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  Mapping Atomic Motions with Electrons: Toward the Quantum Limit to Imaging Chemistry

Li, Z., Gyawali, S., Ischenko, A. A., Hayes, S. A., & Miller, R. J. D. (2020). Mapping Atomic Motions with Electrons: Toward the Quantum Limit to Imaging Chemistry. ACS Photonics, 7(2), 296-320. doi:10.1021/acsphotonics.9b01008.

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Li, Z.1, 2, Author              
Gyawali, S.3, Author
Ischenko, A. A.4, Author
Hayes, S. A.2, Author              
Miller, R. J. D.2, 5, Author              
1State Key Laboratory for Mesoscopic Physics, School of Physics, Peking University, ou_persistent22              
2Miller Group, Atomically Resolved Dynamics Department, Max Planck Institute for the Structure and Dynamics of Matter, Max Planck Society, ou_1938288              
3Department of Mathematics and Logistics, Jacobs University Bremen, ou_persistent22              
4Institute of Fine Chemical Technologies, MIREA - Russian Technological University, ou_persistent22              
5Departments of Chemistry and Physics, University of Toronto, ou_persistent22              


Free keywords: atomically resolved reaction dynamics, key reaction modes, femtosecond time-resolved electron diffraction, time-resolved real-space imaging, quantum tomography, fundamental space time limits to imaging chemistry
 Abstract: Recent advances in ultrafast electron and X-ray diffraction have pushed imaging of structural dynamics into the femtosecond time domain, that is, the fundamental time scale of atomic motion. New physics can be reached beyond the scope of traditional diffraction or reciprocal space imaging. By exploiting the high time resolution, it has been possible to directly observe the collapse of nearly innumerable possible nuclear motions to a few key reaction modes that direct chemistry. It is this reduction in dimensionality in the transition state region that makes chemistry a transferable concept, with the same class of reactions being applicable to synthetic strategies to nearly arbitrary levels of complexity. The ability to image the underlying key reaction modes has been achieved with resolution to relative changes in atomic positions to better than 0.01 Å, that is, comparable to thermal motions. We have effectively reached the fundamental space-time limit with respect to the reaction energetics and imaging the acting forces. In the process of ensemble measured structural changes, we have missed the quantum aspects of chemistry. This perspective reviews the current state of the art in imaging chemistry in action and poses the challenge to access quantum information on the dynamics. There is the possibility with the present ultrabright electron and X-ray sources, at least in principle, to do tomographic reconstruction of quantum states in the form of a Wigner function and density matrix for the vibrational, rotational, and electronic degrees of freedom. Accessing this quantum information constitutes the ultimate demand on the spatial and temporal resolution of reciprocal space imaging of chemistry. Given the much shorter wavelength and corresponding intrinsically higher spatial resolution of current electron sources over X-rays, this Perspective will focus on electrons to provide an overview of the challenge on both the theory and the experimental fronts to extract the quantum aspects of molecular dynamics.


Language(s): eng - English
 Dates: 2019-12-092019-07-212019-12-182020-02-19
 Publication Status: Published in print
 Pages: 25
 Publishing info: -
 Table of Contents: -
 Rev. Type: Peer
 Identifiers: DOI: 10.1021/acsphotonics.9b01008
 Degree: -



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Project name : This work was supported by the Max Planck Society, with contributions from the Cluster of Excellence “The Hamburg Centre for Ultrafast Imaging” of the Deutsche Forschungsgemeinschaft (DFG), EXC 1074, Project ID 194651731. A.A.I. acknowledges support by RFBR Grant 16-29-1167 OFI_m and partial support by Grant 16-29-11741 OFI_m.
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Source 1

Title: ACS Photonics
Source Genre: Journal
Publ. Info: Washington, DC : American Chemical Society
Pages: - Volume / Issue: 7 (2) Sequence Number: - Start / End Page: 296 - 320 Identifier: ISSN: 2330-4022
CoNE: https://pure.mpg.de/cone/journals/resource/2330-4022