Coexistence of Urbach-Tail-Like Localized States and Metallic Conduction Channels in Nitrogen-Doped 3D Curved Graphene

Yoichi Tanabe; Yoshikazu Ito; Katsuaki Sugawara; Samuel Jeong; Tatsuhiko Ohto; Tomohiko Nishiuchi; Naoaki Kawada; Shojiro Kimura; Christopher Florencio Aleman; Takashi Takahashi; Motoko Kotani; Mingwei Chen

doi:10.1002/adma.202205986

Coexistence of Urbach-Tail-Like Localized States and Metallic Conduction Channels in Nitrogen-Doped 3D Curved Graphene

Adv Mater. 2022 Dec;34(51):e2205986. doi: 10.1002/adma.202205986. Epub 2022 Nov 18.

Authors

Yoichi Tanabe¹, Yoshikazu Ito², Katsuaki Sugawara^{3

4

5

6}, Samuel Jeong², Tatsuhiko Ohto⁷, Tomohiko Nishiuchi⁸, Naoaki Kawada¹, Shojiro Kimura⁹, Christopher Florencio Aleman¹⁰, Takashi Takahashi⁴, Motoko Kotani^{4

11}, Mingwei Chen¹⁰

Affiliations

¹ Department of Applied Science, Okayama University of Science, Okayama, 700-0005, Japan.
² Institute of Applied Physics, Graduate School of Pure and Applied Sciences, University of Tsukuba, Tsukuba, Ibaraki, 305-8573, Japan.
³ Department of Physics, Graduate School of Science, Tohoku University, Sendai, 980-8578, Japan.
⁴ Advanced Institute for Materials Research, Tohoku University, Sendai, 980-8577, Japan.
⁵ Center for Spintronics Research Network, Tohoku University, Sendai, 980-8577, Japan.
⁶ Precursory Research for Embryonic Science and Technology (PRESTO), Japan Science and Technology Agency (JST), Tokyo, 102-0076, Japan.
⁷ Graduate School of Engineering Science, Osaka University, 1-3 Machikaneyama, Toyonaka, 560-8531, Japan.
⁸ Department of Chemistry, Graduate School of Science, Osaka University, 1-1 Machikaneyama, Toyonaka, Osaka, 560-0043, Japan.
⁹ Institute for Materials Research, Tohoku University, Katahira 2-1-1, Sendai, 980-8577, Japan.
¹⁰ Department of Materials Science and Engineering, Johns Hopkins University, Baltimore, MD, 21218, USA.
¹¹ Mathematical Institute, Graduate School of Science, Tohoku University, Sendai, 980-8578, Japan.

PMID: 36208073
DOI: 10.1002/adma.202205986

Abstract

Nitrogen (N) doping is one of the most effective approaches to tailor the chemical and physical properties of graphene. By the interplay between N dopants and 3D curvature of graphene lattices, N-doped 3D graphene displays superior performance in electrocatalysis and solar-energy harvesting for energy and environmental applications. However, the electrical transport properties and the electronic states, which are the key factors to understand the origins of the N-doping effect in 3D graphene, are still missing. The electronic properties of N-doped 3D graphene are systematically investigated by an electric-double-layer transistor method. It is demonstrated that Urbach-tail-like localized states are located around the neutral point of N-doped 3D graphene with the background metallic transport channels. The dual nature of electronic states, generated by the synergistic effect of N dopants and 3D curvature of graphene, can be the electronic origin of the high electrocatalysis, enhanced molecular adsorption, and light absorption of N-doped 3D graphene.

Keywords: 3D curved surfaces; Urbach tail; electrical transport; graphene; nitrogen doping.

Abstract

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