Theoretical Rationalization of the Singlet–Triplet Gap in OLEDs Materials: Impact of Charge-Transfer Character
| العنوان: | Theoretical Rationalization of the Singlet–Triplet Gap in OLEDs Materials: Impact of Charge-Transfer Character |
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| المؤلفون: | Won Joong Son, Luca Muccioli, Mónica Moral, Juan Carlos Sancho-García, Yoann Olivier |
| المساهمون: | Moral, M, Muccioli, L., Son, W.-J., Olivier, Y., Sancho-Garcia, J.C., Universidad de Alicante. Departamento de Química Física, Química Cuántica, Departamento de Quımica Fısica [Alicante], Universidad de Alicante, Dipartimento di Chimica Industriale ‘‘Toso Montanari’’, Alma Mater Studiorum Università di Bologna [Bologna] (UNIBO), Laboratoire de Chimie des Polymères Organiques (LCPO), Centre National de la Recherche Scientifique (CNRS)-Institut Polytechnique de Bordeaux-Ecole Nationale Supérieure de Chimie, de Biologie et de Physique (ENSCBP)-Université de Bordeaux (UB)-Institut de Chimie du CNRS (INC), Team 4 LCPO : Polymer Materials for Electronic, Energy, Information and Communication Technologies, Centre National de la Recherche Scientifique (CNRS)-Institut Polytechnique de Bordeaux-Ecole Nationale Supérieure de Chimie, de Biologie et de Physique (ENSCBP)-Université de Bordeaux (UB)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS)-Institut Polytechnique de Bordeaux-Ecole Nationale Supérieure de Chimie, de Biologie et de Physique (ENSCBP)-Université de Bordeaux (UB)-Institut de Chimie du CNRS (INC), Samsung Adv Inst Technol, S. Korea, Samsung Advanced Institute of Technology (SAIT), Samsung-Samsung, Univ Mons, Lab Chem Novel Mat, Belgium, Université de Mons (UMons) |
| المصدر: | RUA. Repositorio Institucional de la Universidad de Alicante Universidad de Alicante (UA) Journal of Chemical Theory and Computation Journal of Chemical Theory and Computation, American Chemical Society, 2015, 11 (1), pp.168-177. ⟨10.1021/ct500957s⟩ |
| بيانات النشر: | American Chemical Society (ACS), 2014. |
| سنة النشر: | 2014 |
| مصطلحات موضوعية: | ORGANIC SEMICONDUCTORS, Exciton, LIGHT-EMITTING-DIODES, Nanotechnology, Molecular physics, Molecular engineering, DENSITY-FUNCTIONAL THEORY, CONFIGURATION-INTERACTION, Charge-transfer character, OLED, OLEDs materials, Química Física, Singlet state, Physical and Theoretical Chemistry, ACTIVATED DELAYED FLUORESCENCE, Physics, Computer Science Applications1707 Computer Vision and Pattern Recognition, Configuration interaction, DISPERSION CORRECTIONS, Computer Science Applications, Organic semiconductor, [CHIM.POLY]Chemical Sciences/Polymers, EXCITED-STATES, HIGH-PERFORMANCE, Excited state, TAMM-DANCOFF APPROXIMATION, Singlet–triplet gap, Density functional theory, FIELD-EFFECT TRANSISTORS |
| الوصف: | New materials for OLED applications with low singlet–triplet energy splitting have been recently synthesized in order to allow for the conversion of triplet into singlet excitons (emitting light) via a Thermally Activated Delayed Fluorescence (TADF) process, which involves excited-states with a non-negligible amount of Charge-Transfer (CT). The accurate modeling of these states with Time-Dependent Density Functional Theory (TD-DFT), the most used method so far because of the favorable trade-off between accuracy and computational cost, is however particularly challenging. We carefully address this issue here by considering materials with small (high) singlet–triplet gap acting as emitter (host) in OLEDs and by comparing the accuracy of TD-DFT and the corresponding Tamm-Dancoff Approximation (TDA), which is found to greatly reduce error bars with respect to experiments thanks to better estimates for the lowest singlet–triplet transition. Finally, we quantitatively correlate the singlet–triplet splitting values with the extent of CT, using for it a simple metric extracted from calculations with double-hybrid functionals, that might be applied in further molecular engineering studies. 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), and the work in Mons was supported by the “Programme d’Excellence de la Région Wallonne” (OPTI2MAT project) and FNRS-FRFC. |
| وصف الملف: | STAMPA |
| تدمد: | 1549-9626 1549-9618 |
| الوصول الحر: | https://explore.openaire.eu/search/publication?articleId=doi_dedup___::b01a4f5206e9cf2bccdb02f4197a563dTest https://doi.org/10.1021/ct500957sTest |
| حقوق: | OPEN |
| رقم الانضمام: | edsair.doi.dedup.....b01a4f5206e9cf2bccdb02f4197a563d |
| قاعدة البيانات: | OpenAIRE |
| تدمد: | 15499626 15499618 |
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