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Statements

Subject Item
n2:RIV%2F49777513%3A23220%2F14%3A43924172%21RIV15-MSM-23220___
rdf:type
skos:Concept n19:Vysledek
rdfs:seeAlso
http://10.1021/jp506959m
dcterms:description
We have observed highly efficient intrinsic phosphorescence of a neat sigma-conjugated polymer, poly(biphenyl-4-ylmethylsilylene) (PBMSi). At low temperatures, PBMSi solid films featured ?15% phosphorescence quantum yield, which is unusually high for purely organic conjugated polymers and is comparable to that of organometallic polymers. Exciton dynamics in PBMSi was studied by ultrafast fluorescence and time-gated delayed emission measurements. It was shown that the phosphorescence of PBMSi originates from the radiative decay of triplets on the pí-conjugated biphenyl group constituting the lowest triplet state, T1, which is populated under the excitation of the sigma-conjugated polymer backbone, i.e., with energy well below the lowest singlet excited state of the biphenyl group itself. The nature of the excited states in PBMSi was further investigated by performing quantum-mechanical calculations of the model compound. The calculations showed that the lowest singlet excited state has charge-transfer (CT) character involving different parts of the same macromolecule. Energetically this state lies very close to the CT triplet excited state. We argue that the intramolecular CT state is responsible for the strongly enhanced intersystem crossing (ISC) in PBMSi due to the small positive CT singlet?triplet energy splitting, which is itself a consequence of a weak exchange interaction of a spatially separated electron and hole in the CT state. This study suggests a new molecular-level engineering approach for enhancement of the ISC, enabling efficient conversion of primary excited singlets into triplets in conjugated polymers without involving a heavy atom effect while leaving the rate of radiative T1 ? S0 transition virtually unaffected. We have observed highly efficient intrinsic phosphorescence of a neat sigma-conjugated polymer, poly(biphenyl-4-ylmethylsilylene) (PBMSi). At low temperatures, PBMSi solid films featured ?15% phosphorescence quantum yield, which is unusually high for purely organic conjugated polymers and is comparable to that of organometallic polymers. Exciton dynamics in PBMSi was studied by ultrafast fluorescence and time-gated delayed emission measurements. It was shown that the phosphorescence of PBMSi originates from the radiative decay of triplets on the pí-conjugated biphenyl group constituting the lowest triplet state, T1, which is populated under the excitation of the sigma-conjugated polymer backbone, i.e., with energy well below the lowest singlet excited state of the biphenyl group itself. The nature of the excited states in PBMSi was further investigated by performing quantum-mechanical calculations of the model compound. The calculations showed that the lowest singlet excited state has charge-transfer (CT) character involving different parts of the same macromolecule. Energetically this state lies very close to the CT triplet excited state. We argue that the intramolecular CT state is responsible for the strongly enhanced intersystem crossing (ISC) in PBMSi due to the small positive CT singlet?triplet energy splitting, which is itself a consequence of a weak exchange interaction of a spatially separated electron and hole in the CT state. This study suggests a new molecular-level engineering approach for enhancement of the ISC, enabling efficient conversion of primary excited singlets into triplets in conjugated polymers without involving a heavy atom effect while leaving the rate of radiative T1 ? S0 transition virtually unaffected.
dcterms:title
Highly efficient intrinsic phosphorescence from a sigma?conjugated poly(silylene) polymer Highly efficient intrinsic phosphorescence from a sigma?conjugated poly(silylene) polymer
skos:prefLabel
Highly efficient intrinsic phosphorescence from a sigma?conjugated poly(silylene) polymer Highly efficient intrinsic phosphorescence from a sigma?conjugated poly(silylene) polymer
skos:notation
RIV/49777513:23220/14:43924172!RIV15-MSM-23220___
n3:aktivita
n12:P
n3:aktivity
P(ED2.1.00/03.0094)
n3:cisloPeriodika
40
n3:dodaniDat
n11:2015
n3:domaciTvurceVysledku
n18:5801737
n3:druhVysledku
n13:J
n3:duvernostUdaju
n16:S
n3:entitaPredkladatele
n14:predkladatel
n3:idSjednocenehoVysledku
19141
n3:idVysledku
RIV/49777513:23220/14:43924172
n3:jazykVysledku
n10:eng
n3:klicovaSlova
polymer semiconductor; light emitting diode; polysilan; photoluminescence
n3:klicoveSlovo
n9:photoluminescence n9:polysilan n9:light%20emitting%20diode n9:polymer%20semiconductor
n3:kodStatuVydavatele
US - Spojené státy americké
n3:kontrolniKodProRIV
[96592A40CDF9]
n3:nazevZdroje
The Journal of Physical Chemistry C
n3:obor
n6:JA
n3:pocetDomacichTvurcuVysledku
1
n3:pocetTvurcuVysledku
10
n3:projekt
n4:ED2.1.00%2F03.0094
n3:rokUplatneniVysledku
n11:2014
n3:svazekPeriodika
118
n3:tvurceVysledku
Gulbinas, V. Genoe, J. Augulis, R. Sulskus, J. Valkunas, L. Kadashchuk, A. Skryshevski, Yu. Toliautas, S. Vakhnin, A. Nešpůrek, Stanislav
n3:wos
000343016800012
s:issn
1932-7447
s:numberOfPages
12
n15:doi
10.1021/jp506959m
n20:organizacniJednotka
23220