TY - JOUR A1 - Müller, Ulrich A1 - Spenst, Peter A1 - Kagerer, Philipp A1 - Stolte, Matthias A1 - Würthner, Frank A1 - Pflaum, Jens T1 - Photon‐Correlation Studies on Multichromophore Macrocycles of Perylene Dyes JF - Advanced Optical Materials N2 - Organic dyes offer unique properties for their application as room temperature single photon emitters. By means of photon‐correlation, the emission characteristics of macrocyclic para‐xylylene linked perylene bisimide (PBI) trimers and tetramers dispersed in polymethyl methacrylate matrices are analyzed. The optical data indicate that, despite of the strong emission enhancement of PBI trimers and tetramers according to their larger number of chromophores, the photon‐correlation statistics still obeys that of single photon emitters. Moreover, driving PBI trimers and tetramers at higher excitation powers, saturated emission behavior for monomers is found while macrocycle emission is still far‐off saturation but shows enhanced fluctuations. This observation is attributed to fast singlet–singlet annihilation, i.e., faster than the radiative lifetime of the excited S1 state, and the enlarged number of conformational arrangements of multichromophores in the polymeric host. Finally, embedding trimeric PBI macrocycles in active organic light‐emitting diode matrices, electrically driven bright fluorescence together with an indication for antibunching at room temperature can be detected. This, so far, has only been observed for phosphorescent emitters that feature much longer lifetimes of the excited states and, thus, smaller radiative recombination rates. The results are discussed in the context of possible effects on the g(2) behavior of molecular emitters. KW - multichromophores KW - organic light emitting diodes KW - perylene dyes KW - photon‐correlation KW - single photon emission Y1 - 2022 U6 - http://nbn-resolving.de/urn/resolver.pl?urn:nbn:de:bvb:20-opus-287219 VL - 10 IS - 14 ER - TY - JOUR A1 - Bunzmann, Nikolai A1 - Krugmann, Benjamin A1 - Weissenseel, Sebastian A1 - Kudriashova, Liudmila A1 - Ivaniuk, Khrystyna A1 - Stakhira, Pavlo A1 - Cherpak, Vladyslav A1 - Chapran, Marian A1 - Grybauskaite‐Kaminskiene, Gintare A1 - Grazulevicius, Juozas Vidas A1 - Dyakonov, Vladimir A1 - Sperlich, Andreas T1 - Spin‐ and Voltage‐Dependent Emission from Intra‐ and Intermolecular TADF OLEDs JF - Advanced Electronic Materials N2 - Organic light emitting diodes (OLEDs) based on thermally activated delayed fluorescence (TADF) utilize molecular systems with a small energy splitting between singlet and triplet states. This can either be realized in intramolecular charge transfer states of molecules with near‐orthogonal donor and acceptor moieties or in intermolecular exciplex states formed between a suitable combination of individual donor and acceptor materials. Here, 4,4′‐(9H,9′H‐[3,3′‐bicarbazole]‐9,9′‐diyl)bis(3‐(trifluoromethyl) benzonitrile) (pCNBCzoCF\(_{3}\)) is investigated, which shows intramolecular TADF but can also form exciplex states in combination with 4,4′,4′′‐tris[phenyl(m‐tolyl)amino]triphenylamine (m‐MTDATA). Orange emitting exciplex‐based OLEDs additionally generate a sky‐blue emission from the intramolecular emitter with an intensity that can be voltage‐controlled. Electroluminescence detected magnetic resonance (ELDMR) is applied to study the thermally activated spin‐dependent triplet to singlet up‐conversion in operating devices. Thereby, intermediate excited states involved in OLED operation can be investigated and the corresponding activation energy for both, intra‐ and intermolecular based TADF can be derived. Furthermore, a lower estimate is given for the extent of the triplet wavefunction to be ≥ 1.2 nm. Photoluminescence detected magnetic resonance (PLDMR) reveals the population of molecular triplets in optically excited thin films. Overall, the findings allow to draw a comprehensive picture of the spin‐dependent emission from intra‐ and intermolecular TADF OLEDs. KW - color tuning KW - exciplexes KW - organic light emitting diodes KW - spin KW - triplets Y1 - 2021 U6 - http://nbn-resolving.de/urn/resolver.pl?urn:nbn:de:bvb:20-opus-224434 VL - 7 IS - 3 ER -