Brauße, FelixGoldsztejn, GildasAmini, KasraBoll, RebeccaBari, SadiaBomme, CédricBrouard, MarkBurt, Michaelde Miranda, Barbara CunhaDüsterer, StefanErk, BenjaminGéléoc, MarieGeneaux, RomainGentleman, Alexander S.Guillemin, RenaudIsmail, IyasJohnsson, PerJournel, LoïcKierspel, ThomasKöckert, HansjochenKüpper, JochenLablanquie, PascalLahl, JanLee, Jason W. L.Mackenzie, Stuart R.Maclot, SylvainManschwetus, BastianMereshchenko, Andrey S.Mullins, TerenceOlshin, Pavel K.Palaudoux, JérômePatchkovskii, SergueiPenent, FrancisPiancastelli, Maria NovellaRompotis, DimitriosRuchon, ThierryRudenko, ArtemSavelyev, EvgenySchirmel, NoraTechert, SimoneTravnikova, OksanaTrippel, SebastianUnderwood, Jonathan G.Vallance, ClaireWiese, JossSimon, MarcHolland, David M. P.Marchenko, TatianaRouzée, ArnaudRolles, Daniel2019-04-172019-04-172018-04-27http://hdl.handle.net/2097/39540Citation: Brauße, F., Goldsztejn, G., Amini, K., Boll, R., Bari, S., Bomme, C., … Rolles, D. (2018). Time-resolved inner-shell photoelectron spectroscopy: From a bound molecule to an isolated atom. Physical Review A, 97(4). https://doi.org/10.1103/PhysRevA.97.043429Due 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.en-USThis Item is protected by copyright and/or related rights. You are free to use this Item in any way that is permitted by the copyright and related rights legislation that applies to your use. For other uses you need to obtain permission from the rights-holder(s).PhotodissociationSingle- and few-photon ionization & excitationX-ray beams & opticsText