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Influence of orbital symmetry on diffraction imaging with rescattering electron wave packets

The ability to directly follow and time-resolve the rearrangement of the nuclei within molecules is a frontier of science that requires atomic spatial and few-femtosecond temporal resolutions. While laser-induced electron diffraction can meet these requirements, it was recently concluded that molecu...

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Autores principales: Pullen, M. G., Wolter, B., Le, A. -T., Baudisch, M., Sclafani, M., Pires, H., Schröter, C. D., Ullrich, J., Moshammer, R., Pfeifer, T., Lin, C. D., Biegert, J.
Formato: Online Artículo Texto
Lenguaje:English
Publicado: Nature Publishing Group 2016
Materias:
Acceso en línea:https://www.ncbi.nlm.nih.gov/pmc/articles/PMC4917885/
https://www.ncbi.nlm.nih.gov/pubmed/27329236
http://dx.doi.org/10.1038/ncomms11922
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author Pullen, M. G.
Wolter, B.
Le, A. -T.
Baudisch, M.
Sclafani, M.
Pires, H.
Schröter, C. D.
Ullrich, J.
Moshammer, R.
Pfeifer, T.
Lin, C. D.
Biegert, J.
author_facet Pullen, M. G.
Wolter, B.
Le, A. -T.
Baudisch, M.
Sclafani, M.
Pires, H.
Schröter, C. D.
Ullrich, J.
Moshammer, R.
Pfeifer, T.
Lin, C. D.
Biegert, J.
author_sort Pullen, M. G.
collection PubMed
description The ability to directly follow and time-resolve the rearrangement of the nuclei within molecules is a frontier of science that requires atomic spatial and few-femtosecond temporal resolutions. While laser-induced electron diffraction can meet these requirements, it was recently concluded that molecules with particular orbital symmetries (such as π(g)) cannot be imaged using purely backscattering electron wave packets without molecular alignment. Here, we demonstrate, in direct contradiction to these findings, that the orientation and shape of molecular orbitals presents no impediment for retrieving molecular structure with adequate sampling of the momentum transfer space. We overcome previous issues by showcasing retrieval of the structure of randomly oriented O(2) and C(2)H(2) molecules, with π(g) and π(u) symmetries, respectively, and where their ionization probabilities do not maximize along their molecular axes. While this removes a serious bottleneck for laser-induced diffraction imaging, we find unexpectedly strong backscattering contributions from low-Z atoms.
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spelling pubmed-49178852016-07-07 Influence of orbital symmetry on diffraction imaging with rescattering electron wave packets Pullen, M. G. Wolter, B. Le, A. -T. Baudisch, M. Sclafani, M. Pires, H. Schröter, C. D. Ullrich, J. Moshammer, R. Pfeifer, T. Lin, C. D. Biegert, J. Nat Commun Article The ability to directly follow and time-resolve the rearrangement of the nuclei within molecules is a frontier of science that requires atomic spatial and few-femtosecond temporal resolutions. While laser-induced electron diffraction can meet these requirements, it was recently concluded that molecules with particular orbital symmetries (such as π(g)) cannot be imaged using purely backscattering electron wave packets without molecular alignment. Here, we demonstrate, in direct contradiction to these findings, that the orientation and shape of molecular orbitals presents no impediment for retrieving molecular structure with adequate sampling of the momentum transfer space. We overcome previous issues by showcasing retrieval of the structure of randomly oriented O(2) and C(2)H(2) molecules, with π(g) and π(u) symmetries, respectively, and where their ionization probabilities do not maximize along their molecular axes. While this removes a serious bottleneck for laser-induced diffraction imaging, we find unexpectedly strong backscattering contributions from low-Z atoms. Nature Publishing Group 2016-06-22 /pmc/articles/PMC4917885/ /pubmed/27329236 http://dx.doi.org/10.1038/ncomms11922 Text en Copyright © 2016, Nature Publishing Group, a division of Macmillan Publishers Limited. All Rights Reserved. http://creativecommons.org/licenses/by/4.0/ This work is licensed under a Creative Commons Attribution 4.0 International License. The images or other third party material in this article are included in the article's Creative Commons license, unless indicated otherwise in the credit line; if the material is not included under the Creative Commons license, users will need to obtain permission from the license holder to reproduce the material. To view a copy of this license, visit http://creativecommons.org/licenses/by/4.0/
spellingShingle Article
Pullen, M. G.
Wolter, B.
Le, A. -T.
Baudisch, M.
Sclafani, M.
Pires, H.
Schröter, C. D.
Ullrich, J.
Moshammer, R.
Pfeifer, T.
Lin, C. D.
Biegert, J.
Influence of orbital symmetry on diffraction imaging with rescattering electron wave packets
title Influence of orbital symmetry on diffraction imaging with rescattering electron wave packets
title_full Influence of orbital symmetry on diffraction imaging with rescattering electron wave packets
title_fullStr Influence of orbital symmetry on diffraction imaging with rescattering electron wave packets
title_full_unstemmed Influence of orbital symmetry on diffraction imaging with rescattering electron wave packets
title_short Influence of orbital symmetry on diffraction imaging with rescattering electron wave packets
title_sort influence of orbital symmetry on diffraction imaging with rescattering electron wave packets
topic Article
url https://www.ncbi.nlm.nih.gov/pmc/articles/PMC4917885/
https://www.ncbi.nlm.nih.gov/pubmed/27329236
http://dx.doi.org/10.1038/ncomms11922
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