Simultaneous imaging of vibrational, rotational, and electronic wave packet dynamics in a triatomic molecule

Fuente: arXiv
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Autori principali: Lam, Huynh Van Sa, Hoang, Van-Hung, Venkatachalam, Anbu Selvam, Bhattacharyya, Surjendu, Chen, Keyu, Jacob, Sina, Kudagama, Sanduni, Nguyen, Tu Thanh, Rolles, Daniel, Thumm, Uwe, Rudenko, Artem, Kumarappan, Vinod
Natura: Preprint
Pubblicazione: 2024
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author Lam, Huynh Van Sa
Hoang, Van-Hung
Venkatachalam, Anbu Selvam
Bhattacharyya, Surjendu
Chen, Keyu
Jacob, Sina
Kudagama, Sanduni
Nguyen, Tu Thanh
Rolles, Daniel
Thumm, Uwe
Rudenko, Artem
Kumarappan, Vinod
author_facet Lam, Huynh Van Sa
Hoang, Van-Hung
Venkatachalam, Anbu Selvam
Bhattacharyya, Surjendu
Chen, Keyu
Jacob, Sina
Kudagama, Sanduni
Nguyen, Tu Thanh
Rolles, Daniel
Thumm, Uwe
Rudenko, Artem
Kumarappan, Vinod
contents Light-induced molecular dynamics often involve the excitation of several electronic, vibrational, and rotational states. Since the ensuing electronic and nuclear motion determines the pathways and outcomes of photoinduced reactions, our ability to monitor and understand these dynamics is crucial for molecular physics, physical chemistry, and photobiology. However, characterizing this complex motion represents a significant challenge when different degrees of freedom are strongly coupled. 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) and quantum mechanical wave packet simulations, we directly map the bending vibrations of the molecule, show how the vibrational wave packet is influenced by molecular alignment, and elucidate the consequences of nuclear motion for the coupling between the two lowest electronic states of the cation. Our results demonstrate that multi-coincident CEI can be an efficient experimental tool for characterizing coupled electronic and nuclear motion in polyatomic molecules.
format Preprint
id arxiv_https___arxiv_org_abs_2408_07958
institution arXiv
publishDate 2024
record_format arxiv
spellingShingle Simultaneous imaging of vibrational, rotational, and electronic wave packet dynamics in a triatomic molecule
Lam, Huynh Van Sa
Hoang, Van-Hung
Venkatachalam, Anbu Selvam
Bhattacharyya, Surjendu
Chen, Keyu
Jacob, Sina
Kudagama, Sanduni
Nguyen, Tu Thanh
Rolles, Daniel
Thumm, Uwe
Rudenko, Artem
Kumarappan, Vinod
Chemical Physics
Atomic and Molecular Clusters
Optics
Quantum Physics
Light-induced molecular dynamics often involve the excitation of several electronic, vibrational, and rotational states. Since the ensuing electronic and nuclear motion determines the pathways and outcomes of photoinduced reactions, our ability to monitor and understand these dynamics is crucial for molecular physics, physical chemistry, and photobiology. However, characterizing this complex motion represents a significant challenge when different degrees of freedom are strongly coupled. 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) and quantum mechanical wave packet simulations, we directly map the bending vibrations of the molecule, show how the vibrational wave packet is influenced by molecular alignment, and elucidate the consequences of nuclear motion for the coupling between the two lowest electronic states of the cation. Our results demonstrate that multi-coincident CEI can be an efficient experimental tool for characterizing coupled electronic and nuclear motion in polyatomic molecules.
title Simultaneous imaging of vibrational, rotational, and electronic wave packet dynamics in a triatomic molecule
topic Chemical Physics
Atomic and Molecular Clusters
Optics
Quantum Physics
url https://arxiv.org/abs/2408.07958