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dc.contributor.authorLi, Huifang
dc.contributor.authorLi, Hong
dc.contributor.authorXun, Sangni
dc.contributor.authorBredas, Jean-Luc
dc.date.accessioned2020-11-11T11:37:54Z
dc.date.available2020-11-11T11:37:54Z
dc.date.issued2020-10-28
dc.date.submitted2020-07-13
dc.identifier.citationLi, H., Li, H., Xun, S., & Brédas, J.-L. (2020). Doping Modulation of the Charge Injection Barrier between a Covalent Organic Framework Monolayer and Graphene. Chemistry of Materials, 32(21), 9228–9237. doi:10.1021/acs.chemmater.0c02913
dc.identifier.issn0897-4756
dc.identifier.issn1520-5002
dc.identifier.doi10.1021/acs.chemmater.0c02913
dc.identifier.urihttp://hdl.handle.net/10754/665896
dc.description.abstractThe rapid development in the design and synthesis of covalent organic frameworks (COFs) brings opportunities in tuning their electronic and magnetic properties and expanding their applications. Controlled chemical doping is a traditional route to modulate the charge carrier injection and transport properties in organic molecular and polymeric semiconductors; it represents a natural strategy that, however, has not been explored systematically for COF monolayers (2D COFs), especially when interfaced with inorganic substrates. Here, considering alkali metal (Na) atoms as conventional dopants, we investigate at the Density Functional Theory level the n-type doping of the porphyrin-based COF, COF366-OMe, in the form of both a freestanding monolayer or as interacting with a graphene substrate. The COF monolayer and COF/graphene complex are found to be efficiently n-doped by accepting a full electron from each Na dopant. On the COF/graphene complex, while a Na atom binds more strongly to the COF than to graphene, the transferred electron distributes between them. As a result, the Fermi level of graphene shifts above the Dirac point, whereas the conduction band minimum of the 2D COF strongly stabilizes; the consequence is a marked reduction in the electron injection barrier between the graphene sheet and the 2D COF. Our study highlights the key role that controlled chemical doping of COFs can play in tuning their charge injection and transport properties for optoelectronic applications.
dc.description.sponsorshipWe are grateful to Prof. M. Crommie and his group at UC Berkeley for many stimulating discussions. The work at the University of Arizona was supported by the Army Research Office, under the Multidisciplinary University Research Initiative (MURI) Award No. W911NF-15-1-0447 and under Award No. W911NF-17-1-0339, and by the University of Arizona. H.F.L. thanks the National Natural Science Foundation of China (Nos. 21403037 and 51676103) for funding as well as the KAUST Supercomputing Laboratory. The computational work was supported in part by a grant of computer time from the DOD High Performance Computing Modernization Program.
dc.publisherAmerican Chemical Society (ACS)
dc.relation.urlhttps://pubs.acs.org/doi/10.1021/acs.chemmater.0c02913
dc.rightsThis document is the Accepted Manuscript version of a Published Work that appeared in final form in Chemistry of Materials, copyright © American Chemical Society after peer review and technical editing by the publisher. To access the final edited and published work see https://pubs.acs.org/doi/10.1021/acs.chemmater.0c02913.
dc.titleDoping Modulation of the Charge Injection Barrier between a Covalent Organic Framework Monolayer and Graphene
dc.typeArticle
dc.identifier.journalChemistry of Materials
dc.rights.embargodate2021-11-28
dc.eprint.versionPost-print
dc.contributor.institutionCollege of Electromechanical Engineering, Shandong Engineering Laboratory for Preparation and Application of High-performance Carbon-Materials, Qingdao University of Science & Technology, Qingdao, Shandong 266061, China
dc.contributor.institutionDepartment of Chemistry and Biochemistry, The University of Arizona, Tucson, Arizona 85721-0088, United States
dc.contributor.institutionSchool of Chemistry and Biochemistry and Center for Organic Photonics and Electronics, Georgia Institute of Technology, Atlanta, Georgia 30332-0400, United States
dc.contributor.institutionCollege of Environmental Science and Engineering, Hunan University, Changsha 410082, China
dc.identifier.volume32
dc.identifier.issue21
dc.identifier.pages9228-9237
dc.date.accepted2020-10-15
kaust.acknowledged.supportUnitKAUST Supercomputing Laboratory
kaust.acknowledged.supportUnitSupercomputing Laboratory.
dc.date.published-online2020-10-28
dc.date.published-print2020-11-10


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