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

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 () and Xueguang Ren ()
Additional contact information
Jiaqi Zhou: Xi’an Jiaotong University
Lu Wu: Jilin University
Michal Belina: Department of Physical Chemistry
Anna D. Skitnevskaya: A. E. Favorsky Irkutsk Institute of Chemistry of the Siberian Branch of the Russian Academy of Sciences
Shaokui Jia: Xi’an Jiaotong University
Xiaorui Xue: Xi’an Jiaotong University
Xintai Hao: Xi’an Jiaotong University
Qingrui Zeng: Xi’an Jiaotong University
Qibo Ma: Xi’an Jiaotong University
Yongtao Zhao: Xi’an Jiaotong University
Xiaokai Li: Jilin University
Lanhai He: Jilin University
Sizuo Luo: Jilin University
Dongdong Zhang: Jilin University
Chuncheng Wang: Jilin University
Alexander B. Trofimov: A. E. Favorsky Irkutsk Institute of Chemistry of the Siberian Branch of the Russian Academy of Sciences
Petr Slavíček: Department of Physical Chemistry
Dajun Ding: Jilin University
Xueguang Ren: Xi’an Jiaotong University

Nature Communications, 2025, vol. 16, issue 1, 1-10

Abstract: Abstract 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.

Date: 2025
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DOI: 10.1038/s41467-025-61305-z

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