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Nat Commun. 2017 Dec 22;8(1):2266. doi: 10.1038/s41467-017-02437-9.

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

Author information

1
Institut für Kernphysik, J. W. Goethe Universität, Max-von-Laue-Str. 1, 60438, Frankfurt, Germany.
2
Departamento de Química, Universidad Autónoma de Madrid, 28049, Madrid, Spain.
3
Universität Kassel, Heinr.-Plett-Strasse 40, 34132, Kassel, Germany.
4
Institut für Experimentalphysik, Universität Hamburg, Luruper Chaussee 149, 22761, Hamburg, Germany.
5
FS-PE, Deutsches Elektronen-Synchrotron DESY, Notkestrasse 85, 22607, Hamburg, Germany.
6
FS-FLASH-D, Deutsches Elektronen-Synchrotron DESY, Notkestrasse 85, 22607, Hamburg, Germany.
7
Chemical Sciences Division, Lawrence Berkeley National Laboratory, Berkeley, CA, 94720, USA.
8
Department of Physics, University of Nevada Reno, 1664 N. Virginia Street, Reno, NV, 89557, USA.
9
Department of Theoretical Physics, Saratov State University, 83 Astrakhanskaya, Saratov, 410012, Russia.
10
Research School of Physical Sciences, The Australian National University, Canberra, ACT, 0200, Australia.
11
Department of Physics and CREOL College of Optics & Photonics, University of Central Florida, Orlando, FL 32816, USA.
12
Departamento de Química, Universidad Autónoma de Madrid, 28049, Madrid, Spain. fernando.martin@uam.es.
13
Instituto Madrileo de Estudios Avanzados en Nanociencia, 28049, Madrid, Spain. fernando.martin@uam.es.
14
Condensed Matter Physics Center (IFIMAC), Universidad Autónoma de Madrid, 28049, Madrid, Spain. fernando.martin@uam.es.
15
Institut für Kernphysik, J. W. Goethe Universität, Max-von-Laue-Str. 1, 60438, Frankfurt, Germany. doerner@atom.uni-frankfurt.de.

Abstract

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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