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

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

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 res...

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Bibliographic Details
Main Authors: Brauße, F, Goldsztejn, G, Amini, K, Boll, R, Bari, S, Bomme, C, Brouard, M, Burt, M, De Miranda, B, Düsterer, S, Erk, B, Géléoc, M, Geneaux, R, Gentleman, A, Guillemin, R, Ismail, I, Johnsson, P, Journel, L, Kierspel, T, Köckert, H, Küpper, J, Lablanquie, P, Lahl, J, Lee, J, Mackenzie, S, Maclot, S, Manschwetus, B, Mereshchenko, A, Mullins, T, Olshin, P, Palaudoux, J, Patchkovskii, S, Penent, F, Piancastelli, M, Rompotis, D, Ruchon, T, Rudenko, A, Savelyev, E, Schirmel, N, Techert, S, Travnikova, O, Trippel, S, Underwood, J, Vallance, C, Wiese, J, Simon, M, Holland, D, Marchenko, T, Rouzée, A, Rolles, D
Format: Journal article
Published: American Physical Society 2018
Description
Summary: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 ( CH 3 I ) is investigated by ionization above the iodine 4 d 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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