We expose significant changes in the emission color of carbazole-based thermally activated delayed fluorescence (TADF) emitters that arise from the presence of persistent dimer states in thin films and organic light-emitting diodes (OLEDs). Direct photoexcitation of this dimer state in 1,2,3,5-tetrakis(carbazol-9-yl)-4,6-dicyanobenzene (4CzIPN) reveals the significant influence of dimer species on the color purity of its photoluminescence and electroluminescence. The dimer species is sensitive to the sample preparation method, and its enduring presence contributes to the widely reported concentration-mediated red shift in the photoluminescence and electroluminescence of evaporated thin films. This discovery has implications on the usability of these, and similar, molecules for OLEDs and explains disparate electroluminescence spectra presented in the literature for these compounds. The dimerization-controlled changes observed in the TADF process and photoluminescence efficiency mean that careful consideration of dimer states is imperative in the design of future TADF emitters and the interpretation of previously reported studies of carbazole-based TADF materials.
We examine the impact of various annihilation processes on the laser threshold current density of a multilayer organic laser diode by numerical simulation. Our self-consistent numerical model treats the dynamics of electrons, holes, and singlet as well as triplet excitons in the framework of a drift-diffusion model. The resulting particle distributions enter into an optical model. In our approach, a three layer waveguide structure is taken into account and the resulting laser rate equations are solved. Various annihilation processes are included as reactions between the different particle species in the device employing typical annihilation rates and material properties of organic semiconductors. By systematically varying the device dimensions and the annihilation rate coefficients, the dominating quenching processes are identified. The threshold current density is found to depend sensitively on the thickness of the emission layer. The influence of annihilation processes on the threshold current density is quantified as a function of the emission layer thickness and various annihilation rate coefficients. Using typical annihilation rate coefficients singlet-polaron annihilation is found to be the dominating quenching process. Maximum annihilation rate coefficients are calculated allowing a threshold current density below 1kA∕cm2. Singlet-triplet annihilation is recognized as another main loss process for singlet excitons. In our model the singlet exciton density is increased by triplet-triplet annihilation whereas it is diminished by singlet-triplet annihilation. The ratio of the rate coefficients for singlet-triplet and triplet-triplet annihilations is identified to be critical for the total number of singlet excitons being quenched by triplet excitons.
A simplified state model and associated rate equations are used to extract the reverse intersystem crossing and other key rate constants from transient photoluminescence measurements of two high performance thermally activated delayed fluorescence materials. The values of the reverse intersystem crossing rate constant are in close agreement with established methods, but do not require a priori assumption of exponential decay kinetics, nor any additional steady state measurements. The model is also applied to measurements at different temperatures and found to reproduce previously reported thermal activation energies for the thermally activated delayed fluorescence process. Transient absorption measurements provide independent confirmation that triplet decay channels (neglected here) have no adverse effect on the fitting.
The authors present organic semiconductor distributed feedback lasers based on thin films of the conjugated polymer poly[9,9-dioctylfluorene-co-9,9-di(4-methoxy-phenyl)fluorene] and employing an improved resonator design. In order to combine the advantages of first- and second-order distributed feedback resonators, the authors utilize a mixed-order grating design: A second-order Bragg scattering region that provides efficient vertical outcoupling of the laser radiation is surrounded by first-order scattering regions that give rise to strong feedback. By optimizing the film thickness to obtain laser oscillation at the polymer maximum gain wavelength, a very low laser threshold of 45pJ∕pulse (≈36nJ∕cm2) was realized with this resonator concept.
We report on the fabrication of low threshold distributed feedback (DFB) polymer lasers based on a polyfluorene derivative containing statistical binaphthyl units (BN-PFO). First- and second-order feedback lasers have been realized. The emission was tuned in the wavelength range from 438to459nm by varying the grating period and the film thickness. A threshold energy of 280pJ/pulse was observed in second-order DFB structures, which could be further reduced to 160pJ/pulse by employing first-order feedback in electron beam lithographically patterned structures with a period of 140nm. In these first-order structures, laser oscillation at both edges of the photonic stop band was observed. These very low threshold values render BN-PFO a very promising material for future electrically pumped organic semiconductor laser diodes.
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