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

Schiros, Theanne; Nordlund, Dennis; Palova, Lucia; Zhao, Liuyan; Levendorf, Mark; Jaye, Cherno; Reichman, David; Park, Jiwoong; Hybertsen, Mark; Pasupathy, Abhay

doi:10.1021/acsnano.6b01318

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

Journal Article · Tue Jun 21 00:00:00 EDT 2016 · ACS Nano

DOI:https://doi.org/10.1021/acsnano.6b01318· OSTI ID:1336131

Schiros, Theanne ^[1]; Nordlund, Dennis ^[2]; Palova, Lucia ^[3]; Zhao, Liuyan ^[4]; Levendorf, Mark ^[5]; Jaye, Cherno ^[6]; Reichman, David ^[3]; Park, Jiwoong ^[5]; Hybertsen, Mark ^[7]; Pasupathy, Abhay ^[4]

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
SLAC National Accelerator Lab., Menlo Park, CA (United States). Stanford Synchrotron Radiation Lightsource
Columbia Univ., New York, NY (United States). Dept. of Chemistry
Columbia Univ., New York, NY (United States). Dept. of Physics
Cornell Univ., Ithaca, NY (United States). Chemistry Dept.
National Inst. of Standards and Technology, Gaithersburg, MD (United States). Materials Measurement Lab.
Brookhaven National Lab. (BNL), Upton, NY (United States). Center for Functional Nanomaterials

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 > 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.

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Research Organization:: Brookhaven National Laboratory (BNL), Upton, NY (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES)

Grant/Contract Number:: SC00112704

OSTI ID:: 1336131

Report Number(s):: BNL-112597-2016-JA; R&D Project: 16068; KC0403020

Journal Information:: ACS Nano, Vol. 10, Issue 7; ISSN 1936-0851

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

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Cited by: 44 works

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

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