In studying interactions between intense laser fields and atoms or molecules,the role of electron correlation effects on the dynamical response is an important and pressing issue to address.Utilizing Bohmian mechanics...In studying interactions between intense laser fields and atoms or molecules,the role of electron correlation effects on the dynamical response is an important and pressing issue to address.Utilizing Bohmian mechanics(BM),we have theoretically explored the two-electron correlation characteristics while generating high-order harmonics in xenon atoms subjected to intense laser fields.We initially employed Bohmian trajectories to reproduce the dynamics of the electrons and subsequently utilized time-frequency analysis spectra to ascertain the emission time windows for high-order harmonics.Within these time windows,we classified the nuclear region Bohmian trajectories and observed that intense high-order harmonics are solely generated when paired Bohmian particles(BPs)concurrently appear in the nuclear region and reside there for a duration within a re-collision time window.Furthermore,our analysis of characteristic trajectories producing high-order harmonics led us to propose a two-electron re-collision model to elucidate this phenomenon.The study demonstrates that intense high-order harmonics are only generated when both electrons are in the ground state within the re-collision time window.This work discusses the implications of correlation effects between two electrons and offers valuable insights for studying correlation in multi-electron high-order harmonic generation.展开更多
The geometric structure parameters and radial density distribution of 1s2s1S excited state of the two-electron atomic system near the critical nuclear charge Z_(c)were calculated in detail under tripled Hylleraas basi...The geometric structure parameters and radial density distribution of 1s2s1S excited state of the two-electron atomic system near the critical nuclear charge Z_(c)were calculated in detail under tripled Hylleraas basis set.Contrary to the localized behavior observed in the ground and the doubly excited 2p^(23)Pe states,for this state our results identify that while the behavior of the inner electron increasingly resembles that of a hydrogen-like atomic system,the outer electron in the excited state exhibits diffused hydrogen-like character and becomes perpendicular to the inner electron as nuclear charge Z approaches Z_(c).This study provides insights into the electronic structure and stability of the two-electron system in the vicinity of the critical nuclear charge.展开更多
Precise energy eigenvalues of metastable bound doubly excited 1,3Fe states originating from 2 pnf(n=4–6)configuration of helium-like ions(Z=2–4)under weakly coupled plasma(WCP)environment have been estimated within ...Precise energy eigenvalues of metastable bound doubly excited 1,3Fe states originating from 2 pnf(n=4–6)configuration of helium-like ions(Z=2–4)under weakly coupled plasma(WCP)environment have been estimated within the framework of Ritz variational method.The wavefunction is expanded in explicitly correlated Hylleraas type basis set.The screened Coulomb potential is consideredas mimic the WCP environment.The atomic systems tend towards gradual instability and the number of excited metastable bound states reduces with increasing plasma strength.The wavelengths corresponding to 2 pnf(1,3F^e)→2 pnf(1,3Do)(n=4–6;n′=3–6)transitions occurring between doubly excited states of plasma embedded two-electron ions are also reported.展开更多
The ionization dynamics of two-electron atom in an intense laser field is studied by the Bohmian mechanics(BM)theory, and the xenon atomic potential function is used as a model. The single ionization process and doubl...The ionization dynamics of two-electron atom in an intense laser field is studied by the Bohmian mechanics(BM)theory, and the xenon atomic potential function is used as a model. The single ionization process and double ionization process are calculated by the BM theory and their results are in good agreement with those calculated by numerically solving the time-dependent Schrodinger equation. The analyses of the types, trajectories, and forces of Bohmian particles(BPs)undergoing the single and double ionizations indicate that the re-collision process accounts for a considerable proportion in the singly ionized cases. Furthermore, the analysis of the work done by the external force acting on the BPs shows that the quantum force plays an important role in the re-collision process. This work is helpful in understanding the ionization of two-electron atom in an intense laser field.展开更多
Using the basic ingredient of two-body problem, we propose accurate algebraic solutions in a closed form for the ground state of helium and helium-like atoms. These simple but explicit expressions involve exact screen...Using the basic ingredient of two-body problem, we propose accurate algebraic solutions in a closed form for the ground state of helium and helium-like atoms. These simple but explicit expressions involve exact screening parameters for each system considered and provide an insight into their physical structure. The energy eigenvalues have been exactly calculated for atoms with nuclear charge Z in the range 1 ≤ Z ≤ 12, clarifying the relation between the screening parameteter and Z.展开更多
Electrocatalytic oxygen reduction via a two-electron pathway(2e^(-)-ORR)is a promising and eco-friendly route for producing hydrogen peroxide(H_(2)O_(2)).Single-atom catalysts(SACs)typically show excellent selectivity...Electrocatalytic oxygen reduction via a two-electron pathway(2e^(-)-ORR)is a promising and eco-friendly route for producing hydrogen peroxide(H_(2)O_(2)).Single-atom catalysts(SACs)typically show excellent selectivity towards 2e^(-)-ORR due to their unique electronic structures and geometrical configurations.The very low density of single-atom active centers,however,often leads to unsatisfactory H_(2)O_(2)yield rate,significantly inhibiting their practical feasibility.Addressing this,we herein introduce fluorine as a secondary doping element into conventional SACs,which does not directly coordinate with the singleatom metal centers but synergize with them in a remote manner.This strategy effectively activates the surrounding carbon atoms and converts them into highly active sites for 2e^(-)-ORR.Consequently,a record-high H_(2)O_(2)yield rate up to 27 mol g^(-1)h^(-1)has been achieved on the Mo–F–C catalyst,with high Faradaic efficiency of 90%.Density functional theory calculations further confirm the very kinetically facile 2e^(-)-ORR over these additional active sites and the superiority of Mo as the single-atom center to others.This strategy thus not only provides a high-performance electrocatalyst for 2e^(-)-ORR but also should shed light on new strategies to significantly increase the active centers number of SACs.展开更多
The variation of the inner electronic cloud of a two-electron system when the outer elec-tron is moving far away or coming close is investigated in this paper mainly by analyzingthe shape-density. The geometric charac...The variation of the inner electronic cloud of a two-electron system when the outer elec-tron is moving far away or coming close is investigated in this paper mainly by analyzingthe shape-density. The geometric character and features of internal motion of the ~1S^e heliumstates having different K--numbers have been shown, the mechanism for energy transfer andthe details of radial-radial correlation have been inspected. The motion of the inner electroniccloud as a whole is found to be strongly correlated with the motion of the outer electron.展开更多
By using the path integral approach, we investigate the problem of Hooke＇s atom （two electrons interacting with Coulomb potential in an external harmonic-oscillator potential） in an arbitrary time-dependent electri...By using the path integral approach, we investigate the problem of Hooke＇s atom （two electrons interacting with Coulomb potential in an external harmonic-oscillator potential） in an arbitrary time-dependent electric field. For a certain infinite set of discrete oscillator frequencies, we obtain the analytical solutions. The ground state polarization of the atom is then calculated. The same result is also obtained through linear response theory.展开更多
Lithium-sulfur (Li-S) batteries have gained great attention due to the high theoretical energy density and low cost,yet their further commercialization has been obstructed by the notorious shuttle effect and sluggish ...Lithium-sulfur (Li-S) batteries have gained great attention due to the high theoretical energy density and low cost,yet their further commercialization has been obstructed by the notorious shuttle effect and sluggish redox dynamics.Herein,we supply a strategy to optimize the electron structure of Ni_(2)P by concurrently introducing B-doped atoms and P vacancies in Ni_(2)P (Vp-B-Ni_(2)P),thereby enhancing the bidirectional sulfur conversion.The study indicates that the simultaneous introduction of B-doped atoms and P vacancies in Ni_(2)P causes the redistribution of electron around Ni atoms,bringing about the upward shift of d-band center of Ni atoms and effective d-p orbital hybridization between Ni atoms and sulfur species,thus strengthening the chemical anchoring for lithium polysulfides (LiPSs) as well as expediting the bidirectional conversion kinetics of sulfur species.Meanwhile,theoretical calculations reveal that the incorporation of B-doped atoms and P vacancies in Ni_(2)P selectively promotes Li2S dissolution and nucleation processes.Thus,the Li-S batteries with Vp-B-Ni_(2)P-separators present outstanding rate ability of 777 m A h g^(-1)at 5 C and high areal capacity of 8.03 mA h cm^(-2)under E/S of 5μL mg^(-1)and sulfur loading of 7.20 mg cm^(-2).This work elucidates that introducing heteroatom and vacancy in metal phosphide collaboratively regulates the electron structure to accelerate bidirectional sulfur conversion.展开更多
Exploiting non-precious metal catalysts with excellent oxygen reduction reaction(ORR)performance for energy devices is paramount essential for the green and sustainable society development.Herein,low-cost,high-perform...Exploiting non-precious metal catalysts with excellent oxygen reduction reaction(ORR)performance for energy devices is paramount essential for the green and sustainable society development.Herein,low-cost,high-performance biomass-derived ORR catalysts with an asymmetric Fe-N_(3)P configuration was prepared by a simple pyrolysis-etching technique,where carboxymethyl cellulose(CMC)was used as the carbon source,urea and 1,10-phenanthroline iron complex(FePhen)as additives,and Na_(3)PO_(4)as the phosphorus dopant and a pore-forming agent.The CMC-derived FeNPC catalyst displayed a large specific area(BET:1235 m^(2)g^(-1))with atomically dispersed Fe-N_(3)P active sites,which exhibited superior ORR activity and stability in alkaline solution(E_(1/2)=0.90 V vs.RHE)and Zn-air batteries(P_(max)=149 mW cm^(-2))to commercial Pt/C catalyst(E_(1/2)=0.87 V,P_(max)=118 mW cm^(-2))under similar experimental conditions.This work provides a feasible and costeffective route toward highly efficient ORR catalysts and their application to Zn-air batteries for energy conversion.展开更多
The T_(1)(Al_(2) CuLi)phase is one of the most effective strengthening nanoscale-precipitate in Al-Cu alloys with Li.However,its formation and evolution still need to be further clarified during aging due to the compl...The T_(1)(Al_(2) CuLi)phase is one of the most effective strengthening nanoscale-precipitate in Al-Cu alloys with Li.However,its formation and evolution still need to be further clarified during aging due to the complex precipitation sequences.Here,a detailed investigation has been carried out on the atomic struc-tural evolution of T_(1) precipitate in an aged Al-Cu-Li-Mg-Ag alloy using state-of-the-art Cs-corrected high-angle annular dark field(HAADF)-coupled with integrated differential phase contrast(iDPC)-scanning transmission electron microscopy(STEM)and energy-dispersive X-ray spectroscopy(EDXS)techniques.An intermediate T_(1)’phase between T_(1p) and T_(1) phase,with a crystal structure and orientation rela-tionship consistent with T_(1),but exhibiting different atomic occupancy and chemical composition was found.We observed the atomic structural transformation from T_(1p) to T_(1)’phase(fcc→hcp),involving only 1/12<112>Al shear component.DFT calculation results validated our proposed structural models and the precipitation sequence.Besides,the distributions of minor solute elements(Ag,Mg,and Zn)in the pre-cipitates exhibited significant differences.These findings may contribute to a further understanding of the nucleation mechanism of T_(1) precipitate.展开更多
Combustion dynamics are a critical factor in determining the performance and reliabilityof a chemical propulsion engine.The underlying processes include liquid atomization,evaporation,mixing,and chemical reactions.Thi...Combustion dynamics are a critical factor in determining the performance and reliabilityof a chemical propulsion engine.The underlying processes include liquid atomization,evaporation,mixing,and chemical reactions.This paper presents a high-fidelity numerical study of liquidatomization and spray combustion under high-pressure conditions,emphasizing the effects of pres-sure oscillations on the flow evolution and combustion dynamics.The theoretical framework isbased on the three-dimensional conservation equations for multiphase flows and turbulent combus-tion.The numerical solution is achieved using a coupling method of volume-of-fluid and Lagran-gian particle tracking.The Zhuang-Kadota-Sutton(ZKS)high-pressure evaporation model andthe eddy breakup-Arrhenius combustion model are employed.Simulations are conducted for amodel combustion chamber with impinging-jet injectors using liquid oxygen and kerosene as pro-pellants.Both conditions with and without inlet and outlet pressure oscillations are considered.Thefindings reveal that pressure oscillations amplify flow fluctuations and can be characterized usingkey physical parameters such as droplet evaporation,chemical reaction,and chamber pressure.The spectral analysis uncovers the axial variations of the dominant and secondary frequenciesand their amplitudes in terms of the characteristic physical quantities.This research helps establisha methodology for exploring the coupling effect of liquid atomization and spray combustion.It alsoprovides practical insights into their responses to pressure oscillations during the occurrence ofcombustion instability.This information can be used to enhance the design and operation ofliquid-fueled propulsion engines.展开更多
We present the experimental demonstration of nondestructive detection of ^(171)Yb atoms in a magneto-optical trap(MOT) based on phase shift measurement induced by the atoms on a weak off-resonant laser beam. After loa...We present the experimental demonstration of nondestructive detection of ^(171)Yb atoms in a magneto-optical trap(MOT) based on phase shift measurement induced by the atoms on a weak off-resonant laser beam. After loading a green MOT of ^(171)Yb atoms, the phase shift is obtained with a two-color Mach–Zehnder interferometer by means of ±45 MHz detuning with respect to the ^(1)S_(0)–^(1)P_(1) transition. We measured a phase shift of about 100 mrad corresponding to an atom count of around 5 × 10^(5). This demonstrates that it is possible to obtain the number of atoms without direct destructive measurement compared with the absorption imaging method. This scheme could be an important approach towards a high-precision lattice clock for clock operation through suppression of the impact of the Dick effect.展开更多
Exploration of stable metal single-site supported porous graphitic carbon nitride(PCN)nanostructures and the development of maximum atom utilization for enhanced photocatalytic oxidation of antibiotics remains a chall...Exploration of stable metal single-site supported porous graphitic carbon nitride(PCN)nanostructures and the development of maximum atom utilization for enhanced photocatalytic oxidation of antibiotics remains a challenge in current research.This work proposed a one-step thermal copolymerization to obtain Cu(Ⅰ)doping porous carbon nitride(CUCN)through a spontaneously reducing atmosphere by urea in a covered crucible.The obtained CUCN had crumpled ultrathin nanosheets and mesoporous structures,which possessed higher specific surface areas than PCN.From X-ray absorption near edge structure(XANES)and Fourier transform extended X-ray absorption fine structure(FT-EXAFS)spectra analysis,the Cu doping existed in the oxidation state of Cu(Ⅰ)as single atoms anchored on the 2D layers of CN through two N neighbors,thereby facilitating efficient pathways for the transfer of photoexcited charge carriers.Furthermore,the photoluminescence(PL)spectra,electrochemical impedance spectra(EIS)and transient photocurrent response test proved the improved separation and transfer of photoexcited charge carriers for Cu(Ⅰ)introduction.Consequently,the photocatalytic activity of CUCN was much better than that of PCN for antibiotics norfloxacin(NOR),with 4.7-fold higher degradation reaction rate constants.From species-trapping experiments and density function theory(DFT)calculations,the Cu single atoms in Cu-N_(2)served as catalytic sites that could accelerate charge transfer and facilitate the adsorption of molecular oxygen to produce active species.The stable Cu(Ⅰ)embedded in the layer structure led to the excellent recycling test and remained stable after four runs of degradation and even thermal regenerated treatment.The degradation paths of NOR by CUCN under visible light were also demonstrated.Our work sheds light on a sustainable and practical approach for achieving stable metal single-atom doping and enhancing photocatalytic degradation of aqueous pollutants.展开更多
Atomic surfaces are strictly required by high-performance devices of diamond.Nevertheless,diamond is the hardest material in nature,leading to the low material removal rate(MRR)and high surface roughness during machin...Atomic surfaces are strictly required by high-performance devices of diamond.Nevertheless,diamond is the hardest material in nature,leading to the low material removal rate(MRR)and high surface roughness during machining.Noxious slurries are widely used in conventional chemical mechanical polishing(CMP),resulting in the possible pollution to the environment.Moreover,the traditional slurries normally contain more than four ingredients,causing difficulties to control the process and quality of CMP.To solve these challenges,a novel green CMP for single crystal diamond was developed,consisting of only hydrogen peroxide,diamond abrasive and Prussian blue(PB)/titania catalyst.After CMP,atomic surface is achieved with surface roughness Sa of 0.079 nm,and the MRR is 1168 nm·h^(-1).Thickness of damaged layer is merely 0.66 nm confirmed by transmission electron microscopy(TEM).X-ray photoelectron spectroscopy,electron paramagnetic resonance and TEM reveal that·OH radicals form under ultraviolet irradiation on PB/titania catalyst.The·OH radicals oxidize diamond,transforming it from monocrystalline to amorphous atomic structure,generating a soft amorphous layer.This contributes the high MRR and formation of atomic surface on diamond.The developed novel green CMP offers new insights to achieve atomic surface of diamond for potential use in their high-performance devices.展开更多
Broadband transparent films play a pivotal role in various applications such as lenses and solar cells,particularly porous structured transparent films exhibit significant potential.This study investigates a porous Si...Broadband transparent films play a pivotal role in various applications such as lenses and solar cells,particularly porous structured transparent films exhibit significant potential.This study investigates a porous SiO_(2) refractive index gradient anti-reflective film prepared by atomic layer deposition(ALD).A porous SiO_(2) film with gradual porosity was obtained by phosphoric acid etching of Al_(2)O_(3)/SiO_(2) multilayers with gradient Al2O3 ratios,achieving a gradual decrease in refractive index from the substrate to the surface.The film exhibited an average transmittance as high as 97.8%within the wavelength range from 320 nm to 1200 nm.The environmental adaptability was further enhanced by surface modification using rare earth oxide(REO)La_(2)O_(3),resulting in formation of a lotus leaf-like structure and achieving a water contact angle of 100.0°.These data proved that the modification significantly improved hydrophobic self-cleaning capability while maintaining exceptional transparency of the film.The surface structure of the modified film remained undamaged even after undergoing wipe testing,demonstrating its excellent surface durability.展开更多
Polymeric perylene diimide(PDI)has been evidenced as a good candidate for photocatalytic water oxidation,yet the origin of the photocatalytic oxygen evolution activity remains unclear and needs further exploration.Her...Polymeric perylene diimide(PDI)has been evidenced as a good candidate for photocatalytic water oxidation,yet the origin of the photocatalytic oxygen evolution activity remains unclear and needs further exploration.Herein,with crystal and atomic structures of the self-assembled PDI revealed from the X-ray diffraction pattern,the electronic structure is theoretically illustrated by the first-principles density functional theory calculations,suggesting the suitable band structure and the direct electronic transition for efficient photocatalytic oxygen evolution over PDI.It is confirmed that the carbonyl O atoms on the conjugation structure serve as the active sites for oxygen evolution reaction by the crystal orbital Hamiltonian group analysis.The calculations of reaction free energy changes indicate that the oxygen evolution reaction should follow the reaction pathway of H_(2)O→^(*)OH→^(*)O→^(*)OOH→^(*)O_(2)with an overpotential of 0.81 V.Through an in-depth theoretical computational analysis in the atomic and electronic structures,the origin of photocatalytic oxygen evolution activity for PDI is well illustrated,which would help the rational design and modification of polymeric photocatalysts for efficient oxygen evolution.展开更多
Single-atom catalysts(SACs),in which isolated metal atoms such as palladium(Pd)are anchored on solid supports,promise breakthroughs in energy conversion and catalysis.However,balancing their activity(reaction speed)an...Single-atom catalysts(SACs),in which isolated metal atoms such as palladium(Pd)are anchored on solid supports,promise breakthroughs in energy conversion and catalysis.However,balancing their activity(reaction speed)and stability(longevity)remains challenging,as the interplay between metal atoms,supports,and reactants is poorly understood.展开更多
The so-called close-coupled gas atomization process involves melting a metal and using a high-pressure gas jet positioned close to the melt stream to rapidly break it into fine,spherical powder particles.This techniqu...The so-called close-coupled gas atomization process involves melting a metal and using a high-pressure gas jet positioned close to the melt stream to rapidly break it into fine,spherical powder particles.This technique,adapted for blast furnace slag granulation using a circular seam nozzle,typically aims to produce solid slag particles sized 30–140μm,thereby allowing the utilization of slag as a resource.This study explores the atomization dynamics of liquid blast furnace slag,focusing on the effects of atomization pressure.Primary atomization is simulated using a combination of the Volume of Fluid(VOF)method and the Shear Stress Transport k-ωturbulence model,while secondary atomization is analyzed through the Discrete Phase Model(DPM).The results reveal that primary atomization progresses in three stages:the slag column transforms into an umbrella-shaped liquid film,whose leading edge fragments into particles while forming a cavity-like structure,which is eventually torn into ligaments.This primary deformation is driven by the interplay of airflow velocity in the recirculation zone and the guide tube outlet pressure(Fp).Increasing the atomization pressure amplifies airflow velocity,recirculation zone size,expansion and shock waves,though the guide tube outlet pressure variations remain irregular.Notably,at 4.5 MPa,the primary deformation is most pronounced.Secondary atomization yields finer slag particles as a result of more vigorous primary atomization.For this pressure,the smallest average particle size and the highest yield of particles within the target range(30–140μm)are achieved.展开更多
Electrochemical nitrogen reduction reaction(ENRR)is emerging as a favorable option to the power-intensive Haber-Bosch process for ammonia synthesis.However,obstacles such as poor selectivity,low production rates,and c...Electrochemical nitrogen reduction reaction(ENRR)is emerging as a favorable option to the power-intensive Haber-Bosch process for ammonia synthesis.However,obstacles such as poor selectivity,low production rates,and competition against the hydrogen evolution reaction hinder its practical implementation.To address these,the design of highly active catalysts is critical.Single-atom catalysts(SACs)have shown great potential because of their maximized atom utilization,but their limited stability and low metal loading restrict their performances.On the other hand,dual-atom catalysts(DACs)are atomic catalysts with two metal atoms nearby and offer enhanced electrocatalytic performances by aligning with the N≡N bond to enhance N2 reduction efficiency,potentially overcoming the limitations of SAC.This review discusses recent advances in SACs and more importantly DACs for ENRR,highlighting their advantages,limitations,and the need for advanced characterization techniques to better understand catalyst behavior.The review concludes by underscoring the importance of research to optimize these catalysts for efficient and sustainable nitrogen fixation.展开更多
基金Project supported by the Natural Science Foundation(General Project)of Jilin Province,China(Grant No.20230101283JC)。
文摘In studying interactions between intense laser fields and atoms or molecules,the role of electron correlation effects on the dynamical response is an important and pressing issue to address.Utilizing Bohmian mechanics(BM),we have theoretically explored the two-electron correlation characteristics while generating high-order harmonics in xenon atoms subjected to intense laser fields.We initially employed Bohmian trajectories to reproduce the dynamics of the electrons and subsequently utilized time-frequency analysis spectra to ascertain the emission time windows for high-order harmonics.Within these time windows,we classified the nuclear region Bohmian trajectories and observed that intense high-order harmonics are solely generated when paired Bohmian particles(BPs)concurrently appear in the nuclear region and reside there for a duration within a re-collision time window.Furthermore,our analysis of characteristic trajectories producing high-order harmonics led us to propose a two-electron re-collision model to elucidate this phenomenon.The study demonstrates that intense high-order harmonics are only generated when both electrons are in the ground state within the re-collision time window.This work discusses the implications of correlation effects between two electrons and offers valuable insights for studying correlation in multi-electron high-order harmonic generation.
基金supported by the National Natural Science Foundation of China(Grant Nos.12074295,12304271,and 12104420).
文摘The geometric structure parameters and radial density distribution of 1s2s1S excited state of the two-electron atomic system near the critical nuclear charge Z_(c)were calculated in detail under tripled Hylleraas basis set.Contrary to the localized behavior observed in the ground and the doubly excited 2p^(23)Pe states,for this state our results identify that while the behavior of the inner electron increasingly resembles that of a hydrogen-like atomic system,the outer electron in the excited state exhibits diffused hydrogen-like character and becomes perpendicular to the inner electron as nuclear charge Z approaches Z_(c).This study provides insights into the electronic structure and stability of the two-electron system in the vicinity of the critical nuclear charge.
基金Supported under Grant No. EMR/2017/000737 from DST-SERB, Govt. of India, Grant No. 23(Sanc.)/ST/P/S&T/16G-35/2017 from DHESTB, Govt. of West Bengal, Indiaby the DHESTB,Govt.of West Bengal,India under Grant No.249(Sanc.)/ST/P/S&T/16G-26/2017
文摘Precise energy eigenvalues of metastable bound doubly excited 1,3Fe states originating from 2 pnf(n=4–6)configuration of helium-like ions(Z=2–4)under weakly coupled plasma(WCP)environment have been estimated within the framework of Ritz variational method.The wavefunction is expanded in explicitly correlated Hylleraas type basis set.The screened Coulomb potential is consideredas mimic the WCP environment.The atomic systems tend towards gradual instability and the number of excited metastable bound states reduces with increasing plasma strength.The wavelengths corresponding to 2 pnf(1,3F^e)→2 pnf(1,3Do)(n=4–6;n′=3–6)transitions occurring between doubly excited states of plasma embedded two-electron ions are also reported.
基金Project supported by the Jilin Provincial Science and Technology Development Plan Program for Excellent Youth Talents,China(Grant No.20180520174JH)the National Natural Science Foundation of China(Grant Nos.11704145,11904050,11774129,11747007,11534004,and 12074145).
文摘The ionization dynamics of two-electron atom in an intense laser field is studied by the Bohmian mechanics(BM)theory, and the xenon atomic potential function is used as a model. The single ionization process and double ionization process are calculated by the BM theory and their results are in good agreement with those calculated by numerically solving the time-dependent Schrodinger equation. The analyses of the types, trajectories, and forces of Bohmian particles(BPs)undergoing the single and double ionizations indicate that the re-collision process accounts for a considerable proportion in the singly ionized cases. Furthermore, the analysis of the work done by the external force acting on the BPs shows that the quantum force plays an important role in the re-collision process. This work is helpful in understanding the ionization of two-electron atom in an intense laser field.
文摘Using the basic ingredient of two-body problem, we propose accurate algebraic solutions in a closed form for the ground state of helium and helium-like atoms. These simple but explicit expressions involve exact screening parameters for each system considered and provide an insight into their physical structure. The energy eigenvalues have been exactly calculated for atoms with nuclear charge Z in the range 1 ≤ Z ≤ 12, clarifying the relation between the screening parameteter and Z.
基金supported by the National Natural Science Foundation of China(Nos.22179093 and 21905202)。
文摘Electrocatalytic oxygen reduction via a two-electron pathway(2e^(-)-ORR)is a promising and eco-friendly route for producing hydrogen peroxide(H_(2)O_(2)).Single-atom catalysts(SACs)typically show excellent selectivity towards 2e^(-)-ORR due to their unique electronic structures and geometrical configurations.The very low density of single-atom active centers,however,often leads to unsatisfactory H_(2)O_(2)yield rate,significantly inhibiting their practical feasibility.Addressing this,we herein introduce fluorine as a secondary doping element into conventional SACs,which does not directly coordinate with the singleatom metal centers but synergize with them in a remote manner.This strategy effectively activates the surrounding carbon atoms and converts them into highly active sites for 2e^(-)-ORR.Consequently,a record-high H_(2)O_(2)yield rate up to 27 mol g^(-1)h^(-1)has been achieved on the Mo–F–C catalyst,with high Faradaic efficiency of 90%.Density functional theory calculations further confirm the very kinetically facile 2e^(-)-ORR over these additional active sites and the superiority of Mo as the single-atom center to others.This strategy thus not only provides a high-performance electrocatalyst for 2e^(-)-ORR but also should shed light on new strategies to significantly increase the active centers number of SACs.
基金Project supported by the National Natural Science Foundation of China.
文摘The variation of the inner electronic cloud of a two-electron system when the outer elec-tron is moving far away or coming close is investigated in this paper mainly by analyzingthe shape-density. The geometric character and features of internal motion of the ~1S^e heliumstates having different K--numbers have been shown, the mechanism for energy transfer andthe details of radial-radial correlation have been inspected. The motion of the inner electroniccloud as a whole is found to be strongly correlated with the motion of the outer electron.
基金Supported by the National Natural Science Foundation of China under Grant No.10805029ZheJiang NSF under Grant No.R6090717the K.C.Wong Magna Foundation of Ningbo University
文摘By using the path integral approach, we investigate the problem of Hooke＇s atom （two electrons interacting with Coulomb potential in an external harmonic-oscillator potential） in an arbitrary time-dependent electric field. For a certain infinite set of discrete oscillator frequencies, we obtain the analytical solutions. The ground state polarization of the atom is then calculated. The same result is also obtained through linear response theory.
基金Institute of Technology Research Fund Program for Young Scholars21C Innovation Laboratory Contemporary Amperex Technology Co.,Limited,Ninde, 352100, China (21C–OP-202314)。
文摘Lithium-sulfur (Li-S) batteries have gained great attention due to the high theoretical energy density and low cost,yet their further commercialization has been obstructed by the notorious shuttle effect and sluggish redox dynamics.Herein,we supply a strategy to optimize the electron structure of Ni_(2)P by concurrently introducing B-doped atoms and P vacancies in Ni_(2)P (Vp-B-Ni_(2)P),thereby enhancing the bidirectional sulfur conversion.The study indicates that the simultaneous introduction of B-doped atoms and P vacancies in Ni_(2)P causes the redistribution of electron around Ni atoms,bringing about the upward shift of d-band center of Ni atoms and effective d-p orbital hybridization between Ni atoms and sulfur species,thus strengthening the chemical anchoring for lithium polysulfides (LiPSs) as well as expediting the bidirectional conversion kinetics of sulfur species.Meanwhile,theoretical calculations reveal that the incorporation of B-doped atoms and P vacancies in Ni_(2)P selectively promotes Li2S dissolution and nucleation processes.Thus,the Li-S batteries with Vp-B-Ni_(2)P-separators present outstanding rate ability of 777 m A h g^(-1)at 5 C and high areal capacity of 8.03 mA h cm^(-2)under E/S of 5μL mg^(-1)and sulfur loading of 7.20 mg cm^(-2).This work elucidates that introducing heteroatom and vacancy in metal phosphide collaboratively regulates the electron structure to accelerate bidirectional sulfur conversion.
基金supported by the National Natural Science Foundation of China(No.21571062)the Program for Professor of Special Appointment(Eastern Scholar)at the Shanghai Institutions of Higher Learning to JGL,and the Fundamental Research Funds for the Central Universities(No.222201717003)。
文摘Exploiting non-precious metal catalysts with excellent oxygen reduction reaction(ORR)performance for energy devices is paramount essential for the green and sustainable society development.Herein,low-cost,high-performance biomass-derived ORR catalysts with an asymmetric Fe-N_(3)P configuration was prepared by a simple pyrolysis-etching technique,where carboxymethyl cellulose(CMC)was used as the carbon source,urea and 1,10-phenanthroline iron complex(FePhen)as additives,and Na_(3)PO_(4)as the phosphorus dopant and a pore-forming agent.The CMC-derived FeNPC catalyst displayed a large specific area(BET:1235 m^(2)g^(-1))with atomically dispersed Fe-N_(3)P active sites,which exhibited superior ORR activity and stability in alkaline solution(E_(1/2)=0.90 V vs.RHE)and Zn-air batteries(P_(max)=149 mW cm^(-2))to commercial Pt/C catalyst(E_(1/2)=0.87 V,P_(max)=118 mW cm^(-2))under similar experimental conditions.This work provides a feasible and costeffective route toward highly efficient ORR catalysts and their application to Zn-air batteries for energy conversion.
基金supported by the Pre-research fund(No.412130024).
文摘The T_(1)(Al_(2) CuLi)phase is one of the most effective strengthening nanoscale-precipitate in Al-Cu alloys with Li.However,its formation and evolution still need to be further clarified during aging due to the complex precipitation sequences.Here,a detailed investigation has been carried out on the atomic struc-tural evolution of T_(1) precipitate in an aged Al-Cu-Li-Mg-Ag alloy using state-of-the-art Cs-corrected high-angle annular dark field(HAADF)-coupled with integrated differential phase contrast(iDPC)-scanning transmission electron microscopy(STEM)and energy-dispersive X-ray spectroscopy(EDXS)techniques.An intermediate T_(1)’phase between T_(1p) and T_(1) phase,with a crystal structure and orientation rela-tionship consistent with T_(1),but exhibiting different atomic occupancy and chemical composition was found.We observed the atomic structural transformation from T_(1p) to T_(1)’phase(fcc→hcp),involving only 1/12<112>Al shear component.DFT calculation results validated our proposed structural models and the precipitation sequence.Besides,the distributions of minor solute elements(Ag,Mg,and Zn)in the pre-cipitates exhibited significant differences.These findings may contribute to a further understanding of the nucleation mechanism of T_(1) precipitate.
基金supported by the National Natural Science Foundation of China(Nos.U23B6009 and 12272050)。
文摘Combustion dynamics are a critical factor in determining the performance and reliabilityof a chemical propulsion engine.The underlying processes include liquid atomization,evaporation,mixing,and chemical reactions.This paper presents a high-fidelity numerical study of liquidatomization and spray combustion under high-pressure conditions,emphasizing the effects of pres-sure oscillations on the flow evolution and combustion dynamics.The theoretical framework isbased on the three-dimensional conservation equations for multiphase flows and turbulent combus-tion.The numerical solution is achieved using a coupling method of volume-of-fluid and Lagran-gian particle tracking.The Zhuang-Kadota-Sutton(ZKS)high-pressure evaporation model andthe eddy breakup-Arrhenius combustion model are employed.Simulations are conducted for amodel combustion chamber with impinging-jet injectors using liquid oxygen and kerosene as pro-pellants.Both conditions with and without inlet and outlet pressure oscillations are considered.Thefindings reveal that pressure oscillations amplify flow fluctuations and can be characterized usingkey physical parameters such as droplet evaporation,chemical reaction,and chamber pressure.The spectral analysis uncovers the axial variations of the dominant and secondary frequenciesand their amplitudes in terms of the characteristic physical quantities.This research helps establisha methodology for exploring the coupling effect of liquid atomization and spray combustion.It alsoprovides practical insights into their responses to pressure oscillations during the occurrence ofcombustion instability.This information can be used to enhance the design and operation ofliquid-fueled propulsion engines.
基金Project supported by the National Natural Science Foundation of China (Grant Nos. U20A2075,11803072,and 12374467)the Innovation Program for Quantum Science and Technology (Grant No. 2021ZD0300902)the Hubei Provincial Science and Technology Major Project (Grant No. ZDZX2022000004)。
文摘We present the experimental demonstration of nondestructive detection of ^(171)Yb atoms in a magneto-optical trap(MOT) based on phase shift measurement induced by the atoms on a weak off-resonant laser beam. After loading a green MOT of ^(171)Yb atoms, the phase shift is obtained with a two-color Mach–Zehnder interferometer by means of ±45 MHz detuning with respect to the ^(1)S_(0)–^(1)P_(1) transition. We measured a phase shift of about 100 mrad corresponding to an atom count of around 5 × 10^(5). This demonstrates that it is possible to obtain the number of atoms without direct destructive measurement compared with the absorption imaging method. This scheme could be an important approach towards a high-precision lattice clock for clock operation through suppression of the impact of the Dick effect.
基金supported by the National Natural Science Foundation of China(Nos.52070103 and 22102102)Zhejiang Provincial Natural Science Foundation of China(Nos.LY21E090004 and LQ22B050004)+1 种基金Ningbo Public Welfare Science and Technology Program(No.2021S025)Ningbo Youth Leading Talent Project(No.2024QL038).
文摘Exploration of stable metal single-site supported porous graphitic carbon nitride(PCN)nanostructures and the development of maximum atom utilization for enhanced photocatalytic oxidation of antibiotics remains a challenge in current research.This work proposed a one-step thermal copolymerization to obtain Cu(Ⅰ)doping porous carbon nitride(CUCN)through a spontaneously reducing atmosphere by urea in a covered crucible.The obtained CUCN had crumpled ultrathin nanosheets and mesoporous structures,which possessed higher specific surface areas than PCN.From X-ray absorption near edge structure(XANES)and Fourier transform extended X-ray absorption fine structure(FT-EXAFS)spectra analysis,the Cu doping existed in the oxidation state of Cu(Ⅰ)as single atoms anchored on the 2D layers of CN through two N neighbors,thereby facilitating efficient pathways for the transfer of photoexcited charge carriers.Furthermore,the photoluminescence(PL)spectra,electrochemical impedance spectra(EIS)and transient photocurrent response test proved the improved separation and transfer of photoexcited charge carriers for Cu(Ⅰ)introduction.Consequently,the photocatalytic activity of CUCN was much better than that of PCN for antibiotics norfloxacin(NOR),with 4.7-fold higher degradation reaction rate constants.From species-trapping experiments and density function theory(DFT)calculations,the Cu single atoms in Cu-N_(2)served as catalytic sites that could accelerate charge transfer and facilitate the adsorption of molecular oxygen to produce active species.The stable Cu(Ⅰ)embedded in the layer structure led to the excellent recycling test and remained stable after four runs of degradation and even thermal regenerated treatment.The degradation paths of NOR by CUCN under visible light were also demonstrated.Our work sheds light on a sustainable and practical approach for achieving stable metal single-atom doping and enhancing photocatalytic degradation of aqueous pollutants.
基金financial support from the National Key Research and Development Program of China(2018YFA0703400)the Fundamental Research Funds for the Provincial Universities of Zhejiang(GK239909299001021)+1 种基金the Ninth China Association for Science and Technology Youth Talent Lift Project Support Plan(KYZ015324002)the Changjiang Scholars Program of Chinese Ministry of Education。
文摘Atomic surfaces are strictly required by high-performance devices of diamond.Nevertheless,diamond is the hardest material in nature,leading to the low material removal rate(MRR)and high surface roughness during machining.Noxious slurries are widely used in conventional chemical mechanical polishing(CMP),resulting in the possible pollution to the environment.Moreover,the traditional slurries normally contain more than four ingredients,causing difficulties to control the process and quality of CMP.To solve these challenges,a novel green CMP for single crystal diamond was developed,consisting of only hydrogen peroxide,diamond abrasive and Prussian blue(PB)/titania catalyst.After CMP,atomic surface is achieved with surface roughness Sa of 0.079 nm,and the MRR is 1168 nm·h^(-1).Thickness of damaged layer is merely 0.66 nm confirmed by transmission electron microscopy(TEM).X-ray photoelectron spectroscopy,electron paramagnetic resonance and TEM reveal that·OH radicals form under ultraviolet irradiation on PB/titania catalyst.The·OH radicals oxidize diamond,transforming it from monocrystalline to amorphous atomic structure,generating a soft amorphous layer.This contributes the high MRR and formation of atomic surface on diamond.The developed novel green CMP offers new insights to achieve atomic surface of diamond for potential use in their high-performance devices.
文摘Broadband transparent films play a pivotal role in various applications such as lenses and solar cells,particularly porous structured transparent films exhibit significant potential.This study investigates a porous SiO_(2) refractive index gradient anti-reflective film prepared by atomic layer deposition(ALD).A porous SiO_(2) film with gradual porosity was obtained by phosphoric acid etching of Al_(2)O_(3)/SiO_(2) multilayers with gradient Al2O3 ratios,achieving a gradual decrease in refractive index from the substrate to the surface.The film exhibited an average transmittance as high as 97.8%within the wavelength range from 320 nm to 1200 nm.The environmental adaptability was further enhanced by surface modification using rare earth oxide(REO)La_(2)O_(3),resulting in formation of a lotus leaf-like structure and achieving a water contact angle of 100.0°.These data proved that the modification significantly improved hydrophobic self-cleaning capability while maintaining exceptional transparency of the film.The surface structure of the modified film remained undamaged even after undergoing wipe testing,demonstrating its excellent surface durability.
基金supported by National Natural Science Foundation of China(No.523B2070,No.52225606).
文摘Polymeric perylene diimide(PDI)has been evidenced as a good candidate for photocatalytic water oxidation,yet the origin of the photocatalytic oxygen evolution activity remains unclear and needs further exploration.Herein,with crystal and atomic structures of the self-assembled PDI revealed from the X-ray diffraction pattern,the electronic structure is theoretically illustrated by the first-principles density functional theory calculations,suggesting the suitable band structure and the direct electronic transition for efficient photocatalytic oxygen evolution over PDI.It is confirmed that the carbonyl O atoms on the conjugation structure serve as the active sites for oxygen evolution reaction by the crystal orbital Hamiltonian group analysis.The calculations of reaction free energy changes indicate that the oxygen evolution reaction should follow the reaction pathway of H_(2)O→^(*)OH→^(*)O→^(*)OOH→^(*)O_(2)with an overpotential of 0.81 V.Through an in-depth theoretical computational analysis in the atomic and electronic structures,the origin of photocatalytic oxygen evolution activity for PDI is well illustrated,which would help the rational design and modification of polymeric photocatalysts for efficient oxygen evolution.
文摘Single-atom catalysts(SACs),in which isolated metal atoms such as palladium(Pd)are anchored on solid supports,promise breakthroughs in energy conversion and catalysis.However,balancing their activity(reaction speed)and stability(longevity)remains challenging,as the interplay between metal atoms,supports,and reactants is poorly understood.
基金the Tangshan University Doctor Innovation Fund(Project Number:1402306).
文摘The so-called close-coupled gas atomization process involves melting a metal and using a high-pressure gas jet positioned close to the melt stream to rapidly break it into fine,spherical powder particles.This technique,adapted for blast furnace slag granulation using a circular seam nozzle,typically aims to produce solid slag particles sized 30–140μm,thereby allowing the utilization of slag as a resource.This study explores the atomization dynamics of liquid blast furnace slag,focusing on the effects of atomization pressure.Primary atomization is simulated using a combination of the Volume of Fluid(VOF)method and the Shear Stress Transport k-ωturbulence model,while secondary atomization is analyzed through the Discrete Phase Model(DPM).The results reveal that primary atomization progresses in three stages:the slag column transforms into an umbrella-shaped liquid film,whose leading edge fragments into particles while forming a cavity-like structure,which is eventually torn into ligaments.This primary deformation is driven by the interplay of airflow velocity in the recirculation zone and the guide tube outlet pressure(Fp).Increasing the atomization pressure amplifies airflow velocity,recirculation zone size,expansion and shock waves,though the guide tube outlet pressure variations remain irregular.Notably,at 4.5 MPa,the primary deformation is most pronounced.Secondary atomization yields finer slag particles as a result of more vigorous primary atomization.For this pressure,the smallest average particle size and the highest yield of particles within the target range(30–140μm)are achieved.
基金supported by the National Research Foundation of Korea(2022R1C1C2005786,RS-2023-00256106,RS-2023-00207831,RS-2024-00346153).
文摘Electrochemical nitrogen reduction reaction(ENRR)is emerging as a favorable option to the power-intensive Haber-Bosch process for ammonia synthesis.However,obstacles such as poor selectivity,low production rates,and competition against the hydrogen evolution reaction hinder its practical implementation.To address these,the design of highly active catalysts is critical.Single-atom catalysts(SACs)have shown great potential because of their maximized atom utilization,but their limited stability and low metal loading restrict their performances.On the other hand,dual-atom catalysts(DACs)are atomic catalysts with two metal atoms nearby and offer enhanced electrocatalytic performances by aligning with the N≡N bond to enhance N2 reduction efficiency,potentially overcoming the limitations of SAC.This review discusses recent advances in SACs and more importantly DACs for ENRR,highlighting their advantages,limitations,and the need for advanced characterization techniques to better understand catalyst behavior.The review concludes by underscoring the importance of research to optimize these catalysts for efficient and sustainable nitrogen fixation.
