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<p>Proton transfer underpins number of chemical and biochemical processes, yet its sub-100 fs dynamics have rarely been captured in real time. Here, we report direct and time-resolved observation of ionizing radiation-induced proton transfer in a heteroaromatic hydrate: the pyrrole-water complex. Both the electron-impact and strong-field laser experiments create a locally and doubly charged pyrrole unit (C<sub>4</sub>H<sub>5</sub>N<sup>2+</sup>), which immediately (within 60 fs) donates a proton to the adjacent H<sub>2</sub>O, generating deprotonated C<sub>4</sub>H<sub>4</sub>N<sup>+</sup> and hydronium H<sub>3</sub>O<sup>+</sup> cations that subsequently undergo Coulomb explosion. The electron-impact experiments directly revealed initial states and provided dynamical insights through fragment ions and electron coincidence momentum imaging. The strong-field femtosecond laser experiments tracked the ultrafast dynamics of proton transfer; complementary ab initio calculations unraveled the dynamical details. The 50-60 fs proton transfer qualifies as one of the fastest acid-base reactions observed to date. This study offers a novel perspective on radiation-induced proton transfer in hydrated biomolecules.</p>

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State- and time-resolved observation of ultrafast intermolecular proton transfer in hydrated biomolecules

  • 期刊论文

  • 出版模式：

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  • 发表日期：

    2025年7月1日

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  • Jiaqi Zhou,
  • Lu Wu,
  • Michal Belina,
  • Anna D. Skitnevskaya,
  • Shaokui Jia,
  • Xiaorui Xue,
  • Xintai Hao,
  • Qingrui Zeng,
  • Qibo Ma,
  • Yongtao Zhao,
  • Xiaokai Li,
  • Lanhai He,
  • Sizuo Luo,
  • Dongdong Zhang,
  • Chuncheng Wang,
  • Alexander B. Trofimov,
  • Petr Slavíček,
  • Dajun Ding,
  • Xueguang Ren

摘要

Proton transfer underpins number of chemical and biochemical processes, yet its sub-100 fs dynamics have rarely been captured in real time. Here, we report direct and time-resolved observation of ionizing radiation-induced proton transfer in a heteroaromatic hydrate: the pyrrole-water complex. Both the electron-impact and strong-field laser experiments create a locally and doubly charged pyrrole unit (C4H5N2+), which immediately (within 60 fs) donates a proton to the adjacent H2O, generating deprotonated C4H4N+ and hydronium H3O+ cations that subsequently undergo Coulomb explosion. The electron-impact experiments directly revealed initial states and provided dynamical insights through fragment ions and electron coincidence momentum imaging. The strong-field femtosecond laser experiments tracked the ultrafast dynamics of proton transfer; complementary ab initio calculations unraveled the dynamical details. The 50-60 fs proton transfer qualifies as one of the fastest acid-base reactions observed to date. This study offers a novel perspective on radiation-induced proton transfer in hydrated biomolecules.