High order Correlation polarization potential for vibrational excitation scattering of diatomic molecules by low-energy electrons

This paper introduces a correlation--polarization potential with high order terms for vibrational excitation in electron--molecule scattering. The new polarization potential generalizes the two-term approximation so that it can better reflect the dependence of correlation and polarization effects on the position coordinate of the scattering electron. It applies the new potential on the vibrational excitation scattering from N₂ in an energy range which includes the ²П_g shape resonance. The good agreement of theoretical resonant peaks with experiments shows that polarization potentials with high order terms are important and should be included in vibrational excitation scattering.     

运用球高斯分布极化势研究低能电子与H2 分子碰撞的振动激发动量迁移散射截面

用最近改进的球高斯分布(distributed spherical Gaussian,DSG)极化势模型,在振动密耦合框架下和基于量子力学从头计算的静电势、交换势的基础上,研究了低能电子与H₂分子碰撞振动激发的动量迁移散射截面(momentum transfer cross section,MTCS).通过包含18个振动波函数、5个分波和16个分子对称性,得到了0<E≤10 eV时收敛性很好的ν=0→ν'=0,1,2,3等几个振动跃迁通道和总的MTCS,并与其他实验和理论得到的值进行了比较和分析. 关键词： 2分子碰撞')" href="#">H₂分子碰撞 动量迁移散射截面 振动激发 球高斯分布极化势     

低能电子与氢分子碰撞的振动激发积分散射截面的研究

采用振动密耦合方法,研究了低能电子与H₂分子碰撞的振动激发积分散射截面.研究表明,使用18个Morse振动波函数、5个分波和4个对称性可以得到收敛的0→0,0→1,0→2和0→3积分散射截面;而且振动波函数的性质和振动能级的精确性会直接影响振动激发散射势能和振动激发积分散射截面.计算结果与实验符合得很好. 关键词： 电子散射 振动激发 2分子')" href="#">H₂分子 积分截面     

Studies on differential cross-sections of e–N2 scattering

The differential cross-sections (DCS) of the low-energy electron–N ₂ scattering are studied using the vibrational close-coupling (VCC) method and vibrational scattering potentials which include static, exchange and polarization contributions. The polarization is obtained based on the ‘better than adiabatic dipole’ (BTAD) and the ‘distributed spherical Gaussian’ (DSG) respectively. The converged (0 → 0, 0 → 1, 0 → 2, 0 → 3) DCS are obtained with the impact energies being the resonance's first two elastic scattering peaks?–?approximately 1.90 eV and 2.10 eV. Calculations from both polarization potentials agree with experimental results.     

Studies on vibrational excitation differential cross-sections of low-energy electron scattering from N2 molecule

The vibrational excitation differential cross-sections (DCS) of low-energy electron-N₂ scattering are studied using vibrational close-coupling (VCC) method and vibrational scattering potentials which include static, exchange and polarization contributions. By including the contributions of 18 partial waves, 20 vibrational states, and 16 molecular symmetries (up to Λ=7), the converged vibrational excitation (0↦2, 0↦3, 0↦4) DCS agree well with experimental results. Also obtained are converged vibrational (1↦0, 1↦1, 1↦2, 1↦3) DCS, with the impact energies being those of the main resonant peaks (1.92 eV, 1.90 eV, 1.62 eV, 1.63 eV).     

基于严格交换势的低能电子与H2分子碰撞振动激发散射截面的研究

严格交换势用于研究低能电子与H₂分子的弹性和非弹性散射截面,线性代数方法和R-矩阵传播子相结合求解基于振动密耦合方法的积分-微分耦合方程组,由此得到收敛的(0→0,0→1,0→2)散射微分截面和积分截面.理论计算结果与目前优秀的实验值和其他理论计算值进行了比较,表明基于振动密耦合方程的严格交换势在低能电子与H₂分子振动激发散射中有重要作用. 关键词： 严格交换势 2分子振动激发')" href="#">H₂分子振动激发 微分截面 积分截面     

低能电子与氮分子碰撞振动激发动量迁移截面的研究

采用作者改进的振动密耦合方法和基于量子力学从头计算的静电势、交换势、相关极化势,研究了低能电子与N₂振动激发散射动量迁移截面. 计算结果与试验符合较好. 关键词： 动量迁移截面 低能电子 分子碰撞 振动激发     

Modelling electron-N2 scattering in the resonant region

Quantum calculations of the resonant vibrational excitation of N₂ by electron impact are carried out using a model potential for exchange and correlation-polarization forces and exact static interaction. The inelastic process is treated within a coupled channel, space-frame formulation and final cross-sections are tested for convergence within less than of their values. Comparison with the experiments yields very good agreement with the latter data in the resonance region and suggests possible extension to calculations near the threshold openings for rovibrational inelastic processes induced by electron impact.     

Spontaneous Raman scattering: a useful tool for investigating the afterglow of nanosecond scale discharges in air

Nanosecond scale discharges are considered an interesting way for assisting combustion by enhancing either flame stabilization or ignition. Better understanding of energy deposit and radical species production processes is still required under pressure conditions normally encountered in combustion. The purpose of the present paper is to show that spontaneous Raman scattering, seldom used to investigate nanosecond pulsed discharges, is a useful measurement method for investigating the energy deposit of these discharges. The advantage of spontaneous Raman scattering is described by analyzing N₂ and O₂ spectra during the post-discharge of a filamentary nanosecond air discharge under atmospheric pressure, using phase-locked average spectra. The main advantages of spontaneous Raman scattering measurements are that they allow line-wise probing of different species with the same experimental setup and the determination of vibrational distribution by comparison with theoretical modeling over a wide range of vibrational levels (from v=0 to v=20 for N₂). The model proposed takes into account the high level of vibrational excitation and the strong non-equilibrium observed, allowing the characterization of the vibrational relaxation over the complete post-discharge duration. Although the rotational structure is not resolved, the rotational temperature and thus translational temperature are determined with a moderate uncertainty for T above 500 K.     

Vibrational and rotational excitation effects of the N(2D) + D2(X1Σg +) → ND(X3Σ+) + D(2S) reaction

The effects of the rovibrational excitation of reactants in the N(²D) + D₂(X¹Σ_g⁺) → ND(X³Σ⁺) + D(²S) reaction are calculated in a collision energy range from the threshold to 1.0 eV using the time-dependent wave packet approach and a second-order split operator. The reaction probability, integral cross-section, differential cross-section and rate constant of the title reaction are calculated. The integral cross-section and rate constant of the initial states v = 0, j = 0, 1, are in good agreement with experimental data available in the literature. The rotational excitation of the D₂ molecule has little effect on reaction probability, integral cross-section and the rate constant, but it increased the sideways and forward scattering signals. The vibrational excitation of the D₂ molecule reduced the threshold and broke up the forward–backward symmetry of the differential cross-section; it also increased the forward scattering signals. This may be because the vibrational excitation of the D₂ molecule reduced the lifetime of the intermediate complex.     

用振动密耦合方法研究低能电子与N2分子碰撞的振动激发微分散射截面

采用振动密耦合方法,分别应用球高斯分布极化势和优于绝热极化势,及基于量子力学从头计算的静电、交换势,得到入射电子能量2.40eV时0→2和0→3的振动激发微分散射截面,与目前优秀的实验值比较,获得了满意的结果,并从理论上分析了整个计算过程中可能影响微分散射截面精度的主要物理因素. 关键词： 分子碰撞 微分散射截面 振动激发 相互作用势     

Correlation-polarization effects in electron-atom scattering

The correlation-polarization (CP) model-potential, given by O’Connell and Lane (1983) as well as Padial and Norcross (1984) is examined for the elastic scattering of electrons by oxygen atoms, at intermediate energies. The correlation potential is found to be stronger than necessary at low energies. Two model polarization potentials based on the CP model, are suggested and employed to thee ⁻ — O scattering at 8.7, 30, 50 and 100 eV energies. The calculated total cross-sections agree in general with the other data at these energies.     

O3+与H2碰撞中非解离电荷转移过程的全量子计算

应用全量子的分子轨道强耦合方法,研究了基态的O³⁺(2s²2p ²P)与氢分子碰撞的非解离电荷转移过程,计算了不同方位角(25°,45°,89°),能量分别为100,500,1000和5000eV/u时的单电子俘获的振动分辨的态选择截面及相应的微分截面.分子轨道强耦合计算中采用了自旋耦合价带理论计算的三原子分子势能面和径向耦合矩阵元.对氢分子的自身转动,采用无限阶的冲量近似方法;对体系的电子运动同H₂或H^{+< 关键词： 非解离电荷转移过程 全量子的分子轨道强耦合方法 无限阶冲量近似 振动冲量近似国家自然科学基金(批准号：10604011 10574020)和国家高技术研究发展计划(863)惯性约束聚变领域资助的课题.}     

Theoretical prediction of a linear isomer for NeBr2(X1Γg + an ab initio approach

A supermolecular approach is used to predict the stationary structures of the NeBr₂(X¹Γ_g ⁺) van der Waals cluster. The intermolecular potential is calculated using the single and double excitation coupled-cluster method with non-iterative perturbation treatment of triple excitations [CCSD(T)]. Relativistic effects are included for the Br atoms using effective core potentials (ECPs) and their efficiency is tested for Br₂ and NeBr₂ molecules. Our results for NeBr₂ show minima for both linear and T-shaped configurations, in accord with previous ab initio calculations for rare gas-Br₂ species. The dependence of the interaction potential, as a function of the Br-Br bond, is also presented. Finally, vibrational analysis is carried out to examine the stability of the two isomers including zero-point vibrational energy effects.     

Differential cross section surfaces for low energy scattering of electrons and positrons from rare gas atoms

The differential cross sections for scattering of electrons and positrons from He, Ne, Ar, Kr, and Xe at projectile energies below the inelastic thresholds are calculated using a model potential approach in which the interaction between the projectile and the target atom is partitioned into static, exchange (for electrons), and correlation-polarization parts. Two different forms of the parameter-free correlation-polarization potential are suggested; in both cases the correlation-polarization potential is determined by smoothly matching the asymptotic form of the polarization potential (1/r ⁴) to the correlation potential at the outermost orbital radius of the target atom. The results of angular distributions are presented in the form of contours of constant differential cross sections as well as in the form of differential cross section surfaces in three-dimensional plots. Both of these presentations display the locations of the principal maxima and minima of the differential cross sections as well as the critical points in a very useful manner.     

Optical conductivity and electron interaction in the one-dimensional metal K2Pt (CN)4 Br0.3 · 3H2O

Experimental and theoretical investigations of the optical conductivity of K₂Pt (CN)₄Br_0,3 · 3H₂O single crystals for phonon energies near the plasma edge are reported. The imaginary part of the dielectric function is determined by only two scattering processes: Elastic scattering of holes by the Coulomb potentials of randomly distributed Br-ions and inelastic scattering by excitation of plasmons.     

The sub-bandgap energy loss satellites in the RIXS spectra of beryllium compounds

Resonant X-ray inelastic scattering spectra have been measured in BeO, phenakite (Be₂SiO₄) and chrysoberyl (BeAl₂O₄) with the excitation energy near the beryllium K edge.The RIXS spectra excited in the vicinity of the Be 1s core resonance show two principal features: the scattering on a valence excitation (which at higher excitation energies verges into the characteristic K_α emission), and a remarkably strong energy loss sideband to the elastic scattering peak. The energy loss shoulder appears to result from lattice relaxation in the absorption site. The comparison of the RIXS spectra of phenakite, chrysoberyl and BeO shows that the strength of the low energy sideband differs greatly; it is strongest in BeO and weakest in phenakite. The Si 2p RIXS spectra of phenakite also display a similar strong sub-bandgap energy loss tail.To gain further insight to this process, transitions in a system with a single vibrational mode have been modelled. The phonon relaxation has been simulated empirically by “smearing” the photoabsortion-populated vibrational levels with lower levels. This simple model is able to qualitatively explain this wide energy loss shoulder.     

Vibrationally elastice − — H2O scattering at intermediate energies

Vibrationally elastic total cross-sections ofe ⁻—H₂O scattering are calculated at intermediate energiesE _i=10–300 eV. The interaction potentials are treated in spherical models. The dipole rotational excitation, which is significant but not dominant above 10 eV, is treated incoherently. Effects of electronic excitation-ionization, significant above 30 eV or so, are considered through a complex optical potential. A dynamically distorted charge-density is employed to calculate the imaginary part of the complex potential. Comparisons are made with recent theoretical and experimental data. The mutual agreement is better in total cross-sections than in differential cross-sections.     

Vibrationally inelastic scattering of H∼ ions from H2, N2, O2 and CO2

State-resolved measurements are presented for vibrational excitation of H₂, N₂, O₂ and CO₂ by H^? impact in the collision energy rangeE _cm=20–180 eV and for scattering in the forward direction (0±0.5°). The data obtained from the measurements are the relative intensities and differential cross sections for vibrational excitation up toν′=4, the transition probabilitiesP _0→ν′ and the vibrational energy transferΔE _vib. For the systems H^?-H₂, N₂, O₂ the vibrational inelasticity increases in the order H₂-N₂-O₂. The mechanism for vibrational excitation in these systems is due to transient charge transfer from the H^? ion into antibonding orbitals of the target molecule which provides a bond stretching force during the collision. For H₂ and N₂, the results are compared with corresponding measurements for H⁺ scattering where the interaction mechanism is quite different. In the case of CO₂, vibrational excitation in forward scattering is caused primarily by the long-range dipole interaction. The spectra are very similar for H^?-CO₂ and H⁺-CO₂. Finer details are attributed to the influence of transient charge transfer and valence interactions.