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Time-resolved inner-shell photoelectron spectroscopy: From a bound molecule to an isolated atom

Felix Brauße 1 Gildas Goldsztejn 1 Kasra Amini 2 Rebecca Boll 3 Sadia Bari 3 Cédric Bomme 3 Mark Brouard 2 Michael Burt 2 Barbara Cunha de Miranda 4 Stefan Düsterer 3 Benjamin Erk 3 Marie Géléoc 5, 6 Romain Géneaux 5, 7 Alexander Gentleman 2 Renaud Guillemin 4 Iyas Ismail 4 Per Johnsson 8 Loïc Journel 4 Thomas Kierspel 9, 10 Hansjochen Köckert 2 Jochen Küpper 9, 10 Pascal Lablanquie 4 Jan Lahl 8 Jason Lee 2 Stuart Mackenzie 2 Sylvain Maclot 8 Bastian Manschwetus 3 Andrey Mereshchenko 11 Terence Mullins 9 Pavel Olshin 11 Jerome Palaudoux 4 Serguei Patchkovskii 1 Francis Penent 4, 12 Maria Novella Piancastelli 4, 12 Dimitrios Rompotis 3 Thierry Ruchon 5, 7 Artem Rudenko 13 Evgeny Savelyev 3 Nora Schirmel 3 Simone Simon 3, 14 Oksana Travnikova 4 Sebastian Trippel 9, 10 Jonathan Underwood 15 Claire Vallance 2 Joss Wiese 9 Marc Simon 4 David Holland Tatiana Marchenko 4 Arnaud Rouzée 1 Daniel Rolles 13
Abstract : Due to its element and site specificity, inner-shell photoelectron spectroscopy is a widely used technique to probe the chemical structure of matter. Here, we show that time-resolved inner-shell photoelectron spectroscopy can be employed to observe ultrafast chemical reactions and the electronic response to the nuclear motion with high sensitivity. The ultraviolet dissociation of iodomethane (CH3I) is investigated by ionization above the iodine 4d edge, using time-resolved inner-shell photoelectron and photoion spectroscopy. The dynamics observed in the photoelectron spectra appear earlier and are faster than those seen in the iodine fragments. The experimental results are interpreted using crystal-field and spin-orbit configuration interaction calculations, and demonstrate that time-resolved inner-shell photoelectron spectroscopy is a powerful tool to directly track ultrafast structural and electronic transformations in gas-phase molecules.
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Submitted on : Friday, October 12, 2018 - 2:57:12 PM
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Felix Brauße, Gildas Goldsztejn, Kasra Amini, Rebecca Boll, Sadia Bari, et al.. Time-resolved inner-shell photoelectron spectroscopy: From a bound molecule to an isolated atom. Physical Review A, American Physical Society, 2018, 97 (4), ⟨10.1103/PhysRevA.97.043429⟩. ⟨cea-01894499⟩



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