激光溅射Cu等离子体与气相CH3CN团簇的反应

用激光溅射 -分子束技术研究了Cu等离子体与乙腈团簇的气相反应 .观察到Cu+ (CH3 CN) n、CH2 CN+ (CH3 CN) n、H+ (CH3 CN) n 和CH3 CHCN+ (CH3 CN) n 四个种类的团簇离子 .考察了等离子体作用于脉冲分子束的不同位置 ,对团簇产物的种类和尺寸大小的影响 .实验结果表明 ,Cu+ (CH3 CN) n 是由Cu+ 与乙腈团簇直接缔合而成 ,CH2 CN+ (CH3 CN) n、H+ (CH3 CN) n 主要是激光等离子体中的电子与乙腈团簇碰撞电离产生的 ,而CH3 CHCN+ (CH3 CN) n 是由乙腈团簇离子内的离子 分子反应生成的 .     

Cu+、Ag+、Au+与乙硫醇的气相化学反应

利用激光溅射-分子束的技术,结合反射飞行时间质谱计,研究了Cu+、Ag+、Au+与乙硫醇的气相化学反应.结果显示这三种金属离子与(CH3CH2SH)n反应形成一系列团簇离子M+(CH3CH2SH)n,且团簇离子尺寸不一样.Ag+、Au+与乙硫醇的反应还生成了(CH3CH2SH)+n,由此推测Cu+、Ag+、Au+与乙硫醇团簇的反应存在两种通道,一种通道是生成M+(CH3CH2SH)n,另一种是生成(CH3CH2SH)+n.Cu+、Au+与乙硫醇的反应还生成了M+(H2S)(M=Cu、Au),但是实验中没有观察到Ag+(H2S),理论计算表明Ag+(H2S)很不稳定.另外,分析产物离子M+(CH3CH2SH)n的强度发现,n=1～2之间存在明显的强度突变现象.     

A1等离子体与甲醇团簇的反应

利用激光烧蚀-分子束法(LA-MB)对激光烧蚀金属铝靶产生的Al等离子体与脉冲分子束超声膨胀产生的(CH3OH)n团簇在气相条件下的反应进行了研究.烧蚀激光相对于脉冲分子束之间的延时不同,观测到团簇离子序列及团簇尺寸的变化,反映出脉冲分子束状态对反应条件及激光烧蚀等离子体状态的影响.在激光烧蚀发生于脉冲分子束的前段,主要反应产物为Al (CH3OH)n,但团簇尺寸较小;在烧蚀发生于脉冲分子束的中段,主要产物为H (CH3OH)n,团簇尺寸增大,强度减弱;在烧蚀发生于脉冲分子束的后段,观测到尺寸更大的水合质子化团簇H (H2O)m(CH3OH)n.结合团簇离子速度分布的特征,对团簇的产生机理进行了讨论.     

Cu~+、Ag~+、Au~+与乙硫醇的气相化学反应

利用激光溅射 分子束的技术 ,结合反射飞行时间质谱计 ,研究了Cu+、Ag+、Au+与乙硫醇的气相化学反应。结果显示这三种金属离子与 (CH3 CH2 SH) n 反应形成一系列团簇离子M+(CH3 CH2 SH) n,且团簇离子尺寸不一样。Ag+、Au+与乙硫醇的反应还生成了 (CH3 CH2 SH) +n ,由此推测Cu+、Ag+、Au+与乙硫醇团簇的反应存在两种通道 ,一种通道是生成M+(CH3 CH2 SH) n,另一种是生成 (CH3 CH2 SH) +n 。Cu+、Au+与乙硫醇的反应还生成了M+(H2 S) (M =Cu、Au) ,但是实验中没有观察到Ag+(H2 S) ,理论计算表明Ag+(H2 S)很不稳定。另外 ,分析产物离子M+(CH3 CH2 SH) n 的强度发现 ,n =1～ 2之间存在明显的强度突变现象     

钨离子团簇与N2分子的反应性

利用激光蒸发团簇源产生Wn团簇束,团簇束通过一个充有N2气体分 子的低压反应池,利用飞行时间质谱探测反应产物,在类单次碰撞条件下研究了W+10 -W+50和N2分子的反应性,在室温条件下测量了N2分子与W+n团簇反应的 反应几率。团簇尺寸在10～26原子的团簇与N2分子的反应几率与团簇尺寸有很强的相关性 ,对n=16,22,23的团簇具有比较高的反应性。W+n与N2分子的反应性与Wn与N 2分子的反应性显示出相似的规律性。     

激光作用下甲醇团簇多光子电离质谱研究

YAG脉冲激光的三倍频输出(355 nm)3光子共振电离由脉冲分子束超声膨胀产生的甲醇团簇,观测到质子化的团簇离子序列(CH3OH)nH (n=1~15),其中n=1~3的团簇离子强度明显大于其他尺寸的团簇离子,而n>3的强度随n的增大依次减小,且这种强度分布特征与电离激光相对于脉冲分子束的延时无关,同时对团簇离子的产生受实验条件的影响作了探讨。结合密度泛函密度泛函理论中的B3LYP杂化方法加6-31G 基组水平上的计算,推测了质子化甲醇离子的结构及稳定性,并讨论了甲醇团簇电离后的质子转移反应生成质子化团簇的机理。而对于另一个水合质子化团簇序列H (H2O)(CH3OH)n,由于溶剂化的影响只在较大尺寸时才出现。     

氨与甲醇混合团簇的多光子电离质谱及从头算研究

用多光子电离技术结合飞行时间质谱仪对氨与甲醇混合团簇进行了研究.在脉冲激光波长分别为266nm,355nm和532nm条件下,仅在355nm作用下观测到团簇离子.主要的电离产物为质子化的(CH3OH)n(NH3)mH (n=0~6,m=0~4)混合团簇离子,且各个序列的离子强度随m的增大而减小.经分析,氨与甲醇混合团簇电离后团簇离子发生内部质子化转移反应是形成质子化团簇离子的主要原因.不同尺寸团簇离子信号强度随电离激光光强变化的光强指数曲线显示,团簇均发生四光子电离过程.应用量化计算,构造了质量数较小的几个团簇离子的可能的空间几何构型,发现二元团簇离子(CH3OH)n(NH3)mH 是以NH4 作为内核离子,再通过氢键与其它分子组合而构成团簇离子.     

激光烧蚀Al等离子体与甲醇团簇反应中(CH3OH)nCH3O-的形成

激光烧蚀一分子束(LA-MB)法是研究金属离子与分子团簇反应的有效方法.在气相条件下,用飞行时间质谱观测到激光烧蚀Al等离子体与脉冲分子束超声膨胀产生的甲醇团簇碰撞反应生成的(CH30H)nCH3O-(n=3～23)团簇负离子.实验发现,此序列的团簇负离子主要生成于烧蚀激光作用于脉冲分子束的后段,(CH3OH)3CH3O-离子强度始终远远大于其后的离子,并且这些离子随尺寸大小的分布变化平缓.结合量化计算,在133LYP/6-31G(d)水平上得到(CH3OH)nCH3O-(n=1～4)的可能几何构形,并推断(CH3OH)3CH3O-为-幻数结构.     

自由钨团簇与氮分子反应性的尺寸相关性

用激光蒸发团簇源产生Wn团簇束 ,团簇通过一个充有N2 气体分子的低压反应池 ,利用飞行时间质谱探测反应产物 ,在单次碰撞条件下研究了W+ 10 —W+ 50 和N2 分子的反应性 ,在室温条件下测量了N2 分子与W+ n 团簇反应的反应几率 .n =10— 2 6的团簇与N2 分子的反应几率与团簇尺寸有很强的相关性 ,n =16 ,2 2 ,2 3的团簇有较高的反应性 .W+ n 与N2 分子的反应性与Wn与N2 分子的反应性显示出相似的规律性. A beam of tungsten clusters, seeded in He gas, is produced in a pulsed laser vaporization source. We have studied the size-dependent reactivity of positive tungsten cluster ions with N 2 under single-collision conditions by using laser-vaporization source, low-pressure reaction cell and time-of-flight mass spectrometer. The reaction probability with N 2 molecule was measured as a function of cluster size, W + 10-W + 50, for clusters produced at room temperature...     

乙腈和氨水团簇的激光电离实验研究

在355nm激光波长下应用多光子电离和分子束技术研究了乙腈和氨水的混合团簇,所得的团簇离子以(CH3CN) n、(CH3CN)nNH 3和(CH3CN)n(NH3) 为主,中性团簇以二元团簇(CH3CN)n(NH3)m/(CH3CN)n(NH4OH)m为主.离子产物是来源于中性的二元团簇先吸收部分激光能量解离成稳定的小团簇和碎片,然后再发生分子蒸发和电离的过程,并未发生明显的质子转移反应.     

标量介子场对(ΩΩ)(0+)态生成截面的计算

研究了Ω+Ω→(ΩΩ)0++σ(ε)过程生成(ΩΩ)0+双重子态的截面.结果表明这个过程的生成截面比已计算过的其他Ω+Ω→(ΩΩ)0++X(赝标介子或矢量介子)过程的截面要大一至两个量级.因此这可能是一个值得考虑的(ΩΩ)0+生成途径.     

Gamma-ray transition probabilities in 91Nb+

The lifetimes of 14 excited states in ⁹¹Nb and lower bounds for 5 additional states were measured with the Doppler-shift attenuation method, utilizing the ⁹¹Zr(p, nγ)⁹¹Nb reaction. By using calibrated F(τ) curves, the uncertainty of the stopping power was reduced to about 15 %. Multipole mixing ratios were determined for several transitions from the γ-ray angular distributions. The experimental data on γ-ray transition probabilities were compared with theoretical values. These were calculated using shell-model wave functions based on a ⁸⁸Sr core and active protons in the $\text{2}\text{p}{}_{\mathrm{<mtext>1</mtext><mtext>2</mtext>}}\text{and}\text{1}\text{g}{}_{\mathrm{<mtext>9</mtext><mtext>2</mtext>}}$orbitals. For the negative-parity states also excitations of protons from the $\text{2}\text{p}{}_{\mathrm{<mtext>3</mtext><mtext>2</mtext>}}\text{and}\text{1}\text{f}{}_{\mathrm{<mtext>5</mtext><mtext>2</mtext>}}$ orbitals were taken into account.     

H + reactions from 1.96 to 6.20 MeV

The differential cross sections of ²H(d, d)²H, ²H(d, ³He)n, ²H(d, p)³H and ²H(d, t)p have been measured in a gas scattering chamber at ten bombarding energies between 2.0 and 6.2 MeV with accuracies ranging from ±1.7 % to ±3.4 %. The differential cross section of ²H(d, n)³He has been measured at forward angles to an accuracy of ±2.5 % at the same energies using a time-of-flight detection system. The neutron detection efficiency was calibrated from the ²H(d, ³He)n cross sections, so the neutron production cross sections reported here do not depend on any previous neutron measurements. The ²H(d, ³He)n cross sections have been converted into ²H(d, n) ³He cross sections and Legendre polynomial fits are given for the complete angular distributions of ²H(d, n)³He.     

The break-up reaction p0 + d → p1 + p2+ n at E0 = 16 MeV

The break-up reaction p₀ + d → p₁ + p₂ + n has been studied at E₀ = 16 MeV in kinematically complete p₁-p₂ coincidence experiments with special regard to n-p final-state interactions (f.s.i.) and p₁-p₂ quasifree scattering (q.f.s.). The absolute differential cross section has been measured for n-p f.s.i. c.m. production angles from 60° to 140° and for four pairs of angles with strong contributions due to q.f.s. Calculations with separable nucleon-nucleon potentials based on the Faddeev equations are in good agreement with the data obtained. In general, the shape of the experimental differential cross section is well reproduced. Discrepancies of up to 30 % in the worst cases arise between the absolute values of the theoretical predictions and the experimental data.     

Experimental search for B = 2, T= 0 states in the d + d → d + X reaction

A search for isoscalar dibaryonic resonances by means of missing-mass spectra in the d + d → d + X reaction has been attempted using deuteron beams of T = 2.29,2.00 and 1.65 GeV. The results do not show any evidence for a narrow peak with a limit of $\text{30 nb}\text{GeV}{}^2$ for a 15 MeV width or a broad enhancement which could be unambiguously attributed to a dibaryonic resonance.     

反应物分子初始振动激发对H+CH~+→C~++H_2反应的影响

在CH_2~+体系的电子基态势能面上运用准经典轨线方法,研究了当碰撞能E=500 me V时,反应物分子的振动激发对H(~2S)+CH~+(X~1Σ~+)→C+(~2P)+H_2(X1_gΣ~+)反应的反应概率、反应截面和立体动力学性质的影响.分别计算了两矢量相关k-j′的P(θ_r)分布,三矢量相关k-k′-j′的P(φr)分布以及反应产物的四个极化微分截面.结果表明,产物分子转动角动量不仅在Y轴方向有取向效应,还定于Y轴的正方向.并且发现,随着振动量子数的增加,对反应体系产物分布的影响就越明显.     

Total reaction cross section for 12C + 16O below the Coulomb barrier

The energy dependence of the total reaction cross section, σ(E), for ¹²C + ¹⁶O has been measured over the range E_c.m. = 4–12 MeV, by detecting γ-rays from the various possible residual nuclei with two large NaI(Tl) detectors placed close to the target. This technique for measuring total reaction cross sections was explored in some detail and shown to yield reliable values for σ(E). Although the principal emphasis of this work was placed on obtaining reliable cross sections, a preliminary study has been made of the suitability of various methods for extrapolating the cross section to still lower energies. The statistical model provides a good fit with a reasonable value for the strength function, 〈γ²〉/〈D〉 = 6.8 × 10^?2, over the range E_c.m. = 6.5–12 MeV, but predicts cross sections which are much too large for E_c.m. < 6.5 MeV. Optical model fits at low energies are especially sensitive to the radius and diffuseness of the imaginary component of the potential and, since these are still poorly known at present, such extrapolations may be wrong by orders of magnitude. A simple barrier penetration model gives a moderately good fit to the data and seems to provide the safest extrapolation to lower energies at the present time. It is clear, however, that our knowledge of the heavy-ion reaction mechanism at low energies is incomplete, and that cross-section measurements at still lower energies are needed to establish the correct procedure for extrapolating heavy-ion reaction cross sections to low energies.     

用精确的量子力学方法研究N + OD反应的动力学性质

采用close coupling (CC)方法,在3A’’势能面上[Guadagnini R, Schatz G C, Walch S P. Global potential energy surface for the lowest 1A’, 3A’’, and 1A’’ states of HNO [J]. J. Chem. Phys., 1995,10:774],我们利用量子含时波包方法对N + OH的同位素反应—N + OD进行了研究。在0.0-0.8 eV的平动能范围内,选态的反应几率受共振结构支配。利用 -shifting方法计算,我们得到了基态的速率常数,并对分子间的同位素效应进行了研究。     

Cl+CH4反应的含时量子动力学研究

基于新的势能面,运用半刚性振动转子靶(SVRT)模型和含时波包法对Cl+CH4→HCl+CH3反应体系进行了计算,给出了反应过程中体系的振动、转动及空间立体效应对该反应的反应几率和反应阈能的影响,并计算了基态的总散射截面和热速率常数.