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The Impact of Functionalization on the Stability, Work Function, and Photoluminescence of Reduced Graphene Oxide

Kumar, Priyank V. and Bernardi, Marco and Grossman, Jeffrey C. (2013) The Impact of Functionalization on the Stability, Work Function, and Photoluminescence of Reduced Graphene Oxide. ACS Nano, 7 (2). pp. 1638-1645. ISSN 1936-0851. doi:10.1021/nn305507p. https://resolver.caltech.edu/CaltechAUTHORS:20150923-134905213

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Abstract

Reduced graphene oxide (rGO) is a promising material for a variety of thin-film optoelectronic applications. Two main barriers to its widespread use are the lack of (1) fabrication protocols leading to tailored functionalization of the graphene sheet with oxygen-containing chemical groups, and (2) understanding of the impact of such functional groups on the stability and on the optical and electronic properties of rGO. We carry out classical molecular dynamics and density functional theory calculations on a large set of realistic rGO structures to decompose the effects of different functional groups on the stability, work function, and photoluminescence. Our calculations indicate the metastable nature of carbonyl-rich rGO and its favorable transformation to hydroxyl-rich rGO at room temperature via carbonyl-to-hydroxyl conversion reactions near carbon vacancies and holes. We demonstrate a significant tunability in the work function of rGO up to 2.5 eV by altering the composition of oxygen-containing functional groups for a fixed oxygen concentration, and of the photoluminescence emission by modulating the fraction of epoxy and carbonyl groups. Taken together, our results guide the application of tailored rGO structures in devices for optoelectronics and renewable energy.


Item Type:Article
Related URLs:
URLURL TypeDescription
http://dx.doi.org/10.1021/nn305507pDOIArticle
http://pubs.acs.org/doi/abs/10.1021/nn305507pPublisherArticle
http://pubs.acs.org/doi/suppl/10.1021/nn305507pPublisherSupporting Information
ORCID:
AuthorORCID
Bernardi, Marco0000-0001-7289-9666
Grossman, Jeffrey C.0000-0003-1281-2359
Additional Information:© 2013 American Chemical Society. Received for review November 27, 2012 and accepted January 23, 2013. Publication Date (Web): January 31, 2013. The authors acknowledge financial support from the Solar Frontiers Program at MIT. We thank NERSC and Teragrid for providing computational resources. The authors declare no competing financial interest.
Funders:
Funding AgencyGrant Number
Massachusetts Institute of Technology (MIT)UNSPECIFIED
TeraGridUNSPECIFIED
Subject Keywords:reduced graphene oxide; molecular dynamics; density functional theory; work function; stability; photoluminescence; functional groups
Issue or Number:2
DOI:10.1021/nn305507p
Record Number:CaltechAUTHORS:20150923-134905213
Persistent URL:https://resolver.caltech.edu/CaltechAUTHORS:20150923-134905213
Official Citation:The Impact of Functionalization on the Stability, Work Function, and Photoluminescence of Reduced Graphene Oxide Priyank V. Kumar, Marco Bernardi, and Jeffrey C. Grossman ACS Nano 2013 7 (2), 1638-1645 DOI: 10.1021/nn305507p
Usage Policy:No commercial reproduction, distribution, display or performance rights in this work are provided.
ID Code:60444
Collection:CaltechAUTHORS
Deposited By: George Porter
Deposited On:23 Sep 2015 21:01
Last Modified:10 Nov 2021 22:34

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