Imaging transient molecular configurations in UV-excited diiodomethane

Fuente: arXiv
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Main Authors: Venkatachalam, Anbu Selvam, Lam, Huynh Van Sa, Bhattacharyya, Surjendu, Kaderiya, Balram, Wang, Enliang, Ding, Yijue, Greenman, Loren, Rudenko, Artem, Rolles, Daniel
Format: Preprint
Published: 2025
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author Venkatachalam, Anbu Selvam
Lam, Huynh Van Sa
Bhattacharyya, Surjendu
Kaderiya, Balram
Wang, Enliang
Ding, Yijue
Greenman, Loren
Rudenko, Artem
Rolles, Daniel
author_facet Venkatachalam, Anbu Selvam
Lam, Huynh Van Sa
Bhattacharyya, Surjendu
Kaderiya, Balram
Wang, Enliang
Ding, Yijue
Greenman, Loren
Rudenko, Artem
Rolles, Daniel
contents Femtosecond structural dynamics of diiodomethane ($\mathrm{CH_2I_2}$) triggered by ultraviolet (UV) photoabsorption at 290 nm and 330 nm are studied using time-resolved coincident Coulomb explosion imaging driven by a near-infrared probe pulse. We map the dominant single-photon process, the cleavage of the carbon-iodine bond producing rotationally excited $\mathrm{CH_2I}$ radical, identify the contributions of the three-body ($\mathrm{CH_2} + \mathrm{I} + \mathrm{I}$) dissociation and molecular iodine formation channels, which are primarily driven by the absorption of more than one UV photon, and demonstrate the existence of a weak reaction pathway involving the formation of short-lived transient species resembling iso-$\mathrm{CH_2I{-}I}$ geometries with a slightly shorter I-I separation compared to the ground-state $\mathrm{CH_2I_2}$. These transient molecular configurations, which can be separated from the other channels by applying a set of conditions on the correlated momenta of three ionic fragments, are formed within approximately 100 fs after the initial photoexcitation and decay within the next 100 fs.
format Preprint
id arxiv_https___arxiv_org_abs_2506_07289
institution arXiv
publishDate 2025
record_format arxiv
spellingShingle Imaging transient molecular configurations in UV-excited diiodomethane
Venkatachalam, Anbu Selvam
Lam, Huynh Van Sa
Bhattacharyya, Surjendu
Kaderiya, Balram
Wang, Enliang
Ding, Yijue
Greenman, Loren
Rudenko, Artem
Rolles, Daniel
Chemical Physics
Atomic and Molecular Clusters
Femtosecond structural dynamics of diiodomethane ($\mathrm{CH_2I_2}$) triggered by ultraviolet (UV) photoabsorption at 290 nm and 330 nm are studied using time-resolved coincident Coulomb explosion imaging driven by a near-infrared probe pulse. We map the dominant single-photon process, the cleavage of the carbon-iodine bond producing rotationally excited $\mathrm{CH_2I}$ radical, identify the contributions of the three-body ($\mathrm{CH_2} + \mathrm{I} + \mathrm{I}$) dissociation and molecular iodine formation channels, which are primarily driven by the absorption of more than one UV photon, and demonstrate the existence of a weak reaction pathway involving the formation of short-lived transient species resembling iso-$\mathrm{CH_2I{-}I}$ geometries with a slightly shorter I-I separation compared to the ground-state $\mathrm{CH_2I_2}$. These transient molecular configurations, which can be separated from the other channels by applying a set of conditions on the correlated momenta of three ionic fragments, are formed within approximately 100 fs after the initial photoexcitation and decay within the next 100 fs.
title Imaging transient molecular configurations in UV-excited diiodomethane
topic Chemical Physics
Atomic and Molecular Clusters
url https://arxiv.org/abs/2506.07289