Density functional theory for the description of charge-transfer processes at TTF/TCNQ interfaces

Handle URI:
http://hdl.handle.net/10754/597927
Title:
Density functional theory for the description of charge-transfer processes at TTF/TCNQ interfaces
Authors:
Van Regemorter, Tanguy; Guillaume, Maxime; Sini, Gjergji; Sears, John S.; Geskin, Victor; Brédas, Jean-Luc; Beljonne, David; Cornil, Jérôme
Abstract:
In the field of organic electronics, a central issue is to assess how the frontier electronic levels of two adjacent organic layers align with respect to one another at the interface. This alignment can be driven by the presence of a partial charge transfer and the formation of an interface dipole; it plays a key role for instance in determining the rates of exciton dissociation or exciton formation in organic solar cells or light-emitting diodes, respectively. Reliably modeling the processes taking place at these interfaces remains a challenge for the computational chemistry community. Here, we review our recent theoretical work on the influence of the choice of density functional theory (DFT) methodology on the description of the charge-transfer character in the ground state of TTF/ TCNQ model complexes and interfaces. Starting with the electronic properties of the isolated TTF and TCNQ molecules and then considering the charge transfer and resulting interface dipole in TTF/TCNQ donor-acceptor stacks and bilayers, we examine the impact of the choice of DFT functional in describing the interfacial electronic structure. Finally, we employ computations based on periodic boundary conditions to highlight the impact of depolarization effects on the interfacial dipole moment. © Springer-Verlag 2012.
Citation:
Van Regemorter T, Guillaume M, Sini G, Sears JS, Geskin V, et al. (2012) Density functional theory for the description of charge-transfer processes at TTF/TCNQ interfaces. Theoretical Chemistry Accounts 131. Available: http://dx.doi.org/10.1007/s00214-012-1273-0.
Publisher:
Springer Science + Business Media
Journal:
Theoretical Chemistry Accounts
Issue Date:
15-Sep-2012
DOI:
10.1007/s00214-012-1273-0
Type:
Article
ISSN:
1432-881X; 1432-2234
Sponsors:
The authors acknowledge the European project MINOTOR (FP7-NMP-228424) for financial support. The work in Mons is also partly supported by the Interuniversity Attraction Pole IAP 6/27 of the Belgian Federal Government and by the Belgian National Fund for Scientific Research (FNRS/FRFC). J.C. and D. B. are FNRS Research Fellows. The work at Georgia Tech has been partly supported by the Center for Advanced Molecular Photovoltaics, Award No. KUS-C1-015-21, made by King Abdullah University of Science and Technology (KAUST); the Georgia Research Alliance; and the STC Program of the National Science Foundation under Award DMR-0120967.
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Full metadata record

DC FieldValue Language
dc.contributor.authorVan Regemorter, Tanguyen
dc.contributor.authorGuillaume, Maximeen
dc.contributor.authorSini, Gjergjien
dc.contributor.authorSears, John S.en
dc.contributor.authorGeskin, Victoren
dc.contributor.authorBrédas, Jean-Lucen
dc.contributor.authorBeljonne, Daviden
dc.contributor.authorCornil, Jérômeen
dc.date.accessioned2016-02-25T12:59:01Zen
dc.date.available2016-02-25T12:59:01Zen
dc.date.issued2012-09-15en
dc.identifier.citationVan Regemorter T, Guillaume M, Sini G, Sears JS, Geskin V, et al. (2012) Density functional theory for the description of charge-transfer processes at TTF/TCNQ interfaces. Theoretical Chemistry Accounts 131. Available: http://dx.doi.org/10.1007/s00214-012-1273-0.en
dc.identifier.issn1432-881Xen
dc.identifier.issn1432-2234en
dc.identifier.doi10.1007/s00214-012-1273-0en
dc.identifier.urihttp://hdl.handle.net/10754/597927en
dc.description.abstractIn the field of organic electronics, a central issue is to assess how the frontier electronic levels of two adjacent organic layers align with respect to one another at the interface. This alignment can be driven by the presence of a partial charge transfer and the formation of an interface dipole; it plays a key role for instance in determining the rates of exciton dissociation or exciton formation in organic solar cells or light-emitting diodes, respectively. Reliably modeling the processes taking place at these interfaces remains a challenge for the computational chemistry community. Here, we review our recent theoretical work on the influence of the choice of density functional theory (DFT) methodology on the description of the charge-transfer character in the ground state of TTF/ TCNQ model complexes and interfaces. Starting with the electronic properties of the isolated TTF and TCNQ molecules and then considering the charge transfer and resulting interface dipole in TTF/TCNQ donor-acceptor stacks and bilayers, we examine the impact of the choice of DFT functional in describing the interfacial electronic structure. Finally, we employ computations based on periodic boundary conditions to highlight the impact of depolarization effects on the interfacial dipole moment. © Springer-Verlag 2012.en
dc.description.sponsorshipThe authors acknowledge the European project MINOTOR (FP7-NMP-228424) for financial support. The work in Mons is also partly supported by the Interuniversity Attraction Pole IAP 6/27 of the Belgian Federal Government and by the Belgian National Fund for Scientific Research (FNRS/FRFC). J.C. and D. B. are FNRS Research Fellows. The work at Georgia Tech has been partly supported by the Center for Advanced Molecular Photovoltaics, Award No. KUS-C1-015-21, made by King Abdullah University of Science and Technology (KAUST); the Georgia Research Alliance; and the STC Program of the National Science Foundation under Award DMR-0120967.en
dc.publisherSpringer Science + Business Mediaen
dc.subjectDFTen
dc.subjectInterface dipoleen
dc.subjectInterfacesen
dc.subjectOrganic electronicsen
dc.subjectPartial charge transferen
dc.subjectTTF/TCNQen
dc.titleDensity functional theory for the description of charge-transfer processes at TTF/TCNQ interfacesen
dc.typeArticleen
dc.identifier.journalTheoretical Chemistry Accountsen
dc.contributor.institutionUniversité de Mons, Mons, Belgiumen
dc.contributor.institutionGeorgia Institute of Technology, Atlanta, United Statesen
dc.contributor.institutionUniversite de Cergy-Pontoise, Cergy-Pontoise, Franceen
kaust.grant.fundedcenterCenter for Advanced Molecular Photovoltaics (CAMP)en
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