Scholarlink

<p>Solvation plays a key role in many photochemical and biological processes. Yet, direct atomic-scale observation of solvent reorganization around photoexcited molecules containing only light atoms has so far remained elusive. Here, we use time-resolved X-ray scattering at an X-ray free-electron laser to track with a &#xa0;~&#xa0;120 fs time resolution the photoinduced ultrafast rearrangement of polar acetonitrile solvent molecules around an organic hemithioindigo chromophore. The experiments reveal that the solvation shell reorganizes with a &#xa0;~&#xa0;0.3 ps time constant driven by photoinduced charge transfer in the chromophore, and then reequilibrates over &#xa0;~&#xa0;3 ps as the excited state population returns to the ground state. These results demonstrate the viability of using ultrashort X-ray pulses to directly visualize the motion of light atoms in solution, paving the way for atomic-scale understanding and control of photoinduced processes in biological and synthetic photoactive organic molecules.</p>

错误：搜索内容不能为空，请输入英文关键词
错误：关键词超出字数限制，请精简
高级检索

Tracking polar solvation dynamics of a photoexcited organic chromophore with ultrafast X-ray scattering

  • 期刊论文

  • 出版模式：

    开放获取

  • 发表日期：

    2026年4月13日

查看全文
  • Kerstin M. Mitterer,
  • Elli Selenius,
  • Morten L. Haubro,
  • Magnus A. H. Christiansen,
  • Verena Markmann,
  • Bianca L. Hansen,
  • Mikkel Krell-Jørgensen,
  • Joseph G. F. Hoock,
  • Victor Lorentzen,
  • Emma V. Beale,
  • Philip J. M. Johnson,
  • David J. Gosztola,
  • Claudio Cirelli,
  • Camila Bacellar,
  • Asmus O. Dohn,
  • Luca Laraia,
  • Klaus B. Møller,
  • Kristoffer Haldrup,
  • Gianluca Levi,
  • Martin M. Nielsen

摘要

Solvation plays a key role in many photochemical and biological processes. Yet, direct atomic-scale observation of solvent reorganization around photoexcited molecules containing only light atoms has so far remained elusive. Here, we use time-resolved X-ray scattering at an X-ray free-electron laser to track with a  ~ 120 fs time resolution the photoinduced ultrafast rearrangement of polar acetonitrile solvent molecules around an organic hemithioindigo chromophore. The experiments reveal that the solvation shell reorganizes with a  ~ 0.3 ps time constant driven by photoinduced charge transfer in the chromophore, and then reequilibrates over  ~ 3 ps as the excited state population returns to the ground state. These results demonstrate the viability of using ultrashort X-ray pulses to directly visualize the motion of light atoms in solution, paving the way for atomic-scale understanding and control of photoinduced processes in biological and synthetic photoactive organic molecules.