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首页> 外文学位 >Time-resolved IR diode laser spectroscopy: Kinetics and product distribution determination of transient photoproducts formed by UV excimer laser photolysis of irony pentacarbonyl.
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Time-resolved IR diode laser spectroscopy: Kinetics and product distribution determination of transient photoproducts formed by UV excimer laser photolysis of irony pentacarbonyl.

机译：时间分辨红外二极管激光光谱法：测定五羰基铁的紫外准分子激光光解形成的瞬态光产物的动力学和产物分布。

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摘要

Time-resolved IR spectroscopy (TRIS) is employed to identify and study the iron carbonyl and CO photofragments of UV photolyzed Fe(CO){dollar}sb5{dollar}. Photofragment reactions with Fe(CO){dollar}sb5{dollar} result in the formation of dinuclear and polynuclear species, some with reaction cross-section on the order of single collisions. Reactions taking place orders of magnitude more slowly are consistent with spin forbidden processes.; Addition of a tunable IR diode laser as the probe source for the TRIS experiments has advantages over a conventional CO laser probe source including a wider tuning range, better long timescale stability and the ability to tune off vibrationally and rotationally excited CO. The IR diode laser permits observation of polynuclear species absorbing at {dollar}>{dollar}2040 cm{dollar}sp{lcub}-1{rcub}{dollar}, measurement of the concentration of vibrationally excited CO and a much higher resolution analysis of the iron carbonyl absorptions.; A number of previously unknown species as well as species observed for the first time in the gas-phase have been detected. TRIS assignments were made for the mononuclear iron carbonyl species: Fe(CO) and excited states of Fe(CO){dollar}sb3{dollar} and Fe(CO){dollar}sb4{dollar}. Assignments for observed dinuclear species included: Fe{dollar}sb2{dollar}(CO){dollar}sb6{dollar}, Fe{dollar}sb2{dollar}(CO){dollar}sb7{dollar}, multiple isomers of Fe{dollar}sb2{dollar}(CO){dollar}sb8{dollar} and two isomers of Fe{dollar}sb2{dollar}(CO){dollar}sb9{dollar}. Formation of Fe{dollar}sb3{dollar}(CO){dollar}sb{lcub}12{rcub}{dollar} was also observed. Reaction rates for these processes as well as for Fe(CO){dollar}sb4{dollar} + O{dollar}sb2{dollar} and Fe(CO){dollar}sb4{dollar} + H{dollar}sb2{dollar} are reported.; Quantitative distributions of photoproducts produced following 193, 248 and 351 nm photolysis were obtained. Approximate distributions of excited Fe(CO){dollar}sb4{dollar}* formed on 351 nm and excited Fe(CO){dollar}sb3{dollar}* formed on 248 nm photolysis were measured and are reported. A qualitative CO photoproduct distribution was also measured and is reported. The photofragment and CO product distribution measured in this study are compared to those measured in prior molecular beam studies of the photodissociation of Fe(CO){dollar}sb5{dollar}.
机译：时间分辨红外光谱法（TRIS）用于鉴定和研究UV光解的Fe（CO）{sb5 {dollar}的羰基铁和CO的光碎片。与Fe（CO）{sb5 {sb5 {dollar}}的光致碎裂反应导致双核和多核物质的形成，其中一些反应横截面按一次碰撞的顺序排列。反应发生的速度较慢的数量级与自旋禁止过程一致。为TRIS实验添加可调谐IR二极管激光器作为探测源具有优于常规CO激光器探测源的优点，包括更宽的调谐范围，更好的长时间刻度稳定性以及能够消除振动和旋转激发的CO的能力。允许观察多核物质在{dollar}> {dollar} 2040 cm {dollar} sp {lcub} -1 {rcub} {dollar}处的吸收，振动激发CO浓度的测量以及羰基铁的更高分辨率分析吸收。已检测到许多先前未知的物种以及在气相中首次观察到的物种。对单核羰基铁物种进行了TRIS分配：Fe（CO）以及Fe（CO）{dol} sb3 {dol}和Fe（CO）{dol} sb4 {dol}的激发态。观察到的双核物种的赋值包括：Fe {dollar} sb2 {dollar}（CO）{dollar} sb6 {dollar}，Fe {dollar} sb2 {dollar}（CO）{dollar} sb7 {dollar}，Fe {的多个异构体美元} sb2 {dollar}（CO）{dollar} sb8 {dollar}和Fe {dollar} sb2 {dollar}（CO）{dollar} sb9 {dollar}的两个异构体。还观察到Fe {美元} sb3 {美元}（CO）{美元} sb {lcub} 12 {rcub} {美元}的形成。这些过程以及Fe（CO）{dollar} sb4 {dollar} + O {dollar} sb2 {dollar}和Fe（CO）{dollar} sb4 {dollar} + H {dollar} sb2 {dollar}的反应速率被报告。获得了在193、248和351 nm光解后产生的光产物的定量分布。测量并报告了在351 nm处形成的激发Fe（CO）{sb4 {dollar} *和在248 nm处形成的激发Fe（CO）{sb3 {dollar} *}的近似分布。还测量并报告了定性的CO光产品分布。将本研究中测得的光碎度和CO产物分布与先前对Fe（CO）{sb5 {dollar}}的光解离的分子束研究中测得的结果进行比较。

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