Photon‐Correlation Studies on Multichromophore Macrocycles of Perylene Dyes. Issue 14 (29th May 2022)

• Record Type: Journal Article
• Authors: Müller, Ulrich; Spenst, Peter; Kagerer, Philipp; Stolte, Matthias; Würthner, Frank; Pflaum, Jens
• Is Part Of: Advanced optical materials. Volume 10:Issue 14(2022)
• Page Start: n/a
• Page End: n/a
• Publication Date: 2022-05-29
• Subjects: multichromophores -- organic light emitting diodes -- perylene dyes -- photon‐correlation -- single photon emission; Optical materials -- Periodicals; Photonics -- Periodicals; 620.11295
• DOI: 10.1002/adom.202200234
• Languages: English
• ISSNs: 2195-1071

Abstract

Abstract: 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. Abstract : Here, the photophysical properties of single molecule perylene bisimide (PBI) macrocycles are investigated. The disproportionately high fluorescence increase of PBI trimers and tetramers with excitation power indicates the presence of interchromophore multiple‐state processes that conserve the single emitter character of all PBI compounds. Utilizing these processes even further, a proof‐of‐concept organic light‐emitting diode based on PBI trimer single molecules showing bright electro‐fluorescence is demonstrated.