Ultrafast nonadiabatic cascade and subsequent photofragmentation of extreme ultraviolet excited caffeine molecule

Ultrafast XUV chemistry is offering new opportunities to decipher the complex dynamics taking place in highly excited molecular states and thus better understand fundamental natural phenomena as molecule formation in interstellar media. We used ultrashort XUV light pulses to perform XUV pump-IR prob...

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Bibliographic Details
Main Authors: Marciniak, Alexandre (Author) , Kuleff, Alexander I. (Author)
Format: Article (Journal)
Language:English
Published: November 16, 2018
In: The journal of physical chemistry letters
Year: 2018, Volume: 9, Issue: 24, Pages: 6927-6933
ISSN:1948-7185
DOI:10.1021/acs.jpclett.8b02964
Online Access:Verlag, Volltext: https://doi.org/10.1021/acs.jpclett.8b02964
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Author Notes:Alexandre Marciniak, Kaoru Yamazaki, Satoshi Maeda, Maurizio Reduzzi, Victor Despré, Marius Hervé, Mehdi Meziane, Thomas A. Niehaus, Vincent Loriot, Alexander I. Kuleff, Baptiste Schindler, Isabelle Compagnon, Guiseppe Sansone, and Franck Lépine
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Summary:Ultrafast XUV chemistry is offering new opportunities to decipher the complex dynamics taking place in highly excited molecular states and thus better understand fundamental natural phenomena as molecule formation in interstellar media. We used ultrashort XUV light pulses to perform XUV pump-IR probe experiments in caffeine as a model of prebiotic molecule. We observed a 40 fs decay of excited cationic states. Guided by quantum calculations, this time scale is interpreted in terms of a nonadiabatic cascade through a large number of highly correlated states. This shows that the correlation driven nonadiabatic relaxation seems to be a general process for highly excited states, which might impact our understanding of molecular processing in interstellar media.
Item Description:Gesehen am 11.10.2019
Physical Description:Online Resource
ISSN:1948-7185
DOI:10.1021/acs.jpclett.8b02964