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Localization and loss of coherence in molecular double-slit experiments

Zimmermann, Björn and Rolles, Daniel and Langer, Burkhard and Hentges, Rainer and Braune, Markus and Cvejanovic, Slobodan and Geßner, Oliver and Heiser, Franz and Korica, Sanja and Lischke, Toralf and Reinköster, Axel and Viefhaus, Jens and Dörner, Reinhard and McKoy, Vincent and Becker, Uwe (2008) Localization and loss of coherence in molecular double-slit experiments. Nature Physics, 4 (8). pp. 649-655. ISSN 1745-2473. doi:10.1038/nphys993.

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In molecular double-slit experiments, the interference between emitted core electrons of diatomic molecules gives rise to oscillations in the observed electron intensity. Here, we explore this behaviour for photoelectrons emitted from CO and N_2 by soft X-ray ionization in the molecular frame, and we argue that in addition to the undisturbed emission process, intramolecular scattering can lead to electron interference between the scattered and unscattered wave in two ways: two-centre interference between two spatially coherent emitters and one-centre self-interference. The latter is the signature of a loss of spatial coherence. The spatial scale over which the transition from two-centre to one-centre coherence occurs is the de Broglie wavelength of the scattered photoelectron in units of the bond length. These results highlight the fact that the molecular double slit is based on two independent uncertainty principles, Δp_xΔx and ΔEΔt, the second of which causes ongoing tunnelling between the two centres, even after the collapse of the electron wavefunction in real space.

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Additional Information:© 2008 Macmillan Publishers Limited. Received 7 November 2007; Accepted 9 May 2008; Published online 15 June 2008. The authors acknowledge financial support by the Bundesministerium für Bildung und Forschung (BMBF Contract No. 05KS4EB1/3). B.Z. and D.R. thank the Alexander von Humboldt Foundation for a Feodor Lynen fellowship. The authors are grateful to David Shirley for providing the initial beam time for this project at the Advanced Light Source. They also thank E. Moler for his help during this initial period, G. Prümper for his contribution to the development and implementation of the detector and D. Dowek and A. Roy for helpful comments and critical reading of the manuscript. Author contributions: The calculations were carried out by B.Z. and V.M., whereas the measurements and the analysis of the experimental data were done by the other authors.
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Bundesministerium für Bildung und Forschung (BMBF)05KS4EB1/3
Alexander von Humboldt FoundationUNSPECIFIED
Issue or Number:8
Record Number:CaltechAUTHORS:20151027-154124890
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Usage Policy:No commercial reproduction, distribution, display or performance rights in this work are provided.
ID Code:61593
Deposited By: George Porter
Deposited On:28 Oct 2015 18:27
Last Modified:10 Nov 2021 22:51

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