On the interface dipole at the pentacene-fullerene heterojunction: A theoretical study

Mathieu Linares; David Beljonne; Jérôme Cornil; Kelly Lancaster; Jean Luc Brédas; Stijn Verlaak; Alexander Mityashin; Paul Heremans; Andreas Fuchs; Christian Lennartz; Julien Idé; Raphaël Méreau; Philippe Aurel; Laurent Ducasse; Frédéric Castet

doi:10.1021/jp910005g

On the interface dipole at the pentacene-fullerene heterojunction: A theoretical study

Mathieu Linares, David Beljonne, Jérôme Cornil, Kelly Lancaster, Jean Luc Brédas, Stijn Verlaak, Alexander Mityashin, Paul Heremans, Andreas Fuchs, Christian Lennartz, Julien Idé, Raphaël Méreau, Philippe Aurel, Laurent Ducasse, Frédéric Castet^*

^*Corresponding author for this work

Research output: Contribution to journal › Article › peer-review

124 Scopus citations

Abstract

The electronic structure at organic/organic interfaces plays a key role, among others, in defining the quantum efficiency of organics-based photovoltaic cells. Here, we perform quantum-chemical and microelectrostatic calculations on molecular aggregates of various sizes and shapes to characterize the interfacial dipole moment at pentacene/C₆₀ heterojunctions. The results show that the interfacial dipole mostly originates in polarization effects due to the asymmetry in the multipolar expansion of the electronic density distribution between the interacting molecules, rather than in a charge transfer from donor to acceptor. The local dipole is found to fluctuate in sign and magnitude over the interface and appears as a sensitive probe of the relative arrangements of the pentacene and C₆₀ molecules (and of the resulting local electrical fields sensed by the molecular units).

Original language	English (US)
Pages (from-to)	3215-3224
Number of pages	10
Journal	JOURNAL OF PHYSICAL CHEMISTRY C
Volume	114
Issue number	7
DOIs	https://doi.org/10.1021/jp910005g
State	Published - Feb 25 2010
Externally published	Yes

Bibliographical note

KAUST Repository Item: Exported on 2020-10-01
Acknowledged KAUST grant number(s): KUS-C1-015-21
Acknowledgements: The authors acknowledge the European projects MINOTOR (FP7-NMP-228424), MODECOM (NMP3-CT-2006-016434), and ONE-P (NMP3-LA-2008-212311) for financial support. The work in Mons is partly supported by the Interuniversity Attraction Pole IAP 6/27 of the Belgian Federal Governement, and the Belgian National Fund for Scientific Research (FNRS/FRFC). The work at Georgia Tech is partly supported by the STC program of the National Science Foundation under award DMR-0120967 and by the Center for Advanced Molecular Photovoltaics (Award No KUS-C1-015-21 made by King Abdullah University of Science and Technology, KAUST). J.C. and D.B. are FNRS Research Fellows. J.I. is grateful to the “Advanced Material in Aquitaine” program (www.ama-materials.com) for his Ph.D. grant. J.C. thanks University Bordeaux I for a visiting professorship. Calculations were carried out on mainframe computers of the “M3PEC-MESOCENTRE” of University Bordeaux I financed by Conseil Régional d’Aquitaine and the French Ministry of Research and Technology, as well as on the Interuniversity Scientific Calculation Facility (ISCF) installed at Facultés Universitaires Notre-Dame de la Paix (Namur, Belgium), for which the authors gratefully acknowledge the financial support of FNRS-FRFC.
This publication acknowledges KAUST support, but has no KAUST affiliated authors.

ASJC Scopus subject areas

Electronic, Optical and Magnetic Materials
General Energy
Surfaces, Coatings and Films
Physical and Theoretical Chemistry

UN SDGs

This output contributes to the following UN Sustainable Development Goals (SDGs)

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10.1021/jp910005g

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Linares, M., Beljonne, D., Cornil, J., Lancaster, K., Brédas, J. L., Verlaak, S., Mityashin, A., Heremans, P., Fuchs, A., Lennartz, C., Idé, J., Méreau, R., Aurel, P., Ducasse, L., & Castet, F. (2010). On the interface dipole at the pentacene-fullerene heterojunction: A theoretical study. JOURNAL OF PHYSICAL CHEMISTRY C, 114(7), 3215-3224. https://doi.org/10.1021/jp910005g

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abstract = "The electronic structure at organic/organic interfaces plays a key role, among others, in defining the quantum efficiency of organics-based photovoltaic cells. Here, we perform quantum-chemical and microelectrostatic calculations on molecular aggregates of various sizes and shapes to characterize the interfacial dipole moment at pentacene/C60 heterojunctions. The results show that the interfacial dipole mostly originates in polarization effects due to the asymmetry in the multipolar expansion of the electronic density distribution between the interacting molecules, rather than in a charge transfer from donor to acceptor. The local dipole is found to fluctuate in sign and magnitude over the interface and appears as a sensitive probe of the relative arrangements of the pentacene and C60 molecules (and of the resulting local electrical fields sensed by the molecular units).",

author = "Mathieu Linares and David Beljonne and J{\'e}r{\^o}me Cornil and Kelly Lancaster and Br{\'e}das, {Jean Luc} and Stijn Verlaak and Alexander Mityashin and Paul Heremans and Andreas Fuchs and Christian Lennartz and Julien Id{\'e} and Rapha{\"e}l M{\'e}reau and Philippe Aurel and Laurent Ducasse and Fr{\'e}d{\'e}ric Castet",

note = "KAUST Repository Item: Exported on 2020-10-01 Acknowledged KAUST grant number(s): KUS-C1-015-21 Acknowledgements: The authors acknowledge the European projects MINOTOR (FP7-NMP-228424), MODECOM (NMP3-CT-2006-016434), and ONE-P (NMP3-LA-2008-212311) for financial support. The work in Mons is partly supported by the Interuniversity Attraction Pole IAP 6/27 of the Belgian Federal Governement, and the Belgian National Fund for Scientific Research (FNRS/FRFC). The work at Georgia Tech is partly supported by the STC program of the National Science Foundation under award DMR-0120967 and by the Center for Advanced Molecular Photovoltaics (Award No KUS-C1-015-21 made by King Abdullah University of Science and Technology, KAUST). J.C. and D.B. are FNRS Research Fellows. J.I. is grateful to the “Advanced Material in Aquitaine” program (www.ama-materials.com) for his Ph.D. grant. J.C. thanks University Bordeaux I for a visiting professorship. Calculations were carried out on mainframe computers of the “M3PEC-MESOCENTRE” of University Bordeaux I financed by Conseil R{\'e}gional d{\textquoteright}Aquitaine and the French Ministry of Research and Technology, as well as on the Interuniversity Scientific Calculation Facility (ISCF) installed at Facult{\'e}s Universitaires Notre-Dame de la Paix (Namur, Belgium), for which the authors gratefully acknowledge the financial support of FNRS-FRFC. This publication acknowledges KAUST support, but has no KAUST affiliated authors.",

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Linares, M, Beljonne, D, Cornil, J, Lancaster, K, Brédas, JL, Verlaak, S, Mityashin, A, Heremans, P, Fuchs, A, Lennartz, C, Idé, J, Méreau, R, Aurel, P, Ducasse, L & Castet, F 2010, 'On the interface dipole at the pentacene-fullerene heterojunction: A theoretical study', JOURNAL OF PHYSICAL CHEMISTRY C, vol. 114, no. 7, pp. 3215-3224. https://doi.org/10.1021/jp910005g

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AU - Beljonne, David

AU - Cornil, Jérôme

AU - Lancaster, Kelly

AU - Brédas, Jean Luc

AU - Verlaak, Stijn

AU - Mityashin, Alexander

AU - Heremans, Paul

AU - Fuchs, Andreas

AU - Lennartz, Christian

AU - Idé, Julien

AU - Méreau, Raphaël

AU - Aurel, Philippe

AU - Ducasse, Laurent

AU - Castet, Frédéric

N1 - KAUST Repository Item: Exported on 2020-10-01 Acknowledged KAUST grant number(s): KUS-C1-015-21 Acknowledgements: The authors acknowledge the European projects MINOTOR (FP7-NMP-228424), MODECOM (NMP3-CT-2006-016434), and ONE-P (NMP3-LA-2008-212311) for financial support. The work in Mons is partly supported by the Interuniversity Attraction Pole IAP 6/27 of the Belgian Federal Governement, and the Belgian National Fund for Scientific Research (FNRS/FRFC). The work at Georgia Tech is partly supported by the STC program of the National Science Foundation under award DMR-0120967 and by the Center for Advanced Molecular Photovoltaics (Award No KUS-C1-015-21 made by King Abdullah University of Science and Technology, KAUST). J.C. and D.B. are FNRS Research Fellows. J.I. is grateful to the “Advanced Material in Aquitaine” program (www.ama-materials.com) for his Ph.D. grant. J.C. thanks University Bordeaux I for a visiting professorship. Calculations were carried out on mainframe computers of the “M3PEC-MESOCENTRE” of University Bordeaux I financed by Conseil Régional d’Aquitaine and the French Ministry of Research and Technology, as well as on the Interuniversity Scientific Calculation Facility (ISCF) installed at Facultés Universitaires Notre-Dame de la Paix (Namur, Belgium), for which the authors gratefully acknowledge the financial support of FNRS-FRFC. This publication acknowledges KAUST support, but has no KAUST affiliated authors.

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N2 - The electronic structure at organic/organic interfaces plays a key role, among others, in defining the quantum efficiency of organics-based photovoltaic cells. Here, we perform quantum-chemical and microelectrostatic calculations on molecular aggregates of various sizes and shapes to characterize the interfacial dipole moment at pentacene/C60 heterojunctions. The results show that the interfacial dipole mostly originates in polarization effects due to the asymmetry in the multipolar expansion of the electronic density distribution between the interacting molecules, rather than in a charge transfer from donor to acceptor. The local dipole is found to fluctuate in sign and magnitude over the interface and appears as a sensitive probe of the relative arrangements of the pentacene and C60 molecules (and of the resulting local electrical fields sensed by the molecular units).

AB - The electronic structure at organic/organic interfaces plays a key role, among others, in defining the quantum efficiency of organics-based photovoltaic cells. Here, we perform quantum-chemical and microelectrostatic calculations on molecular aggregates of various sizes and shapes to characterize the interfacial dipole moment at pentacene/C60 heterojunctions. The results show that the interfacial dipole mostly originates in polarization effects due to the asymmetry in the multipolar expansion of the electronic density distribution between the interacting molecules, rather than in a charge transfer from donor to acceptor. The local dipole is found to fluctuate in sign and magnitude over the interface and appears as a sensitive probe of the relative arrangements of the pentacene and C60 molecules (and of the resulting local electrical fields sensed by the molecular units).

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On the interface dipole at the pentacene-fullerene heterojunction: A theoretical study

Abstract

Bibliographical note

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