Polaron pair mediated triplet generation in polymer/fullerene blends

Handle URI:
http://hdl.handle.net/10754/346697
Title:
Polaron pair mediated triplet generation in polymer/fullerene blends
Authors:
Dimitrov, Stoichko D. ( 0000-0002-1564-7080 ) ; Wheeler, Scot; Niedzialek, Dorota; Schroeder, Bob C.; Utzat, Hendrik; Frost, Jarvist M. ( 0000-0003-1938-4430 ) ; Yao, Jizhong; Gillett, Alexander; Tuladhar, Pabitra S.; McCulloch, Iain ( 0000-0002-6340-7217 ) ; Nelson, Jenny; Durrant, James R.
Abstract:
Electron spin is a key consideration for the function of organic semiconductors in light-emitting diodes and solar cells, as well as spintronic applications relying on organic magnetoresistance. A mechanism for triplet excited state generation in such systems is by recombination of electron-hole pairs. However, the exact charge recombination mechanism, whether geminate or nongeminate and whether it involves spin-state mixing is not well understood. In this work, the dynamics of free charge separation competing with recombination to polymer triplet states is studied in two closely related polymer-fullerene blends with differing polymer fluorination and photovoltaic performance. Using time-resolved laser spectroscopic techniques and quantum chemical calculations, we show that lower charge separation in the fluorinated system is associated with the formation of bound electron-hole pairs, which undergo spin-state mixing on the nanosecond timescale and subsequent geminate recombination to triplet excitons. We find that these bound electron-hole pairs can be dissociated by electric fields.
KAUST Department:
Physical Sciences and Engineering (PSE) Division
Citation:
Polaron pair mediated triplet generation in polymer/fullerene blends 2015, 6:6501 Nature Communications
Publisher:
Springer Nature
Journal:
Nature Communications
Issue Date:
4-Mar-2015
DOI:
10.1038/ncomms7501
PubMed ID:
25735188
PubMed Central ID:
PMC4366531
Type:
Article
ISSN:
2041-1723
Additional Links:
http://www.nature.com/doifinder/10.1038/ncomms7501
Appears in Collections:
Articles; Physical Sciences and Engineering (PSE) Division

Full metadata record

DC FieldValue Language
dc.contributor.authorDimitrov, Stoichko D.en
dc.contributor.authorWheeler, Scoten
dc.contributor.authorNiedzialek, Dorotaen
dc.contributor.authorSchroeder, Bob C.en
dc.contributor.authorUtzat, Hendriken
dc.contributor.authorFrost, Jarvist M.en
dc.contributor.authorYao, Jizhongen
dc.contributor.authorGillett, Alexanderen
dc.contributor.authorTuladhar, Pabitra S.en
dc.contributor.authorMcCulloch, Iainen
dc.contributor.authorNelson, Jennyen
dc.contributor.authorDurrant, James R.en
dc.date.accessioned2015-03-16T05:11:31Zen
dc.date.available2015-03-16T05:11:31Zen
dc.date.issued2015-03-04en
dc.identifier.citationPolaron pair mediated triplet generation in polymer/fullerene blends 2015, 6:6501 Nature Communicationsen
dc.identifier.issn2041-1723en
dc.identifier.pmid25735188en
dc.identifier.doi10.1038/ncomms7501en
dc.identifier.urihttp://hdl.handle.net/10754/346697en
dc.description.abstractElectron spin is a key consideration for the function of organic semiconductors in light-emitting diodes and solar cells, as well as spintronic applications relying on organic magnetoresistance. A mechanism for triplet excited state generation in such systems is by recombination of electron-hole pairs. However, the exact charge recombination mechanism, whether geminate or nongeminate and whether it involves spin-state mixing is not well understood. In this work, the dynamics of free charge separation competing with recombination to polymer triplet states is studied in two closely related polymer-fullerene blends with differing polymer fluorination and photovoltaic performance. Using time-resolved laser spectroscopic techniques and quantum chemical calculations, we show that lower charge separation in the fluorinated system is associated with the formation of bound electron-hole pairs, which undergo spin-state mixing on the nanosecond timescale and subsequent geminate recombination to triplet excitons. We find that these bound electron-hole pairs can be dissociated by electric fields.en
dc.publisherSpringer Natureen
dc.relation.urlhttp://www.nature.com/doifinder/10.1038/ncomms7501en
dc.rightsThis work is licensed under a Creative Commons Attribution 4.0 International License. The images or other third party material in this article are included in the article’s Creative Commons license, unless indicated otherwise in the credit line; if the material is not included under the Creative Commons license, users will need to obtain permission from the license holder to reproduce the material. To view a copy of this license, visit http://creativecommons.org/licenses/by/4.0/en
dc.titlePolaron pair mediated triplet generation in polymer/fullerene blendsen
dc.typeArticleen
dc.contributor.departmentPhysical Sciences and Engineering (PSE) Divisionen
dc.identifier.journalNature Communicationsen
dc.identifier.pmcidPMC4366531en
dc.eprint.versionPublisher's Version/PDFen
dc.contributor.institutionDepartment of Chemistry, Centre for Plastic Electronics, Imperial College Londonen
dc.contributor.institutionDepartment of Physics, Centre for Plastic Electronics, Imperial College Londonen
dc.contributor.affiliationKing Abdullah University of Science and Technology (KAUST)en
kaust.authorMcCulloch, Iainen

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