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  Mapping atomic motions with ultrabright electrons: towards fundamental limits in space-time resolution

Manz, S., Casandruc, A., Zhang, D., Zhong, Y. P., Loch, R., Marx, A., et al. (2015). Mapping atomic motions with ultrabright electrons: towards fundamental limits in space-time resolution. Faraday Discussions, 177, 467-491. doi:10.1039/C4FD00204K.

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Item Permalink: http://hdl.handle.net/11858/00-001M-0000-0024-BA18-C Version Permalink: http://hdl.handle.net/11858/00-001M-0000-002D-EFAF-F
Genre: Journal Article

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http://dx.doi.org/10.1039/C4FD00204K (Publisher version)
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 Creators:
Manz, Stephanie1, 2, Author              
Casandruc, Albert1, 2, 3, Author              
Zhang, Dongfang1, 2, Author              
Zhong, Yin Peng1, 2, Author              
Loch, Rolf1, 2, Author              
Marx, Alexander1, 2, Author              
Hasegawa, Taisuke1, 2, 4, Author              
Liu, Lai Chung5, Author
Bayesteh, Shima6, Author
Delsim-Hashemi, Hossein7, Author
Hoffmann, Matthias7, Author
Felber, Matthias7, Author
Hachmann, Max7, Author
Mayet, Frank7, Author
Hirscht, Julian1, 2, Author              
Keskin, Sercan1, 2, 3, Author              
Hada, Masaki8, Author
Epp, Sascha1, 2, Author              
Flottmann, Klaus7, Author
Miller, R. J. Dwayne1, 2, 5, 9, Author              
Affiliations:
1Miller Group, Atomically Resolved Dynamics Department, Max Planck Institute for the Structure and Dynamics of Matter, Max Planck Society, ou_1938288              
2Center for Free-Electron Laser Science, Luruper Chaussee 149, Hamburg 22761, Germany, ou_persistent22              
3International Max Planck Research School for Ultrafast Imaging & Structural Dynamics (IMPRS-UFAST), Max Planck Institute for the Structure and Dynamics of Matter, Max Planck Society, ou_2266714              
4Department of Chemical Engineering, Faculty of Engineering Kyoto University Katsura, Nishikyo-ku, Japan, ou_persistent22              
5Departments of Chemistry and Physics, University of Toronto, Toronto, Canada, ou_persistent22              
6Institut für Experimentalphysik, Universität Hamburg, Luruper Chaussee 149, Hamburg 22761, Germany , ou_persistent22              
7DESY, Notkestraße 85, 22607 Hamburg, Germany, ou_persistent22              
8Materials & Structures Laboratory, Tokyo Institute of Technology, Japan & JST-PRESTO, Yokohama 226-8503, Japan, ou_persistent22              
9The Hamburg Centre for Ultrafast Imaging CUI, Universität Hamburg, Luruper Chaussee 149, Hamburg 22761, Germany, ou_persistent22              

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Free keywords: Temporally and Spatially Resolved Molecular Science
 Abstract: The long held objective of directly observing atomic motions during the defining moments of chemistry has been achieved based on ultrabright electron sources that have given rise to a new field of atomically resolved structural dynamics. This class of experiments requires not only simultaneous sub-atomic spatial resolution with temporal resolution on the 100 femtosecond time scale but also has brightness requirements approaching single shot atomic resolution conditions. The brightness condition is in recognition that chemistry leads generally to irreversible changes in structure during the experimental conditions and that the nanoscale thin samples needed for electron structural probes pose upper limits to the available sample or "film" for atomic movies. Even in the case of reversible systems, the degree of excitation and thermal effects require the brightest sources possible for a given space-time resolution to observe the structural changes above background. Further progress in the field, particularly to the study of biological systems and solution reaction chemistry, requires increased brightness and spatial coherence, as well as an ability to tune the electron scattering cross-section to meet sample constraints. The electron bunch density or intensity depends directly on the magnitude of the extraction field for photoemitted electron sources and electron energy distribution in the transverse and longitudinal planes of electron propagation. This work examines the fundamental limits to optimizing these parameters based on relativistic electron sources using re-bunching cavity concepts that are now capable of achieving 10 femtosecond time scale resolution to capture the fastest nuclear motions. This analysis is given for both diffraction and real space imaging of structural dynamics in which there are several orders of magnitude higher space-time resolution with diffraction methods. The first experimental results from the Relativistic Electron Gun for Atomic Exploration (REGAE) are given that show the significantly reduced multiple electron scattering problem in this regime, which opens up micron scale systems, notably solution phase chemistry, to atomically resolved structural dynamics.

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Language(s): eng - English
 Dates: 2014-10-142014-11-122015-01-292015-04-01
 Publication Status: Published in print
 Pages: 25
 Publishing info: -
 Table of Contents: -
 Rev. Method: Peer
 Identifiers: DOI: 10.1039/C4FD00204K
 Degree: -

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Title: Faraday Discussions
  Abbreviation : Faraday Discuss.
Source Genre: Journal
 Creator(s):
Affiliations:
Publ. Info: London : Royal Society of Chemistry
Pages: - Volume / Issue: 177 Sequence Number: - Start / End Page: 467 - 491 Identifier: ISSN: 1359-6640
CoNE: /journals/resource/954925269326