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    我所低溫F+H2反應研究取得新進展

      近日,我所肖春雷研究員、孫志剛研究員、張東輝院士和楊學明院士團隊,與美國馬里蘭大學M. Alexander教授、伯克利大學D. Neumark教授合作,研究了低溫下F+H2反應中共振增強隧穿效應,以及探索了其在星際化學中對于產生HF的貢獻,相關結果發表在《自然-化學》(Nature Chemistry)上。

      1997年,科學家在星際云中首次觀測到了HF的存在。近幾年,赫歇爾空間天文臺發現,HF在星際空間是普遍存在的。而HF在星際空間,只能通過F+H2反應才能產生。但是F+H2反應具有1.8kcal/mol高度的勢壘(78meV,相當于800K的高溫),在星際空間的低溫下(大約10K左右),這個反應有效發生的具體機制暫不明確,因為即使考慮到通常量子力學的隧穿效應,這個反應也是極難進行的。按照通常量子力學隧穿效應去估計,星際空間的HF的含量是不可能被觀測到的。

      在過去兩年,肖春雷和楊學明領導的團隊,對現有H原子里德堡態標示時間飛渡譜的交叉分子束裝置進行了顯著改進,使其能夠對低至~1meV碰撞能的F+H2反應的微分截面進行測量。他們利用改進的交叉分子束裝置,詳細測量了碰撞能1~35meV范圍內的后向散射譜。在此后向散射譜上,他們于碰撞能大約5meV的位置觀測到了一個獨立的譜峰;而于20meV的位置,觀測到了輕微的振蕩。此外,根據孫志剛等人計算的高精度的FH2-離子的電離能,發現后向散射譜的這兩個特征,是和Neumark等人所測得的負離子光電子能譜上過渡態的譜峰精確對應。

      為了揭示實驗所觀測到的后向散射譜特征,孫志剛等人采用自行發展的非絕熱量子波包動力學方法,進行了詳細的動力學分析。理論分析清晰的表明,位于5meV能量處的后向散射譜峰,是精確對應于F+H2反應的基態共振態;而位于20meV能量出的后向散射譜,是精確對應于F+H2反應的激發態共振態。而基態反應共振態對于低溫下F+H2反應有顯著作用。如果將共振態所導致的共振增強效應移除,F+H2(v=0,j=0)在10K以下的溫度下的反應速率常數,會降低三個數量級以上。因此,F+H2在低溫時的反應性,其實是通過反應共振態所增強的隧穿效應而產生的,而不是通常簡單的隧穿效應。通過精確的理論計算,該工作進而給出了F+H2反應在較寬溫度范圍的速率常數,這對于星際化學過程的精確模擬和研究具有重要的意義。(文/圖 楊天罡)

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