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Title: Periodic density functional LDA and GGA study of CO adsorption at the (001) surface of MgO

Abstract

The deficiencies of the local density approximation (LDA) to describe weakly adsorbed species on ionic surfaces are exposed in the current study of CO on the (001) surface of MgO. The authors applied a periodic formulation of density functional theory with crystal orbitals and charge density expanded as linear combinations of atomic orbitals of Gaussian form. The binding was investigated for four orientations of the CO molecule; either the carbon or oxygen atom of CO down over either the surface magnesium cation or oxygen anion. The authors find that the carbon down over the magnesium cation is the only noticeably attractive configuration, when basis set superposition error is corrected for, and estimate the binding energy of CO to be 1.9 kcal/mol for the Perdew, Burke, and Enzerhof (PBE96) functional. The binding energy obtained in the LDA approximation is as large as 7.4 kcal/mol. For the C-down-over-Mg configuration, the CO stretching frequency shift is only 4 cm{sup {minus}1} for the PBE96 functional. This binding energy, vibrational shift, and analysis of density of states indicate that little chemical bonding accompanies the adsorption. The values of binding energy and vibrational shift support a suggestion by Nygren and Pettersson that the CO adsorption discussedmore » by He et al. actually takes place at defect sites on the (001) surface of MgO.« less

Authors:
; ; ; ; ;
Publication Date:
Research Org.:
Pacific Northwest National Lab., Richland, WA (US)
Sponsoring Org.:
USDOE
OSTI Identifier:
20075909
DOE Contract Number:  
AC06-76RL01830
Resource Type:
Journal Article
Journal Name:
Journal of Physical Chemistry B: Materials, Surfaces, Interfaces, amp Biophysical
Additional Journal Information:
Journal Volume: 104; Journal Issue: 19; Other Information: PBD: 18 May 2000; Journal ID: ISSN 1089-5647
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE; MAGNESIUM OXIDES; CARBON MONOXIDE; MATHEMATICAL MODELS; CRYSTAL MODELS; ADSORPTION; SURFACES

Citation Formats

Snyder, J.A., Alfonso, D.R., Jaffe, J.E., Lin, Z., Hess, A.C., and Gutowski, M. Periodic density functional LDA and GGA study of CO adsorption at the (001) surface of MgO. United States: N. p., 2000. Web. doi:10.1021/jp000820y.
Snyder, J.A., Alfonso, D.R., Jaffe, J.E., Lin, Z., Hess, A.C., & Gutowski, M. Periodic density functional LDA and GGA study of CO adsorption at the (001) surface of MgO. United States. doi:10.1021/jp000820y.
Snyder, J.A., Alfonso, D.R., Jaffe, J.E., Lin, Z., Hess, A.C., and Gutowski, M. Thu . "Periodic density functional LDA and GGA study of CO adsorption at the (001) surface of MgO". United States. doi:10.1021/jp000820y.
@article{osti_20075909,
title = {Periodic density functional LDA and GGA study of CO adsorption at the (001) surface of MgO},
author = {Snyder, J.A. and Alfonso, D.R. and Jaffe, J.E. and Lin, Z. and Hess, A.C. and Gutowski, M.},
abstractNote = {The deficiencies of the local density approximation (LDA) to describe weakly adsorbed species on ionic surfaces are exposed in the current study of CO on the (001) surface of MgO. The authors applied a periodic formulation of density functional theory with crystal orbitals and charge density expanded as linear combinations of atomic orbitals of Gaussian form. The binding was investigated for four orientations of the CO molecule; either the carbon or oxygen atom of CO down over either the surface magnesium cation or oxygen anion. The authors find that the carbon down over the magnesium cation is the only noticeably attractive configuration, when basis set superposition error is corrected for, and estimate the binding energy of CO to be 1.9 kcal/mol for the Perdew, Burke, and Enzerhof (PBE96) functional. The binding energy obtained in the LDA approximation is as large as 7.4 kcal/mol. For the C-down-over-Mg configuration, the CO stretching frequency shift is only 4 cm{sup {minus}1} for the PBE96 functional. This binding energy, vibrational shift, and analysis of density of states indicate that little chemical bonding accompanies the adsorption. The values of binding energy and vibrational shift support a suggestion by Nygren and Pettersson that the CO adsorption discussed by He et al. actually takes place at defect sites on the (001) surface of MgO.},
doi = {10.1021/jp000820y},
journal = {Journal of Physical Chemistry B: Materials, Surfaces, Interfaces, amp Biophysical},
issn = {1089-5647},
number = 19,
volume = 104,
place = {United States},
year = {2000},
month = {5}
}