Journal
PROCEEDINGS OF THE NATIONAL ACADEMY OF SCIENCES OF THE UNITED STATES OF AMERICA
Volume 108, Issue 18, Pages 7302-7306Publisher
NATL ACAD SCIENCES
DOI: 10.1073/pnas.1018534108
Keywords
photoelectron spectroscopy; molecular spectroscopy; molecular ionization; density functional theory; quantum chemistry
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Funding
- Ministerio de Ciencia e Innovacion (Spain) [FIS2010-15127, ACI2008-0777, CSD2007-00010]
- European Cooperation in Science and Technology Action [CM0702]
- DOE [DE-AC02-05CH11231]
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Vibrationally resolved valence-shell photoionization spectra of H(2), N(2) and CO have been measured in the photon energy range 20-300 eV using third-generation synchrotron radiation. Young's double-slit interferences lead to oscillations in the corresponding vibrational ratios, showing that the molecules behave as two-center electron-wave emitters and that the associated interferences leave their trace in the angle-integrated photoionization cross section. In contrast to previous work, the oscillations are directly observable in the experiment, thereby removing any possible ambiguity related to the introduction of external parameters or fitting functions. A straightforward extension of an original idea proposed by Cohen and Fano [Cohen HD, Fano U (1966) Phys Rev 150: 30] confirms this interpretation and shows that it is also valid for diatomic heteronuclear molecules. Results of accurate theoretical calculations are in excellent agreement with the experimental findings.
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