Journal
NATURE COMMUNICATIONS
Volume 10, Issue -, Pages -Publisher
NATURE PUBLISHING GROUP
DOI: 10.1038/s41467-019-10060-z
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Funding
- X-ray Free-Electron Laser Utilization Research Project
- X-ray Free-Electron Laser Priority Strategy Program of the Ministry of Education, Culture, Sports, Science, and Technology of Japan (MEXT)
- Proposal Program of SACLA Experimental Instruments of RIKEN
- Japan Society for the Promotion of Science (JSPS) KAKENHI [JP15K17487, JP16H04091, JP18K05022]
- MEXT
- Research Program of Dynamic Alliance for Open Innovation Bridging Human, Environment and Materials in Network Joint Research Center for Materials and Devices
- European Research Council Advanced Investigator Grant [692657]
- IMRAM project
- JSPS KAKENHI [JP16J02270]
- Academy of Finland
- Tohoku University Institute
- Swedish Research Council
- Swedish Foundation
- DFG through QUTIF Priority Programme
- Cross-ministerial Strategic Innovation Promotion Program
- Chemical Sciences, Geosciences, and Biosciences Division, Office of Basic Energy Sciences, Office of Science, US Department of Energy [DE-FG02-86ER13491]
- [2013B8058]
- [2015A8056]
- [2015B8057]
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The increasing availability of X-ray free-electron lasers (XFELs) has catalyzed the development of single-object structural determination and of structural dynamics tracking in realtime. Disentangling the molecular-level reactions triggered by the interaction with an XFEL pulse is a fundamental step towards developing such applications. Here we report real-time observations of XFEL-induced electronic decay via short-lived transient electronic states in the diiodomethane molecule, using a femtosecond near-infrared probe laser. We determine the lifetimes of the transient states populated during the XFEL-induced Auger cascades and find that multiply charged iodine ions are issued from short-lived (similar to 20 fs) transient states, whereas the singly charged ones originate from significantly longer-lived states (similar to 100 fs). We identify the mechanisms behind these different time scales: contrary to the short-lived transient states which relax by molecular Auger decay, the long-lived ones decay by an interatomic Coulombic decay between two iodine atoms, during the molecular fragmentation.
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