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中國科大在單分子電致上轉換發光的實驗觀察與機理研究中取得進展

文章來源:中國科學技術大學   發布時間:2019-05-10  【字號:     】  

  最近,中國科學技術大學單分子科學團隊的董振超研究小組,通過掃描隧道顯微鏡(STM)誘導單分子電致發光技術,首次清晰地展示了單個分子在電激勵下的上轉化發光行為,并通過與深圳大學教授李曉光等合作,從理論上揭示了其微觀機制。國際物理學術期刊《物理評論快報》于53日在線發表了這項成果。

  上轉換發光通常指材料吸收低能光子但發出高能光子的反斯托克斯過程,這一現象在激光信息技術、紅外探測、生物醫學等領域有巨大的應用前景。電激勵下的上轉化發光過程中,有機分子吸收由STM注入的低能電子,并在其弛豫過程中發射出高能光子。這一過程涉及分子電子能態、分子間以及分子與周圍環境間的相互作用,深入理解這些相互競爭與制約的微觀過程,對其在有機光電轉換器件、光催化和光合成等方面的應用有著至關重要的意義。

    中國科大單分子科學團隊長期致力于發展將STM高空間分辨表征與光學技術高靈敏探測相結合的技術,特別是通過巧妙調控隧道結納腔等離激元的寬頻、局域與增強特性,拓展了測量極限,為在單分子水平上觀測和調控分子的光電行為提供了有力手段。他們利用高度局域化的隧穿電子作為激發源,研究了氯化鈉脫耦合層表面上的單個酞菁分子的電致熒光,不僅發現了反常的電致上轉換發光現象,還清晰地展示了分子發光強度的三個不同偏壓區域。尤其值得指出的是,該工作在單分子水平上觀測到電致上轉換發光現象,有力排除了此前對這類體系中上轉換機制的一些猜測,同時不同偏壓區域的觀測也為分析和理解上轉換機制提供了豐富的數據。以此為基礎的理論分析進一步表明,兩種不同的分子激發機制——非彈性電子散射和載流子注入——之間的微妙競爭導致了不同偏壓區域不同的發光現象。基于對上述兩種激發機制以及對系統其它潛在激發態的定量分析,研究團隊首次提出了以自旋三重態作為中間過渡態,同時結合非彈性電子散射和載流子注入兩種激發過程的單分子上轉換發光機制。

  陳功與駱陽為這篇文章的共同第一作者。該系列研究工作得到基金委、科技部、中科院、教育部、安徽省等的支持。

  論文鏈接

 

  圖注:(a) STM誘導單分子電致發光的實驗構型示意圖;(b) 三種不同偏壓下單分子電致發光光譜,展示了單分子的上轉換發光現象;(c) 單分子電致發光強度的偏壓依賴關系。




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