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Ultraviolet-light-triggered isomerization of Rydberg-excited propanal: Real-time capture of ultrafast structural evolution and dynamics investigation

机译:瑞德伯格兴奋的丙凌紫外线触发异构化:超快结构演化和动力学调查的实时捕获

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摘要

Structure rearrangement processes, such as isomerization, are attracting extensive interest as a potential carrier in molecular scale electronics design. UV-light-triggered isomerization of Rydberg-excited propanal with two UV photons has been investigated with time-resolved photoelectron spectroscopy. By following the photoionization from 3s Rydberg states in the time domain, the ultrafast structural evolution and the corresponding photoisomerization dynamics are observed and tracked in real-time. The conversion barrier for isomerization from cis-propanal to gauche isomer is estimated to be about 1500 +/- 100 cm(-1) experimentally. Both the photoisomerization yield and the conversion rate have shown strong dependence on the excitation energy. It is observed that whether vibration modes are selectively excited or not, cis-to-gauche photoisomerization of propanal in 3s Rydberg state occurs once the excitation energy is higher than the conversion barrier without any vibrational excitation specificity. This yields a powerful approach to studying structural evolution dynamics in large molecules, which may have applications in molecular devices.
机译:结构重排过程,如异构化,作为分子尺度电子学设计的潜在载体,正引起人们的广泛兴趣。用时间分辨光电子能谱研究了里德堡激发丙醛与两个紫外光子的紫外光引发异构化反应。通过在时域内跟踪3s里德堡态的光电离,实时观察和跟踪了超高速结构演化和相应的光异构化动力学。实验估计顺式丙醛异构化为gauche异构体的转化势垒约为1500+/-100 cm(-1)。光异构化产率和转化率都表现出强烈的激发能依赖性。研究发现,无论振动模式是否被选择性激发,当激发能高于转化势垒时,丙醛在3s里德堡态发生顺式到gauche式光异构化,而没有任何振动激发特异性。这为研究大分子中的结构演化动力学提供了一种强有力的方法,可能在分子器件中有应用。

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  • 来源
    《The Journal of Chemical Physics》 |2021年第5期|共7页
  • 作者单位

    Chinese Acad Sci Innovat Acad Precis Measurement Sci &

    Technol Wuhan Inst Phys &

    Math State Key Lab Magnet Resonance &

    Atom &

    Mol Phys Wuhan 430071 Peoples R China;

    Chinese Acad Sci Innovat Acad Precis Measurement Sci &

    Technol Wuhan Inst Phys &

    Math State Key Lab Magnet Resonance &

    Atom &

    Mol Phys Wuhan 430071 Peoples R China;

    Chinese Acad Sci Innovat Acad Precis Measurement Sci &

    Technol Wuhan Inst Phys &

    Math State Key Lab Magnet Resonance &

    Atom &

    Mol Phys Wuhan 430071 Peoples R China;

    Chinese Acad Sci Innovat Acad Precis Measurement Sci &

    Technol Wuhan Inst Phys &

    Math State Key Lab Magnet Resonance &

    Atom &

    Mol Phys Wuhan 430071 Peoples R China;

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  • 原文格式 PDF
  • 正文语种 eng
  • 中图分类 物理化学(理论化学)、化学物理学;
  • 关键词

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