Design Strategy for Ag(I)-Based Thermally Activated Delayed Fluorescence Reaching an Efficiency Breakthrough

A design strategy for the development of Ag­(I)-based materials for thermally activated delayed fluorescence (TADF) is presented. Although Ag­(I) complexes usually do not show TADF, the designed material, Ag­(dbp)­(P2-nCB) [dbp = 2,9-di-n-butyl-1,10-phenanthroline, and P2-nCB = nido-carborane-bis­(d...

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Published inChemistry of materials Vol. 29; no. 4; pp. 1708 - 1715
Main Authors Shafikov, Marsel Z, Suleymanova, Alfiya F, Czerwieniec, Rafał, Yersin, Hartmut
Format Journal Article
LanguageEnglish
Published American Chemical Society 28.02.2017
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Abstract A design strategy for the development of Ag­(I)-based materials for thermally activated delayed fluorescence (TADF) is presented. Although Ag­(I) complexes usually do not show TADF, the designed material, Ag­(dbp)­(P2-nCB) [dbp = 2,9-di-n-butyl-1,10-phenanthroline, and P2-nCB = nido-carborane-bis­(diphenylphosphine)], shows a TADF efficiency breakthrough exhibiting an emission decay time of τ­(TADF) = 1.4 μs at a quantum yield of ΦPL = 100%. This is a consequence of three optimized parameters. (i) The strongly electron-donating negatively charged P2-nCB ligand destabilizes the 4d orbitals and leads to low-lying charge (CT) states of MLL′CT character, with L and L′ being the two different ligands, thus giving a small energy separation between the lowest singlet S1 and triplet T1 state of ΔE(S1–T1) = 650 cm–1 (80 meV). (ii) The allowedness of the S1 → S0 transition is more than 1 order of magnitude higher than those found for other TADF metal complexes, as shown experimentally and by time-dependent density functional theory calculations. Both parameters favor a short TADF decay time. (iii) The high quantum efficiency is dominantly related to the rigid molecular structure of Ag­(dbp)­(P2-nCB), resulting from the design strategy of introducing n-butyl substitutions at positions 2 and 9 of phenanthroline that sterically interact with the phenyl groups of the P2-nCB ligand. In particular, the shortest TADF decay time of τ­(TADF) = 1.4 μs at a ΦPL value of 100%, reported so far, suggests the use of this outstanding material for organic light-emitting diodes (OLEDs). Importantly, the emission of Ag­(dbp)­(P2-nCB) is not subject to concentration quenching. Therefore, it may be applied even as a 100% emission layer.
AbstractList A design strategy for the development of Ag­(I)-based materials for thermally activated delayed fluorescence (TADF) is presented. Although Ag­(I) complexes usually do not show TADF, the designed material, Ag­(dbp)­(P2-nCB) [dbp = 2,9-di-n-butyl-1,10-phenanthroline, and P2-nCB = nido-carborane-bis­(diphenylphosphine)], shows a TADF efficiency breakthrough exhibiting an emission decay time of τ­(TADF) = 1.4 μs at a quantum yield of ΦPL = 100%. This is a consequence of three optimized parameters. (i) The strongly electron-donating negatively charged P2-nCB ligand destabilizes the 4d orbitals and leads to low-lying charge (CT) states of MLL′CT character, with L and L′ being the two different ligands, thus giving a small energy separation between the lowest singlet S1 and triplet T1 state of ΔE(S1–T1) = 650 cm–1 (80 meV). (ii) The allowedness of the S1 → S0 transition is more than 1 order of magnitude higher than those found for other TADF metal complexes, as shown experimentally and by time-dependent density functional theory calculations. Both parameters favor a short TADF decay time. (iii) The high quantum efficiency is dominantly related to the rigid molecular structure of Ag­(dbp)­(P2-nCB), resulting from the design strategy of introducing n-butyl substitutions at positions 2 and 9 of phenanthroline that sterically interact with the phenyl groups of the P2-nCB ligand. In particular, the shortest TADF decay time of τ­(TADF) = 1.4 μs at a ΦPL value of 100%, reported so far, suggests the use of this outstanding material for organic light-emitting diodes (OLEDs). Importantly, the emission of Ag­(dbp)­(P2-nCB) is not subject to concentration quenching. Therefore, it may be applied even as a 100% emission layer.
Author Shafikov, Marsel Z
Suleymanova, Alfiya F
Czerwieniec, Rafał
Yersin, Hartmut
AuthorAffiliation Universität Regensburg
Institut für Physikalische und Theoretische Chemie
I. Postovsky Institute of Organic Synthesis
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  givenname: Rafał
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  email: hartmut.yersin@ur.de
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Snippet A design strategy for the development of Ag­(I)-based materials for thermally activated delayed fluorescence (TADF) is presented. Although Ag­(I) complexes...
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Title Design Strategy for Ag(I)-Based Thermally Activated Delayed Fluorescence Reaching an Efficiency Breakthrough
URI http://dx.doi.org/10.1021/acs.chemmater.6b05175
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