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arXiv · 1111.2569

Electronic energy level alignment at metal-molecule interfaces with a GW approach

Isaac Tamblyn·Pierre Darancet·Su Ying Quek·Stanimir A. Bonev·Jeffrey B. Neaton
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Abstract

Using density functional theory and many-body perturbation theory within a GW approximation, we calculate the electronic structure of a metal-molecule interface consisting of benzene diamine (BDA) adsorbed on Au(111). Through direct comparison with photoemission data, we show that a conventional G$_0$W$_0$ approach can underestimate the energy of the adsorbed molecular resonance relative to the Au Fermi level by up to 0.8 eV. The source of this discrepancy is twofold: a 0.7 eV underestimate of the gas phase ionization energy (IE), and a 0.2 eV overestimate of the Au work function. Refinements to self-energy calculations within the GW framework that account for deviations in both the Au work function and BDA gas-phase IE can result in an interfacial electronic level alignment in quantitative agreement with experiment.

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Isaac Tamblyn, Pierre Darancet, Su Ying Quek, Stanimir A. Bonev, Jeffrey B. Neaton. 2011-11-10. Electronic energy level alignment at metal-molecule interfaces with a GW approach. https://doi.org/10.1103/physrevb.84.201402

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