Benzene and Pyridine on Silicon (001): A Trial Ground for Long Range Corrections in Density Functional Theory

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DOI

  • Oliver Warschkow, Sydney University, Sydney
  • ,
  • J.M. Bennett, Sydney University, Sydney
  • ,
  • J. A. Miwa
  • G. P. Lopinski, Natl Res Council Canada, National Research Council Canada
  • ,
  • F. Rosei, Univ Quebec, University of Quebec, Geotop
  • ,
  • D. R. McKenzie, Sydney University, Sydney
  • ,
  • Nigel A. Marks, Curtin University

The adsorption chemistry of benzene and pyridine on the silicon (001) surface is characterized by two prominent adsorbate configurations: a precursor structure bonded to a single Si Si dimer and a "tight-bridge" configuration that connects two adjacent dimers. We examine here the performance of 20 density functionals in predicting the relative stability of these two configurations. Discrepancies between the predicted and experimentally observed preferred structures highlight the importance of long-range exact-exchange terms in these adsorbate systems. These terms, however, tend to be detrimental to the prediction of adsorption and activation energies. We discuss this conundrum in terms of systematic exchange-correlation errors that scale with the number of molecule-surface bonds.

Original languageEnglish
JournalThe Journal of Physical Chemistry Part C
Volume121
Issue19
Pages (from-to)10484-10500
Number of pages17
ISSN1932-7447
DOIs
Publication statusPublished - 18 May 2017

    Research areas

  • GENERALIZED-GRADIENT-APPROXIMATION, SCANNING-TUNNELING-MICROSCOPY, BINDING STATE CONVERSION, ELECTRONIC-STRUCTURE, DISPERSION CORRECTIONS, CORRELATION-ENERGY, SURFACE-CHEMISTRY, SI(100) SURFACE, ADSORPTION, ACCURACY

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