期刊
SCIENCE
卷 345, 期 6194, 页码 288-291出版社
AMER ASSOC ADVANCEMENT SCIENCE
DOI: 10.1126/science.1253607
关键词
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资金
- Max Planck Society
- Chemical Sciences, Geosciences, and Biosciences Division, Office of Basic Energy Sciences, Office of Science, U.S. Department of Energy
- Kansas National Science Foundation Experimental Program to Stimulate Competitive Research (NSF EPSCoR) First Award
- Helmholtz Gemeinschaft through the Young Investigator Program
- excellence cluster The Hamburg Centre for Ultrafast Imaging - Structure, Dynamics and Control of Matter at the Atomic Scale of the Deutsche Forschungsgemeinschaft
Studies of charge transfer are often hampered by difficulties in determining the charge localization at a given time. Here, we used ultrashort x-ray free-electron laser pulses to image charge rearrangement dynamics within gas-phase iodomethane molecules during dissociation induced by a synchronized near-infrared (NIR) laser pulse. Inner-shell photoionization creates positive charge, which is initially localized on the iodine atom. We map the electron transfer between the methyl and iodine fragments as a function of their interatomic separation set by the NIR-x-ray delay. We observe signatures of electron transfer for distances up to 20 angstroms and show that a realistic estimate of its effective spatial range can be obtained from a classical over-the-barrier model. The presented technique is applicable for spatiotemporal imaging of charge transfer dynamics in a wide range of molecular systems.
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