Computationally Guided Molecular Design to Minimize the LE/CT Gap in D-π-A Fluorinated Triarylboranes for Efficient TADF via D and π-Bridge Tuning

Ayush K. Narsaria, Florian Rauch, Johannes Krebs, Peter Endres, Alexandra Friedrich, Ivo Krummenacher, Holger Braunschweig, Maik Finze, Jörn Nitsch, F. Matthias Bickelhaupt*, Todd B. Marder

*Corresponding author for this work

Research output: Contribution to JournalArticleAcademicpeer-review


In this combined experimental and theoretical study, a computational protocol is reported to predict the excited states in D-π-A compounds containing the B(FXyl)2 (FXyl = 2,6-bis(trifluoromethyl)phenyl) acceptor group for the design of new thermally activated delayed fluorescence (TADF) emitters. To this end, the effect of different donor and π-bridge moieties on the energy gaps between local and charge-transfer singlet and triplet states is examined. To prove this computationally aided design concept, the D-π-B(FXyl)2 compounds 1–5 were synthesized and fully characterized. The photophysical properties of these compounds in various solvents, polymeric film, and in a frozen matrix were investigated in detail and show excellent agreement with the computationally obtained data. Furthermore, a simple structure–property relationship is presented on the basis of the molecular fragment orbitals of the donor and the π-bridge, which minimize the relevant singlet–triplet gaps to achieve efficient TADF emitters.

Original languageEnglish
Article number2002064
Pages (from-to)1-15
Number of pages15
JournalAdvanced Functional Materials
Issue number31
Early online date2 Jun 2020
Publication statusPublished - 1 Aug 2020


A.K.N. and F.R. contributed equally to this work. Financial support from the Julius-Maximilians-Universit?t W?rzburg and the Netherlands Organisation for Scientific Research (NWO) is gratefully acknowledged. T.B.M. thanks the Bavarian State Ministry of Science, Research, and the Arts for the Collaborative Research Network ?Solar Technologies go Hybrid? for funding. F.M.B. thanks the Industrial Partnership Program (IPP) ?Computational Sciences for Energy Research? (project 14CSER011) which is part of the Netherlands Organization for Scientific Research (NWO) and is co-financed by Shell Global Solutions International B.V. J.N. thanks the Deutsche Forschungsgemeinschaft for a Research Fellowship (NI 1737/1-1) and a DFG Return Fellowship (NI 1737/2-1). A.K.N. thanks Erik van Lenthe for stimulating discussions on modeling the energy gaps. B2pin2 was kindly donated by AllyChem Co. Ltd. (Dalian, China). All authors thank Verena Borawski for preparing the TOC.

FundersFunder number
Verena Borawski
Shell Global Solutions International
Deutsche ForschungsgemeinschaftNI 1737/1‐1, NI 1737/2‐1
Nederlandse Organisatie voor Wetenschappelijk Onderzoek
Bayerisches Staatsministerium für Wissenschaft, Forschung und Kunst14CSER011
Julius-Maximilians-Universität Würzburg


    • boron
    • charge transfer
    • delayed fluorescence
    • organic light-emitting diodes
    • singlet–triplet gap quantum efficiency


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