Concentric dopant segregation in CVD-grown N-doped graphene single crystals

Heteroatom doping in graphene leads to bandgap opening and tunable electronic, magnetic and optical properties, which are important for graphene-based electronics applications. In recent years, scalable growth of nitrogen-doped graphene (NG) by chemical vapor deposition (CVD) has been extensively st...

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Main Authors: Lin, Jinjun, Tay, Roland Yingjie, Li, Hongling, Jing, Lin, Tsang, Siu Hon, Bolker, Asaf, Saguy, Cecile, Teo, Edwin Hang Tong
Other Authors: School of Electrical and Electronic Engineering
Format: Journal Article
Language:English
Published: 2019
Subjects:
Online Access:https://hdl.handle.net/10356/88943
http://hdl.handle.net/10220/48351
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author Lin, Jinjun
Tay, Roland Yingjie
Li, Hongling
Jing, Lin
Tsang, Siu Hon
Bolker, Asaf
Saguy, Cecile
Teo, Edwin Hang Tong
author2 School of Electrical and Electronic Engineering
author_facet School of Electrical and Electronic Engineering
Lin, Jinjun
Tay, Roland Yingjie
Li, Hongling
Jing, Lin
Tsang, Siu Hon
Bolker, Asaf
Saguy, Cecile
Teo, Edwin Hang Tong
author_sort Lin, Jinjun
collection NTU
description Heteroatom doping in graphene leads to bandgap opening and tunable electronic, magnetic and optical properties, which are important for graphene-based electronics applications. In recent years, scalable growth of nitrogen-doped graphene (NG) by chemical vapor deposition (CVD) has been extensively studied because of its potential for practical applications. A phenomenon that occurs exclusively for CVD-grown NG films is the segregation of doping concentration. However, most studies to date are conducted using highly polycrystalline NG films comprising small grain sizes. It is still unknown whether dopant segregation occurs in single crystalline NG domains. Here, we used hexamethylenetetramine ((CH2)6N4) as a single-source solid precursor to grow hexagonal-shaped monolayer NG single crystals of ∼20 µm on Cu substrates. The NG single crystals exhibit discrete concentric hexagonal rings comprising N depleted regions as determined by Raman spectroscopy. Supported by scanning tunneling microscopy experiments, we propose that the segregation of N dopants is caused by a competing N attachment mechanism to either zigzag or Klein edges during growth; where the former should result in higher N concentration and the latter with lower N concentration. This work provides critical insights into the growth mechanism of CVD-grown NG and enables new opportunities to engineer the properties of graphene by fabrication of lateral heterostructures.
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spelling ntu-10356/889432020-09-26T22:17:37Z Concentric dopant segregation in CVD-grown N-doped graphene single crystals Lin, Jinjun Tay, Roland Yingjie Li, Hongling Jing, Lin Tsang, Siu Hon Bolker, Asaf Saguy, Cecile Teo, Edwin Hang Tong School of Electrical and Electronic Engineering School of Materials Science & Engineering Temasek Laboratories Nitrogen-doped Graphene DRNTU::Engineering::Electrical and electronic engineering Chemical Vapor Deposition Heteroatom doping in graphene leads to bandgap opening and tunable electronic, magnetic and optical properties, which are important for graphene-based electronics applications. In recent years, scalable growth of nitrogen-doped graphene (NG) by chemical vapor deposition (CVD) has been extensively studied because of its potential for practical applications. A phenomenon that occurs exclusively for CVD-grown NG films is the segregation of doping concentration. However, most studies to date are conducted using highly polycrystalline NG films comprising small grain sizes. It is still unknown whether dopant segregation occurs in single crystalline NG domains. Here, we used hexamethylenetetramine ((CH2)6N4) as a single-source solid precursor to grow hexagonal-shaped monolayer NG single crystals of ∼20 µm on Cu substrates. The NG single crystals exhibit discrete concentric hexagonal rings comprising N depleted regions as determined by Raman spectroscopy. Supported by scanning tunneling microscopy experiments, we propose that the segregation of N dopants is caused by a competing N attachment mechanism to either zigzag or Klein edges during growth; where the former should result in higher N concentration and the latter with lower N concentration. This work provides critical insights into the growth mechanism of CVD-grown NG and enables new opportunities to engineer the properties of graphene by fabrication of lateral heterostructures. ASTAR (Agency for Sci., Tech. and Research, S’pore) Accepted version 2019-05-24T02:27:28Z 2019-12-06T17:14:17Z 2019-05-24T02:27:28Z 2019-12-06T17:14:17Z 2018 Journal Article Lin, J., Tay, R. Y., Li, H., Jing, L., Tsang, S. H., Bolker, A., . . . Teo, E. H. T. (2018). Concentric dopant segregation in CVD-grown N-doped graphene single crystals. Applied Surface Science, 454, 121-129. doi:10.1016/j.apsusc.2018.05.132 0169-4332 https://hdl.handle.net/10356/88943 http://hdl.handle.net/10220/48351 10.1016/j.apsusc.2018.05.132 en Applied Surface Science © 2018 Elsevier B.V. All rights reserved. This paper was published in Applied Surface Science and is made available with permission of Elsevier B.V. 30 p. application/pdf
spellingShingle Nitrogen-doped Graphene
DRNTU::Engineering::Electrical and electronic engineering
Chemical Vapor Deposition
Lin, Jinjun
Tay, Roland Yingjie
Li, Hongling
Jing, Lin
Tsang, Siu Hon
Bolker, Asaf
Saguy, Cecile
Teo, Edwin Hang Tong
Concentric dopant segregation in CVD-grown N-doped graphene single crystals
title Concentric dopant segregation in CVD-grown N-doped graphene single crystals
title_full Concentric dopant segregation in CVD-grown N-doped graphene single crystals
title_fullStr Concentric dopant segregation in CVD-grown N-doped graphene single crystals
title_full_unstemmed Concentric dopant segregation in CVD-grown N-doped graphene single crystals
title_short Concentric dopant segregation in CVD-grown N-doped graphene single crystals
title_sort concentric dopant segregation in cvd grown n doped graphene single crystals
topic Nitrogen-doped Graphene
DRNTU::Engineering::Electrical and electronic engineering
Chemical Vapor Deposition
url https://hdl.handle.net/10356/88943
http://hdl.handle.net/10220/48351
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