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首頁> 外文學(xué)位 >Infrared spectroscopy of the hydroxyl radical-carbon monoxide reactant complex and the isoelectronic hydroxy radical-nitrogen complex as a probe of the hydroxy radical + carbon monoxide goes to hydrocarboxyl radical reaction pathway.
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Infrared spectroscopy of the hydroxyl radical-carbon monoxide reactant complex and the isoelectronic hydroxy radical-nitrogen complex as a probe of the hydroxy radical + carbon monoxide goes to hydrocarboxyl radical reaction pathway.

機(jī)譯：羥基自由基-一氧化碳反應(yīng)物配合物和作為羥基自由基+一氧化碳的探針的等電子羥基自由基-氮配合物的紅外光譜進(jìn)入了氫羧基自由基反應(yīng)路徑。

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Infrared spectroscopy has been used to characterize a hydrogen-bonded complex between the OH and CO reactants that lies directly along the OH + CO ↔ HOCO → H + CO2 reaction coordinate. The spectroscopic experiments have accessed the pure OH overtone stretch as well as combination bands involving intermolecular bend and spin-orbit excitation of the linear OH-CO reactant complex. The geometry, OH spectral shift, binding energy, and vibrational frequencies derived from these measurements are in good accord with complementary ab initio calculations inspired by the experimental work. The experimentally observed geared bend and H-atom bend vibrations are of special interest because they probe portions of the reaction path leading to trans-HOCO formation.; Infrared excitation of the OH-CO complex also supplies sufficient energy to surmount the low barrier to reaction or break the weak intermolecular bond, thereby initiating reactive or inelastic scattering dynamics. The rotational distribution of the inelastically scattered OH (v = 1) fragments is bimodal, revealing that vibrational predissociation proceeds by vibration-to-vibration and vibration-to-rotation and/or translation energy transfer mechanisms. The relative intensities of the OH overtone and combination bands are shown to differ in infrared action and fluorescence depletion measurements, providing preliminary evidence that the OH-CO reactant complex decays by both inelastic and reactive decay processes upon geared bend or H-atom bend excitation.; Analogous spectroscopic and dynamical studies of the isoelectronic OH-N 2 complex in the OH overtone region provide a valuable point of comparison, since this nonreactive system decays exclusively by vibrational predissociation through a vibration-to-vibration mechanism. Infrared spectroscopic studies of the OH-N2 complex are used as the basis for a model of the coupling between the electronic angular momentum of the OH radical and the vibrational angular momentum of the intermolecular bending modes, which is directly applicable to the OH + CO system.
機(jī)譯：紅外光譜已被用來表征OH和CO反應(yīng)物之間的氫鍵配合物，該配合物直接位于OH + CO?HOCO→H + CO2反應(yīng)坐標(biāo)上。光譜實(shí)驗(yàn)已經(jīng)獲得了純OH泛音拉伸以及涉及線性O(shè)H-CO反應(yīng)物配合物的分子間彎曲和自旋軌道激發(fā)的組合帶。從這些測量中得出的幾何形狀，OH光譜位移，結(jié)合能和振動(dòng)頻率與實(shí)驗(yàn)工作所啟發(fā)的補(bǔ)充從頭算式非常吻合。實(shí)驗(yàn)觀察到的齒輪彎曲和H原子彎曲的振動(dòng)特別令人關(guān)注，因?yàn)樗鼈兲綔y了導(dǎo)致反式HOCO形成的反應(yīng)路徑部分。 OH-CO絡(luò)合物的紅外激發(fā)也提供了足夠的能量，以克服反應(yīng)的低勢壘或破壞弱的分子間鍵，從而啟動(dòng)反應(yīng)性或非彈性散射動(dòng)力學(xué)。非彈性分散的OH（v = 1）碎片的旋轉(zhuǎn)分布是雙峰的，表明振動(dòng)預(yù)離解是通過振動(dòng)到振動(dòng)以及振動(dòng)到旋轉(zhuǎn)和/或平移能量轉(zhuǎn)移機(jī)制進(jìn)行的。 OH泛音和組合譜帶的相對強(qiáng)度在紅外作用和熒光消耗測量中顯示出不同，從而提供了初步證據(jù)，表明在齒輪彎曲或H原子彎曲激發(fā)下，OH-CO反應(yīng)物復(fù)合物會(huì)通過非彈性和反應(yīng)性衰變過程而衰變。 ;對OH泛音區(qū)中的等電子OH-N 2配合物的光譜和動(dòng)力學(xué)研究提供了有價(jià)值的比較點(diǎn)，因?yàn)樵摲欠磻?yīng)性系統(tǒng)僅通過通過振動(dòng)-振動(dòng)機(jī)制進(jìn)行的振動(dòng)預(yù)離解而衰減。 OH-N2配合物的紅外光譜研究被用作OH自由基的電子角動(dòng)量與分子間彎曲模式的振動(dòng)角動(dòng)量之間耦合模型的基礎(chǔ)，該模型直接適用于OH + CO系統(tǒng)。

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