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

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. Finally, our study paves the way for future time resolved correlation imaging at FELs and laser based X-ray sources.

Authors:
 [1];  [2];  [1];  [1];  [1];  [1];  [1];  [1]; ORCiD logo [3];  [4];  [4];  [5];  [5];  [6];  [1];  [7];  [1];  [8];  [9];  [10] more »;  [2];  [11];  [1]; ORCiD logo [1] « less
  1. Goethe Univ., Frankfurt (Germany). Inst. fur Kernphysik
  2. Autonomous Univ. of Madrid (Spain). Dept. de Quimica
  3. Univ. Kassel, Kassel (Germany)
  4. Univ. of Hamburg (Germany). Inst. fur Experimentalphysik
  5. Deutsches Elektronen-Synchrotron (DESY), Hamburg (Germany)
  6. Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). Chemical Sciences Division
  7. Univ. of Nevada, Reno, NV (United States). Dept. of Physics
  8. Saratov State Univ. (Russian Federation). Dept. of Theoretical Physics
  9. Australian National Univ., Canberra, ACT (Australia). Research School of Physical Sciences and Engineering
  10. Autonomous Univ. of Madrid (Spain). Dept. de Quimica; Univ. of Central Florida, Orlando, FL (United States). Dept. of Physics and CREOL College of Optics & Photonic
  11. Autonomous Univ. of Madrid (Spain). Dept. de Quimica; Inst. Madrileo de Estudios Avanzados en Nanociencia, Madrid (Spain); Autonomous Univ. of Madrid (Spain). Condensed Matter Physics Center (IFIMAC)
Publication Date:
Research Org.:
Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)
OSTI Identifier:
1432225
Grant/Contract Number:  
AC02-05CH11231
Resource Type:
Accepted Manuscript
Journal Name:
Nature Communications
Additional Journal Information:
Journal Volume: 8; Journal Issue: 1; Journal ID: ISSN 2041-1723
Publisher:
Nature Publishing Group
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; 71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSICS

Citation Formats

Waitz, M., Bello, R. Y., Metz, D., Lower, J., Trinter, F., Schober, C., Keiling, M., Lenz, U., Pitzer, M., Mertens, K., Martins, M., Viefhaus, J., Klumpp, S., Weber, T., Schmidt, L. Ph. H., Williams, J. B., Schoffler, M. S., Serov, V. V., Kheifets, A. S., Argenti, L., Palacios, A., Martin, F., Jahnke, T., and Dorner, R. Imaging the square of the correlated two-electron wave function of a hydrogen molecule. United States: N. p., 2017. Web. doi:10.1038/s41467-017-02437-9.
Waitz, M., Bello, R. Y., Metz, D., Lower, J., Trinter, F., Schober, C., Keiling, M., Lenz, U., Pitzer, M., Mertens, K., Martins, M., Viefhaus, J., Klumpp, S., Weber, T., Schmidt, L. Ph. H., Williams, J. B., Schoffler, M. S., Serov, V. V., Kheifets, A. S., Argenti, L., Palacios, A., Martin, F., Jahnke, T., & Dorner, R. Imaging the square of the correlated two-electron wave function of a hydrogen molecule. United States. doi:10.1038/s41467-017-02437-9.
Waitz, M., Bello, R. Y., Metz, D., Lower, J., Trinter, F., Schober, C., Keiling, M., Lenz, U., Pitzer, M., Mertens, K., Martins, M., Viefhaus, J., Klumpp, S., Weber, T., Schmidt, L. Ph. H., Williams, J. B., Schoffler, M. S., Serov, V. V., Kheifets, A. S., Argenti, L., Palacios, A., Martin, F., Jahnke, T., and Dorner, R. Fri . "Imaging the square of the correlated two-electron wave function of a hydrogen molecule". United States. doi:10.1038/s41467-017-02437-9. https://www.osti.gov/servlets/purl/1432225.
@article{osti_1432225,
title = {Imaging the square of the correlated two-electron wave function of a hydrogen molecule},
author = {Waitz, M. and Bello, R. Y. and Metz, D. and Lower, J. and Trinter, F. and Schober, C. and Keiling, M. and Lenz, U. and Pitzer, M. and Mertens, K. and Martins, M. and Viefhaus, J. and Klumpp, S. and Weber, T. and Schmidt, L. Ph. H. and Williams, J. B. and Schoffler, M. S. and Serov, V. V. and Kheifets, A. S. and Argenti, L. and Palacios, A. and Martin, F. and Jahnke, T. and Dorner, R.},
abstractNote = {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. Finally, our study paves the way for future time resolved correlation imaging at FELs and laser based X-ray sources.},
doi = {10.1038/s41467-017-02437-9},
journal = {Nature Communications},
number = 1,
volume = 8,
place = {United States},
year = {2017},
month = {12}
}

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    Works referencing / citing this record:

    The photon‐ion merged‐beams experiment PIPE at PETRA III—The first five years
    journal, April 2019

    • Schippers, Stefan; Buhr, Ticia; Borovik, Alexander
    • X-Ray Spectrometry, Vol. 49, Issue 1
    • DOI: 10.1002/xrs.3035

    The photon‐ion merged‐beams experiment PIPE at PETRA III—The first five years
    text, January 2019

    • Schippers, Stefan; Buhr, Ticia; Borovik, Alexander
    • Deutsches Elektronen-Synchrotron, DESY, Hamburg
    • DOI: 10.3204/pubdb-2019-02368