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

Abstract

Using density functional theory (DFT) with van der Waals functionals, 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 based on many-body perturbation theory within the GW approximation, we obtain approximate self-energy corrections to the DFT highest occupied molecular orbital (HOMO) energy associated with BDA adsorbate phases. As a result, 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.

Authors:
 [1];  [1];  [1];  [2];  [3]
  1. Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States); Univ. of California, Berkeley, CA (United States)
  2. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
  3. Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States); Univ. of California, Berkeley, CA (United States); Kavli Energy NanoSciences Institute at Berkeley, Berkeley, CA (United States)
Publication Date:
Research Org.:
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States); Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)
OSTI Identifier:
1245359
Alternate Identifier(s):
OSTI ID: 1243156; OSTI ID: 1379246
Grant/Contract Number:  
AC02-05CH11231; AC05-00OR22725; AC02-05-CH11231
Resource Type:
Accepted Manuscript
Journal Name:
Physical Review B
Additional Journal Information:
Journal Volume: 93; Journal Issue: 12; Journal ID: ISSN 2469-9950
Publisher:
American Physical Society (APS)
Country of Publication:
United States
Language:
English
Subject:
74 ATOMIC AND MOLECULAR PHYSICS

Citation Formats

Li, Guo, Rangel, Tonatiuh, Liu, Zhen -Fei, Cooper, Valentino R., and Neaton, Jeffrey B. Energy level alignment of self-assembled linear chains of benzenediamine on Au(111) from first principles. United States: N. p., 2016. Web. doi:10.1103/PhysRevB.93.125429.
Li, Guo, Rangel, Tonatiuh, Liu, Zhen -Fei, Cooper, Valentino R., & Neaton, Jeffrey B. Energy level alignment of self-assembled linear chains of benzenediamine on Au(111) from first principles. United States. doi:10.1103/PhysRevB.93.125429.
Li, Guo, Rangel, Tonatiuh, Liu, Zhen -Fei, Cooper, Valentino R., and Neaton, Jeffrey B. Thu . "Energy level alignment of self-assembled linear chains of benzenediamine on Au(111) from first principles". United States. doi:10.1103/PhysRevB.93.125429. https://www.osti.gov/servlets/purl/1245359.
@article{osti_1245359,
title = {Energy level alignment of self-assembled linear chains of benzenediamine on Au(111) from first principles},
author = {Li, Guo and Rangel, Tonatiuh and Liu, Zhen -Fei and Cooper, Valentino R. and Neaton, Jeffrey B.},
abstractNote = {Using density functional theory (DFT) with van der Waals functionals, 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 based on many-body perturbation theory within the GW approximation, we obtain approximate self-energy corrections to the DFT highest occupied molecular orbital (HOMO) energy associated with BDA adsorbate phases. As a result, 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.},
doi = {10.1103/PhysRevB.93.125429},
journal = {Physical Review B},
number = 12,
volume = 93,
place = {United States},
year = {2016},
month = {3}
}

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