Electron density plays an important role in determining the properties of functional materials.Revealing the electron density distribution experimentally in real space can help to tune the properties of materials.Spin...Electron density plays an important role in determining the properties of functional materials.Revealing the electron density distribution experimentally in real space can help to tune the properties of materials.Spinel Li Mn2 O4 is one of the most promising cathode candidates because of its high voltage,low cost,and non-toxicity,but suffers severe capacity fading during electrochemical cycling due to the Mn dissolution.Real-space measurement of electron distribution of Li Mn2 O4 experimentally can provide direct evaluation on the strength of Mn–O bond and give an explanation of the structure stability.Here,through high energy synchrotron powder x-ray diffraction(SPXRD),accurate electron density distribution in spinel Li Mn2 O4 has been investigated based on the multipole model.The electron accumulation between Mn and O atoms in deformation density map indicates the shared interaction of Mn–O bond.The quantitative topological analysis at bond critical points shows that the Mn–O bond is relatively weak covalent interaction due to the oxygen loss.These findings suggest that oxygen stoichiometry is the key factor for preventing the Mn dissolution and capacity fading.展开更多
The distributions of traps and electron density in the interfaces between polyimide （PI） matrix and Al2O3 nanoparticles are researched using the isothermal decay current and the small-angle x-ray scattering （SAXS）...The distributions of traps and electron density in the interfaces between polyimide （PI） matrix and Al2O3 nanoparticles are researched using the isothermal decay current and the small-angle x-ray scattering （SAXS） tests. According to the electron density distribution for quasi two-phase mixture doped by spherical nanoparticles, the electron densities in the interfaces of PI/Al2O3 nanocomposite films are evaluated. The trap level density and carrier mobility in the interface are studied. The experimental results show that the distribution and the change rate of the electron density in the three layers of interface are different, indicating different trap distributions in the interface layers. There is a maximum trap level density in the second layer, where the maximum trap level density for the nanocomposite film doped by 25 wt% is 1.054 × 10^22 eV·m^-3 at 1.324eV, resulting in the carrier mobility reducing. In addition, both the thickness and the electron density of the nanocomposite film interface increase with the addition of the doped Al2O3 contents. Through the study on the trap level distribution in the interface, it is possible to further analyze the insulation mechanism and to improve the performance of nano-dielectric materials.展开更多
Electron momentum distributions for 4a1 orbitals of serial freon molecules CFaC1, CF2Cl2, and CFCl3 （CFxC14-x, x=1-3） have been reanalyzed due to the severe discrepancies between theory and experiment in low momentu...Electron momentum distributions for 4a1 orbitals of serial freon molecules CFaC1, CF2Cl2, and CFCl3 （CFxC14-x, x=1-3） have been reanalyzed due to the severe discrepancies between theory and experiment in low momentum region. The tentative calculations using equilibrium geometries of molecular ions have exhibited a great improvement in agreement with the experimental data, which suggests that the molecular geometry distortion may be responsible for the observed high intensities at p〈0.5 a.u.. Further analyses show that the severe discrepancies at low momentum region mainly arise from the influence of molecular geometry distortion on C-Cl bonding electron density distributions.展开更多
A three-dimensional fluid model for surface-wave plasma （SWP）, to investigate the discharge characteristics of a rectangular SWP source working in a steady state, was presented. The simulation is performed for diffe...A three-dimensional fluid model for surface-wave plasma （SWP）, to investigate the discharge characteristics of a rectangular SWP source working in a steady state, was presented. The simulation is performed for different gas pressures in argon and different deposited powers. The results showed that there is a peak of plasma density at a distance of 2 cm to 3 cm from the plasma-quartz interface whose position depends mainly on the gas pressure but not the deposited power. The spatial distributions of plasma parameters and their dependence on the gas pressure and deposited power are also presented and discussed. Using this model a good agreement between the simulation results and the available experimental data is obtained.展开更多
Electron density distributions of 2-aminoethanol （2AE） and 2-amino-l-propanol （2AP） are calculated in both the coordinate and the momentum spaces using the B3LYP/TZVP method. Using the dual space analysis, molecul...Electron density distributions of 2-aminoethanol （2AE） and 2-amino-l-propanol （2AP） are calculated in both the coordinate and the momentum spaces using the B3LYP/TZVP method. Using the dual space analysis, molecular orbital signatures of the methyl substituent in 2AP are identified with respect to 2AE. Relaxations of the geometry and the valence orbital in 2AP are found to be due to the insertion of the methyl group. Five orbitals, not four orbitals, are identified as the methyl signatures. They are orbital 5a in the core shell, orbitals 9a and 10a in the inner valence shell, and orbitals 15a and 16a in the outer valence. In the inner valence shell, the attachment of methyl to 2AE causes a splitting of its orbital 8a into orbitals 9a and 10a of 2AP, whereas in the outer valence shell, the methyl group results in the insertion of an additional orbital pair of 15a and 16a. The frontier molecular orbitals 21a, 20a, and 19a are found to have no significant role in the methylation of 2AE.展开更多
基金Beijing Natural Science Foundation,China(Grant No.Z190010)the National Key Research and Development Program of China(Grant No.2019YFA0308500)+2 种基金the Strategic Priority Research Program of Chinese Academy of Sciences(Grant No.XDB07030200)Key Research Projects of Frontier Science of Chinese Academy of Sciences(Grant No.QYZDB-SSW-JSC035)the National Natural Science Foundation of China(Grant Nos.51421002,51672307,51991344,52025025,and 52072400).
文摘Electron density plays an important role in determining the properties of functional materials.Revealing the electron density distribution experimentally in real space can help to tune the properties of materials.Spinel Li Mn2 O4 is one of the most promising cathode candidates because of its high voltage,low cost,and non-toxicity,but suffers severe capacity fading during electrochemical cycling due to the Mn dissolution.Real-space measurement of electron distribution of Li Mn2 O4 experimentally can provide direct evaluation on the strength of Mn–O bond and give an explanation of the structure stability.Here,through high energy synchrotron powder x-ray diffraction(SPXRD),accurate electron density distribution in spinel Li Mn2 O4 has been investigated based on the multipole model.The electron accumulation between Mn and O atoms in deformation density map indicates the shared interaction of Mn–O bond.The quantitative topological analysis at bond critical points shows that the Mn–O bond is relatively weak covalent interaction due to the oxygen loss.These findings suggest that oxygen stoichiometry is the key factor for preventing the Mn dissolution and capacity fading.
基金Supported by the National Natural Science Foundation of China under Grant Nos 51337002,51077028,51502063 and 51307046the Foundation of Harbin Science and Technology Bureau of Heilongjiang Province under Grant No RC2014QN017034
文摘The distributions of traps and electron density in the interfaces between polyimide （PI） matrix and Al2O3 nanoparticles are researched using the isothermal decay current and the small-angle x-ray scattering （SAXS） tests. According to the electron density distribution for quasi two-phase mixture doped by spherical nanoparticles, the electron densities in the interfaces of PI/Al2O3 nanocomposite films are evaluated. The trap level density and carrier mobility in the interface are studied. The experimental results show that the distribution and the change rate of the electron density in the three layers of interface are different, indicating different trap distributions in the interface layers. There is a maximum trap level density in the second layer, where the maximum trap level density for the nanocomposite film doped by 25 wt% is 1.054 × 10^22 eV·m^-3 at 1.324eV, resulting in the carrier mobility reducing. In addition, both the thickness and the electron density of the nanocomposite film interface increase with the addition of the doped Al2O3 contents. Through the study on the trap level distribution in the interface, it is possible to further analyze the insulation mechanism and to improve the performance of nano-dielectric materials.
基金V. ACKNOWLEDGMENTS This work was supported by the National Natural Science Foundation of China （No.10734040） and the Chinese Academy of Science Knowledge Promotion Project （No.KJCXI-YW-N30）. The authors also gratefully acknowledge Professor C. E. Brion from University of British Columbia （UBC） in Canada for supplying the HEMS and RESFOLD programs.
文摘Electron momentum distributions for 4a1 orbitals of serial freon molecules CFaC1, CF2Cl2, and CFCl3 （CFxC14-x, x=1-3） have been reanalyzed due to the severe discrepancies between theory and experiment in low momentum region. The tentative calculations using equilibrium geometries of molecular ions have exhibited a great improvement in agreement with the experimental data, which suggests that the molecular geometry distortion may be responsible for the observed high intensities at p〈0.5 a.u.. Further analyses show that the severe discrepancies at low momentum region mainly arise from the influence of molecular geometry distortion on C-Cl bonding electron density distributions.
文摘A three-dimensional fluid model for surface-wave plasma （SWP）, to investigate the discharge characteristics of a rectangular SWP source working in a steady state, was presented. The simulation is performed for different gas pressures in argon and different deposited powers. The results showed that there is a peak of plasma density at a distance of 2 cm to 3 cm from the plasma-quartz interface whose position depends mainly on the gas pressure but not the deposited power. The spatial distributions of plasma parameters and their dependence on the gas pressure and deposited power are also presented and discussed. Using this model a good agreement between the simulation results and the available experimental data is obtained.
基金Project supported by the Foundation of Henan Educational Committee, China (Grant No. 2011A140015)
文摘Electron density distributions of 2-aminoethanol （2AE） and 2-amino-l-propanol （2AP） are calculated in both the coordinate and the momentum spaces using the B3LYP/TZVP method. Using the dual space analysis, molecular orbital signatures of the methyl substituent in 2AP are identified with respect to 2AE. Relaxations of the geometry and the valence orbital in 2AP are found to be due to the insertion of the methyl group. Five orbitals, not four orbitals, are identified as the methyl signatures. They are orbital 5a in the core shell, orbitals 9a and 10a in the inner valence shell, and orbitals 15a and 16a in the outer valence. In the inner valence shell, the attachment of methyl to 2AE causes a splitting of its orbital 8a into orbitals 9a and 10a of 2AP, whereas in the outer valence shell, the methyl group results in the insertion of an additional orbital pair of 15a and 16a. The frontier molecular orbitals 21a, 20a, and 19a are found to have no significant role in the methylation of 2AE.
