Ultrafast structural dynamics of pyrrole trimer probed by Coulomb explosion imaging

doi:10.1088/1674-1056/ae3556

Abstract The ultrafast structural dynamics of the pyrrole trimer induced by femtosecond laser pulses have been investigated using the Coulomb explosion imaging technique. Coincidence measurements of the three-body dissociation channel ($\mathrm{(C_4H_5N)_3^{3+}} \rightarrow 3\ \mathrm{C_4H_5N^+}$) reveal the geometric configuration and fragmentation behavior of the trimer in the gas phase. Analysis of the kinetic energy release (KER) and fragment angular distributions, combined with Dalitz-plot reconstruction, indicates that the pyrrole trimer predominantly adopts a stable equilateral triangular (cyclic) configuration. Ab initio molecular dynamics (AIMD) simulations show that the experimental KER distribution can be reproduced only when the structural evolution proceeds along the ground state of the trimer dication within $\sim 50$ fs. These results demonstrate that significant intracluster structural rearrangement occurs on an ultrafast timescale during multiple ionization, highlighting the strong coupling between electronic excitation and nuclear motion even in relatively large molecular clusters.

Keywords: strong-field ionization pyrrole trimer fragmentation dynamics Coulomb explosion

Received: 14 November 2025
Revised: 28 December 2025
Accepted manuscript online: 08 January 2026

PACS:	33.80.Rv	(Multiphoton ionization and excitation to highly excited states (e.g., Rydberg states))
	36.40.-c	(Atomic and molecular clusters)
	36.40.Wa	(Charged clusters)

Fund: Project supported by the Innovation Program for Quantum Science and Technology (Grant No. 2024ZD0300700) and the National Natural Science Foundation of China (Grant Nos. 12525411, 92261201, 12274179, 12325406, and 12334011).

Corresponding Authors: Lanhai He, Chuncheng Wang
E-mail: helanhai@jlu.edu.cn;ccwang@jlu.edu.cn

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Lu Wu(武璐), Di Zhou(周迪), Shengpeng Zhou(周胜鹏), Zejin Liu(刘泽槿), Xinhui Wang(王馨慧), Jiaqi Zhou(周家琪), Xiaoge Zhao(赵晓戈), Xiyue Lu(卢喜悦), Xiaokai Li(李孝开), Yizhang Yang(杨译章), Xueguang Ren(任雪光), Lanhai He(赫兰海), and Chuncheng Wang(王春成) Ultrafast structural dynamics of pyrrole trimer probed by Coulomb explosion imaging 2026 Chin. Phys. B 35 043302

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Ultrafast structural dynamics of pyrrole trimer probed by Coulomb explosion imaging

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