Vibrational properties of organic donor-acceptor molecular crystals: Anthracene-pyromellitic-dianhydride (PMDA) as a case study

Handle URI:
http://hdl.handle.net/10754/584256
Title:
Vibrational properties of organic donor-acceptor molecular crystals: Anthracene-pyromellitic-dianhydride (PMDA) as a case study
Authors:
Fonari, A.; Corbin, N. S. ( 0000-0001-6074-7948 ) ; Vermeulen, D.; Goetz, K. P.; Jurchescu, O. D.; McNeil, L. E. ( 0000-0001-8926-9548 ) ; Bredas, Jean-Luc ( 0000-0001-7278-4471 ) ; Coropceanu, V.
Abstract:
We establish a reliable quantum-mechanical approach to evaluate the vibrational properties of donor-acceptor molecular crystals. The anthracene-PMDA (PMDA = pyromellitic dianhydride) crystal, where anthracene acts as the electron donor and PMDA as the electron acceptor, is taken as a representative system for which experimental non-resonance Raman spectra are also reported. We first investigate the impact that the amount of nonlocal Hartree-Fock exchange (HFE) included in a hybrid density functional has on the geometry, normal vibrational modes, electronic coupling, and electron-vibrational (phonon) couplings. The comparison between experimental and theoreticalRaman spectra indicates that the results based on the αPBE functional with 25%-35% HFE are in better agreement with the experimental results compared to those obtained with the pure PBE functional. Then, taking αPBE with 25% HFE, we assign the vibrational modes and examine their contributions to the relaxation energy related to the nonlocal electron-vibration interactions. The results show that the largest contribution (about 90%) is due to electron interactions with low-frequency vibrational modes. The relaxation energy in anthracene-PMDA is found to be about five times smaller than the electronic coupling.
KAUST Department:
Solar and Photovoltaic Engineering Research Center (SPERC); Physical Sciences and Engineering (PSE) Division
Citation:
Vibrational properties of organic donor-acceptor molecular crystals: Anthracene-pyromellitic-dianhydride (PMDA) as a case study 2015, 143 (22):224503 The Journal of Chemical Physics
Publisher:
AIP Publishing
Journal:
The Journal of Chemical Physics
Issue Date:
10-Dec-2015
DOI:
10.1063/1.4936965
Type:
Article
ISSN:
0021-9606; 1089-7690
Additional Links:
http://scitation.aip.org/content/aip/journal/jcp/143/22/10.1063/1.4936965
Appears in Collections:
Articles; Physical Sciences and Engineering (PSE) Division; Solar and Photovoltaic Engineering Research Center (SPERC)

Full metadata record

DC FieldValue Language
dc.contributor.authorFonari, A.en
dc.contributor.authorCorbin, N. S.en
dc.contributor.authorVermeulen, D.en
dc.contributor.authorGoetz, K. P.en
dc.contributor.authorJurchescu, O. D.en
dc.contributor.authorMcNeil, L. E.en
dc.contributor.authorBredas, Jean-Lucen
dc.contributor.authorCoropceanu, V.en
dc.date.accessioned2015-12-21T08:30:08Zen
dc.date.available2015-12-21T08:30:08Zen
dc.date.issued2015-12-10en
dc.identifier.citationVibrational properties of organic donor-acceptor molecular crystals: Anthracene-pyromellitic-dianhydride (PMDA) as a case study 2015, 143 (22):224503 The Journal of Chemical Physicsen
dc.identifier.issn0021-9606en
dc.identifier.issn1089-7690en
dc.identifier.doi10.1063/1.4936965en
dc.identifier.urihttp://hdl.handle.net/10754/584256en
dc.description.abstractWe establish a reliable quantum-mechanical approach to evaluate the vibrational properties of donor-acceptor molecular crystals. The anthracene-PMDA (PMDA = pyromellitic dianhydride) crystal, where anthracene acts as the electron donor and PMDA as the electron acceptor, is taken as a representative system for which experimental non-resonance Raman spectra are also reported. We first investigate the impact that the amount of nonlocal Hartree-Fock exchange (HFE) included in a hybrid density functional has on the geometry, normal vibrational modes, electronic coupling, and electron-vibrational (phonon) couplings. The comparison between experimental and theoreticalRaman spectra indicates that the results based on the αPBE functional with 25%-35% HFE are in better agreement with the experimental results compared to those obtained with the pure PBE functional. Then, taking αPBE with 25% HFE, we assign the vibrational modes and examine their contributions to the relaxation energy related to the nonlocal electron-vibration interactions. The results show that the largest contribution (about 90%) is due to electron interactions with low-frequency vibrational modes. The relaxation energy in anthracene-PMDA is found to be about five times smaller than the electronic coupling.en
dc.language.isoenen
dc.publisherAIP Publishingen
dc.relation.urlhttp://scitation.aip.org/content/aip/journal/jcp/143/22/10.1063/1.4936965en
dc.rightsArchived with thanks to The Journal of Chemical Physicsen
dc.titleVibrational properties of organic donor-acceptor molecular crystals: Anthracene-pyromellitic-dianhydride (PMDA) as a case studyen
dc.typeArticleen
dc.contributor.departmentSolar and Photovoltaic Engineering Research Center (SPERC)en
dc.contributor.departmentPhysical Sciences and Engineering (PSE) Divisionen
dc.identifier.journalThe Journal of Chemical Physicsen
dc.eprint.versionPublisher's Version/PDFen
dc.contributor.institutionSchool of Chemistry and Biochemistry and Center for Organic Photonics and Electronics, Georgia Institute of Technology, Atlanta, Georgia 30332-0400, USAen
dc.contributor.institutionSchool of Chemistry and Biochemistry and Center for Organic Photonics and Electronics, Georgia Institute of Technology, Atlanta, Georgia 30332-0400, USAen
dc.contributor.institutionDepartment of Physics and Astronomy, University of North Carolina at Chapel Hill, Chapel Hill, North Carolina 27599-3255, USAen
dc.contributor.institutionDepartment of Physics, Wake Forest University, Winston-Salem, North Carolina 27109-7507, USAen
dc.contributor.institutionDepartment of Physics, Wake Forest University, Winston-Salem, North Carolina 27109-7507, USAen
dc.contributor.institutionDepartment of Physics and Astronomy, University of North Carolina at Chapel Hill, Chapel Hill, North Carolina 27599-3255, USAen
dc.contributor.institutionSchool of Chemistry and Biochemistry and Center for Organic Photonics and Electronics, Georgia Institute of Technology, Atlanta, Georgia 30332-0400, USAen
dc.contributor.institutionSchool of Chemistry and Biochemistry and Center for Organic Photonics and Electronics, Georgia Institute of Technology, Atlanta, Georgia 30332-0400, USAen
dc.contributor.affiliationKing Abdullah University of Science and Technology (KAUST)en
kaust.authorBredas, Jean-Lucen
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