Energy level alignment of self-assembled linear chains of benzenediamine on Au(111) from first principles

Guo Li, Tonatiuh Rangel, Zhen Fei Liu, Valentino R. Cooper, Jeffrey B. Neaton

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Abstract

Using density functional theory (DFT) with a van der Waals density functional, we calculate the adsorption energetics and geometry of benzenediamine (BDA) molecules on Au(111) surfaces. Our results demonstrate that the reported self-assembled linear chain structure of BDA, stabilized via hydrogen bonds between amine groups, is energetically favored over previously studied monomeric phases. Moreover, using a model, which includes nonlocal polarization effects from the substrate and the neighboring molecules and incorporates many-body perturbation theory calculations within the GW approximation, we obtain approximate self-energy corrections to the DFT highest occupied molecular orbital (HOMO) energy associated with BDA adsorbate phases. We find that, independent of coverage, the HOMO energy of the linear chain phase is lower relative to the Fermi energy than that of the monomer phase, and in good agreement with values measured with ultraviolet photoelectron spectroscopy and x-ray photoelectron spectroscopy.

Original languageEnglish
Article number125429
JournalPhysical Review B
Volume93
Issue number12
DOIs
StatePublished - Mar 24 2016

Funding

This work was supported by the Director, Office of Science, Office of Basic Energy Sciences, Materials Sciences and Engineering Division, of the U.S. Department of Energy under Contract No. DE-AC02-05-CH11231. Work at the Molecular Foundry was supported by the Office of Science, Office of Basic Energy Sciences and by the U.S. Department of Energy under Contract No. DE-AC02-05CH11231. Work by V.R.C. was supported by the U.S. DOE, Office of Science, Basic Energy Sciences, Materials Sciences and Energy Division. All calculations were carried out at NERSC.

FundersFunder number
Materials Sciences and Energy Division
U.S. Department of EnergyDE-AC02-05-CH11231
Office of Science
Basic Energy Sciences
Division of Materials Sciences and Engineering

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