Product state distributions and rotational polarization for the crossed beam reactions of Ca with F2 and NF3

Product state distributions of the CaF products from the thermal crossed beam reactions Ca + F₂ and Ca + NF₃ have been measured using laser induced fluorescence (LIF) techniques. We obtain information about the rotational and vibrational distributions by generating synthetic band profiles and comparing them with those observed. The inverted vibrational distributions indicate direct reaction mechanisms. For Ca + F₂ the fractionf′ of energy is nearly half going into product translation and the remainder being devided nearly equally between product rotation and vibration. For Ca + NF₃ the largest fraction of the available reaction exoergicity goes into vibrational excitation of the newly formed CaF products. In addition, we have probed the rotational polarization of CaF product molecules. This gives direct information on the role of angular momentum alignment in reactive scattering.     

Advanced adiabatic approximation for momentum distributions of ejected electrons in slow atomic collisions

The problem of determination of momentum distributions of ejected electrons in slow atomic collisions is studied within the impact-parameter method by using a dynamic adiabatic basis which takes into account the correct boundary conditions. An expression is obtained which relates the momentum distribution of the ejected electrons with a coherent sum of the delocalized dynamic adiabatic eigenstates (elementary wavepackets). The form of the momentum distribution exactly coincides with the form of the total wavepacket in configuration space. General formulas are applied to a model problem of electron detachment in the process in which the electron-atom interactions are described by the zero-range potentials. In the example considered, the momentum distribution of ejected electrons, in the center-of-mass frame, exhibits a maximum located in the scattering plane on the circle of radius (in atomic units), where v is the relative collision velocity and is the impact parameter. Received: 5 October 1998     

Poincaré-sphere equivalent for light beams containing orbital angular momentum

The polarization state of a light beam is related to its spin angular momentum and can be represented on the Poincaré sphere. We propose a sphere for light beams in analogous orbital angular momentum states. Using the Poincaré-sphere equivalent, we interpret the rotational frequency shift for light beams with orbital angular momentum [Phys. Rev. Lett. 80, 3217 (1998)] as a dynamically evolving geometric phase.     

甲基自由基在212.5 nm的光分解:母体内能态的激发对产物态分布的影响

利用里德堡氢原子飞渡时间谱的方法,进行了甲基自由基在212.5nm 的光解动力学的实验研究.甲基自由基来自于碘甲烷分子在266nm 的光分解.实验测量了不同振动态的甲基自由基通过3s 电子激发态解离的产物 CH_2自由基的平动能分布和角分布,并从平动能分布得到了 CH_2自由基的转动布居.实验同时详细地研究了母体分子甲基自由基的振动和转动激发对光解动力学的影响.实验结果表明母体分乙甲基自由基的伞形振动对于产物的转动激发和角分布均有较大的影响,而母体分子的转动激发只对产物的角分布有较明显的影响.     

Investigation on phase and shape transitions in the hot rotating nucleus <Superscript>154</Superscript>Dy

A statistical theory for hot rotating nuclei incorporating deformation, collective and non-collective rotational degrees of freedom, shell effects and pairing correlations is used to investigate the occurrence of phase and shape transitions in the hot rotating deformed nucleus ¹⁵⁴Dy . The interplay of various degrees of freedom and their influence on the behavior of nuclei formed as fused compounds in heavy-ion reactions are studied. A phase transition from the superfluid to normal state in the nucleus with increasing temperature and angular momentum is observed. The effect of pairing on the level density parameter and nucleon separation energy has been analyzed and is found to be substantial. The neutron and proton separation energies extracted as a function of the angular momentum and temperature is found to decrease sharply for particular angular momentum states of the nucleus due to shape transitions from prolate collective to oblate non-collective at higher temperatures.     

Isotope effect on the stereodynamics for the collision reaction H＋LiF（v = 0, j = 0） → HF＋Li

Stereodynamics for the reaction H+LiF(v=0, j=0) → HF+Li and its isotopic variants on the ground-state (1 2 A′) potential energy surface (PES) are studied by employing the quasi-classical trajectory (QCT) method. At a collision energy of 1.0 eV, product rotational angular momentum distributions P (θr), P (φr), and P (θr ,φr), are calculated in the center-of-mass (CM) frame. The results demonstrate that the product rotational angular momentum j′ is not only aligned along the direction perpendicular to the reagent relative velocity vector k, but also oriented along the negative y axis. The four generalized polarization-dependent differential cross sections (PDDCSs) are also computed. The PDDCS 00 distribution shows a preferential forward scattering for the product angular distribution in each of the three isotopic reactions, which indicates that the title collision reaction is a direct reaction mechanism. The isotope effect on the stereodynamics is revealed and discussed in detail.     

Effects of reagent's rotational and vibrational excitations on reaction O(3P) + H2 H2(ν = 0, 3, j = 0, 3; 5; 7; 9; 12; 15) → OH + H

To investigate the effect of reagent's rotational and vibrational excitations on the stereo-dynamics of reaction product, the title reaction is theoretically simulated using the quasi-classical trajectory (QCT) method on the ³A" and ³A′ potential energy surfaces (PESs). The reaction cross section is considered as the only scalar property in this work at four different collision energies. Furthermore the vector properties including two polarization-dependent differential cross sections (PDDCSs), the angular distributions of product' rotational momentum are discussed at one fixed collision energy. Effects of reagents' rotational excitation on the reaction do exist regularly.     

Electron angular distributions in double photoionization: Use of effective Sommerfeld parameters

We present calculations of the fivefold differential cross-section (FDCS) for double photoionization of helium at excess energies of 6 and 20 eV above threshold. Our results are obtained using for the final double-continuum state a product of three Coulomb wave functions, with the Sommerfeld parameters modified to describe the strength of interaction of any two particles affected by the third particle. Our calculations are compared with recent absolute measurements by D?rner et al. (Phys. Rev. A 57, 1074 (1998)), both in coplanar and non-coplanar geometries. Very good agreement is obtained for the shape of the angular distributions, and differences in the absolute magnitude exist in comparison with the standard choice of Sommerfeld parameters. Received: 17 July 1998 / Received in final form and Accepted: 23 October 1998     

C (~3P)+NO (X~2Ⅱ)→CN (X~2∑+)+O (~3P) 反应的矢量相关研究

采用准经典轨线方法研究了三个不同碰撞能下,反应C(~3P)+NO (X~2∏)→CN (X~2∑+)+O(~3P) 在Nyman等拟合的两个势能面(~2A″和~2A′)上反应物与产物之间的矢量相关.结果表明在两个势能面上产物的转动角动量矢量不仅取向,而且沿着y轴垂直于散射平面定向,产物的角动量定向依赖于碰撞能和势能面.同时,计算的四个重整化极化依赖微分截面显示产物在三个散射角被强烈极化,这与在两个势能面上的三个过渡态有关.     

Dynamics of photoinduced reactions at oxide surfaces

This report summarizes our work on UV-laser induced desorption of small molecules and atoms from transition metal oxides. The systems presented serve as examples for a simple photochemical reaction, the fission of the molecule surface bond. State resolved detection methods were used to record the final state distributions of the desorbing neutral molecules. Detailed results on the systems NO/NiO(1 1 1) and CO/Cr₂O₃ (0 0 0 1) are presented. The experiments include investigations on stereodynamic aspects like the angular distributions of the desorbing molecules and, in the case of CO desorption, the rotational alignment with respect to the surface normal. Large desorption cross sections of (6 ± 1) · 10^–17 cm² for NO and (3.5 ± 1) · 10^–17 cm² for CO have been found for the desorption at 6.4 eV. The wavelength dependence indicates that the primary excitation step is substrate induced. The final state distributions show a high degree of translational, rotational and vibrational excitation and are clearly nonthermal of origin. The results are consistent with the formation of a negative ion intermediate state of the adsorbate. This observation is supported from a comparison to former results on NO/NiO(1 0 0) for which extensive ab initio calculations including electronically excited states exist. A spin state dependence of the vibrational excitation of NO could only be observed for NO/NiO(1 1 1) and is absent for NO/NiO(1 0 0). We attribute this observation to a spin state dependent coupling of the desorbing molecule to the surface in case the spin lattice orientation of the surface shows a preferential orientation. In the (111) plane the spin orientation is parallel within neighbour nickel ions while it is alternating in the (1 0 0) plane. For both systems studied the velocity component parallel to the surface is constant leading to a strong peaking along the surface normal for the fast molecules. The change from a preferred helicopter rotation (angular momentum vector aligned parallel to the surface normal) to a cartwheel motion (angular momentum vector aligned perpendicular to the surface normal) with increasing rotational excitation for desorption of the flat lying CO is consistent with a change of bonding geometry during the desorption process.     

Levinson theorem for Dirac particles in one dimension

The scattering of Dirac particles by symmetric potentials in one dimension is studied. A Levinson theorem is established. By this theorem, the number of bound states with even(odd)-parity, n₊ (n_-), is related to the phase shifts [] of scattering states with the same parity at zero momentum as follows: The theorem is verified by several simple examples. Received 26 August 1998 and Received in final form 18 January 1999     

Double photoionization of rotating linear molecules

This communication presents a theoretical study of the angular distribution of one or both of the two electrons emitted in one-photon, one-step double ionization of a linear molecule. Experiments which do or do not detect spin of the photoelectrons have been considered. Effects of molecular rotation on double photoionization have been studied in both Hund's coupling schemes (a) and (b) by using parity-adapted states. Selection rules obtained in this paper are very different from those derived earlier for single photoionization and for Auger decay following the absorption of a photon in a rotating linear molecule. It is shown that complete specification of the spin-unresolved and of spin-resolved angular distributions of both photoelectrons require, respectively, three and seven parameters which depend, among other things, on their energies as well as directions of emission. The approach developed in this paper has been used to analyze spin-unresolved double photoionization in the shell of the molecule. The angular distribution is quite different depending on whether or not molecular rotation has been taken into account. Also, it is found to change significantly for different rotational transitions. Effects of electron-electron correlation are clearly manifested even in non-coincident, both rotationally resolved--as well as unresolved--double photoionization. Received: 7 August 1998     

反应物振动激发对O(3P)+D2→OD+D立体动力学的影响

运用准经典轨线方法,基于Roger的³A"势能面,在碰撞能为104.5 kJ/mol时对O(³P)+D₂反应的立体动力学性质进行了理论研究. 详细讨论与产物矢量相关的的极化分布函数以及四个极化微分反应截面进行了. 结果表明,产物OD的立体动力学性质对反应物分子H_{2相似文献}   

Theory of angular momentum waves in solid ortho-hydrogen

The Theory of angular momentum waves in pure ortho-hydrogen is presented in the Bloch spin wave approximation. Since there is a large energy gap between the ground state and the excitation this approximation can be justified. Quadrupole-quadrupole interaction of nearest neighbours is used. We have derived some dispersion curves and the spectrum.