Imaging the square of the correlated two-electron wave function of a hydrogen molecule

  • The toolbox for imaging molecules is well-equipped today. Some techniques visualize the geometrical structure, others the electron density or electron orbitals. Molecules are many-body systems for which the correlation between the constituents is decisive and the spatial and the momentum distribution of one electron depends on those of the other electrons and the nuclei. Such correlations have escaped direct observation by imaging techniques so far. Here, we implement an imaging scheme which visualizes correlations between electrons by coincident detection of the reaction fragments after high energy photofragmentation. With this technique, we examine the H2 two-electron wave function in which electron–electron correlation beyond the mean-field level is prominent. We visualize the dependence of the wave function on the internuclear distance. High energy photoelectrons are shown to be a powerful tool for molecular imaging. Our study paves the way for future time resolved correlation imaging at FELs and laser based X-ray sources.

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Author:Markus Waitz, Roger Y. Bello, Daniel Metz, Julian Lower, Florian Trinter, Carl Schober, Marco Keiling, Ute Lenz, Martin Pitzer, Karolin Mertens, Michael Martins, Jens Viefhaus, Stephan Klumpp, Thorsten WeberORCiDGND, Lothar SchmidtGND, Joshua B. WilliamsORCiD, Markus S. SchöfflerORCiDGND, Vladislav V. Serov, Anatoli Kheifets, Luca Argenti, Alicia Palacios, Fernando Martín, Till JahnkeORCiDGND, Reinhard DörnerORCiDGND
URN:urn:nbn:de:hebis:30:3-455748
DOI:https://doi.org/10.1038/s41467-017-02437-9
ISSN:2041-1723
Pubmed Id:https://pubmed.ncbi.nlm.nih.gov/29273745
Parent Title (English):Nature Communications
Publisher:Nature Publishing Group UK
Place of publication:[London]
Document Type:Article
Language:English
Year of Completion:2017
Date of first Publication:2017/12/22
Publishing Institution:Universitätsbibliothek Johann Christian Senckenberg
Release Date:2018/01/25
Tag:Atomic and molecular interactions with photons; Chemical physics; Electronic structure of atoms and molecules; Techniques and instrumentation
Volume:8
Issue:1, Art. 2266
Page Number:8
First Page:1
Last Page:8
Note:
Open Access: This article is licensed under a Creative Commons Attribution 4.0 International License, which permits use, sharing, adaptation, distribution and reproduction in any medium or format, as long as you give appropriate credit to the original author(s) and the source, provide a link to the Creative Commons license, and indicate if changes were made. The images or other third party material in this article are included in the article’s Creative Commons license, unless indicated otherwise in a credit line to the material. If material is not included in the article’s Creative Commons license and your intended use is not permitted by statutory regulation or exceeds the permitted use, you will need to obtain permission directly from the copyright holder. To view a copy of this license, visit http://creativecommons.org/ licenses/by/4.0/. © The Author(s) 2017
Note:
Publisher correction erschienen in: Nature Communications, 9.2018, Nr. 1, Art. 2259, doi:10.1038/s41467-018-04740-5
HeBIS-PPN:425782506
Institutes:Physik / Physik
Dewey Decimal Classification:5 Naturwissenschaften und Mathematik / 53 Physik / 530 Physik
Sammlungen:Universitätspublikationen
Licence (German):License LogoCreative Commons - Namensnennung 4.0