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Title: Atomistic Interrogation of B–N Co-dopant Structures and Their Electronic Effects in Graphene

Chemical doping has been demonstrated to be an effective method for producing high-quality, large-area graphene with controlled carrier concentrations and an atomically tailored work function. Furthermore, the emergent optoelectronic properties and surface reactivity of carbon nanostructures are dictated by the microstructure of atomic dopants. Co-doping of graphene with boron and nitrogen offers the possibility to further tune the electronic properties of graphene at the atomic level, potentially creating p- and n-type domains in a single carbon sheet, opening a gap between valence and conduction bands in the 2-D semimetal. When using a suite of high-resolution synchrotron-based X-ray techniques, scanning tunneling microscopy, and density functional theory based computation we visualize and characterize B–N dopant bond structures and their electronic effects at the atomic level in single-layer graphene grown on a copper substrate. We find there is a thermodynamic driving force for B and N atoms to cluster into BNC structures in graphene, rather than randomly distribute into isolated B and N graphitic dopants, although under the present growth conditions, kinetics limit segregation of large B–N domains. We also observe that the doping effect of these BNC structures, which open a small band gap in graphene, follows the B:N ratio (B >more » N, p-type; B < N, n-type; B=N, neutral). We attribute this to the comparable electron-withdrawing and -donating effects, respectively, of individual graphitic B and N dopants, although local electrostatics also play a role in the work function change.« less
Authors:
 [1] ;  [2] ;  [3] ;  [4] ;  [5] ;  [6] ;  [3] ;  [5] ;  [7] ;  [4]
  1. Columbia Univ., New York, NY (United States). Materials Research Science and Engineering Center (MRSEC); State Univ. of New York, NY (United States). Dept. of Science and Mathematics
  2. SLAC National Accelerator Lab., Menlo Park, CA (United States). Stanford Synchrotron Radiation Lightsource
  3. Columbia Univ., New York, NY (United States). Dept. of Chemistry
  4. Columbia Univ., New York, NY (United States). Dept. of Physics
  5. Cornell Univ., Ithaca, NY (United States). Chemistry Dept.
  6. National Inst. of Standards and Technology, Gaithersburg, MD (United States). Materials Measurement Lab.
  7. Brookhaven National Lab. (BNL), Upton, NY (United States). Center for Functional Nanomaterials
Publication Date:
Report Number(s):
BNL-112597-2016-JA
Journal ID: ISSN 1936-0851; R&D Project: 16068; KC0403020
Grant/Contract Number:
SC00112704
Type:
Accepted Manuscript
Journal Name:
ACS Nano
Additional Journal Information:
Journal Volume: 10; Journal Issue: 7; Journal ID: ISSN 1936-0851
Publisher:
American Chemical Society (ACS)
Research Org:
Brookhaven National Laboratory (BNL), Upton, NY (United States)
Sponsoring Org:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE; atomic design; chemical bonding; doping; electronic structure; graphene; scanning tunneling microscopy; work function; X-ray spectroscopy
OSTI Identifier:
1336131