in cellular membranes is closely associated with the realization of the protein functions and it is influenced by various factors such as the post-translational modification of palmitoylation.However,the molecular mechanism of the effect of palmitoylation on membrane protein partitioning into the lipid domains remains elusive.In this work,taking human peripheral myelin protein 22(PMP22)as an example,we employ coarse-grained molecular dynamics simulations to investigate the partitioning of both the natural PMP22 and the palmitoylated PMP22(pal-PMP22)into the lipid domains of model myelin membranes.The results indicate that palmitoylation drives PMP22 to localize at the boundary of the liquid-ordered(Lo)and liquid-disordered(Ld)domains and increases the possibility of PMP22 partitioning into the Lo domains by changing the hydrophobic length of the proteins and perturbing the ordered packing of tails of the saturated lipids in the Lo domains.This work offers some novel insights into the role of palmitoylation in modulating the function of membrane proteins in cellular membranes.展开更多
Here,we report the spin-orbit state-resolved differential cross sections(DCSs)for the prototype barrierless reaction S(^(1)D)+HD.Both product channels,namely H+SD(^(2)Π_(3/2,1/2))and D+SH(^(2)Π_(3/2,1/2)),were measu...Here,we report the spin-orbit state-resolved differential cross sections(DCSs)for the prototype barrierless reaction S(^(1)D)+HD.Both product channels,namely H+SD(^(2)Π_(3/2,1/2))and D+SH(^(2)Π_(3/2,1/2)),were measured by high-resolution crossed molecular beam experiments.The DCSs of the two product channels show an overall forward-backward symmetry,in accordance with statistical model predictions.However,the DCSs for different spin-orbit manifolds show different preferences in forward or backward scattering directions at the same collision energies.This study reveals that,even though the title reaction proceeds via the long-lived complex mechanism,the spin-orbit coupling effects in the product channels play an important role in the reaction process.展开更多
Collision-induced re-laxation process of CH(X^(2)Π,v=0)radical in various bath gases He,Ar,and N_(2)has been investigated ex-perimentally under low-temperature(26-52 K)supersonic flow conditions.The CH radicals were ...Collision-induced re-laxation process of CH(X^(2)Π,v=0)radical in various bath gases He,Ar,and N_(2)has been investigated ex-perimentally under low-temperature(26-52 K)supersonic flow conditions.The CH radicals were generat-ed with internal excitation by multiphoton photolysis of CHBr_(3)at 248 nm,and its rotational temperature was found to relax to the flow temperature in a few microseconds by colliding with bath gas.The relaxation rate coefficients for CH(X^(2)Π,v=0)radical in He,Ar,and N_(2)flow were obtained by time-resolved laser-induced fluorescence measurements,ranging from 10^(-12)cm^(3)·molecule^(-1)·s^(-1)to 10^(-11)cm^(3)·molecule^(-1)·s^(-1).The N_(2)flow exhibits the highest relax-ation rate for CH(X^(2)Π)radical due to its additional rovibrational levels,which allow for more efficient energy dissipation during collisions compared to monoatomic gases.The Ar flow shows a larger relaxation rate than He flow due to its greater polarizability and stronger long-range interaction with the CH(X^(2)Π)radical.展开更多
Heterogeneous catalysis on solid surfaces provides high-value chemicals and is involved in a large fraction of the world’s economic productivity,yet our understanding of this important class of processes remains limi...Heterogeneous catalysis on solid surfaces provides high-value chemicals and is involved in a large fraction of the world’s economic productivity,yet our understanding of this important class of processes remains limited.Thermal reaction rates obtained from experiments on mod-el catalysts provide quantitative data that can reveal reaction mechanisms and provide benchmarks for computational simulations of catalytic processes.This perspective describes a critical advance in measuring these rates:velocity resolved kinetics(VRK).VRK delivers ab-solute rates for elementary surface reactions that are of sufficient accuracy that they may be meaningfully compared to theoretical rate predictions,creating a powerful synergy between theory and experiment.It is now routinely possible to derive fundamental thermochemical quantities,including desorption and adsorption energies,reaction barrier heights,diffusion barrier heights,and lateral adsorbate interaction energies.Reaction mechanisms can also be revealed and reaction intermediates directly detected.The high time resolution of VRK al-lows study of catalytic reactions at the high temperatures typical of conditions present in real catalytic reactors.Current work exploiting the newest and by far the most powerful variant of VRK has only scratched the surface of what is possible,signifying a promising future for re-searchers in this field.展开更多
We report high-resolution velocity map imaging studies of S(^(1)D)atoms formed following excitation on two intense absorption bands of gas phase D_(2)S molecules,centred at wave-lengths~139.1 and~129.1 nm.DS–D bond f...We report high-resolution velocity map imaging studies of S(^(1)D)atoms formed following excitation on two intense absorption bands of gas phase D_(2)S molecules,centred at wave-lengths~139.1 and~129.1 nm.DS–D bond fission is the dominant fragmentation pathway at these wavelengths,yielding SD fragments in both the ground(X)and excited(A)electronic states.Most S(^(1)D)atoms arising via 21A′21A′the rival S atom elimination channel when exciting at~139.1 nm are formed with D_(2)partners,in a wide range of rovibrational levels.The partially resolved structure in the total translational energy distributions,P(ET),derived from the S(^(1)D)atom images,implies two dynamical routes into S(^(1)D)+D_(2)products following non-adiabatic coupling from the photo-excited Rydberg state to the dissociative potential energy surface(PES).Similar D_(2)products are evident in the P(ET)spectra derived from analysis of S(^(1)D)images from D_(2)S photolysis at~129.1 nm,but their contribution is overshadowed by a feature attributable to three-body dissociation to S(^(1)D)+2D fragments.These atomic products are deemed to arise via a natural extension of the dynamics responsible for the previously observed highly rotationally excited SD(A)fragments arising via the rival S–D bond fission pathway:asymmetric bond extension together with a dramatic opening of the interbond angle driven by torques generated after coupling to the highly anisotropic 2^(1)A′PES,leading to a centripetally-driven break-up.展开更多
In this study we theoretically demonstrate ultrahigh-resolution two-dimensional atomic localization within a three-levelλ-type atomic medium via superposition of asymmetric and symmetric standing wave fields.Our anal...In this study we theoretically demonstrate ultrahigh-resolution two-dimensional atomic localization within a three-levelλ-type atomic medium via superposition of asymmetric and symmetric standing wave fields.Our analysis provides an understanding of the precise spatial localization of atomic positions at the atomic level,utilizing advanced theoretical approaches and principles of quantum mechanics.The dynamical behavior of a three-level atomic system is thoroughly analyzed using the density matrix formalism within the realm of quantum mechanics.A theoretical approach is constructed to describe the interaction between the system and external fields,specifically a control field and a probe field.The absorption spectrum of the probe field is thoroughly examined to clarify the spatial localization of the atom within the proposed configuration.A theoretical investigation found that symmetric and asymmetric superposition phenomena significantly influence the localized peaks within a two-dimensional spatial domain.Specifically,the emergence of one and two sharp localized peaks was observed within a one-wavelength domain.We observed notable influences of the intensity of the control field,probe field detuning and decay rates on atomic localization.Ultimately,we have achieved an unprecedented level of ultrahigh resolution and precision in localizing an atom within an area smaller thanλ/35×λ/35.These findings hold promise for potential applications in fields such as Bose-Einstein condensation,nanolithography,laser cooling,trapping of neutral atoms and the measurement of center-of-mass wave functions.展开更多
The development of an analytical method for determining the properties of quantum dots(QDs)is crucial for improving the optical performance of QD-based displays.Therefore,synchrotron-based X-ray photoelectron spectros...The development of an analytical method for determining the properties of quantum dots(QDs)is crucial for improving the optical performance of QD-based displays.Therefore,synchrotron-based X-ray photoelectron spectroscopy(XPS)is designed here to accurately characterize the chemical and structural differences between different QDs.This method enables the determination of the reason for the minimal differences between the optical properties of different QDs depending on the synthesis process,which is difficult to determine using conventional methods alone.Combined with model simulations,the XPS spectra obtained at different photon energies reveal the internal structures and chemical-state distributions of the QDs.In particular,the QD synthesized under optimal conditions demonstrates a relatively lower degree of oxidation of the core and more uniformly stacked ZnSe/ZnS shell layers.The internal structures and chemical-state distributions of QDs are closely related to their optical properties.Finally,the synchrotron-based XPS proposed here can be applied to compare nearly equivalent QDs with slightly different optical properties.展开更多
Anionic redox reaction(ARR)can provide extra capacity beyond transition metal(TM)redox in lithium-rich TM oxide cathodes.Practical ARR application is much hindered by the structure instability,particularly at the surf...Anionic redox reaction(ARR)can provide extra capacity beyond transition metal(TM)redox in lithium-rich TM oxide cathodes.Practical ARR application is much hindered by the structure instability,particularly at the surface.Oxygen release has been widely accepted as the ringleader of surficial structure instability.However,the role of TM in surface stability has been much overlooked,not to mention its interplay with oxygen release.Herein,TM dissolution and oxygen release are comparatively investigated in Li_(1.2)Ni_(0.2)Mn_(0.6)O_(2).Ni is verified to detach from the lattice counter-intuitively despite the overwhelming stoichiometry of Mn,facilitating subsequent oxygen release of the ARR process.Intriguingly,surface reorganization occurs following regulated Ni dissolution,enabling the stabilization of the surface and elimination of oxygen release in turn.Accordingly,a novel optimization strategy is proposed by adding a relaxation step at 4.50 V within the first cycle procedure.Battery performance can be effectively improved,with voltage decay suppressed from 3.44 mV/cycle to 1.60 mV/cycle,and cycle stability improved from 66.77%to 90.01%after 100 cycles.This work provides new perspectives for clarifying ARR surface instability and guidance for optimizing ARR performance.展开更多
Electron-positron colliders operating in the GeV center-of-mass range,or tau-charm energy region,have been proved to enable competitive frontier research due to several unique features.With the progress of high-energy...Electron-positron colliders operating in the GeV center-of-mass range,or tau-charm energy region,have been proved to enable competitive frontier research due to several unique features.With the progress of high-energy physics in the last two decades,a new-generation Tau-Charm factory,called the Super Tau-Charm Facility(STCF),has been actively promoted by the particle physics community in China.STCF has the potential to address fundamental questions such as the essence of color confinement and the matter-antimatter asymmetry within the next decades.The main design goals of the STCF are a center-of-mass energy ranging from 2 to 7 GeV and a luminosity surpassing 5×10^(34)cm^(−2)s^(−1)that is optimized at a center-of-mass energy of 4 GeV,which is approximately 50 times that of the currently operating Tau-Charm factory-BEPCII.The STCF accelerator has two main parts:a double-ring collider with a crab-waist collision scheme and an injector that provides top-up injections for both electron and positron beams.As a typical third-generation electron-positron circular collider,the STCF accelerator faces many challenges in both accelerator physics and technology.In this paper,the conceptual design of the STCF accelerator complex is presented,including the ongoing efforts and plans for technological research and develop-ment,as well as the required infrastructure.The STCF project aims to secure support from the Chinese central government for its construction during the 15th Five-Year Plan(2026-2030).展开更多
The polysulfides shuttle effect represents a great challenge in achieving high capacity and long lifespan of lithium/sulfur(Li/S)cells.A comprehensive understanding of the shuttle-related sulfur speciation and diffusi...The polysulfides shuttle effect represents a great challenge in achieving high capacity and long lifespan of lithium/sulfur(Li/S)cells.A comprehensive understanding of the shuttle-related sulfur speciation and diffusion process is vital for addressing this issue.Herein,we employed in situ/operando X-ray absorption spectroscopy(XAS)to trace the migration of polysulfides across the Li/S cells by precisely monitoring the sulfur chemical speciation at the cathodic electrolyte-separator and electrolyte-anode interfaces,respectively,in a real-time condition.After we adopted a shuttle-suppressing strategy by introducing an electrocatalytic layer of twinborn bismuth sulfide/bismuth oxide nanoclusters in a carbon matrix(BSOC),we found the Li/S cell showed greatly improved sulfur utilization and longer life span.The operando S Kedge XAS results revealed that the BSOC modification was bi-functional:trapping polysulfides and catalyzing conversion of sulfur species simultaneously.We elucidated that the polysulfide trapping-and-catalyzing effect of the BSOC electrocatalytic layer resulted in an effective lithium anode protection.Our results could offer potential stratagem for designing more advanced Li/S cells.展开更多
Here we demonstrate a theory-driven, novel dual-shell coating system of Li_(2)SrSiO_(4) and Al_(2)O_(3), achieved via a facile and scalable sol-gel technique on LiCoO_(2) electrode particles. The optimal thickness of ...Here we demonstrate a theory-driven, novel dual-shell coating system of Li_(2)SrSiO_(4) and Al_(2)O_(3), achieved via a facile and scalable sol-gel technique on LiCoO_(2) electrode particles. The optimal thickness of each coating can lead to increased specific capacity(~185 m Ah/g at 0.5 C-rate) at a cut-off potential of 4.5 V, and greater cycling stability at very high C rates(up to 10 C) in half-cells with lithium metal. The mechanism of this superior performance was investigated using a combination of X-ray and electron characterization methods. It shows that the results of this investigation can inform future studies to identify still better dual-shell coating schemes, achieved by such industrially feasible techniques, for application on similar, nickel-rich cathode materials.展开更多
A hard/soft SmCo5/ Fe nanocomposite magnetic bilayer system is fabricated on x-ray transparent 100-200 nm thin SiaN4 films by magnetron sputtering. The microscopic magnetic domain pattern and its behaviours during mag...A hard/soft SmCo5/ Fe nanocomposite magnetic bilayer system is fabricated on x-ray transparent 100-200 nm thin SiaN4 films by magnetron sputtering. The microscopic magnetic domain pattern and its behaviours during magnetization reversal in the hard and the soft magnetic phases are studied separately by element specific magnetic soft x-ray microscopy at a spatial resolution of better than 25 Nm. We observe that the domain patterns for the soft and hard phases show coherent behaviours in varying magnetic fields. We derive local M（H） curves from the images of Fe and SmCo5 separately and find the switches for hard and soft phases to be the same.展开更多
Fast charging and high-power delivering batteries are highly demanded in mobile electronics,electric vehicles and grid energy storage,but there are full of challenges.The star-material Li_(3)V_(2)(PO_(4))_(3) is demon...Fast charging and high-power delivering batteries are highly demanded in mobile electronics,electric vehicles and grid energy storage,but there are full of challenges.The star-material Li_(3)V_(2)(PO_(4))_(3) is demonstrated as a promising high-rate cathode material meeting the above requirements.Herein,we report the carbon decorated Li_(3)V_(2)(PO_(4))_(3) (LVP/C) cathode prepared via a facile method,which displays a remarkable high-rate capability and long-term cycling performance.Briefly,the prepared LVP/C delivers a high discharge capacity of 122 mAh g^(-1)(-93% of the theoretical capacity) at a high rate up to 20 C and a superior capacity retention of 87.1% after 1000 cycles.Importantly,by applying a combination of X-ray absorption spectroscopy and full-range mapping of resonant inelastic X-ray scattering,we clearly elucidate the structural and chemical evolutions of LVP upon various potentials and cycle numbers.We show unambiguous spectroscopic evidences that the evolution of the hybridization strength between V and O in LVP/C as a consequence of lithiation/delithiation is highly reversible both in the bulk and on the surface during the discharge-charge processes even over extended cycles,which should be responsible for the remarkable electrochemical performance of LVP/C.Our present study provides not only an effective synthesis strategy but also deeper insights into the surface and bulk electrochemical reaction mechanism of LVP,which should be beneficial for the further design of high-performance LVP electrode materials.展开更多
MgAl-LDH（layered double hydroxides） were prepared with CO（NH2）2, NH4 Cl and NH3·H2O by the coprecipitation method, respectively. Corresponding composite membranes were prepared by the coating method. LDHs wer...MgAl-LDH（layered double hydroxides） were prepared with CO（NH2）2, NH4 Cl and NH3·H2O by the coprecipitation method, respectively. Corresponding composite membranes were prepared by the coating method. LDHs were characterized by WAXS, CO2-TPD and SEM. The morphology of the PVC/LDHs composite membranes were characterized by means of SEM. The thermal stability of the membranes was analyzed by air aging box and TGA-FTIR. The SEM results show that nano-particles can be compatible with poly（vinyl chloride）（PVC） matrix homogeneously by the stirring-ultrasound blend method with two steps. Furthermore, the air aging box results proved that MgAl-CO（NH2）2-LDH has the best effect on thermal stability of PVC. TGA-FTIR results show that MgAl-CO（NH2）2-LDH could adsorb more HCl that resulted from the degradation of PVC and improve the pyrolysis temperature of the first degradation stage by 15 K compared with PVC.展开更多
A new photon-in/photon-out endstation at beamline 02B02 of the Shanghai Synchrotron Radiation Facility for studying the electronic structure of energy materials has been constructed and fully opened to users.The endst...A new photon-in/photon-out endstation at beamline 02B02 of the Shanghai Synchrotron Radiation Facility for studying the electronic structure of energy materials has been constructed and fully opened to users.The endstation has the capability to perform soft x-ray absorption spectroscopy in total electron yield and total fluorescence yield modes simultaneously.The photon energy ranges from 40 eV to 2000 eV covering the K-edge of most low Z-elements and the L-edge of 3d transition-metals.The new self-designed channeltron detector allows us to achieve good fluorescence signals at the low photon flux.In addition,we synchronously collect the signals of a standard reference sample and a gold mesh on the upstream to calibrate the photon energy and monitor the beam fluctuation,respectively.In order to cross the pressure gap,in situ gas and liquid cells for soft x-ray absorption spectroscopy are developed to study the samples under realistic working conditions.展开更多
Precisely quantifying transition metal(TM) redox in bulk is a key to understand the fundamental of optimizing cathode materials in secondary batteries. At present, the commonly used methods to probe TM redox are hard ...Precisely quantifying transition metal(TM) redox in bulk is a key to understand the fundamental of optimizing cathode materials in secondary batteries. At present, the commonly used methods to probe TM redox are hard X-ray absorption spectroscopy(hXAS) and soft X-ray absorption spectroscopy(sXAS).However, they are both facing challenges to precisely quantify the valence states of some transition metals such as Mn. In this paper, Mn-L iPFY(inverse partial fluorescence yield) spectra extracted from Mn-L m RIXS(mapping of resonant inelastic X-ray scattering) is adopted to quantify Mn valence states. Mn-L i PFY spectra has been considered as a bulk-sensitive, non-distorted probe of TM valence states.However, the exact precision of this method is still unclear in quantifying practical battery electrodes.Herein, a series of LiMn_(2)O_(4) electrodes with different charge and discharge states are prepared. Based on their electrochemical capacity(generally considered to be very precise), the precision of Mn iPFY in quantifying bulk Mn valence state is confirmed, and the error range is unraveled. Mn-L mRIXS iPFY thus is identified as one of the best methods to quantify the bulk Mn valence state comparing with hXAS and sXAS.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 measure...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
Poor bone quality is a major factor in skeletal fragility in elderly individuals.The molecular mechanisms that establish and maintain bone quality,independent of bone mass,are unknown but are thought to be primarily d...Poor bone quality is a major factor in skeletal fragility in elderly individuals.The molecular mechanisms that establish and maintain bone quality,independent of bone mass,are unknown but are thought to be primarily determined by osteocytes.We hypothesize that the age-related decline in bone quality results from the suppression of osteocyte perilacunar/canalicular remodeling(PLR),which maintains bone material properties.We examined bones from young and aged mice with osteocyte-intrinsic repression of TGFβsignaling(TβRII^(ocy−/−))that suppresses PLR.The control aged bone displayed decreased TGFβsignaling and PLR,but aging did not worsen the existing PLR suppression in male TβRII^(ocy−/−)bone.This relationship impacted the behavior of collagen material at the nanoscale and tissue scale in macromechanical tests.The effects of age on bone mass,density,and mineral material behavior were independent of osteocytic TGFβ.We determined that the decline in bone quality with age arises from the loss of osteocyte function and the loss of TGFβ-dependent maintenance of collagen integrity.展开更多
文摘As an advanced 4^(th) generation synchrotron radiation facility,the Shenzhen Innovation Light-source Facility(SILF)storage ring is based on multi-bend achromat(MBA)lattices,enabling one to two orders of magnitude reduction in beam emittance compared to the 3^(rd) generation storage ring.This significantly enhance the radiation brightness and coherence.The multipole magnets of many types for SILF storage ring are under preliminary design,which require high integral field homogeneity.As a result,a dedicated pole tip optimization procedure with high efficiency is developed for quadrupole and sextupole magnets with Opera-2D^(■)python script.The procedure considers also the 3D field effect which makes the optimization more straightforward.In this paper,the design of the quadrupole and sextupole magnets for SILF storage ring is first presented,followed by a detailed description of the implemented pole shape optimization method.
基金supported by Zhejiang Provincial Natural Science Foundation of China(Grant No.LZ25A040005)the National Natural Science Foundation of China(Grant No.11674287).
文摘The partitioning of membrane proteins into lipid domains in cellular membranes is closely associated with the realization of the protein functions and it is influenced by various factors such as the post-translational modification of palmitoylation.However,the molecular mechanism of the effect of palmitoylation on membrane protein partitioning into the lipid domains remains elusive.In this work,taking human peripheral myelin protein 22(PMP22)as an example,we employ coarse-grained molecular dynamics simulations to investigate the partitioning of both the natural PMP22 and the palmitoylated PMP22(pal-PMP22)into the lipid domains of model myelin membranes.The results indicate that palmitoylation drives PMP22 to localize at the boundary of the liquid-ordered(Lo)and liquid-disordered(Ld)domains and increases the possibility of PMP22 partitioning into the Lo domains by changing the hydrophobic length of the proteins and perturbing the ordered packing of tails of the saturated lipids in the Lo domains.This work offers some novel insights into the role of palmitoylation in modulating the function of membrane proteins in cellular membranes.
基金supported by the National Natural Science Foundation of China(Nos.92476207,22288201)the Chinese Academy of Sciences(No.XBD0970202)+2 种基金the Innovation Program for Quantum Science and Technology(No.2021ZD0303300)the Shenzhen Science and Technology Innovation Committee(No.20220814164755002)the Guangdong Innovative&Entrepreneurial Research Team Program(Nos.2019ZT08L455,2019JC01X091).
文摘Here,we report the spin-orbit state-resolved differential cross sections(DCSs)for the prototype barrierless reaction S(^(1)D)+HD.Both product channels,namely H+SD(^(2)Π_(3/2,1/2))and D+SH(^(2)Π_(3/2,1/2)),were measured by high-resolution crossed molecular beam experiments.The DCSs of the two product channels show an overall forward-backward symmetry,in accordance with statistical model predictions.However,the DCSs for different spin-orbit manifolds show different preferences in forward or backward scattering directions at the same collision energies.This study reveals that,even though the title reaction proceeds via the long-lived complex mechanism,the spin-orbit coupling effects in the product channels play an important role in the reaction process.
基金supported by the National Natural Science Foundation of China(No.22273103)the National Natural Science Foundation of China(NSFC Center for Chemical Dynamics)(No.22288201)+1 种基金Dalian Institute of Chemical Physics(DICP I202230)the Scientific Instrument Developing Project of the Chinese Academy of Sciences(grant GJJSTD20220001)。
文摘Collision-induced re-laxation process of CH(X^(2)Π,v=0)radical in various bath gases He,Ar,and N_(2)has been investigated ex-perimentally under low-temperature(26-52 K)supersonic flow conditions.The CH radicals were generat-ed with internal excitation by multiphoton photolysis of CHBr_(3)at 248 nm,and its rotational temperature was found to relax to the flow temperature in a few microseconds by colliding with bath gas.The relaxation rate coefficients for CH(X^(2)Π,v=0)radical in He,Ar,and N_(2)flow were obtained by time-resolved laser-induced fluorescence measurements,ranging from 10^(-12)cm^(3)·molecule^(-1)·s^(-1)to 10^(-11)cm^(3)·molecule^(-1)·s^(-1).The N_(2)flow exhibits the highest relax-ation rate for CH(X^(2)Π)radical due to its additional rovibrational levels,which allow for more efficient energy dissipation during collisions compared to monoatomic gases.The Ar flow shows a larger relaxation rate than He flow due to its greater polarizability and stronger long-range interaction with the CH(X^(2)Π)radical.
基金support from the Alexander von Humboldt foundationsupport from the National Natural Science Foundation of China(No.22473077)+2 种基金support from the BENCh graduate school,funded by the Deutsche Forschungsgemeinschaft(DFG,German Research Foundation)389479699/GRK2455support from the European Research Council(ERC)under the European Union’s Horizon 2020 research and innovation programme grant agreement No.[833404]support from CRC 1633 Proton Coupled Electron Transfer,Project C02。
文摘Heterogeneous catalysis on solid surfaces provides high-value chemicals and is involved in a large fraction of the world’s economic productivity,yet our understanding of this important class of processes remains limited.Thermal reaction rates obtained from experiments on mod-el catalysts provide quantitative data that can reveal reaction mechanisms and provide benchmarks for computational simulations of catalytic processes.This perspective describes a critical advance in measuring these rates:velocity resolved kinetics(VRK).VRK delivers ab-solute rates for elementary surface reactions that are of sufficient accuracy that they may be meaningfully compared to theoretical rate predictions,creating a powerful synergy between theory and experiment.It is now routinely possible to derive fundamental thermochemical quantities,including desorption and adsorption energies,reaction barrier heights,diffusion barrier heights,and lateral adsorbate interaction energies.Reaction mechanisms can also be revealed and reaction intermediates directly detected.The high time resolution of VRK al-lows study of catalytic reactions at the high temperatures typical of conditions present in real catalytic reactors.Current work exploiting the newest and by far the most powerful variant of VRK has only scratched the surface of what is possible,signifying a promising future for re-searchers in this field.
基金supported by the National Natural Science Foundation of China(Nos.22241304,22225303,22403091,22173100)the Major Program of the National Natural Science Foundation of China(Nos.42494850 and 42494853)+5 种基金the National Natural Science Foundation of China(NSFC Center for Chemical Dynamics(No.22288201))the Strategic Priority Research Program of the Chinese Academy of Sciences(Nos.XDB0970000 and XDB0970200)the Innovation Program for Quantum Science and Technology(No.2021ZD0303304)the Liaoning Revitalization Talents Program(No.XLYC2402046)the Shenzhen Science and Technology Program(No.ZDSYS20200421111001787)Zhenxing Li thanks the Guangdong Science and Technology Program(No.2025A1515012671)。
文摘We report high-resolution velocity map imaging studies of S(^(1)D)atoms formed following excitation on two intense absorption bands of gas phase D_(2)S molecules,centred at wave-lengths~139.1 and~129.1 nm.DS–D bond fission is the dominant fragmentation pathway at these wavelengths,yielding SD fragments in both the ground(X)and excited(A)electronic states.Most S(^(1)D)atoms arising via 21A′21A′the rival S atom elimination channel when exciting at~139.1 nm are formed with D_(2)partners,in a wide range of rovibrational levels.The partially resolved structure in the total translational energy distributions,P(ET),derived from the S(^(1)D)atom images,implies two dynamical routes into S(^(1)D)+D_(2)products following non-adiabatic coupling from the photo-excited Rydberg state to the dissociative potential energy surface(PES).Similar D_(2)products are evident in the P(ET)spectra derived from analysis of S(^(1)D)images from D_(2)S photolysis at~129.1 nm,but their contribution is overshadowed by a feature attributable to three-body dissociation to S(^(1)D)+2D fragments.These atomic products are deemed to arise via a natural extension of the dynamics responsible for the previously observed highly rotationally excited SD(A)fragments arising via the rival S–D bond fission pathway:asymmetric bond extension together with a dramatic opening of the interbond angle driven by torques generated after coupling to the highly anisotropic 2^(1)A′PES,leading to a centripetally-driven break-up.
文摘In this study we theoretically demonstrate ultrahigh-resolution two-dimensional atomic localization within a three-levelλ-type atomic medium via superposition of asymmetric and symmetric standing wave fields.Our analysis provides an understanding of the precise spatial localization of atomic positions at the atomic level,utilizing advanced theoretical approaches and principles of quantum mechanics.The dynamical behavior of a three-level atomic system is thoroughly analyzed using the density matrix formalism within the realm of quantum mechanics.A theoretical approach is constructed to describe the interaction between the system and external fields,specifically a control field and a probe field.The absorption spectrum of the probe field is thoroughly examined to clarify the spatial localization of the atom within the proposed configuration.A theoretical investigation found that symmetric and asymmetric superposition phenomena significantly influence the localized peaks within a two-dimensional spatial domain.Specifically,the emergence of one and two sharp localized peaks was observed within a one-wavelength domain.We observed notable influences of the intensity of the control field,probe field detuning and decay rates on atomic localization.Ultimately,we have achieved an unprecedented level of ultrahigh resolution and precision in localizing an atom within an area smaller thanλ/35×λ/35.These findings hold promise for potential applications in fields such as Bose-Einstein condensation,nanolithography,laser cooling,trapping of neutral atoms and the measurement of center-of-mass wave functions.
基金Advanced Light Source,which is a DOE Office of Science User Facility under contract no.DE-AC02-05CH11231the Basque Government for funding through a PhD Fellowship(Grant no.PRE_2018_2_0285)+1 种基金through Egonlabur Travel Fellowship(Grant no.EP_2018_1_0004)partially supported by an Early Career Award in the Condensed Phase and Interfacial Molecular Science Program,in the Chemical Sciences Geosciences and Biosciences Division of the Office of Basic Energy Sciences of the U.S.Department of Energy under Contract No.DE-AC02-05CH11231.
文摘The development of an analytical method for determining the properties of quantum dots(QDs)is crucial for improving the optical performance of QD-based displays.Therefore,synchrotron-based X-ray photoelectron spectroscopy(XPS)is designed here to accurately characterize the chemical and structural differences between different QDs.This method enables the determination of the reason for the minimal differences between the optical properties of different QDs depending on the synthesis process,which is difficult to determine using conventional methods alone.Combined with model simulations,the XPS spectra obtained at different photon energies reveal the internal structures and chemical-state distributions of the QDs.In particular,the QD synthesized under optimal conditions demonstrates a relatively lower degree of oxidation of the core and more uniformly stacked ZnSe/ZnS shell layers.The internal structures and chemical-state distributions of QDs are closely related to their optical properties.Finally,the synchrotron-based XPS proposed here can be applied to compare nearly equivalent QDs with slightly different optical properties.
基金supported by the National Key Research and Development Program (2019YFA0405601)National Science Foundation of China(No. 22309097, 22179066, 21902179)+1 种基金Shandong Provincial Natural Science Foundation (2023KJ228, ZR2021QE061, ZR202103010205)the Startup Foundation for Advanced Talents in Qingdao University (DC2000005106)
文摘Anionic redox reaction(ARR)can provide extra capacity beyond transition metal(TM)redox in lithium-rich TM oxide cathodes.Practical ARR application is much hindered by the structure instability,particularly at the surface.Oxygen release has been widely accepted as the ringleader of surficial structure instability.However,the role of TM in surface stability has been much overlooked,not to mention its interplay with oxygen release.Herein,TM dissolution and oxygen release are comparatively investigated in Li_(1.2)Ni_(0.2)Mn_(0.6)O_(2).Ni is verified to detach from the lattice counter-intuitively despite the overwhelming stoichiometry of Mn,facilitating subsequent oxygen release of the ARR process.Intriguingly,surface reorganization occurs following regulated Ni dissolution,enabling the stabilization of the surface and elimination of oxygen release in turn.Accordingly,a novel optimization strategy is proposed by adding a relaxation step at 4.50 V within the first cycle procedure.Battery performance can be effectively improved,with voltage decay suppressed from 3.44 mV/cycle to 1.60 mV/cycle,and cycle stability improved from 66.77%to 90.01%after 100 cycles.This work provides new perspectives for clarifying ARR surface instability and guidance for optimizing ARR performance.
基金supported by the National Key Research and Development Program of China(No.2022YFA1602200)the National Natural Science Foundation of China(Nos.12341501 and 12405174)the Hefei Comprehensive National Science Center for the strong support on the STCF key technology research project.
文摘Electron-positron colliders operating in the GeV center-of-mass range,or tau-charm energy region,have been proved to enable competitive frontier research due to several unique features.With the progress of high-energy physics in the last two decades,a new-generation Tau-Charm factory,called the Super Tau-Charm Facility(STCF),has been actively promoted by the particle physics community in China.STCF has the potential to address fundamental questions such as the essence of color confinement and the matter-antimatter asymmetry within the next decades.The main design goals of the STCF are a center-of-mass energy ranging from 2 to 7 GeV and a luminosity surpassing 5×10^(34)cm^(−2)s^(−1)that is optimized at a center-of-mass energy of 4 GeV,which is approximately 50 times that of the currently operating Tau-Charm factory-BEPCII.The STCF accelerator has two main parts:a double-ring collider with a crab-waist collision scheme and an injector that provides top-up injections for both electron and positron beams.As a typical third-generation electron-positron circular collider,the STCF accelerator faces many challenges in both accelerator physics and technology.In this paper,the conceptual design of the STCF accelerator complex is presented,including the ongoing efforts and plans for technological research and develop-ment,as well as the required infrastructure.The STCF project aims to secure support from the Chinese central government for its construction during the 15th Five-Year Plan(2026-2030).
基金financially supported by the National Key R&D Program of China(2016YFB0100100)the National Natural Science Foundation of China(Nos.21433013,U1832218)the support from China Scholarship Council
文摘The polysulfides shuttle effect represents a great challenge in achieving high capacity and long lifespan of lithium/sulfur(Li/S)cells.A comprehensive understanding of the shuttle-related sulfur speciation and diffusion process is vital for addressing this issue.Herein,we employed in situ/operando X-ray absorption spectroscopy(XAS)to trace the migration of polysulfides across the Li/S cells by precisely monitoring the sulfur chemical speciation at the cathodic electrolyte-separator and electrolyte-anode interfaces,respectively,in a real-time condition.After we adopted a shuttle-suppressing strategy by introducing an electrocatalytic layer of twinborn bismuth sulfide/bismuth oxide nanoclusters in a carbon matrix(BSOC),we found the Li/S cell showed greatly improved sulfur utilization and longer life span.The operando S Kedge XAS results revealed that the BSOC modification was bi-functional:trapping polysulfides and catalyzing conversion of sulfur species simultaneously.We elucidated that the polysulfide trapping-and-catalyzing effect of the BSOC electrocatalytic layer resulted in an effective lithium anode protection.Our results could offer potential stratagem for designing more advanced Li/S cells.
基金supported by the U.S. National Science Foundation (CBET-1949870, CBET-2016192, and DMR-1832803)Part of the research was conducted at the Northwest Nanotechnology Infrastructure, a National Nanotechnology Coordinated Infrastructure (NNCI) site at Oregon State University, which is supported, in part, by the U.S. National Science Foundation (NNCI-1542101 and NCC-2025489), and Oregon State University。
文摘Here we demonstrate a theory-driven, novel dual-shell coating system of Li_(2)SrSiO_(4) and Al_(2)O_(3), achieved via a facile and scalable sol-gel technique on LiCoO_(2) electrode particles. The optimal thickness of each coating can lead to increased specific capacity(~185 m Ah/g at 0.5 C-rate) at a cut-off potential of 4.5 V, and greater cycling stability at very high C rates(up to 10 C) in half-cells with lithium metal. The mechanism of this superior performance was investigated using a combination of X-ray and electron characterization methods. It shows that the results of this investigation can inform future studies to identify still better dual-shell coating schemes, achieved by such industrially feasible techniques, for application on similar, nickel-rich cathode materials.
基金Project supported by the Higher Education Commission of Pakistan under International Research Support Initiative Program and partially supported by BES/DOE funding
文摘A hard/soft SmCo5/ Fe nanocomposite magnetic bilayer system is fabricated on x-ray transparent 100-200 nm thin SiaN4 films by magnetron sputtering. The microscopic magnetic domain pattern and its behaviours during magnetization reversal in the hard and the soft magnetic phases are studied separately by element specific magnetic soft x-ray microscopy at a spatial resolution of better than 25 Nm. We observe that the domain patterns for the soft and hard phases show coherent behaviours in varying magnetic fields. We derive local M（H） curves from the images of Fe and SmCo5 separately and find the switches for hard and soft phases to be the same.
基金supported by Collaborative Innovation Center of Suzhou Nano Science & Technologythe Priority Academic Program Development of Jiangsu Higher Education Institutions (PAPD)+5 种基金the 111 roject, Joint International Research Laboratory of Carbon-Based Functional Materials and Devicesthe National Natural Science Foundation of China (11905154)the Natural Science Foundation of the Jiangsu Higher Education Institutions of China (19KJA550004)the Natural Science Foundation of Jiangsu Province (BK20190814)the National Key R&D Program of China (No. 2016YFA0202600)supported by the Director, Office of Science, Office of Basic Energy Sciences, of the U.S. Department of Energy under Contract No. DE-AC02-05CH11231。
文摘Fast charging and high-power delivering batteries are highly demanded in mobile electronics,electric vehicles and grid energy storage,but there are full of challenges.The star-material Li_(3)V_(2)(PO_(4))_(3) is demonstrated as a promising high-rate cathode material meeting the above requirements.Herein,we report the carbon decorated Li_(3)V_(2)(PO_(4))_(3) (LVP/C) cathode prepared via a facile method,which displays a remarkable high-rate capability and long-term cycling performance.Briefly,the prepared LVP/C delivers a high discharge capacity of 122 mAh g^(-1)(-93% of the theoretical capacity) at a high rate up to 20 C and a superior capacity retention of 87.1% after 1000 cycles.Importantly,by applying a combination of X-ray absorption spectroscopy and full-range mapping of resonant inelastic X-ray scattering,we clearly elucidate the structural and chemical evolutions of LVP upon various potentials and cycle numbers.We show unambiguous spectroscopic evidences that the evolution of the hybridization strength between V and O in LVP/C as a consequence of lithiation/delithiation is highly reversible both in the bulk and on the surface during the discharge-charge processes even over extended cycles,which should be responsible for the remarkable electrochemical performance of LVP/C.Our present study provides not only an effective synthesis strategy but also deeper insights into the surface and bulk electrochemical reaction mechanism of LVP,which should be beneficial for the further design of high-performance LVP electrode materials.
基金supported by the Shanghai Municipal Education Commission with“Twelfth Five”scientific connotation construction project(No.nhky-2012-05)foreign visiting scholar fellowship program(No.B-8938-12-0406)Opening Project of Shanghai Key Laboratory of Multiphase Flow and Heat Transfer in Power Engineering
文摘MgAl-LDH（layered double hydroxides） were prepared with CO（NH2）2, NH4 Cl and NH3·H2O by the coprecipitation method, respectively. Corresponding composite membranes were prepared by the coating method. LDHs were characterized by WAXS, CO2-TPD and SEM. The morphology of the PVC/LDHs composite membranes were characterized by means of SEM. The thermal stability of the membranes was analyzed by air aging box and TGA-FTIR. The SEM results show that nano-particles can be compatible with poly（vinyl chloride）（PVC） matrix homogeneously by the stirring-ultrasound blend method with two steps. Furthermore, the air aging box results proved that MgAl-CO（NH2）2-LDH has the best effect on thermal stability of PVC. TGA-FTIR results show that MgAl-CO（NH2）2-LDH could adsorb more HCl that resulted from the degradation of PVC and improve the pyrolysis temperature of the first degradation stage by 15 K compared with PVC.
基金Project supported by the National Natural Science Foundation of China(Grant No.11227902)as part of NSFC ME2 beamline project,Science and Technology Commission of Shanghai Municipality,China(Grant No.14520722100)the National Natural Science Foundation of China(Grant Nos.11905283 and U1632269)
文摘A new photon-in/photon-out endstation at beamline 02B02 of the Shanghai Synchrotron Radiation Facility for studying the electronic structure of energy materials has been constructed and fully opened to users.The endstation has the capability to perform soft x-ray absorption spectroscopy in total electron yield and total fluorescence yield modes simultaneously.The photon energy ranges from 40 eV to 2000 eV covering the K-edge of most low Z-elements and the L-edge of 3d transition-metals.The new self-designed channeltron detector allows us to achieve good fluorescence signals at the low photon flux.In addition,we synchronously collect the signals of a standard reference sample and a gold mesh on the upstream to calibrate the photon energy and monitor the beam fluctuation,respectively.In order to cross the pressure gap,in situ gas and liquid cells for soft x-ray absorption spectroscopy are developed to study the samples under realistic working conditions.
基金the support from the key research and development and promotion of special projects (scientific and technological research) of Henan province (212102210188)the National Natural Science Foundation of China (51604244)the Energy Storage Materials and Processes Key Laboratory of Henan Province Open Fund (2021003)。
文摘Precisely quantifying transition metal(TM) redox in bulk is a key to understand the fundamental of optimizing cathode materials in secondary batteries. At present, the commonly used methods to probe TM redox are hard X-ray absorption spectroscopy(hXAS) and soft X-ray absorption spectroscopy(sXAS).However, they are both facing challenges to precisely quantify the valence states of some transition metals such as Mn. In this paper, Mn-L iPFY(inverse partial fluorescence yield) spectra extracted from Mn-L m RIXS(mapping of resonant inelastic X-ray scattering) is adopted to quantify Mn valence states. Mn-L i PFY spectra has been considered as a bulk-sensitive, non-distorted probe of TM valence states.However, the exact precision of this method is still unclear in quantifying practical battery electrodes.Herein, a series of LiMn_(2)O_(4) electrodes with different charge and discharge states are prepared. Based on their electrochemical capacity(generally considered to be very precise), the precision of Mn iPFY in quantifying bulk Mn valence state is confirmed, and the error range is unraveled. Mn-L mRIXS iPFY thus is identified as one of the best methods to quantify the bulk Mn valence state comparing with hXAS and sXAS.
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.
文摘Poor bone quality is a major factor in skeletal fragility in elderly individuals.The molecular mechanisms that establish and maintain bone quality,independent of bone mass,are unknown but are thought to be primarily determined by osteocytes.We hypothesize that the age-related decline in bone quality results from the suppression of osteocyte perilacunar/canalicular remodeling(PLR),which maintains bone material properties.We examined bones from young and aged mice with osteocyte-intrinsic repression of TGFβsignaling(TβRII^(ocy−/−))that suppresses PLR.The control aged bone displayed decreased TGFβsignaling and PLR,but aging did not worsen the existing PLR suppression in male TβRII^(ocy−/−)bone.This relationship impacted the behavior of collagen material at the nanoscale and tissue scale in macromechanical tests.The effects of age on bone mass,density,and mineral material behavior were independent of osteocytic TGFβ.We determined that the decline in bone quality with age arises from the loss of osteocyte function and the loss of TGFβ-dependent maintenance of collagen integrity.
