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Title: Energy band alignment and electronic states of amorphous carbon surfaces in vacuo and in aqueous environment

In this paper, we obtain the energy band positions of amorphous carbon (a–C) surfaces in vacuum and in aqueous environment. The calculations are performed using a combination of (i) classical molecular dynamics (MD), (ii) Kohn-Sham density functional theory with the Perdew-Burke-Ernzerhof (PBE) exchange-correlation functional, and (iii) the screened-exchange hybrid functional of Heyd, Scuseria, and Ernzerhof (HSE). PBE allows an accurate generation of a-C and the evaluation of the local electrostatic potential in the a-C/water system, HSE yields an improved description of energetic positions which is critical in this case, and classical MD enables a computationally affordable description of water. Our explicit calculation shows that, both in vacuo and in aqueous environment, the a-C electronic states available in the region comprised between the H{sub 2}/H{sub 2}O and O{sub 2}/H{sub 2}O levels of water correspond to both occupied and unoccupied states within the a-C pseudogap region. These are localized states associated to sp{sup 2} sites in a-C. The band realignment induces a shift of approximately 300 meV of the a-C energy band positions with respect to the redox levels of water.
Authors:
 [1] ;  [2] ;  [3] ;  [4] ;  [1]
  1. Department of Electrical Engineering and Automation, Aalto University, Espoo (Finland)
  2. (Finland)
  3. Department of Chemistry, Aalto University, Espoo (Finland)
  4. Department of Applied Physics, COMP Centre of Excellence in Computational Nanoscience, Aalto University, Espoo (Finland)
Publication Date:
OSTI Identifier:
22412964
Resource Type:
Journal Article
Resource Relation:
Journal Name: Journal of Applied Physics; Journal Volume: 117; Journal Issue: 3; Other Information: (c) 2015 AIP Publishing LLC; Country of input: International Atomic Energy Agency (IAEA)
Country of Publication:
United States
Language:
English
Subject:
75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND SUPERFLUIDITY; AMORPHOUS STATE; APPROXIMATIONS; CARBON; DENSITY FUNCTIONAL METHOD; ELECTRONIC STRUCTURE; ENERGY GAP; HYDROGEN; MOLECULAR DYNAMICS METHOD; POTENTIALS; SURFACES; WATER