Imaging coupled vibrational, rotational, and electronic wave packet dynamics in a triatomic molecule

Molecular dynamics triggered by interaction with light often involve the excitation of several electronic, vibrational, and rotational states. Characterizing the resulting coupled electronic and nuclear wave packet motion represents a severe challenge, even for small polyatomic systems. In this Lett...

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Bibliographic Details
Published in:arXiv.org 2024-10
Main Authors: Huynh Van Sa Lam, Van-Hung, Hoang, Anbu Selvam Venkatachalam, Bhattacharyya, Surjendu, Chen, Keyu, Jacob, Sina, Kudagama, Sanduni, Tu Thanh Nguyen, Rolles, Daniel, Thumm, Uwe, Rudenko, Artem, Kumarappan, Vinod
Format: Article
Language:English
Subjects:
Coupling (molecular)
Electron states
Molecular dynamics
Polyatomic molecules
Quantum mechanics
Rotational states
Sulfur dioxide
Wave packets
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Summary:Molecular dynamics triggered by interaction with light often involve the excitation of several electronic, vibrational, and rotational states. Characterizing the resulting coupled electronic and nuclear wave packet motion represents a severe challenge, even for small polyatomic systems. In this Letter, we demonstrate how the interplay between vibrational, rotational, and electronic degrees of freedom governs the evolution of molecular wave packets in the low-lying states of strong-field-ionized sulfur dioxide. Using time-resolved Coulomb explosion imaging (CEI) in combination with quantum mechanical wave packet simulations, we directly map bending vibrations of the molecule, show how the vibrational wave packet is influenced by molecular alignment, and elucidate the role of the coupling between the two lowest electronic states of the cation. A conical intersection between these states couples the bending and asymmetric stretching coordinates, which is clearly reflected in the correlated fragment momenta. Our results suggest that multi-coincident CEI represents an efficient experimental tool for characterizing coupled electronic and nuclear motion in polyatomic molecules.
ISSN:2331-8422