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Spin-spin interactions in organic light-emitting diodes (OLEDs) based on thermally activated delayed fluorescence (TADF) are pivotal because radiative recombination is largely determined by triplet-to-singlet conversion, also called reverse intersystem crossing (RISC). To explore the underlying process, we apply a spin-resonance spectral hole-burning technique to probe electroluminescence. We find that the triplet exciplex states in OLEDs are highly spin-polarized and show that these states can be decoupled from the heterogeneous nuclear environment as a source of spin dephasing and can even be coherently manipulated on a spin-spin relaxation time scale T-2* of 30 ns. Crucially, we obtain the characteristic triplet exciplex spin-lattice relaxation time T-1 in the range of 50 mu s, which far exceeds the RISC time. We conclude that slow spin relaxation rather than RISC is an efficiency-limiting step for intermolecular donor:acceptor systems. Finding TADF emitters with faster spin relaxation will benefit this type of TADF OLEDs.
Microstructural changes and the understanding of their effect on photocurrent generation are key aspects for improving the efficiency of organic photovoltaic devices. We analyze the impact of a systematically increased amount of the solvent additive diiodooctane (DIO) on the morphology of PBDTTT-C:PC71BM blends and related changes in free carrier formation and recombination by combining surface imaging, photophysical and charge extraction techniques. We identify agglomerates visible in AFM images of the 0% DIO blend as PC71BM domains embedded in an intermixed matrix phase. With the addition of DIO, a decrease in the size of fullerene domains along with a demixing of the matrix phase appears for 0.6% and 1% DIO. Surprisingly, transient absorption spectroscopy reveals an efficient photogeneration already for the smallest amount of DIO, although the largest efficiency is found for 3% DIO. It is ascribed to a fine-tuning of the blend morphology in terms of the formation of interpenetrating donor and acceptor phases minimizing geminate and nongeminate recombination as indicated by charge extraction experiments. An increase in the DIO content to 10% adversely affects the photovoltaic performance, most probably due to an inefficient free carrier formation and trapping in a less interconnected donor-acceptor network.