Understanding and controlling the substrate effect on graphene electron-transfer chemistry via reactivity imprint lithography

Qing Hua Wang, Zhong Jin, Ki Kang Kim, Andrew J. Hilmer, Geraldine L.C. Paulus, Chih Jen Shih, Moon Ho Ham, Javier D. Sanchez-Yamagishi, Kenji Watanabe, Takashi Taniguchi, Jing Kong, Pablo Jarillo-Herrero, Michael S. Strano

Research output: Contribution to journalArticlepeer-review

352 Scopus citations

Abstract

Graphene has exceptional electronic, optical, mechanical and thermal properties, which provide it with great potential for use in electronic, optoelectronic and sensing applications. The chemical functionalization of graphene has been investigated with a view to controlling its electronic properties and interactions with other materials. Covalent modification of graphene by organic diazonium salts has been used to achieve these goals, but because graphene comprises only a single atomic layer, it is strongly influenced by the underlying substrate. Here, we show a stark difference in the rate of electron-transfer reactions with organic diazonium salts for monolayer graphene supported on a variety of substrates. Reactions proceed rapidly for graphene supported on SiO 2 and Al 2 O 3 (sapphire), but negligibly on alkyl-terminated and hexagonal boron nitride (hBN) surfaces, as shown by Raman spectroscopy. We also develop a model of reactivity based on substrate-induced electron-hole puddles in graphene, and achieve spatial patterning of chemical reactions in graphene by patterning the substrate.

Original languageEnglish (US)
Pages (from-to)724-732
Number of pages9
JournalNature Chemistry
Volume4
Issue number9
DOIs
StatePublished - Sep 2012
Externally publishedYes

ASJC Scopus subject areas

  • Chemistry(all)
  • Chemical Engineering(all)

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