Isotope-induced partial localization of core electrons in the homonuclear molecule N2

Daniel Rolles, Markus Braune, Slobodan Cvejanović, Oliver Geßner, Rainer Hentges, Sanja Korica, Burkhard Langer, Toralf Lischke, Georg Prümper, Axel Reinköster, Jens Viefhaus, Björn Zimmermann, Vincent McKoy and Uwe Becker ()
Additional contact information
Daniel Rolles: Fritz-Haber-Institut der Max-Planck-Gesellschaft
Markus Braune: Fritz-Haber-Institut der Max-Planck-Gesellschaft
Slobodan Cvejanović: Fritz-Haber-Institut der Max-Planck-Gesellschaft
Oliver Geßner: Fritz-Haber-Institut der Max-Planck-Gesellschaft
Rainer Hentges: Fritz-Haber-Institut der Max-Planck-Gesellschaft
Sanja Korica: Fritz-Haber-Institut der Max-Planck-Gesellschaft
Burkhard Langer: Max-Born-Institut für Nichtlineare Optik und Kurzzeitspektroskopie
Toralf Lischke: Fritz-Haber-Institut der Max-Planck-Gesellschaft
Georg Prümper: Fritz-Haber-Institut der Max-Planck-Gesellschaft
Axel Reinköster: Fritz-Haber-Institut der Max-Planck-Gesellschaft
Jens Viefhaus: Fritz-Haber-Institut der Max-Planck-Gesellschaft
Björn Zimmermann: California Institute of Technology
Vincent McKoy: California Institute of Technology
Uwe Becker: Fritz-Haber-Institut der Max-Planck-Gesellschaft

Nature, 2005, vol. 437, issue 7059, 711-715

Abstract: Abstract Because of inversion symmetry and particle exchange, all constituents of homonuclear diatomic molecules are in a quantum mechanically non-local coherent state; this includes the nuclei and deep-lying core electrons. Hence, the molecular photoemission can be regarded as a natural double-slit experiment1: coherent electron emission originates from two identical sites, and should give rise to characteristic interference patterns2. However, the quantum coherence is obscured if the two possible symmetry states of the electronic wavefunction (‘gerade’ and ‘ungerade’) are degenerate; the sum of the two exactly resembles the distinguishable, incoherent emission from two localized core sites. Here we observe the coherence of core electrons in N2 through a direct measurement of the interference exhibited in their emission. We also explore the gradual transition to a symmetry-broken system of localized electrons by comparing different isotope-substituted species—a phenomenon analogous to the acquisition of partial ‘which-way’ information in macroscopic double-slit experiments3.

Date: 2005
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DOI: 10.1038/nature04040

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