1. Suppressing exciton deconfinement and dissociation for efficient thermally activated delayed fluorescence OLEDs
- Author
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Paulius Imbrasas, Sebastian Reineke, PA Peter Bobbert, Paul-Anton Will, X. de Vries, C. Hauenstein, C. H. L. Weijtens, Katrin Ortstein, Simone Lenk, H. van Eersel, R Reinder Coehoorn, Molecular Materials and Nanosystems, Center for Computational Energy Research, Macromolecular and Organic Chemistry, ICMS Core, and EIRES Chem. for Sustainable Energy Systems
- Subjects
Materials science ,Photoluminescence ,Exciton ,Intermolecular force ,General Physics and Astronomy ,02 engineering and technology ,010402 general chemistry ,021001 nanoscience & nanotechnology ,01 natural sciences ,Deconfinement ,Dissociation (chemistry) ,0104 chemical sciences ,13. Climate action ,Chemical physics ,Molecule ,Emission spectrum ,0210 nano-technology ,HOMO/LUMO - Abstract
The efficiency of organic light-emitting diodes that utilize the principle of thermally activated delayed fluorescence (TADF) depends sensitively on the host material in which the TADF emitter molecules (guests) are embedded. Potential loss processes are "deconfinement,"the transfer of excitons from the guest to the host, and "dissociation,"the formation of intermolecular charge-transfer states. We investigate how both processes can be suppressed by studying the photoluminescence efficiency, emission spectrum, and time-resolved emission intensity of eight thin-film systems in which 5 mol. % of the sky-blue TADF emitter 4-carbazolyl-methylphthalimide (abbreviated here as CzPIMe) is embedded in various host materials. Deconfinement is found to be entirely suppressed if the triplet energy of the host is 0.25 eV or more above that of the guest. For systems allowing for deconfinement, the dependence on the energy difference is consistent with a recent theoretical analysis [C. Hauenstein et al., J. Appl. Phys. 128, 075501 (2020)]. Dissociation, due to hole transfer to a host molecule, is found to be suppressed if the host's highest occupied molecular orbital energy is not more than about 0.2 eV higher than that of the guest. Otherwise, we observe an efficiency loss, a spectral redshift, and the disappearance of distinct prompt and delayed emission regimes. A comprehensive rate-equation model is developed from which we study the sensitivity of these observations to the energy level structure, the intermolecular interaction rates, and the photophysical rates that follow from a fit to the experimental data for the CzPIMe:TCTA [tris (4 - carbazoyl - 9 - ylphenyl) amine] system.
- Published
- 2021
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