D+DBr反应的态-态动力学研究

在0—2.0 eV的碰撞能范围内采用含时量子波包方法和二阶分裂算符传播子对初始量子态为(v_0=0,j_0=0)的D+DBr反应进行了态分辨理论水平上的动力学计算.计算了抽取反应通道D+DBr→Br+D_2和置换反应通道D'+DBr→D+D'Br的反应概率、积分截面、微分截面、产物的振动和转动分布以及速率常数等动力学性质,并与相应的理论和实验结果进行了比较.结果表明:计算的速率常数与实验结果十分符合.微分截面的结果表明:对于抽取反应,前向的剥离反应机制在反应过程中占据主导地位;对于置换反应,头碰头的反弹机制占据主导地位.     

O~++H_2→OH~++H反应的动力学研究

采用含时量子波包方法结合二阶分裂算符传播子对初始态为(v=0, j=0)的O~++H_2→OH~++H反应体系在0.01—1.00 eV的碰撞能范围内进行了态分辨理论水平上的动力学计算.对反应概率、积分截面、微分截面以及固定初始态的热速率常数等动力学信息进行了计算并与文献报道的实验和理论结果进行了比较.结果表明本文的理论结果与实验结果十分符合.从微分截面的散射信息可知,在低碰撞能范围内,插入反应机制在反应中占据主导地位.随着碰撞能的增加,反应机制逐渐由插入机制变为抽取反应机制.     

H+MgH+→Mg++H2反应中由非绝热耦合引起的复合物形成反应机理

一个化学反应的过程可能涉及多个绝热电子态,其中的非绝热耦合对反应机理起着重要的作用. 本文采用含时量子波包方法和轨线面跳跃方法研究了非绝热耦合对H+MgH⁺→Mg⁺+H₂反应的影响. 通过理论计算得到了绝热和非绝热近似下的反应态-态分辨的积分截面. 计算结果表明,当计算中忽略非绝热耦合时,反应遵循直接剥离的反应机理. 然而,当计算中包含非绝热耦合时,在反应过程中可以形成一个长寿命的激发态复合物(MgH₂⁺)^*,进而使反应遵循复合物形成反应机理. 通过轨线面跳跃计算,进一步揭示了直接剥离和复合物形成反应机理. 由非绝热耦合引起的复合物形成反应机理不仅提高了反应的活性,并且对产物的振动态分布具有显著影响.     

D+CD4→CD3+D2反应的四维量子散射计算

运用约化维数量子动力学理论，利用含时波包法，对反应D+CD₄→CD_{3+D2进行了四维量子散射计算.将反应多原子CD4看作双原子D—CD 3，反应D+CD4→CD3+D2看作单原子-双原 子反应，把体系的反应简化为四维散射问题. 波函数的传播采用分裂算符法，为避免格点边界处含时波函数的边界反射，采用了光学吸收 势法，在格点边界处引入光学势，消除边界反射.根据CD4分子的C3v对称性， 选取了Jordan和Gilbert提出的半经验势能面.计算结果表明，反应概率随平动能的变化图像 ，呈现出显著的量子共振特性，这是很多提取反应的共同特征.而不同振动态下的反应概率 随平动能的变化表明，随振动量子数的增大，反应概率有明显提高，且反应阈能明显降低， 这说明反应分子的振动能对分子的碰撞反应有重要贡献.而对基态和第一振动激发态时散射 截面的计算，也证明了这一结论.同时，还分别通过计算量子数j，k，m对反应概率的影响， 对该反应的空间取向效应进行了研究，并与H+CH4→CH3+H2反应进行了比较. 关键词： 含时波包 量子散射 反应概率}     

精确计算n-n重正化链图传播下n+n→２π0反应截面

采用中子n-反中子n与中性介子π⁰强相互作用的Lorentz不变耦合模型,对n-n重正化链图传播子作了有关物理分析及其严格解析计算,获得精确理论计算结果. 进而将此结果用于n+n→2π⁰反应的物理过程分析及其截面的计算研究中,并精确计算出n-n重正化链图传播下n+n→2π⁰反应微分截面. 还将此计算结果与n-n树图和重正化单圈链图传播下n+n→2π⁰反应微分截面作了对比分析,获得了有关辐射修正的重要信息. 此结果对于深 关键词： Lorentz不变耦合模型 重正化链图传播子 微分截面 辐射修正     

H+D2O→HD+OD反应的微分截面:一种全维态-态量子动力学计算

用含时波包方法计算得到H+D₂O→HD+OD反应的第一个初始基态,第一对称（100）和反对称（001）伸缩振动激发态的全维态-态微分截面.计算的三个初始态的微分截面在低碰撞能量下都是很强的后向散射.随着碰撞能量的增加,微分截面越来越宽,伴随着峰的位置逐渐向小角度移动,与标题反应是一个通过抽取机理的直接反应相一致.发现（100）和（001）态不只有几乎完全相同的积分截面,还有基本相同的微分截面-在相同的总能量下和基态反应也接近.反应产生的OD只有很小一部分在v=1态上,其分布几率和基态与振动激发态的相对几率相似,从而证实了Zare等人的实验结果和局域模式图像.另外让人意想不到的是,在相同的总能量下,伸缩激发抑制了产物HD的转动激发.     

C3+与Ne碰撞过程纯电离绝对截面的测量和研究

介绍了离子-原子碰撞过程中双微分绝对截面的计算方法.利用符合技术测量了中能区C³⁺+Ne碰撞系统的纯电离微分绝对截面. 将实验结果与多体经典蒙特卡罗方法计算结果进行对比后发现，纯电离截面随入射能量变化的趋势基本一致，对理论与实验产生差异的原因作了分析. 对多重电离的电离机制分析表明：高价态的反冲离子主要来自于俄歇贡献；随着入射能量的升高，电子-电子间的库仑作用也逐渐显现. 此实验方法可以用于相同实验装置上的各种反应出射道的绝对截面测量，入射离子种类及入射离子能量范围将得到拓展. 关键词： 离子-原子碰撞 绝对截面 纯电离     

中、高能电子被SO2分子散射的微分截面、动量转移截面及弹性积分截面

在考虑分子内成键原子间的电子云重叠效应的基础上, 提出了一种能够准确计算“中、高能电子-分子”散射的微分截面、动量转移截面及弹性积分截面的修正势方法. 利用可加性规则、使用Hartree-Fock波函数并采用被这一方法修正过的复光学势, 在100—1000eV内对电子被SO₂分子散射的微分截面、动量转移截面及弹性积分截面进行了计算, 并将计算结果与实验及其他理论结果进行比较. 结果表明, 利用这一修正过的复光学势及可加性规则获得的微分截面比利用未修正的复光学势及可加性规则得到的结果准 关键词： 可加性规则 微分截面 动量转移截面 电子散射     

中高能电子被O2及CF4分子散射的微分截面、弹性积分截面及动量转移截面

利用可加性规则，使用Roothaan-Hartree-Fock波函数，采用由束缚原子概念修正过的复光 学势，在300—1000eV内若干个能量点处计算了电子被O₂及CF₄分子 散射的微分截面、 弹性积分截面及动量转移截面，并将计算结果与实验结果及其他理论计算结果进行了比较. 比较的结果表明，利用被束缚原子概念修正过的复光学势及可加性规则进行计算，所得微分 散射截面的精度要比利用未修正的复光学势及可加性规则进行计算得到的结果准确得多；同 时，计算得到的弹性积分截面及动量转移截面也比较接近实验值.因此，在复光学势中采用 束缚原子概念可提高电子被分子散射的微分截面、弹性积分截面及动量转移截面的计算准确 度. 关键词： 电子散射 可加性规则 微分截面 弹性积分截面     

将SVRT模型应用到单原子多原子反应F+CH2D2→CH2D/CHD2+DF/HF中

由于含时波包方法具有经典的直观又不乏量子力学的准确 ,选择含时波包方法来处理F +CH2 D2 →CH2 D/CHD2 +DF/HF反应 .把半刚性振转子 (SVRT)模型应用到该反应体系中 ,研究了两个通道中该反应从基态反应物开始在修正过的J1(MJ1)势能面上计算出来了反应几率、积分截面、速率常数 .反应几率随能量变化的图的数值结果给出了振荡结构 ,这些振荡结构是可以和动力学振荡联系起来的 .而这些振荡结构在积分截面随着能量变化的图中就被反应几率求和后的平均结果所掩盖了 .速率常数和实验结果的比较也得到了较好的结果 .     

State-to-state quantum dynamics studies of the H + LiH+ → Li+ + H2 reaction

ABSTRACT

Quantum dynamical calculations of the H?+?LiH⁺?→?Li⁺?+?H₂ reaction were performed based on the potential energy surface (PES) reported by Dong et al. (RSC Adv. 7, 7008 (2017)) using the time-dependent quantum wave packet method in collision energy range from 0.01 to 1.0?eV. Dynamics properties such as reaction probability, integral cross section, differential cross section (DCS), and thermal rate constant of the H?+?LiH⁺?→?Li⁺?+?H₂ reaction were reported at the state-to-state level of theory and compared with available theoretical calculations. The results indicated that present values are in good agreement with results obtained from the quasi-classical trajectory method. However, large differences can be found between present values and previous quantum results. This can be attributed to the different PESs used in the calculation and the CS approximation was adopted in previous theoretical studies. In addition, the ‘rebound’ reaction mechanism was proposed in previous theoretical studies in a high collision energy range. However, the DCS scattering signals calculated in the present work indicated that complex-forming and direct abstract reaction mechanisms are dominant in low and high collision energies, respectively.     

Dynamics studies of O+ + D2 reaction using the time-dependent wave packet method

Based on the potential energy surface (PES) reported by Li et al. (Phys. Chem. Chem. Phys. 20, 1039 (2018)), the initial state dynamics calculation of O⁺?+?D₂ (v?=?0, j?=?0) reaction was conducted using the time-dependent wave packet method with a second order split operator. Dynamics properties such as reaction probability, integral cross section, differential cross section, and distribution of products were calculated and compared with available experimental and theoretical results. The present integral cross section values were in good agreement with experimental results. In addition, the differential cross section indicates that the mechanism of the complex-formation reaction plays a dominant role during the reaction.     

Coupled-Channel Optical Calculations for e＋-Rb Collision at Intermediate Energies

We present the calculation of total cross sections for positron scattering by Rb at intermediate energies by using the coupled-channel optical method, in which an equivalent-local optical potential has been used to describe the continuum and rearrangement process. The present total cross sections are in good agreement with the measurements of Parikh et al. [Phys. Rev. A 47 （1993） 1535] and other theoretical calculation results. Our results show three peaks in the vicinity of 47eV, which have not been found in the previous measurements and theoretical calculations.     

Energy dependence of fusion and reaction cross sections in the 9Be + 12C system

Angular distributions of protons, deuterons. tritons and α-particles were measured for the system ⁹Be + ¹²C at lab energies between 12 and 27 MeV. The compound nucleus model with level densities calculated according to the Gilbert-Cameron formula describes satisfactorily the measured proton, deuteron and triton data. In the α-particle spectra contributions from other processes seem to be present. In the analysis the fusion cut-off angular momentum was adjusted at each energy in order to reproduce correctly the proton, deuteron and triton channels. From this analysis the fusion cross section was determined as a function of the energy. The results were compared with fusion and total reaction cross section values calculated from a potential model with the real part of the interaction potential obtained from the double folding procedure of Satchler.     

α + α scattering phase shifts and values of the reaction cross section near threshold of the 7Li + p and 7Be + n channels

The most recent values of the reaction cross section σ_R published in this journal are not well established and the reasons invoked to discard previous values are shown to be erroneous. In addition, a reanalysis of full angular distributions confirms the complex phase shifts obtained by the present author and the corresponding values of σ_R.     

Effect of reagent vibrational excitation and isotope substitution on the stereo-dynamics of the Ba+HF→BaF+H reaction

Based on an extended London-Eyring-Polanyi-Sato (LEPS) potential energy surface (PES), the Ba + HF reaction has been studied by the quasi-classical trajectory (QCT) method. The reaction integral cross section as a function of collision energy for the Ba + HF → BaF + H reaction is presented and the influence of isotope substitution on the differential cross sections (DCSs) and alignments of the product's rotational angular momentum have also been studied. The results suggest that the integral cross sections increase with increasing collision energy, and the vibrational excitation of the reagent has great influence on the DCS. In addition, the product's rotational polarization is very strong as a result of heavy-heavy-light (HHL) mass combination, and the distinct effect of isotope substitution on the stereodynamics is also revealed.     

Angular momentum polarization of the molecules in the Li + HF reaction

A theoretical analysis of the orientation and alignment of the rotational angular momenta of the reactants and products of the Li + HF(v _r = 0, j _r = 3) → LiF(v, j) + H reaction at a collision energy of E _coll = 0.317 eV is performed. The polarization of the angular momentum of the molecules involved in the reaction is based on the technique of spherical tensor operators (state multipoles). Quantum-mechanical calculations of the S-matrix of the reaction are carried out using the wave packet method. In particular, the influence of the orientation of the angular momentum of the HF reactant on the differential cross section is examined. It is shown that the contribution to the differential cross section comes only from be reactants with an angular momentum perpendicular to the reaction plane. In addition, the angular dependence of the orientation and alignment of the angular momenta of the reaction products are examined. It is shown that, for an isotropic distribution of reactant molecules, the orientation of the angular momenta of the products differs from zero only in the direction perpendicular to the reaction plane. Different experimental geometries, based on radiation enhanced multiphoton ionization, are proposed to detect the predicted effects.     

Multiple scattering effects for quasifree scattering in 3He(d,dd)1H breakup reaction

The differential cross sections for the ³He(d, dd)¹H breakup reaction have been measured in the kinematical region corresponding to quasifree scattering (QFS). The angular dependence of the cross section at the minimum laboratory energy of the unobserved proton has been obtained. The shapes of energy spectra are approximately reproduced by a calculation in the plane-wave impulse approximation (PWIA). As for the angular dependence of the cross section and for the absolute values, the calculation fails to reproduce the experimental results. A calculation with multiple scattering effects reproduces the experimental data well, not only for the shape of the energy spectra but also for the angular dependence. For the absolute cross sections, the ratio of the experimental values to the calculated ones with multiple scattering effects is 0.7 and this value is improved compared with the value of 0.3 obtained by the PWIA calculation.     

Q- and Z-dependence of angular momentum transfer in deeply inelastic collisions of 86Kr with 209Bi

The dependence of the in-plane and out-of-plane angular correlations of fragments from fissioning heavy products on the kinetic energy and Z of the light reaction partner have been measured. From the dependence of the angular correlations on Q-value and hence energy loss, together with existing data from which the total angle-integrated cross section as a function of energy loss can be extracted, we have determined the dependence of the angular momentum transferred to the heavy product on the initial orbital angular momentum or impact parameter. The resulting dependence is qualitatively consistent with the sticking limit for a reaction intermediate of touching deformed fragments. More specific nuclear models generally underestimate the angular momentum transfer, although the one-body proximity-friction model accounts for the major fraction of the angular momentum transfer. A recent model incorporating both one-body proximity friction and collective excitations accounts quite well for the observed angular momentum transfer. The Z-dependendence of the anisotropy shows the importance of angular momentum fractionation for the less probable events, where the Z of the fissioning system is appreciably less than that of the target. The transferred angular momentum is shown to be fairly strongly aligned along the perpendicular to the reaction plane, with alignment values of 0.6 to 0.8. The component of angular momentum not along the perpendicular to the reaction plane is found to be primarily oriented perpendicular rather than parallel to the recoil direction. The absolute fission probabilities are found to be qualitatively consistent with J-dependent calculations using the J-values deduced from the angular correlations.