Dynamic nature of excited states of donor–acceptor TADF materials for OLEDs: how theory can reveal structure–property relationships
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Título: | Dynamic nature of excited states of donor–acceptor TADF materials for OLEDs: how theory can reveal structure–property relationships |
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Autor/es: | Olivier, Yoann | Moral, Mónica | Muccioli, Luca | Sancho-Garcia, Juan-Carlos |
Grupo/s de investigación o GITE: | Química Cuántica |
Centro, Departamento o Servicio: | Universidad de Alicante. Departamento de Química Física |
Palabras clave: | OLEDs | Thermally Activated Delayed Fluorescence (TADF) | Excited states | Donor–acceptor |
Área/s de conocimiento: | Química Física |
Fecha de publicación: | 2017 |
Editor: | Royal Society of Chemistry |
Cita bibliográfica: | Journal of Materials Chemistry C. 2017, 5: 5718-5729. doi:10.1039/C6TC05075A |
Resumen: | Spin statistics greatly limits the efficiency of OLEDs, which might be largely improved upon conversion of triplet into singlet-excited (and thus light-emitting) states via a Thermally Activated Delayed Fluorescence (TADF) process. We theoretically investigate here the combination of some real-life donor (D) and acceptor (A) moieties with the connectivity D–A and D–A–D. We selected phenoxazine (PXZ) and phenylthiazine (PTZ) as electron-donating groups, and 2,5-diphenyl-1,3,4-oxadiazole (OXD), 3,4,5-triphenyl-4H-1,2,4-triazole (TAZ), and 2,5-diphenyl-1,3,4-thiadiazole (TDZ) as their electron-accepting partners. The systematic Tamm–Dancoff Approximation-Density Functional Theory calculations performed allowed us to calculate accurately not only the energy levels of low-lying singlet and triplet-excited states, but also to characterize their Charge-Transfer (CT) or Locally Excited (LE) nature, since the energy difference and the coupling between the 3CT, 3LE, and 1CT states become key to understanding the molecular mechanism involved in this process. We have also studied the role played by the conformational landscape, arising from the thermally accessible range of D–A(–D) torsion angles, in the singlet–triplet energy gap as well as its influence on oscillator strengths. Overall, we rationalize the origin of the higher efficiencies found in real devices for D–A–D molecules, disclosing the underlying structure–property relationships and thus anticipating successful design strategies. |
Patrocinador/es: | This work was partially supported by the Samsung Advanced Institute of Technology (SAIT)’s Global Research Outreach (GRO) Program. In addition, the research in Bordeaux has been funded by the French State grant ANR-10-LABX-0042-AMADEus managed by the French National Research Agency under the initiative of excellence IdEx Bordeaux program (reference ANR-10-IDEX-0003-02). The work in Mons was supported by the “Programme d’Excellence de la Région Wallonne” (OPTI2MAT project) and FNRS-FRFC. Computational resources have been provided by the Consortium des Équipements de Calcul Intensif (CÉCI), funded by the Fonds de la Recherche Scientifique de Belgique (F.R.S.-FNRS) under Grant no. 2.5020.11 as well as the Tier-1 supercomputer of the Fédération Wallonie-Bruxelles, infrastructure funded by the Walloon Region under the grant agreement no. 1117545. Mónica Moral thanks to the E2TP CYTEMA-Santander Program for their financial support. |
URI: | http://hdl.handle.net/10045/67485 |
ISSN: | 2050-7526 (Print) | 2050-7534 (Online) |
DOI: | 10.1039/C6TC05075A |
Idioma: | eng |
Tipo: | info:eu-repo/semantics/article |
Derechos: | © The Royal Society of Chemistry 2017 |
Revisión científica: | si |
Versión del editor: | http://dx.doi.org/10.1039/C6TC05075A |
Aparece en las colecciones: | INV - QC - Artículos de Revistas |
Archivos en este ítem:
Archivo | Descripción | Tamaño | Formato | |
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2017_Olivier_etal_JMaterChemC_final.pdf | Versión final (acceso restringido) | 2,58 MB | Adobe PDF | Abrir Solicitar una copia |
2017_Olivier_etal_JMaterChemC_accepted.pdf | Accepted Manuscript (acceso abierto) | 1,88 MB | Adobe PDF | Abrir Vista previa |
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