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.     

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     

低能电子与H_2分子碰撞振动激发动量迁移散射截面的研究

采用振动密耦合方法及基于量子力学从头计算的静电势、交换势和相关极化势,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.通过包含18个振动波函数、8个分波和16个分子对称性,得到了收敛性很好的ν=0→ν′=0,1,2,3,4等几个振动跃迁通道的动量迁移散射截面值,并在入射电子能量1eVE≤10eV时给出了比以前的理论研究更为合理的总的动量迁移散射截面.     

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     

Measurement of OH spatially resolved spectrum in a wire-plate pulsed streamer discharge

In this study, spatially resolved measurements of the emission intensity of OH (A²Σ↦X²Π, 0-0) and the vibrational temperature of N₂ (C) have been performed during a positive pulsed streamer discharge with a wire-plate electrode configuration at atmospheric pressure. The effects of pulse peak voltage, pulse repetition rate and the added O₂ flow rate on the spatial distributions of the emission intensity of OH (A²Σ↦X²Π, 0-0) and the vibrational temperatures of N₂ (C) perpendicular to the wire in the direction towards the plate (in the radial direction) are investigated. It has been found that the emission intensity of OH (A²Σ↦X²Π, 0-0) increases with increasing pulse peak voltage and pulse repetition rate and decreases with increasing the distance from the wire electrode. When the different oxygen flows are added in N₂ and H₂O mixture gas, the emission intensity of OH (A²Σ↦X²Π, 0-0) decreases with increasing the flow rate of oxygen. The vibrational temperature of N₂ (C) is nearly independent of pulsed peak voltage and pulsed repetition rate, but increases with increasing the added O₂ flow rate and keeps almost constant in the radial direction under the present experimental conditions. This measurement plays a crucial role in understanding the discharge characters of pulsed streamer discharge and establishing the molecule reaction dynamics model of pulsed streamer discharge.     

Electronic excitation and singlet-triplet coupling in uracil tautomers and uracil-water complexes

Electronic spectra of uracil in its diketo (lactam) form and five enol (lactim) tautomeric forms have been investigated by means of combined density functional and configuration interaction methods. We have simulated the effects of hydrogen bonding with a protic solvent by recomputing the spectrum of uracil in the presence of two, four, or six water molecules. Geometries of the electronic ground state and several low-lying excited states have been optimized. Spin-orbit coupling has been determined for correlated wavefunctions employing a non-empirical spin-orbit mean-field approach. In accord with experiment, we find the diketo tautomer to be the most stable one. The calculations confirm that the first absorption band arises from the ¹( π↦π^*) S ₀↦S ₂ excitation. The experimentally observed vibrational structure in this band originates from a breathing mode of the six ring. Complexation with water molecules is seen to cause a significant blue shift of n↦π^* excitations while leaving π↦π^* excitations nearly uninfluenced. Computed radiative lifetimes are presented for the experimentally known weak phosphorescence from the π↦π^* excited T₁ state. Among the uracil lactim tautomers, one is particularly interesting from a spectroscopic point of view. In this tautomer, the π↦π^* excitation gives rise to the S₁ state. Received 18 February 2002 / Received in final form 5 June 2002 Published online 13 September 2002     

Studies on the vibrational excitation differential cross sections of non-resonant e-N2 scattering using augmented polarization potentials

Distributed spherical Gaussian (DSG) correlation-polarization model potentials with higher-order terms and exact exchange effects in single-configuration Slater determinant are taken into account for low-energy vibrational excitation e-N₂ scattering system. The integrodifferential coupled channel equations are solved using a combination of linear-algebraic and R-matrix-propagator algorithms. Analytic Born completion is used to calculate high-order scattering matrix elements in order to obtain convergent differential cross sections. The energy range is set to 4–15 eV which is not tested by the present theoretical method before. The overall agreement of theoretical results with the latest experiments emphasizes the importance of higher-order correlation-polarization potentials and rigorous exchange effects in vibrational excitation scattering.     

Vibrational inelastic electron-H<Subscript>2</Subscript> scattering revisited: numerically converged coupled channels space frame calculations with model interactions

The collisional excitation of the lower vibrational levels of H₂(¹Σ_g⁺) molecules by low-energy electron impact is computed using an empirical model potential and by solving the coupled-channels scattering equations within a space-fixed (SF) frame of reference formulation. Numerically converged partial, integral inelastic and elastic cross-sections are obtained from what is an essentially exact treatment of the dynamics and the results are compared with measurements and with earlier calculations on the same system. The usefulness of the SF method for handling excitation processes at near-threshold collision energies is discussed and analyzed through the calculations of collisional superelastic partial cross-sections down to 10^-2 meV of collision energy.     

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     

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.     

Interaction of Electrons with Indole,Tryptophan, and their Derivatives in the Gas Phase

The electron energy loss spectra (EELS) of indole, 3-indolyl propionic acid, 3-indolealdehyde, 3-dimethylaminomethylindole, tryptophan, and N-acetyl-L-tryptophan in the gas phase upon excitation by monokinetic electrons with an energy of E₀ = 11–50 eV are obtained. The structure of EELS is determined in the main by the indole chromophore; the side groups, except for the C=O group of 3-indolealdehyde, exert an insignificant influence. The energy of the lower triplet level ³L_a is 3.3 eV for indole and its derivatives and 3.2 eV for tryptophan and N-acetyl-L-tryptophan. Four singlet transitions in the region of 4.4–7.2 eV have been identified. The molecules studied, except for tryptophan, fluoresce in the gas phase on excitation by electrons. At low values of E₀ (10–25 eV), the fluorescence spectra are similar and are due to the indole fluorophore. Just as in the case of optical excitation, fluorescence on excitation by electrons is associated with the ¹L_b-S₀ transitions. An increase in the energy E₀ up to 60–80 eV leads to dissociation of a portion of the indole molecules and to the appearance of additional bands in the fluorescence spectrum. __________ Translated from Zhurnal Prikladnoi Spektroskopii, Vol. 72, No. 4, pp. 468–472, July–August, 2005.     

Chemical reactions of water molecules on Ru(0 0 0 1) induced by selective excitation of vibrational modes

Tunneling electrons in a scanning tunneling microscope were used to excite specific vibrational quantum states of adsorbed water and hydroxyl molecules on a Ru(0 0 0 1) surface. The excited molecules relaxed by transfer of energy to lower energy modes, resulting in diffusion, dissociation, desorption, and surface-tip transfer processes. Diffusion of H₂O molecules could be induced by excitation of the O-H stretch vibration mode at 445 meV. Isolated molecules required excitation of one single quantum while molecules bonded to a C atom required at least two quanta. Dissociation of single H₂O molecules into H and OH required electron energies of 1 eV or higher while dissociation of OH required at least 2 eV electrons. In contrast, water molecules forming part of a cluster could be dissociated with electron energies of 0.5 eV.     

Time-dependent analysis of tunneling effect in the formation of ultracold molecules via photoassociation of laser-cooled atoms

The paper contains a time-dependent investigation of the tunneling effect observed in the photoassociation spectrum of Cs₂ and attributed to the 0_g ^-(6s, 6p _3/2) double well. When by photoassociation of two cold cesium atoms a vibrational level of the outer well is populated, tunneling is an efficient mechanism for transferring the population to the inner well (R < 15a ₀), where spontaneous emission may lead to formation of cold molecules in low vibrational levels of the a ³Σ⁺ _u(6s, 6s) electronic state. This tunneling effect is analyzed by wavepackets propagation, first considering the double well potential alone, and following a packet made by a superposition of states initially located at large distances. Characteristic times for the vibration dynamics, corresponding to a beating phenomenon between the two wells, to partial “revival” at large distances, and to maxima in the population localized in the inner well are reported and discussed. Second, we simulate the two-channels a ³Σ⁺ _u(6s, 6s)↦0_g ^-(6s, 6p _3/2) photoassociation at detunings around 2.9 cm^-1: the inner well can be populated either by the excitation of a vibrational level of the external well (resonant excitation), or by tuning the photoassociation laser at the energy of the inner well level which displays tunneling (“off-resonance excitation”). In the first case the photoassociation is efficient, while the tunneling probability is small; in the second, the tunneling probability is large, so that despite the poor efficiency of the photoassociation process, more population can be transferred to the inner well. This second choice is shown to be very sensitive to the laser intensity, which could be used to control the population of the inner well and hence the formation of ultracold molecules in low vibrational levels. Received 19 April 2002 Published online 1st October 2002 RID="a" ID="a"e-mail: francoise.masnou@lac.u-psud.fr     

Femtosecond laser pulse train effect on Doppler profile of cesium resonance lines

We present direct observation of the velocity-selective optical pumping of the Cs ground state hyperfine levels induced by the femtosecond (fs) laser oscillator centered at either D2 (6 ²S_1/2↦6 ²P_3/2, 852 nm) or D1 (6 P_1/2, 894 nm) cesium line. We utilized previously developed modified direct frequency comb spectroscopy (DFCS) which uses a fixed frequency comb for the excitation and a weak cw scanning probe laser centered at the ¹³³Cs 6 ²S_1/2↦6 ²P_3/2 transition (D2 line) for ground levels population monitoring. The frequency comb excitation changes the usual Doppler absorption profile into a specific periodic, comblike structure. The mechanism of the velocity selective population transfer between the Cs ground state hyperfine levels induced by fs pulse train excitation is verified in a theoretical treatment of the multilevel atomic system subjected to a pulse train resonant field interaction.     

Influence of pressure on the relative population of the two lowest vibrational levels of the C <Superscript>3</Superscript> Π<Subscript>u</Subscript> state of nitrogen for electron beam excitation

Continuous and pulsed 12 keV electron beams were used to excite nitrogen within a gas cell at pressures ranging from 10 to 1400 hPa. The pressure dependence of the ratio of photon fluxes for emission from vibrational levels v'=0 and 1 of the C ³Π _u state has been studied. The results confirm the presence of a collisional excitation mechanism populating v'=0, 1 in addition to electron impact excitation. Rate constants of (1.27 ±0.04)×10^-11 cm³s^-1 [ v'=0] and (2.68 ±0.08)×10^-11 cm³s^-1 [ v'=1] were measured for C ³Π _u quenching by ground state nitrogen. For electron beam conditions relative excitation efficiencies of 1:0.59:0.22 for vibrational levels 0, 1 and 2 were calculated. The recorded flux ratios are compared with the predictions given by a vibrational relaxation model.     

Production of a0-mesons in the reactions πN↦a0N and pp↦da0 + at GeV energies

We investigate the reactions πN↦a ₀ N and pp↦da ₀ ⁺ near threshold and at medium energies. An effective Lagragian approach and the Regge pole model are applied to analyze different contributions to the cross-section of the reaction πN↦a ₀ N. These results are used to calculate the differential and total cross-sections of the reaction pp↦da ₀ ⁺ within the framework of the two-step model in which two nucleons produce an a₀-meson via π-meson exchange and fuse to a deuteron. The necessity of new measurements on a₀ production and branching fractions (of its decay to the K and πη channels) is emphasized for clarifying the a₀ structure. Detailed predictions for the reaction pp→da ₀ ⁺ are presented for the energy regime of the proton synchrotron COSY-Jülich. Received: 4 August 2000 / Accepted: 17 September 2000     

Schwingungsanregung von H2-Molekülen durch Zentralstoß mit Li+-Ionen

An apparatus is described for measuring the inelastic differential cross section for vibrational excitation in collisions of diatomic molecules with monoenergetic ions at laboratory energies between 10 and 50 eV. The method consists of measuring the time of flight of single ions with a time amplitude converter and displaying the results on a 100 channel pulse height analyzer. From the shift in the time of flight relative to that expected for elastic scattering the final state of the molecule excited in a single collision is identified. By studying only central collisions with almost zero impact parameter rotational excitation is strongly suppressed. Measured times of flight after collisions of monoenergetic Li⁺ ions with H₂ show that with increasing energy the most probable vibrational quantum jump increases from 0→1 to 0→2,0→3 etc. Contrary to the usual assumption of a small steric factor for vibrational excitation the results show that the inelastic cross section is larger than the elastic cross section. Using reported potential parameters the energy dependence of the most probable excited state is compared with the calculations of Secrest and Johnson for a one-dimensional collinear collision. The satisfactory agreement suggests that the steric factor is close to 1. From measurements at different scattering angles at 10 eV the integral inelastic cross section is found to be about 0.2 Ų corresponding to a differential cross section of 0.4 Ų/sr. Measured values of integral and differential total cross sections for Li⁺-He andLi⁺-H₂ are reported and compared with theory. Direct dissociation of D₂ by Li⁺ in the energy range from 25 to 55 eV was not observed, yielding an upper limit for the cross section of 4 · 10^?4 Ų/sr.     

Tails of the dynamical structure factor of 1D spinless fermions beyond the Tomonaga approximation

We consider one-dimensional (1D) interacting spinless fermions with a non-linear spectrum in a clean quantum wire (non-linear bosonization). We compute diagrammatically the 1D dynamical structure factor, S(ω,q), beyond the Tomonaga approximation focusing on it's tails, |ω| ≫vq, i.e. the 2-pair excitation continuum due to forward scattering. Our methodology reveals three classes of diagrams: two “chiral” classes which bring divergent contributions in the limits ω→±vq, i.e. near the single-pair excitation continuum, and a “mixed” class (so-called Aslamasov-Larkin or Altshuler-Shklovskii type diagrams) which is crucial for the f-sum rule to be satisfied. We relate our approach to the T=0 ones present in the literature. We also consider the case and show that the 2-pair excitation continuum dominates the single-pair one in the range: |q|T/k_F ≪ω±vq ≪T (substantial for q ≪k_F). As applications we first derive the small-momentum optical conductivity due to forward scattering: σ∼1/ω for T ≪ω and σ∼T/ω² for T ≫ω. Next, within the 2-pair excitation continuum, we show that the attenuation rate of a coherent mode of dispersion Ω_q crosses over from , e.g. γ_q ∼|q|³ for an acoustic mode, to , independent of Ω_q, as temperature increases. Finally, we show that the 2-pair excitation continuum yields subleading curvature corrections to the electron-electron scattering rate: , where V is the dimensionless strength of the interaction.     

Separation of dipole and impact scatterings in high resolution electron energy loss spectroscopy: Experiment from model organic material

The interpretation of High Resolution Electron Energy Loss Spectroscopy (HREELS) spectra recorded from polymers remains a difficult task because of (1) the relatively poor resolution achieved on these non-ordered systems, (2) the large number of vibrational features induced by the numerous chemical groups in the monomer unit, (3) the superposition of the dipole, impact and resonant scattering mechanisms. In this report, the study of the physical mechanisms responsible for the electron–molecular vibration coupling is investigated, using a simple model system consisting of a well-ordered film of eicosanoic acid adsorbed on a GeS substrate and an hypothesis supposing that dipole scattering is extinguished in non specular geometry. The ordered character of the molecular layer allowed to separate the dipole from the impact contributions in the signal recorded in specular geometry. The results support the idea that any vibrational mode of an organic compound induced by electron excitation contains both contributions with different relative extent, depending on the chemical nature of the molecular group involved in the vibration and their orientation. Cross section measurements for both interaction mechanisms are in agreement with theoretical prediction, confirming the validity of this new and original method suggested for the separation of the interaction mechanisms. Furthermore, we measured a resonance near 6 eV impact energy as the intensity of the ν(C–D) band is enhanced for this impact energy. This observation again is in agreement with our hypothesis that the impact scattering is the dominant interaction mechanism involved in the vibrational excitation of the C–D group. This study allowed for a model of the geometry of adsorption of the molecule on the substrate. It is confirmed that the eicosanoic acid adsorbs the COO group on the substrate, with the long hydrocarbon chain standing up and the CD₃ terminating group pointing out of the surface.     

Absolute collision cross sections for low energy electron scattering from NO: the role of resonances in elastic scattering and vibrational excitation

Absolute measurements of elastic scattering and vibrational excitation of the NO molecule by low energy electron impact (0.4-2.5 eV) are presented. They show that previous estimates of these cross sections may be in error by as much as a factor of 3 and provide compelling evidence for a reassessment of the balance between elastic scattering and vibrational excitation at incident energies below 2 eV. They also confirm the critical contribution that intermediate negative ion resonances (NO-) make to the various scattering processes for this molecule at low incident energies.