本論文分為兩個研究主題，一是二甲基亞碸（dimethyl sulfoxide, DMSO）的三體光解機制研究，另一是關於偶氮苯（azobenzene, AZB）的異構化研究。在DMSO的光解研究中，我們觀測DMSO分子在200 nm激發下的三體光解過程。我們利用飛秒時間解析之激發-離子化探測和LIF探測分別觀測DMSO光解後的產物CH3和產物SO的成長，與飛秒動能解析飛行質譜術得到飛秒時間解析的甲基產物動能分佈，另外我們也結合理論計算來幫助我們解釋實驗結果，以期完整瞭解DMSO的三體光解過程。我們的研究結果指出當DMSO被激發至S2能態後，有一個在< 50 fs內發生在S2能態的同步三體解離的次要管道，其它主要在S2能態上有一部份在約50 fs進行直接解離產生CH3SO 與高速甲基，另一部份將內轉換至S1能態進而在350 fs解離生成CH3SO 與低速甲基。隨後CH3SO 將快速地內轉換至CH3SO ，形成具較高內能分佈的CH3SO 。上述兩個一級解離所產生的CH3SO ，有一部份具有足夠能量可以進行二次解離，而且在20~90 ps解離生成SO與慢速甲基。
在偶氮苯的研究中，我們首次利用飛秒時間解析之激發-離子化探測技術在氣相中研究AZB的異構化機制，我們發現AZB的瞬時光譜與激發脈衝能量相關，在低激發脈衝能量下所得到的瞬時光譜表示的是中性激發態的動態學表現，其實驗結果與前人的液態實驗結果一致。而在高激發脈衝能量時我們觀察到具有震盪行為的瞬時光譜，經由我們有系統的分析，我們認為這表示的是反式偶氮苯陽離子態的異構化過程的同調震盪（coherent）現象，我們認為這現象可以間接解釋S1能態可以經由N-N鍵旋轉進行異構化。

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