Intermolecular interactions probed by rotational dynamics in gas-phase clusters

Chenxu Lu, Long Xu, Lianrong Zhou, Menghang Shi, Peifen Lu, Wenxue Li, Reinhard Dörner, Kang Lin () and Jian Wu ()
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Chenxu Lu: East China Normal University
Long Xu: Xiamen University
Lianrong Zhou: East China Normal University
Menghang Shi: East China Normal University
Peifen Lu: East China Normal University
Wenxue Li: East China Normal University
Reinhard Dörner: Goethe-Universität Frankfurt am Main
Kang Lin: Zhejiang University
Jian Wu: East China Normal University

Nature Communications, 2024, vol. 15, issue 1, 1-8

Abstract: Abstract The rotational dynamics of a molecule is sensitive to neighboring atoms or molecules, which can be used to probe the intermolecular interactions in the gas phase. Here, we real-time track the laser-driven rotational dynamics of a single N2 molecule affected by neighboring Ar atoms using coincident Coulomb explosion imaging. We find that the alignment trace of N-N axis decays fast and only persists for a few picoseconds when an Ar atom is nearby. We show that the decay rate depends on the rotational geometry of whether the Ar atom stays in or out of the rotational plane of the N2 molecule. Additionally, the vibration of the van der Waals bond is found to be excited through coupling with the rotational N-N axis. The observations are well reproduced by solving the time-dependent Schrödinger equation after taking the interaction potential between the N2 and Ar into consideration. Our results demonstrate that environmental effects on a molecular level can be probed by directly visualizing the rotational dynamics.

Date: 2024
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DOI: 10.1038/s41467-024-48822-z

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