Quasi-classical trajectory study of the stereodynamics of a Ne+H2+→NeH++H reaction

We have carried out a quasi-classical trajectory calculation for the reaction of Ne + H₂⁺ (v=0, j=1) → NeH⁺ + H on the ground state (1²A') using the LZHH potential energy surface constructed by Lü et al. [Lü S J, Zhang P Y, Han K L and He G Z 2010 J. Chem. Phys. 132 014303]. Differential cross sections at many collision energies indicate that the reaction is dominated by forward-scattering. In addition, the NeH⁺ product shows rotationally hot and vibrationally cold distributions. Stereodynamical results indicate that the products are strongly polarized in the direction perpendicular to the scattering plane and that the products rotate mainly in planes parallel to the scattering plane.     

Rotational excitation of CH<Subscript>4</Subscript> by He atoms

Quantum close-coupling and coupled-state approximation scattering calculations for rotational energy transfer of rotationally excited CH₄ due to collisions with He are presented for collision energies between 10⁻⁷ and 3000 cm⁻¹ using the MP4 potential of Calderoni et al. [J. Chem. Phys. 121, 8261 (2004)]. State-to-state cross sections and rate coefficients from selected initial rotational states of CH₄ in symmetries A, E, and F are studied from the ultra-cold to the thermal regime. Comparison of the cross sections with available theoretical results and experimental data show good agreement. Applications to astrophysics and cold laboratory environments are briefly addressed.     

The special features of rotationally resolved differential cross sections of the F + H2 reaction at small scattering angles

We studied the nature and collision energy dependence of the maximum that appears in the angular distributions of the HF (v′ = 3) product of the F + H₂ (v = 0; j = 0, 1, 2) → H + HF (v′, j′) reaction at small scattering angles θ in the center-of-mass frame. This maximum and its increase as the collision energy increased were discovered in the well-known experiment described by D.M. Neumark, A.M. Wodtke, G.N. Robinson, C.C. Hayden, and Y.T. Lee, J. Chem. Phys. 82 (7), 3045 (1985). In order to determine the nature of the maximum, we performed quantum-mechanical simulation of the reaction on the Stark-Werner ground state potential energy surface at collision energies of 1.84, 2.74, and 3.42 kcal/mol corresponding to the above-mentioned experiment and calculated the vibrationally and rotationally resolved differential cross sections dσ_v′j′/dΩ of the reaction. The maximum under consideration was found to be due to a superposition of two effects, namely, the absence of HF (v′ = 3; j′) products with large j′ because of energy restrictions and an increase in the relative amplitude of quantum-mechanical oscillations on dσ_v′j′/dΩ cross sections at small j′ and θ as v′ increased. Oscillations on dσ_3j′ /dΩ cross sections with small j′ are responsible for the maximum observed.     

Xe对NO(X)微分截面和非弹性散射中的碰撞诱导旋转准直

本文对NO(X)-Xe碰撞系统在碰撞能量为519 cm^-1,测量了完全?-双峰分解的微分截面和碰撞引起的旋转准直力矩. 同时结合初始量子态选择,使用六极杆的非均质电场,借助量子态分辨的测量,利用(1+1'')共振增强的多光子电离和速度离子成像. 结果显示,微分截面以及偏振相关的微分截面均显示与从头算势能面上进行的量子力学散射计算[J. K?os etal. J. Chem. Phys. 137, 014312 (2012)]一致. 通过与准经典轨迹、硬壳势能的量子力学散射以及运动近端模型的比较,评估了势能对所测微分截面和碰撞引起的旋转准直力矩的影响.     

Effect of ro-vibrational excitation of NeH~+ on the stereodynamics for the reactions H+NeH~+(v=1-3,j=1,3,5) →H_2~++Ne

The stereodynamics of the abstraction reaction H + NeH+(v = 1-3,j = 1,3,5) → H2+ + Ne is studied theoretically with a quasi-classical trajectory method on a new ab initio potential energy surface [ S J,Zhang P Y,Han K L and He G Z 2012 J.Chem.Phys.132 014303].The effects of vibrational and rotational excitation of reagent molecules on the polarization of the product are investigated.The reaction cross sections,the distributions of P(θr),P(φr),and polarizationdependent differential cross sections(PDDCSs) are calculated.The obtained cross sections indicate that the title reaction is a typical barrierless atom(ion)-ion(molecule) reaction.The initial vibrational excitation and rotational excitation of reagent molecules have distinctly different influences on stereodynamics of the title reaction,and the possible reasons for the differences are presented.     

Laser fields at flat interfaces: II. Plasmon resonances in aluminium photoelectron spectra

Using the model derived in paper I?[G. Ra?eev, Eur. Phys. J. D 66, 167 (2012)], this work presents calculations of the photoelectron spectrum (PES) of low index aluminium surfaces in the 10?C30?eV region. The laser is p or transverse magnetic linearly polarized incident on a flat structureless surface and its fields are modeled in I using the vector potential in the temporal gauge. This model uses a tensor and non-local isotropic (TNLI) susceptibility and solves the classical Ampère-Maxwell equation through the use of the vector potential from the electron density-coupled integro-differential equations (VPED-CIDE). The PE cross sections are the squares of the PE transition moments calculated using the VPED-CIDE vector potential function of the penetration coordinate. The PES is obtained in a one step model using either the Fermi golden rule or the Weisskopf-Wigner (WW) expressions. The WW cross section PES compares favorably with the experimental angle and energy resolved photoelectron yield (AERPY) spectrum of Levinson et?al. [Phys. Rev. Lett. 43, 952 (1979)], Levinson and Plummer [Phys. Rev. B 24, 628 (1981)] for Al(001) and of Barman et?al.?[Phys. Rev. B 58, R4285 (1998)], Barman [Curr. Sci. 88, 54 (2005)] for Al(111) surfaces. As in the experiment, our theoretical AERPY displays the multipole surface plasmon resonance at 11.32/12.75 eV for Al(001)/Al(111), mainly due to the surface contribution |??? _f |p·A|?? _i ?|², the bulk plasmon minimum at 15 eV and the two single particle excitation resonances at about 16 and 22 eV. The nature of the plasmon resonances of the PES is analyzed using the reflectance, the electron density induced by the laser and Feibelman??s parameter d _?? all introduced in paper?I.     

Total cross sections of electron scattering by molecules NF3, PF3, N(CH3)3, P(CH3)3, NH(CH3)2, PH(CH3)2, NH2CH3 and PH2CH3 at 30–5000 eV

Total cross sections of electron scattering by eight molecules NF₃, PF₃, N(CH₃)₃, P(CH₃)₃, NH(CH₃)₂, PH(CH₃)₂, NH₂CH₃ and PH₂CH₃, which have some structural similarities, are calculated at the Hartree-Fork level by the modified additivity rule approach [D.H. Shi, J.F. Sun, Z.L. Zhu, H. Ma, Y.F. Liu, Eur. Phys. J. D 45, 253 (2007); D.H. Shi, J.F. Sun, Y.F. Liu, Z.L. Zhu, X.D. Yang, Chin. Opt. Lett. 4, 192 (2006)]. The modified additivity rule approach takes into considerations that the contributions of the geometric shielding effect vary as the energy of incident electrons, the dimension of target molecule, the number of electrons in the molecule and the number of atoms constituting the molecule. The present investigations cover the impact energy range from 30 to 5000 eV. The quantitative total cross sections are compared with those obtained by experiments and other theories. Excellent agreement is observed even at energies of several tens of eV. It shows that the modified additivity rule approach is applicable to carry out the total cross section calculations of electron scattering by these molecules at intermediate and high energies, in particular over the energy range above 80 eV or so. It proves that the microscopic molecular properties, such as the geometrical size of the target and the number of atoms constituting the molecule, are of crucial importance in the TCS calculations. The new results for PH(CH₃)₂ and PH₂CH₃ are also presented at energies from 30 to 5000 eV, although no experimental and theoretical data are available for comparison. In the present calculations, the atoms are still represented by the spherical complex optical potential, which is composed of static, exchange, polarization and absorption terms.     

Calculated ionization cross sections for proton-fullerene ion collisions

A simple jellium model is constructed in order to obtain one-electron wave functions for the valence electrons of the fullerene. With this jellium wave function we have calculated ionization cross sections for proton-C₆₀ ⁺ collisions in the semiclassical approximation. For higher projectile velocities, for which the semiclassical approximation is valid also for electron impact, theoretical cross sections fit satisfactorily the experimental data of Völpel et al. [Phys. Rev. Lett. 71 (1993) 3439].     

Collisional-radiative model for non-Maxwellian inductively coupled argon plasmas using detailed fine-structure relativistic distorted-wave cross sections

Our recently developed collisional-radiative model which included fine-structure cross sections calculated with a fully relativistic distorted-wave method [R.K. Gangwar, L. Sharma, R. Srivastava, A.D. Stauffer, J. Appl. Phys. 111, 053307 (2012)] has been extended to study non-Maxwellian inductively coupled argon plasmas. We have added more processes to our earlier collisional-radiative model by further incorporating relativistic distorted-wave electron impact cross sections from the 3p ⁵4sJ = 0, 2 metastable states, (1s ₃, 1s ₅ in Paschen’s notation) to the 3p ⁵5p (3p _i ) excited states. The population of various excited levels at different pressures in the range of 1–25 mTorr for an inductively coupled argon plasma have been calculated and compared with the recent optical absorption spectroscopy measurements as well as emission model results of Boffard et al. [Plasma Sources Sci. Technol. 19, 065001 (2010)]. We have also calculated the intensities of two emission lines, 420.1 nm (3p ₉ → 1s ₅) and 419.8 nm (3p ₅ → 1s ₄) and compared with measured intensities reported by Boffard et al. [J. Phys. D 45, 045201 (2012)]. Our results are in good agreement with the measurements.     

Molekularstrahlmessungen von Stoßquerschnitten für Übergänge zwischen definierten Rotationszuständen zwei-atomiger Moleküle

Inelastic collision cross sections for transitions between specified rotational states designated by (J, M) have been measured in a molecular beam apparatus. With an electrostatic four pole field molecules in a specified rotational state are separated out of a molecular beam and focussed into a gas filled scattering chamber. Molecules which have been scattered by less than 1/2° are then collected in a second four pole field, located directly behind the scattering chamber, and are analyzed for their rotational state. From a comparison of the measured pressure dependence with calculated curves a determination of inelastic collision cross sections for specified quantum jumps is possible. Measured inelastic scattering cross sections for the transitions (2,0→3,0) are reported for the gases He, Ne, Ar, Kr, CH₄, SF₆, H₂, O₂, Air, N₂O, H₂O, CF₂Cl₂. The values range between about 5 and 100 Ų in the order indicated. The scattering gases NH₃ und ND₃ yielded larger cross sections of about 600 Ų and, in addition, the transitions (3,0)→(2,0),(1,0)→(2,0), (2,0)→(1,0) and (3,0)→(1,0) were observed. Total cross sections for the same gases were also measured with the apparatus.     

Multielectron processes in collisions of Xe23+ ions with Ar atoms

We report the measurements of relative cross sections for multielectron processes in collisions of Xe²³⁺ ions with argon atoms in the velocity range of 0.65–1.32 a.u. By means of the coincidence time-of-flight (TOF) technique, the final charge states of both the projectile and target ions for each collision event are determined. The present experimental data are compared with the scaling law by Selberg et al. [Phys. Rev. A 54, 4127 (1996)] and the extended classical over-barrier (ECB) model.     

Rotational excitation of NH<Subscript>3</Subscript> and ND<Subscript>3</Subscript> due to He atom collisions

Quantum close-coupling and coupled-states approximation scattering calculations for rotational energy transfer of rotationally excited NH₃ and ND₃ due to collisions with He are presented. Calculations were performed for collision energies between 10^-5 and 10 000 cm^-1 using the NH₃-He potential of Hodges and Wheatley [J. Chem. Phys. 114, 8836 (2001)]. State-to-state and total quenching cross sections from some selected initial states are presented. Rate coefficients for ortho-NH₃ for the quenching 10+→00+ transition were obtained on potentials scaled to reproduce measurements of second virial coefficients with the results showing strong sensitivity to the potential, especially at low temperatures. Significant isotope effects are found in quenching cross sections in the cold to ultracold regime particularly in the region dominated by quasi-bound resonances, ~0.1 to 10 cm^-1. As ammonia has been translationally cooled via Stark deceleration methods, it is a good candidate for experimental study of such effects at cold temperatures. Comparison of rate coefficients with available theoretical results are also presented.     

Quenching vibrations of cesium dimers by He at low and ultralow temperatures: quantum dynamical calculations

This paper analyses in detail the energy redistribution from the upper vibrational levels of Cs dimers, thought to be obtained from initial recombination processes that generate excited internal states of the triplet configuration ³ Σ _u ⁺ . Their quenching is examined as they are made to further collide with ⁴He buffer gas at temperatures below and around 100 mK. The relevant cross sections are computed by using a multichannel quantum dynamical approach and employ a full, ab initio potential energy surface. Due to their smallness (see Ref. [R.B. Ross, J.M. Powers, T. Atashroo, W.C. Ermler, I.A. LaJohn, P. Christiansen, J. Chem. Phys. 93, 6654 (1999)]) the fine structure effects have not been explicitly included in this study. The final, cumulative cross-sections are discussed and analyzed in terms of the overall quenching behavior shown by different initial states of the dimer and in terms of the changing ratios between collisional cooling and vibrational quenching cross sections as a function of trap temperature. The corresponding quenching rates are also computed and analysed.     

Electronic excitation of HgX (X = Cl,Br, I) due to electron and methyl mercury halide collisions

Electronic excitation of HgX (X = Cl, Br, I) radicals in the B-state has been observed as the result of collisions with low energy electrons and methyl mercury halide (CH₃HgX) molecules. The emission intensity has been observed to be much weaker than that observed for electron-HgX₂ collisions under similar experimental conditions. Using the strongest band head of the B-X band system, an attempt has been made to calculate the emission cross section due to electron CH₃HgX collisions at 10 eV electron kinetic energy. For HgCl, HgBr, and HgI radicals, these cross sections are 1 × 10^-18, 7 × 10^-17, and 2 × 10^-17 cm², respectively, with an estimated uncertainty of ±30%. Our measured threshold electron energy for excitation of CH₃HgX molecules and observation of the B-X emission band system and emission cross sections measured at 10 eV are greatly different from those measured by Allision and Zare [Chem. Phys. 35, 263 (1978)].     

Application of R-matrix method to electron-H<Subscript>2</Subscript>S collisions in the low energy range

Electron-H₂S collision process is studied using the R-matrix method. Nine low-lying states of H₂S molecule are considered in the R-matrix formalism to obtain elastic integral, differential, momentum transfer and excitation cross sections for this scattering system. We have represented our target states using configuration interaction (CI) wavefunctions. We obtained adequate representation of vertical spectrum of the target states included in the scattering calculations. The cross sections are compared with the experiment and other theoretical results. We have obtained good agreement for elastic and momentum transfer cross sections with experiment for entire energy range considered. The differential cross sections are in excellent agreement with experiment in the range 3–15 eV. A prominent feature of this calculation is the detection of a shape resonance in ²B₂ symmetry which decays via dissociative electron attachment (DEA). Born correction is applied for the elastic and dipole allowed transition to account for higher partial waves excluded in the R-matrix calculation. The electron energy range is 0.025–15 eV.     

Diffraction scattering of Λ 3 H and Λ 6 He hypernuclei on nuclei with allowance for edge diffuseness, the structure of hypernuclei, and multiple-scattering effects

General formulas for the amplitudes of the diffraction scattering of two-and three-cluster loosely bound nuclei on spherical nuclei for an arbitrary dependence of the profile functions on the impact parameter are represented in a form that is convenient for calculations. The differential cross sections for the elastic scattering of _Λ ³ H and _Λ ⁶ He hypernuclei and the total cross sections are obtained with allowance for the diffuseness of the target-nucleus edge, the binding energy of incident hypernuclei, the ranges of nuclear forces between the clusters in the hypernuclei, and multiple (double and triple) scattering. Changes in the behavior of the cross sections in response to a transition from the two-cluster to the three-cluster model of the aforementioned nuclei are revealed.     

Sub-Coulomb transfer and fission in collisions of129Xe,132Xe and136Xe with238U

Integral cross sections for fission and for one- and two-neutron transfer reactions in the system¹³²Xe+²³⁸U were measured radiochemically in the energy range 0.7≦E/E _Coul≦1. The excitation functions for fission and transfer are found to be essentially parallel below 0.85×E _Coul. Even at the lowest energies the transfer cross sections exceed the fission cross section by more than one order of magnitude. With the other projectiles¹²⁹Xe and¹³⁶Xe different transfer cross sections illustrating their sensitivity for the ground stateQ-values,Q _gg , are observed while the fission cross sections are the same as in the¹³²Xe +²³⁸U reaction. The fission data are interpreted in terms of a continuous transition between Coulomb fission and several transfer-induced fission processes.     

Method for calculating photoionization cross sections of fullerenes in the local density and random phase approximations

A method for calculating the photoionization cross sections of fullerenes taking into account many-electron correlations on the basis of the local density and random phase approximations is proposed and implemented. Calculations are made specifically for fullerenes C₆₀ and C₂₀. It is shown that the photoionization spectrum of C₆₀ acquires a plasmon resonance whose position and magnitude are in good agreement with experimental results [I.V. Hertel, H. Steger, J. de Vries et al., Phys. Rev. Lett. 68, 784 (1992)] and with the results of other calculations [M.J. Puska and R.N. Nieminen, Phys. Rev. A47, 1181 (1993)]. The emergence of a giant resonance is predicted in the photoionization spectrum of fullerene C₂₀ with the center at a photon energy on the order of 27 eV, which corresponds to the frequency of resonant surface plasmon oscillations in a conducting sphere.     

Experimental determination of the scattering length for positron scattering from krypton

We report the first experimentally supported determination of the scattering length for positron scattering from krypton. Our result of  ?10.3 ± 1.5 a.u. compares favourably with that from a convergent close coupling calculation performed as a part of this investigation (?9.5 a.u.), and also with an earlier many body theory calculation of  ?10.1 a.u. from Gribakin and Ludlow [Phys. Rev. A 70, 032720 (2004)] and a polarized-orbital result of  ?10.4 a.u. from McEachran et al. [J. Phys. B 13, 1281 (1980)]. The present experimental scattering length supports the existence of a low-lying positron-krypton virtual state (Surko et al. [J. Phys. B 38, R57 (2005)]) at an energy ε = 0.13 eV.