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dc.contributor.authorDenis, J.-C.
dc.contributor.authorSchumacher, S.
dc.contributor.authorHedley, Gordon James
dc.contributor.authorRuseckas, Arvydas
dc.contributor.authorMorawska, Paulina Olga
dc.contributor.authorWang, Yue
dc.contributor.authorAllard, S.
dc.contributor.authorScherf, U.
dc.contributor.authorTurnbull, Graham A.
dc.contributor.authorSamuel, Ifor David William
dc.contributor.authorGalbraith, I.
dc.date.accessioned2016-05-19T15:30:04Z
dc.date.available2016-05-19T15:30:04Z
dc.date.issued2015-05-07
dc.identifier.citationDenis , J-C , Schumacher , S , Hedley , G J , Ruseckas , A , Morawska , P O , Wang , Y , Allard , S , Scherf , U , Turnbull , G A , Samuel , I D W & Galbraith , I 2015 , ' Subpicosecond exciton dynamics in polyfluorene films from experiment and microscopic theory ' , Journal of Physical Chemistry C , vol. 119 , no. 18 , pp. 9734-9744 . https://doi.org/10.1021/acs.jpcc.5b00680en
dc.identifier.issn1932-7447
dc.identifier.otherPURE: 189278342
dc.identifier.otherPURE UUID: 7b93316a-e6bb-4a2c-b255-e0111caa90e3
dc.identifier.otherScopus: 84929012357
dc.identifier.otherORCID: /0000-0002-2132-7091/work/31037454
dc.identifier.otherORCID: /0000-0001-9114-3522/work/32543063
dc.identifier.otherWOS: 000354339000007
dc.identifier.urihttp://hdl.handle.net/10023/8836
dc.descriptionThe authors acknowledge financial support from the UK EPSRC (Grants EP/E065066/1, EP/E062636/1, EP/J009318/1 and EP/J009019/1), from the EPSRC Scottish Centre for Doctoral training in Condensed Matter Physics and from the European Union Seventh Framework Programme under Grant Agreement 321305.en
dc.description.abstractElectronic energy transfer (EET) in organic materials is a key mechanism that controls the efficiency of many processes, including light harvesting antennas in natural and artificial photosynthesis, organic solar cells, and biological systems. In this paper we have examined EET in solid-state thin-films of polyfluorene, a prototypical conjugated polymer, with ultrafast photoluminescence experiments and theoretical modeling. We observe EET occurring on a 680 ± 300 fs time scale by looking at the depolarisation of photoluminescence. An independent, predictive microscopic theoretical model is built by defining 125 000 chromophores containing both spatial and energetic disorder appropriate for a spin-coated thin film. The model predicts time-dependent exciton dynamics, without any fitting parameters, using the incoherent Förster-type hopping model. Electronic coupling between the chromophores is calculated by an improved version of the usual line-dipole model for resonant energy transfer. Without the need for higher level interactions, we find that the model is in general agreement with the experimentally observed 680 ± 300 fs depolarisation caused by EET. This leads us to conclude that femtosecond EET in polyfluorene can be described well by conventional resonant energy transfer, as long as the relevant microscopic parameters are well captured. The implications of this finding are that dipole-dipole resonant energy transfer can in some circumstances be fully adequate to describe ultrafast EET without needing to invoke strong or intermediate coupling mechanisms.
dc.format.extent11
dc.language.isoeng
dc.relation.ispartofJournal of Physical Chemistry Cen
dc.rightsCopyright © 2015 American Chemical Society. This work is made available online in accordance with the publisher’s policies. This is the author created, accepted version manuscript following peer review and may differ slightly from the final published version. The final published version of this work is available at https://dx.doi.org/10.1021/acs.jpcc.5b00680en
dc.subjectQD Chemistryen
dc.subjectQC Physicsen
dc.subjectNDASen
dc.subject.lccQDen
dc.subject.lccQCen
dc.titleSubpicosecond exciton dynamics in polyfluorene films from experiment and microscopic theoryen
dc.typeJournal articleen
dc.description.versionPostprinten
dc.contributor.institutionUniversity of St Andrews.School of Physics and Astronomyen
dc.contributor.institutionUniversity of St Andrews.Condensed Matter Physicsen
dc.identifier.doihttps://doi.org/10.1021/acs.jpcc.5b00680
dc.description.statusPeer revieweden
dc.identifier.urlhttp://pubs.acs.org/doi/suppl/10.1021/acs.jpcc.5b00680en


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