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Self-consistent GW calculations of electronic transport in thiol- and amine-linked molecular junctions

M. Strange, C. Rostgaard, H. Häkkinen, and K. S. Thygesen
Phys. Rev. B 83, 115108 – Published 4 March 2011

Abstract

The electronic conductance of a benzene molecule connected to gold electrodes via thiol, thiolate, or amino anchoring groups is calculated using nonequilibrium Green functions in combination with the fully self-consistent GW approximation for exchange and correlation. The calculated conductance of benzenedithiol and benzenediamine is one-fifth that predicted by standard density functional theory (DFT), in very good agreement with experiments. In contrast, the widely studied benzenedithiolate structure is found to have a significantly higher conductance due to the unsaturated sulfur bonds. These findings suggest that more complex gold-thiolate structures where the thiolate anchors are chemically passivated by Au adatoms are responsible for the measured conductance. Analysis of the energy level alignment obtained with DFT, Hartree-Fock, and GW reveals the importance of self-interaction corrections (exchange) on the molecule and dynamical screening at the metal-molecule interface. The main effect of the GW self-energy is to renormalize the level positions; however, its influence on the shape of molecular resonances also affects the conductance. Non-self-consistent G0W0 calculations, starting from either DFT or Hartree-Fock, yield conductance values within 50% of the self-consistent GW results.

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  • Received 14 January 2011

DOI:https://doi.org/10.1103/PhysRevB.83.115108

©2011 American Physical Society

Authors & Affiliations

M. Strange1,2, C. Rostgaard1, H. Häkkinen2, and K. S. Thygesen1,*

  • 1Center for Atomic-scale Materials Design, Department of Physics, Technical University of Denmark, DK-2800 Kgs. Lyngby, Denmark
  • 2Departments of Physics and Chemistry, University of Jyväskylä, FI-40014 Jyväskylä, Finland

  • *thygesen@fysik.dtu.dk

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Vol. 83, Iss. 11 — 15 March 2011

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