期刊
PHYSICAL REVIEW A
卷 97, 期 4, 页码 -出版社
AMER PHYSICAL SOC
DOI: 10.1103/PhysRevA.97.043429
关键词
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资金
- UK EPSRC [EP/G00224X/1, EP/L005913/1]
- EU (FP7 EU People ITN Project) [238671]
- EU (MEDEA project within the Horizon research and innovation programme under the Marie Skodowska-Curie Grant) [641789]
- STFC through PNPAS award
- mini-IPS grant [ST/J002895/1]
- ISIS Innovation Ltd.
- Max Planck Society
- BMBF [05K10KT2]
- EPSRC
- Merton College
- RSC
- Chemical Sciences, Geosciences, and Biosciences Division, Office of Basic Energy Sciences, Office of Science, U. S. Department of Energy [DE-FG02-86ER13491]
- Helmholtz Gemeinschaft through the Helmholtz Young Investigator Program
- Helmholtz Networking and Initiative Funds
- excellence cluster The Hamburg Center for Ultrafast Imaging-Structure, Dynamics and Control of Matter at the Atomic Scale of the Deutsche Forschungsgemeinschaft [CUI, DFG-EXC1074]
- Helmholtz Virtual Institute Dynamic Pathways in Multidimensional Landscapes [419]
- French Agence Nationale de la Recherche (ANR) through XSTASE project [ANR-14-CE32-0010]
- French Agence Nationale de la Recherche (ANR) through the ATTOMEMU-CHO project [ANR-16-CE30-0001]
- Deutsche Forschungsgemeinschaft [B03/SFB755, C02/SFB1073]
- Swedish Research Council
- Swedish Foundation for Strategic Research
- German-Russian Interdisciplinary Science Center - German Federal Foreign Office via the German Academic Exchange Service (DAAD) [G-RISC, C-2015a-6, C-2015b-6, C-2016b-7]
- Saint-Petersburg State University
- Deutsche Forschungsgemeinschaft (DFG) [RO 4577/1-1]
- Deutsche Forschungsgemeinschaft (DFG-ERA grant) [VR 76/1-1]
- Oxford University
- EPSRC [EP/L005913/1, EP/G00224X/1] Funding Source: UKRI
- Engineering and Physical Sciences Research Council [EP/L005913/1] Funding Source: researchfish
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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