Exciton efficiency beyond the spin statistical limit in organic light emitting diodes based on anthracene derivatives

Nidhi Sharma; Michael Yin Wong; David Hall; Eduard Spuling; Francisco Tenopala Carmona; Alberto Privitera; Graeme Jeffrey Copley; David Bradford Cordes; Alexandra Martha Zoya Slawin; Caroline Murawski; Malte Christian Gather; David Beljonne; Yoann Olivier; Ifor D. W. Samuel; Eli Zysman-Colman

doi:10.1039/C9TC06356K

Exciton efficiency beyond the spin statistical limit in organic light emitting diodes based on anthracene derivatives

Nidhi Sharma, Michael Yin Wong, David Hall, Eduard Spuling, Francisco Tenopala Carmona, Alberto Privitera, Graeme Jeffrey Copley, David Bradford Cordes, Alexandra Martha Zoya Slawin, Caroline Murawski, Malte Christian Gather, David Beljonne, Yoann Olivier, Ifor D. W. Samuel, Eli Zysman-Colman^*

^*Corresponding author for this work

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

Abstract

We report two donor-acceptor (D-A) materials based on a cyanoanthracene acceptor paired with diphenylamine (DPAAnCN) and carbazole (CzAnCN) donor moieties. These compounds show hybrid locally excited (LE) charge-transfer (CT) excited states (HLCT), which we demonstrated through a combined photophysical and computational study. Vacuum- deposited organic light emitting diodes (OLEDs) using these HLCT emitters exhibit maximum external quantum efficiencies (EQE_max) close to 6%, with impressive exciton utilization efficiency (Φs) of >50%, far exceeding the spin statistic limit of 25%. We rule out triplet-triplet annihilation and thermally activated delayed fluorescence as triplet harvesting mechanisms along with horizontal orientation of emitters to enhance light outcoupling and, instead, propose a “hot exciton” channel involving the nearly isoenergetic T₂ and S₁ states.

Original language	English
Pages (from-to)	3773-3783
Journal	Journal of Materials Chemistry C
Volume	8
Issue number	11
Early online date	28 Jan 2020
DOIs	https://doi.org/10.1039/C9TC06356K
Publication status	Published - 21 Mar 2020

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Copyright © 2020 The Author(s). This work has been made available online in accordance with publisher policies or with permission. Permission for further reuse of this content should be sought from the publisher or the rights holder. This is the author created accepted manuscript following peer review and may differ slightly from the final published version. The final published version of this work is available at https://doi.org/10.1039/C9TC06356K
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Sharma, N., Wong, M. Y., Hall, D., Spuling, E., Tenopala Carmona, F., Privitera, A., Copley, G. J., Cordes, D. B., Slawin, A. M. Z., Murawski, C., Gather, M. C., Beljonne, D., Olivier, Y., Samuel, I. D. W., & Zysman-Colman, E. (2020). Exciton efficiency beyond the spin statistical limit in organic light emitting diodes based on anthracene derivatives. Journal of Materials Chemistry C, 8(11), 3773-3783. https://doi.org/10.1039/C9TC06356K

@article{a3f7b61283bf4aaabbcddf5e0eabf86a,

title = "Exciton efficiency beyond the spin statistical limit in organic light emitting diodes based on anthracene derivatives",

abstract = "We report two donor-acceptor (D-A) materials based on a cyanoanthracene acceptor paired with diphenylamine (DPAAnCN) and carbazole (CzAnCN) donor moieties. These compounds show hybrid locally excited (LE) charge-transfer (CT) excited states (HLCT), which we demonstrated through a combined photophysical and computational study. Vacuum- deposited organic light emitting diodes (OLEDs) using these HLCT emitters exhibit maximum external quantum efficiencies (EQEmax) close to 6\%, with impressive exciton utilization efficiency (Φs) of >50\%, far exceeding the spin statistic limit of 25\%. We rule out triplet-triplet annihilation and thermally activated delayed fluorescence as triplet harvesting mechanisms along with horizontal orientation of emitters to enhance light outcoupling and, instead, propose a “hot exciton” channel involving the nearly isoenergetic T2 and S1 states.",

author = "Nidhi Sharma and Wong, \{Michael Yin\} and David Hall and Eduard Spuling and \{Tenopala Carmona\}, Francisco and Alberto Privitera and Copley, \{Graeme Jeffrey\} and Cordes, \{David Bradford\} and Slawin, \{Alexandra Martha Zoya\} and Caroline Murawski and Gather, \{Malte Christian\} and David Beljonne and Yoann Olivier and Samuel, \{Ifor D. W.\} and Eli Zysman-Colman",

note = "E.Z.-C. acknowledges the University of St Andrews and the Leverhulme Trust (RPG- 2016-047) for financial support. E.Z.-C. and I.D.W.S. thank EPSRC (EP/P010482/1) for support. We thank EPSRC UK National Mass Spectrometry Facility at Swansea University for analytical services. The work in Mons was supported by the European Union{\textquoteright}s Horizon 2020 research and innovation program under Grant Agreement N°. 646176 (EXTMOS project). Computational resources have been provided by the Consortium des {\'E}quipements de Calcul Intensif (C{\'E}CI), funded by the Fonds de la Recherche Scientifiques de Belgique (F.R.S.- FNRS) under Grant No. 2.5020.11. C.M. and G.C acknowledge funding by the European Commission through a Marie Sk{\l}odowska Curie fellowship (No. 703387 and 799302, respectively). M.C.G. acknowledges funding from EPSRC (EP/R010595/1). A.P. acknowledges the European Union{\textquoteright}s Horizon 2020 research and innovation programme under Marie Sklodowska Curie Grant agreement No. 722651 (SEPOMO project). EPR measurements were performed in the Centre for Advanced ESR (CAESR), located in the Department of Chemistry of the University of Oxford, and this work was supported by the EPSRC (EP/L011972/1). ",

year = "2020",

month = mar,

day = "21",

doi = "10.1039/C9TC06356K",

language = "English",

volume = "8",

pages = "3773--3783",

journal = "Journal of Materials Chemistry C",

issn = "2050-7526",

publisher = "Royal Society of Chemistry",

number = "11",

}

Sharma, N, Wong, MY, Hall, D, Spuling, E, Tenopala Carmona, F, Privitera, A, Copley, GJ, Cordes, DB , Slawin, AMZ, Murawski, C, Gather, MC, Beljonne, D, Olivier, Y, Samuel, IDW & Zysman-Colman, E 2020, 'Exciton efficiency beyond the spin statistical limit in organic light emitting diodes based on anthracene derivatives', Journal of Materials Chemistry C, vol. 8, no. 11, pp. 3773-3783. https://doi.org/10.1039/C9TC06356K

TY - JOUR

T1 - Exciton efficiency beyond the spin statistical limit in organic light emitting diodes based on anthracene derivatives

AU - Sharma, Nidhi

AU - Wong, Michael Yin

AU - Hall, David

AU - Spuling, Eduard

AU - Tenopala Carmona, Francisco

AU - Privitera, Alberto

AU - Copley, Graeme Jeffrey

AU - Cordes, David Bradford

AU - Slawin, Alexandra Martha Zoya

AU - Murawski, Caroline

AU - Gather, Malte Christian

AU - Beljonne, David

AU - Olivier, Yoann

AU - Samuel, Ifor D. W.

AU - Zysman-Colman, Eli

N1 - E.Z.-C. acknowledges the University of St Andrews and the Leverhulme Trust (RPG- 2016-047) for financial support. E.Z.-C. and I.D.W.S. thank EPSRC (EP/P010482/1) for support. We thank EPSRC UK National Mass Spectrometry Facility at Swansea University for analytical services. The work in Mons was supported by the European Union’s Horizon 2020 research and innovation program under Grant Agreement N°. 646176 (EXTMOS project). Computational resources have been provided by the Consortium des Équipements de Calcul Intensif (CÉCI), funded by the Fonds de la Recherche Scientifiques de Belgique (F.R.S.- FNRS) under Grant No. 2.5020.11. C.M. and G.C acknowledge funding by the European Commission through a Marie Skłodowska Curie fellowship (No. 703387 and 799302, respectively). M.C.G. acknowledges funding from EPSRC (EP/R010595/1). A.P. acknowledges the European Union’s Horizon 2020 research and innovation programme under Marie Sklodowska Curie Grant agreement No. 722651 (SEPOMO project). EPR measurements were performed in the Centre for Advanced ESR (CAESR), located in the Department of Chemistry of the University of Oxford, and this work was supported by the EPSRC (EP/L011972/1).

PY - 2020/3/21

Y1 - 2020/3/21

N2 - We report two donor-acceptor (D-A) materials based on a cyanoanthracene acceptor paired with diphenylamine (DPAAnCN) and carbazole (CzAnCN) donor moieties. These compounds show hybrid locally excited (LE) charge-transfer (CT) excited states (HLCT), which we demonstrated through a combined photophysical and computational study. Vacuum- deposited organic light emitting diodes (OLEDs) using these HLCT emitters exhibit maximum external quantum efficiencies (EQEmax) close to 6%, with impressive exciton utilization efficiency (Φs) of >50%, far exceeding the spin statistic limit of 25%. We rule out triplet-triplet annihilation and thermally activated delayed fluorescence as triplet harvesting mechanisms along with horizontal orientation of emitters to enhance light outcoupling and, instead, propose a “hot exciton” channel involving the nearly isoenergetic T2 and S1 states.

AB - We report two donor-acceptor (D-A) materials based on a cyanoanthracene acceptor paired with diphenylamine (DPAAnCN) and carbazole (CzAnCN) donor moieties. These compounds show hybrid locally excited (LE) charge-transfer (CT) excited states (HLCT), which we demonstrated through a combined photophysical and computational study. Vacuum- deposited organic light emitting diodes (OLEDs) using these HLCT emitters exhibit maximum external quantum efficiencies (EQEmax) close to 6%, with impressive exciton utilization efficiency (Φs) of >50%, far exceeding the spin statistic limit of 25%. We rule out triplet-triplet annihilation and thermally activated delayed fluorescence as triplet harvesting mechanisms along with horizontal orientation of emitters to enhance light outcoupling and, instead, propose a “hot exciton” channel involving the nearly isoenergetic T2 and S1 states.

UR - https://www.scopus.com/pages/publications/85082297917

U2 - 10.1039/C9TC06356K

DO - 10.1039/C9TC06356K

M3 - Article

SN - 2050-7526

VL - 8

SP - 3773

EP - 3783

JO - Journal of Materials Chemistry C

JF - Journal of Materials Chemistry C

IS - 11

ER -

Exciton efficiency beyond the spin statistical limit in organic light emitting diodes based on anthracene derivatives

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H2020-MSCA-redTADF: H2020 MSCA IF 2017 (Graeme Copley)

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TADF Emitters for OLEDs - Eli Zysman: TADF Emitters for OLEDs