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首页> 外文期刊>The journal of physical chemistry, A. Molecules, spectroscopy, kinetics, environment, & general theory >Mechanisms and Relative ates of MX_2~* Chemiluminescence in the Reactions of Ca,Sr,and Ba(~1s) Atos with Dihalogen Molecules
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Mechanisms and Relative ates of MX_2~* Chemiluminescence in the Reactions of Ca,Sr,and Ba(~1s) Atos with Dihalogen Molecules

机译：Ca，Sr和Ba（〜1s）原子与二卤分子反应中MX_2〜*化学发光的机理及相关原因

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摘要

Chemiluminescent reactions of ground state(Ca,Sr,and Ba)atoms with (Cl_2,Br_2,I_2,ICl,and IBr)were studied in a beam-gas arrangement.The MX_2~* pseudo-continua were measured as a function of target gas pressure in the 0.0001-0.25 Pa range.To identify the main reaction channels that contribute to MX_2~* formation and to otain their relative contributions,kinetic models were fitted to the data.The following channels were considered:(1) radiative two-body recombination(R2BR),(2)radiative three-body recombination(R3BR),(3)two consecutive harpooing steps involving MX~+ intermediate (two-step chemiluminescent reaction TSCR),and (4) combinations of the above.On their own,none of the mechanisms (1-3)provide satisfactory data fits.The best agreement is obtained by a model involving both (R2BR),(2) radiative three-body recombination(R3BR),(3)two consecutive harpooing steps involving MX~+ intermediate (two-step chemiluminescent reaction TSCR),and (4) combinations of the above.On their own,none of the mechanisms (1-3) provide satisfactory datafits.The best agreement is obtained by a model involving both R2BR and TSCR.The ranching ratios of these channels were determined for #rho#=0-0.25Pa.At 0.16 Pa these RWBR fractios vary from 7% (for Ca,Sr+ICl)to 79% (for Ba+IBr).Absolute CL cross sections and lower limits of photon yields were estimated by cross-calibrations.Photon yields for R2BR varied from 0.0004% to 0.037,depending on the collision partners.
机译：研究了束流-气体排列中基态（Ca，Sr和Ba）原子与（Cl_2，Br_2，I_2，ICl和IBr）的化学发光反应。测量了MX_2〜*伪连续谱与目标的关系气体压力在0.0001-0.25 Pa范围内。为确定有助于MX_2〜*形成的主要反应通道并获得其相对贡献，将动力学模型拟合到数据中。考虑以下通道：（1）辐射二体重组（R2BR），（2）辐射三体重组（R3BR），（3）两个连续的涉及MX〜+中间体的两步键合（两步化学发光反应TSCR）和（4）上述的组合。 （1-3）中没有一个机制提供令人满意的数据拟合。通过（R2BR），（2）辐射三体重组（R3BR），（3）两个连续的涉及MX〜+中间体（两步化学发光反应TSCR），以及以上（4）的组合。 （1-3）提供了令人满意的数据拟合。通过同时涉及R2BR和TSCR的模型获得了最佳一致性。确定了这些通道的放牧率，用于＃rho＃= 0-0.25Pa。在0.16 Pa时，这些RWBR分数变化从7％（Ca，Sr + ICl）到79％（Ba + IBr）。通过交叉校准估计了绝对CL截面和光子产率的下限.R2BR的光子产率在0.0004％到0.037之间变化，取决于在碰撞伙伴上。

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