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  Mapping molecular motions leading to charge delocalization with ultrabright electrons

Gao, M., Lu, C., Jean-Ruel, H., Liu, L. C., Marx, A., Onda, K., et al. (2013). Mapping molecular motions leading to charge delocalization with ultrabright electrons. Nature, 496(7445), 343-346. doi:10.1038/nature12044.

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http://dx.doi.org/10.1038/nature12044 (Publisher version)


Gao, Meng1, 2, Author              
Lu, Cheng1, Author
Jean-Ruel, Hubert1, 2, Author              
Liu, Lai Chung1, 2, Author              
Marx, Alexander2, Author              
Onda, Ken3, 4, Author
Koshihara, Shin-ya5, 6, Author
Nakano, Yoshiaki7, Author
Shao, Xiangfeng7, Author
Hiramatsu, Takaaki8, Author
Saito, Gunzi8, Author
Yamochi, Hideki7, Author
Cooney, Ryan R.1, 2, Author              
Moriena, Gustavo1, 2, Author              
Sciaini, Germán1, 2, Author              
Miller, R. J. Dwayne1, 2, Author              
1Department of Chemistry and Physics, University of Toronto, 80 St. George Street, Toronto, Ontario M5S 3H6, Canada, ou_persistent22              
2Atomically Resolved Structural Dynamics Division, Max Planck Research Department for Structural Dynamics, Department of Physics, University of Hamburg, External Organizations, ou_2173636              
3Interactive Research Center of Science, Tokyo Institute of Technology, Nagatsuta, Midori-ku, Yokohama 226-8502, Japan, ou_persistent22              
4PRESTO, Japan Science and Technology Agency, Honcho, Kawaguchi 332-0012, Japan, ou_persistent22              
5Department of Chemistry and Materials Science, Tokyo Institute of Technology, Ōokayama, Meguro-ku, Tokyo 152-8551, Japan, ou_persistent22              
6CREST, Japan Science and Technology Agency (JST), 5-3, Yonbancho, Chiyoda-ku, Tokyo 102-8666, Japan, ou_persistent22              
7Research Center for Low Temperature and Materials Sciences, Kyoto University, Sakyo-ku, Kyoto 606-8501, Japan, ou_persistent22              
8Faculty of Agriculture, Meijo University, Shiogamaguchi 1-501 Tempaku-ku, Nagoya 468-8502, Japan, ou_persistent22              


Free keywords: Characterization and analytical techniques; Imaging techniques
 Abstract: Ultrafast processes can now be studied with the combined atomic spatial resolution of diffraction methods and the temporal resolution of femtosecond optical spectroscopy by using femtosecond pulses of electrons or hard X-rays as structural probes. However, it is challenging to apply these methods to organic materials, which have weak scattering centres, thermal lability, and poor heat conduction. These characteristics mean that the source needs to be extremely bright to enable us to obtain high-quality diffraction data before cumulative heating effects from the laser excitation either degrade the sample or mask the structural dynamics. Here we show that a recently developed, ultrabright femtosecond electron source makes it possible to monitor the molecular motions in the organic salt (EDO-TTF)2PF6 as it undergoes its photo-induced insulator-to-metal phase transition. After the ultrafast laser excitation, we record time-delayed diffraction patterns that allow us to identify hundreds of Bragg reflections with which to map the structural evolution of the system. The data and supporting model calculations indicate the formation of a transient intermediate structure in the early stage of charge delocalization (less than five picoseconds), and reveal that the molecular motions driving its formation are distinct from those that, assisted by thermal relaxation, convert the system into a metallic state on the hundred-picosecond timescale. These findings establish the potential of ultrabright femtosecond electron sources for probing the primary processes governing structural dynamics with atomic resolution in labile systems relevant to chemistry and biology.


Language(s): eng - English
 Dates: 2012-08-102013-02-202013-04-172013-04-18
 Publication Status: Published in print
 Pages: 4
 Publishing info: -
 Table of Contents: -
 Rev. Type: Peer
 Identifiers: DOI: 10.1038/nature12044
 Degree: -



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Title: Nature
Source Genre: Journal
Publ. Info: London : Nature Publishing Group
Pages: - Volume / Issue: 496 (7445) Sequence Number: - Start / End Page: 343 - 346 Identifier: ISSN: 0028-0836
CoNE: https://pure.mpg.de/cone/journals/resource/954925427238