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  Capturing Chemistry in Action with Electrons: Realization of Atomically Resolved Reaction Dynamics

Ischenko, A. A., Weber, P. M., & Miller, R. J. D. (2017). Capturing Chemistry in Action with Electrons: Realization of Atomically Resolved Reaction Dynamics. Chemical Reviews, 117(16), 11066-11124. doi:10.1021/acs.chemrev.6b00770.

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Item Permalink: http://hdl.handle.net/11858/00-001M-0000-002D-5F14-2 Version Permalink: http://hdl.handle.net/11858/00-001M-0000-002D-E942-F
Genre: Journal Article

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Capturing Chemistry in Action with Electrons.pdf (Publisher version), 25MB
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 Creators:
Ischenko, Anatoly A.1, Author
Weber, Peter M.2, Author
Miller, R. J. Dwayne3, 4, Author              
Affiliations:
1Institute of Fine Chemical Technologies, Moscow Technological University, Vernadskogo 86, 119571 Moscow, Russia, ou_persistent22              
2Department of Chemistry, Brown University, 324 Brook Street, 02912 Providence, Rhode Island, United States, ou_persistent22              
3Miller Group, Atomically Resolved Dynamics Department, Max Planck Institute for the Structure and Dynamics of Matter, Max Planck Society, ou_1938288              
4Departments of Chemistry and Physics, University of Toronto, 80 St. George, M5S 3H6 Toronto, Canada, ou_persistent22              

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 Abstract: One of the grand challenges in chemistry has been to directly observe atomic motions during chemical processes. The depiction of the nuclear configurations in space-time to understand barrier crossing events has served as a unifying intellectual theme connecting the different disciplines of chemistry. This challenge has been cast as an imaging problem in which the technical issues reduce to achieving not only sufficient simultaneous space-time resolution but also brightness for sufficient image contrast to capture the atomic motions. This objective has been met with electrons as the imaging source. The review chronicles the first use of electron structural probes to study reactive intermediates, to the development of high bunch charge electron pulses with sufficient combined spatial-temporal resolution and intensity to literally light up atomic motions, as well as the means to characterize the electron pulses in terms of temporal brightness and image reconstruction. The use of femtosecond Rydberg spectroscopy as a novel means to use internal electron scattering within the molecular reference frame to obtain similar information on reaction dynamics is also discussed. The focus is on atomically resolved chemical reaction dynamics with pertinent references to work in other areas and forms of spectroscopy that provide additional information. Effectively, we can now directly observe the far-from-equilibrium atomic motions involved in barrier crossing and categorize chemistry in terms of a power spectrum of a few dominant reaction modes. It is this reduction in dimensionality that makes chemical reaction mechanisms transferrable to seemingly arbitrarily complex (large N) systems, up to molecules as large as biological macromolecules (N > 1000 atoms). We now have a new way to reformulate reaction mechanisms using an experimentally determined dynamic mode basis that in combination with recent theoretical advances has the potential to lead to a new conceptual basis for chemistry that forms a natural link between structure and dynamics.

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Language(s): eng - English
 Dates: 2016-11-152017-06-07
 Publication Status: Published online
 Pages: 59
 Publishing info: -
 Table of Contents: -
 Rev. Method: Peer
 Identifiers: DOI: 10.1021/acs.chemrev.6b00770
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Title: Chemical Reviews
  Abbreviation : Chem. Rev.
Source Genre: Journal
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Publ. Info: Washington, DC. : American Chemical Society
Pages: - Volume / Issue: 117 (16) Sequence Number: - Start / End Page: 11066 - 11124 Identifier: ISSN: 0009-2665
CoNE: /journals/resource/954925389243