Investigación

 

Nature of the bonding, surface relaxation and charge transfer of Au dimmers on an MgO(100) surface

 

C. Quintanar^a, R. Caballero^a, J. Ulises Reveles^b, and S.N. Khanna^b

 

^a Facultad de Ciencias, Universidad Nacional Autónoma de México, Ciudad Universitaria, 04510 México, D.F., México. e–mail: cqs@matrix.super.unam.mx

^b Physics Department, Virginia Commonwealth University, Richmond, Virginia, 23284–2000, USA.

 

Recibido el 12 de mayo de 2011.
Aceptado el 15 de diciembre de 2011.

 

Abstract

First principles electronic structure investigations of the nature of adsorption, relaxation of the atoms near the adsorption site, and the charging of the Au₂ particle on the relaxed–rumpled MgO(100) surface have been carried out within the density functional theory–cluster–embedding approach. The investigations focus on an Au₂ molecule, perpendicular to the surface, adsorbed at different locations. Three bonding sites are studied: a five coordinated oxygen regular terrace site O_5c, an F_s neutral color center (two electrons in an O vacancy), and an F⁺_s positive charged color center (one electron in an O vacancy). The studies indicate that large relaxation of the neighboring atoms and large charge transfer occurs for an Au₂ over the color centers. An analysis of the one–electron energy levels of the Au dimer, the MgO surface and the Au₂MgO(100) complex for each absorption site allows us to rationalize the nature of the bonding, surface relaxation, calculated absorption and dimerization energies and electron charge transfers.

Keywords: Supported gold nanoparticles; gold catalysis; density functional theory; metal oxides.

 

PACS: 61.72.Ji; 68.47.Jn

 

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Acknowledgments

C.Q. acknowledges Prof. Dennis R. Salahub forvaluable discussions. R.C and C.Q. acknowledge financial support by the PAPIIT–UNAM IN116912–3 project and Proyecto Universitario de Tecnología Ambiental PUNTA–UNAM. S.N.K. and J.U.R. acknowledges support from the MURI grant from the Air Force Office of Scientific Research grant. Part of the calculations was performed on the computational equipment of DGSCA UNAM, particularly at the super computer Kan–Balam.

 

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