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Journal of Chemical Physics / Volume 115 / Issue 9 / ARTICLES / Surfaces, Interfaces, and Materials

J. Chem. Phys. 115, 4292 (2001); http://dx.doi.org/10.1063/1.1391253 (8 pages)

Charge transfer and “band lineup” in molecular electronic devices: A chemical and numerical interpretation

Yongqiang Xue1,2, Supriyo Datta2, and Mark A. Ratner1

1Department of Chemistry and Materials Research Center, Northwestern University, Evanston, Illinois 60208
2School of Electrical and Computer Engineering, Purdue University, West Lafayette, Indiana 47907

(Received 7 March 2001; accepted 19 June 2001)

We present first-principles based calculation of charge transfer and “band lineup” in molecular electronic devices using as an example the device formed by a phenyldithiolate molecule bridging two gold electrodes and local-spin-density-functional theory with a Gaussian-type orbital basis. We show that significant charge transfer from the metal to the molecule occurs, reflecting the partially ionic character of the sulfur–gold bond and localized in the interfacial region. Such charge transfer increases the electrostatic potential in the molecule which changes the molecular energy level structures. The interaction between the molecular orbitals under the self-consistent potential and the surface metal states determines the lineup of molecular levels relative to the metal Fermi level. We also discuss the implications of our work on device engineering at the molecular scale. © 2001 American Institute of Physics.

© 2001 American Institute of Physics

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KEYWORDS and PACS

Keywords

molecular electronics, charge exchange, GTO calculations, Fermi level, density functional theory

PACS

  • 85.65.+h

    Molecular electronic devices

  • 34.70.+e

    Charge transfer

  • 71.15.Mb

    Density functional theory, local density approximation, gradient and other corrections

ARTICLE DATA

Digital Object Identifier
http://dx.doi.org/10.1063/1.1391253

PUBLICATION DATA

ISSN

0021-9606 (print)  
1089-7690 (online)

Publisher

$abstract.society.value is a Member of CrossRef American Institute of Physics

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