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dc.contributor.authorJoshi, Trinity
dc.contributor.authorChen, Chen
dc.contributor.authorLi, Huifang
dc.contributor.authorDiercks, Christian S.
dc.contributor.authorWang, Gaoqiang
dc.contributor.authorWaller, Peter J.
dc.contributor.authorLi, Hong
dc.contributor.authorBredas, Jean-Luc
dc.contributor.authorYaghi, Omar M.
dc.contributor.authorCrommie, Michael F.
dc.date.accessioned2018-12-31T14:01:42Z
dc.date.available2018-12-31T14:01:42Z
dc.date.issued2018-11-28
dc.identifier.citationJoshi T, Chen C, Li H, Diercks CS, Wang G, et al. (2018) Local Electronic Structure of Molecular Heterojunctions in a Single-Layer 2D Covalent Organic Framework. Advanced Materials: 1805941. Available: http://dx.doi.org/10.1002/adma.201805941.
dc.identifier.issn0935-9648
dc.identifier.doi10.1002/adma.201805941
dc.identifier.urihttp://hdl.handle.net/10754/630649
dc.description.abstractThe synthesis of a single-layer covalent organic framework (COF) with spatially modulated internal potentials provides new opportunities for manipulating the electronic structure of molecularly defined materials. Here, the fabrication and electronic characterization of COF-420: a single-layer porphyrin-based square-lattice COF containing a periodic array of oriented, type II electronic heterojunctions is reported. In contrast to previous donor-acceptor COFs, COF-420 is constructed from building blocks that yield identical cores upon reticulation, but that are bridged by electrically asymmetric linkers supporting oriented electronic dipoles. Scanning tunneling spectroscopy reveals staggered gap (type II) band alignment between adjacent molecular cores in COF-420, in agreement with first-principles calculations. Hirshfeld charge analysis indicates that dipole fields from oriented imine linkages within COF-420 are the main cause of the staggered electronic structure in this square grid of atomically-precise heterojunctions.
dc.description.sponsorshipT.J., C.C., H.L., and C.S.D. contributed equally to this work. This research was supported by the Army Research Office Multidisciplinary University Research Initiative (MURI) program under grant no. W911NF-15-1-0447 (STM spectroscopy), by the Army Research Office grant no. W911NF-17-1-0339 to Georgia Tech (DFT calculations), by the U.S. Department of Energy, Office of Basic Energy Sciences Nanomachine Program under contract no. DEAC02-05CH11231 (COF sample preparation), and by the joint KACST-UC Berkeley Center for Nanomaterials and Clean Energy (molecular synthesis). The KAUST IT Research Computing Team and the KAUST Supercomputing Laboratory are gratefully acknowledged for providing generous computational resources for part of our theoretical work. T.J. acknowledges support from the National Science Foundation (NSF) Graduate Research Fellowship Program under grant no. DGE 1106400. C.S.D. acknowledges support from a Kavli ENSI Philomathia Graduate Student Fellowship. P.J.W. acknowledges the Berkeley Center for Green Chemistry and NSF for support through a Systems Approach to Green Energy Integrative Graduate Education and Research Traineeship (1144885). G.W. acknowledges fellowship support from the National Natural Science Foundation of China under grant no. 61622116, the Strategic Priority Research Program of Chinese Academy of Sciences under grant no. XDB28010200, and the International Partnership Program of Chinese Academy of Sciences under grant no. 112111KYSB20160061.
dc.publisherWiley
dc.relation.urlhttps://onlinelibrary.wiley.com/doi/full/10.1002/adma.201805941
dc.relation.urlhttps://doi.org/10.1002/adma.201805941
dc.rightsArchived with thanks to Wiley
dc.rightsThis file is an open access version redistributed from: https://doi.org/10.1002/adma.201805941
dc.subjectDensity functional theory
dc.subjectelectronic structure
dc.subjectCovalent Organic Frameworks
dc.subjectScanning Tunneling Microscopy And Spectroscopy
dc.subjectType Ii Heterojunctions
dc.titleLocal Electronic Structure of Molecular Heterojunctions in a Single-Layer 2D Covalent Organic Framework
dc.typeArticle
dc.contributor.departmentKAUST Solar Center (KSC)
dc.contributor.departmentLaboratory for Computational and Theoretical Chemistry of Advanced Materials
dc.contributor.departmentMaterial Science and Engineering Program
dc.contributor.departmentPhysical Science and Engineering (PSE) Division
dc.identifier.journalAdvanced Materials
dc.rights.embargodate2019-11-28
dc.eprint.versionPost-print
dc.contributor.institutionDepartment of Physics; University of California - Berkeley; Berkeley CA 94720 USA
dc.contributor.institutionMaterials Sciences Division; Lawrence Berkeley National Laboratory; Berkeley CA 94720 USA
dc.contributor.institutionDepartment of Chemistry; Kavli Energy NanoScience Institute and Berkeley Global Science Institute; University of California - Berkeley; Berkeley CA 94720 USA
dc.contributor.institutionSchool of Chemistry and Biochemistry & Center for Organic Photonics and Electronics; Georgia Institute of Technology; 901 Atlantic Drive NW Atlanta GA 30332-0400 USA
dc.contributor.institutionKavli Energy NanoScience Institute; University of California Berkeley; Lawrence Berkeley National Laboratory; Berkeley CA 94720 USA
kaust.personLi, Huifang
kaust.personLi, Hong
kaust.personBredas, Jean-Luc
refterms.dateFOA2020-01-23T10:31:40Z


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