Observing the Structural Evolution in the Photodissociation of Diiodomethane with Femtosecond Solution X-Ray Scattering

Matthijs R. Panman; Elisa Biasin; Oskar Berntsson; Markus Hermann; Stephan Niebling; Ashley J. Hughes; Joachim Kübel; Kalina Atkovska; Emil Gustavsson; Amke Nimmrich; Asmus O. Dohn; Mads Laursen; Diana B. Zederkof; Alireza Honarfar; Kensuke Tono; Tetsuo Katayama; Shigeki Owada; Tim B. Van Driel; Kasper  Kjær; Martin M. Nielsen; Jan Davidsson; Jens Uhlig; Kristoffer Haldrup; Jochen S. Hub; Sebastian Westenhoff

doi:10.1103/PhysRevLett.125.226001

Observing the Structural Evolution in the Photodissociation of Diiodomethane with Femtosecond Solution X-Ray Scattering

Matthijs R. Panman, Elisa Biasin, Oskar Berntsson, Markus Hermann, Stephan Niebling, Ashley J. Hughes, Joachim Kübel, Kalina Atkovska, Emil Gustavsson, Amke Nimmrich, Asmus O. Dohn, Mads Laursen, Diana B. Zederkof, Alireza Honarfar, Kensuke Tono, Tetsuo Katayama, Shigeki Owada, Tim B. Van Driel, Kasper Kjær, Martin M. NielsenJan Davidsson, Jens Uhlig, Kristoffer Haldrup, Jochen S. Hub, Sebastian Westenhoff

Department of Physics

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Abstract

Resolving the structural dynamics of the initial steps of chemical reactions is challenging. We report the femtosecond time-resolved wide-angle X-ray scattering of the photodissociation of diiodomethane in cyclohexane. The data reveal with structural detail how the molecule dissociates into radicals, how the radicals collide with the solvent, and how they form the photoisomer. We extract how translational and rotational kinetic energy is dispersed into the solvent. We also find that 85% of the primary radical pairs are confined to their original solvent cage and discuss how this influences the downstream recombination reactions.

Original language	English
Article number	226001
Journal	Physical Review Letters
Volume	125
Issue number	22
Number of pages	7
ISSN	0031-9007
DOIs	https://doi.org/10.1103/PhysRevLett.125.226001
Publication status	Published - 2020

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Panman, M. R., Biasin, E., Berntsson, O., Hermann, M., Niebling, S., Hughes, A. J., Kübel, J., Atkovska, K., Gustavsson, E., Nimmrich, A., Dohn, A. O., Laursen, M., Zederkof, D. B., Honarfar, A., Tono, K., Katayama, T., Owada, S., Van Driel, T. B., Kjær, K., ... Westenhoff, S. (2020). Observing the Structural Evolution in the Photodissociation of Diiodomethane with Femtosecond Solution X-Ray Scattering. Physical Review Letters, 125(22), Article 226001. https://doi.org/10.1103/PhysRevLett.125.226001

@article{eb1ddb7bd63f4d76a1a7cc059022c57a,

title = "Observing the Structural Evolution in the Photodissociation of Diiodomethane with Femtosecond Solution X-Ray Scattering",

abstract = "Resolving the structural dynamics of the initial steps of chemical reactions is challenging. We report the femtosecond time-resolved wide-angle X-ray scattering of the photodissociation of diiodomethane in cyclohexane. The data reveal with structural detail how the molecule dissociates into radicals, how the radicals collide with the solvent, and how they form the photoisomer. We extract how translational and rotational kinetic energy is dispersed into the solvent. We also find that 85% of the primary radical pairs are confined to their original solvent cage and discuss how this influences the downstream recombination reactions.",

author = "Panman, {Matthijs R.} and Elisa Biasin and Oskar Berntsson and Markus Hermann and Stephan Niebling and Hughes, {Ashley J.} and Joachim K{\"u}bel and Kalina Atkovska and Emil Gustavsson and Amke Nimmrich and Dohn, {Asmus O.} and Mads Laursen and Zederkof, {Diana B.} and Alireza Honarfar and Kensuke Tono and Tetsuo Katayama and Shigeki Owada and {Van Driel}, {Tim B.} and Kasper Kj{\ae}r and Nielsen, {Martin M.} and Jan Davidsson and Jens Uhlig and Kristoffer Haldrup and Hub, {Jochen S.} and Sebastian Westenhoff",

year = "2020",

doi = "10.1103/PhysRevLett.125.226001",

language = "English",

volume = "125",

journal = "Physical Review Letters",

issn = "0031-9007",

publisher = "American Physical Society",

number = "22",

}

Panman, MR, Biasin, E, Berntsson, O, Hermann, M, Niebling, S, Hughes, AJ, Kübel, J, Atkovska, K, Gustavsson, E, Nimmrich, A, Dohn, AO, Laursen, M, Zederkof, DB, Honarfar, A, Tono, K, Katayama, T, Owada, S, Van Driel, TB, Kjær, K, Nielsen, MM, Davidsson, J, Uhlig, J, Haldrup, K, Hub, JS & Westenhoff, S 2020, 'Observing the Structural Evolution in the Photodissociation of Diiodomethane with Femtosecond Solution X-Ray Scattering', Physical Review Letters, vol. 125, no. 22, 226001. https://doi.org/10.1103/PhysRevLett.125.226001

TY - JOUR

T1 - Observing the Structural Evolution in the Photodissociation of Diiodomethane with Femtosecond Solution X-Ray Scattering

AU - Panman, Matthijs R.

AU - Biasin, Elisa

AU - Berntsson, Oskar

AU - Hermann, Markus

AU - Niebling, Stephan

AU - Hughes, Ashley J.

AU - Kübel, Joachim

AU - Atkovska, Kalina

AU - Gustavsson, Emil

AU - Nimmrich, Amke

AU - Dohn, Asmus O.

AU - Laursen, Mads

AU - Zederkof, Diana B.

AU - Honarfar, Alireza

AU - Tono, Kensuke

AU - Katayama, Tetsuo

AU - Owada, Shigeki

AU - Van Driel, Tim B.

AU - Kjær, Kasper

AU - Nielsen, Martin M.

AU - Davidsson, Jan

AU - Uhlig, Jens

AU - Haldrup, Kristoffer

AU - Hub, Jochen S.

AU - Westenhoff, Sebastian

PY - 2020

Y1 - 2020

N2 - Resolving the structural dynamics of the initial steps of chemical reactions is challenging. We report the femtosecond time-resolved wide-angle X-ray scattering of the photodissociation of diiodomethane in cyclohexane. The data reveal with structural detail how the molecule dissociates into radicals, how the radicals collide with the solvent, and how they form the photoisomer. We extract how translational and rotational kinetic energy is dispersed into the solvent. We also find that 85% of the primary radical pairs are confined to their original solvent cage and discuss how this influences the downstream recombination reactions.

AB - Resolving the structural dynamics of the initial steps of chemical reactions is challenging. We report the femtosecond time-resolved wide-angle X-ray scattering of the photodissociation of diiodomethane in cyclohexane. The data reveal with structural detail how the molecule dissociates into radicals, how the radicals collide with the solvent, and how they form the photoisomer. We extract how translational and rotational kinetic energy is dispersed into the solvent. We also find that 85% of the primary radical pairs are confined to their original solvent cage and discuss how this influences the downstream recombination reactions.

U2 - 10.1103/PhysRevLett.125.226001

DO - 10.1103/PhysRevLett.125.226001

M3 - Journal article

C2 - 33315438

SN - 0031-9007

VL - 125

JO - Physical Review Letters

JF - Physical Review Letters

IS - 22

M1 - 226001

ER -

Observing the Structural Evolution in the Photodissociation of Diiodomethane with Femtosecond Solution X-Ray Scattering

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