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Effect of exciton diffusion on the triplet-triplet annihilation rate in organic semiconductor host-guest systems
摘要： We study the contribution of triplet exciton diffusion to the efficiency loss resulting from F?rster-type triplet-triplet annihilation (TTA) in organic phosphorescent semiconductor host-guest systems, using kinetic Monte Carlo (KMC) simulations. Our study focusses on diffusion due to F?rster-type guest-guest transfer, but includes also a comparison with simulation results for the case of Dexter-type guest-guest transfer. The simulations are carried out for a wide range of F?rster radii, and for guest concentrations up to 100 mol%, with the purpose to support analyses of time-resolved photoluminescence experiments probing TTA. We find that the relative contribution of diffusion to the TTA-induced efficiency loss may be deduced quite accurately from a quantitative experimental measure for the shape of the time-dependent photoluminescence intensity, the so-called r ratio. For small guest concentrations and F?rster radii that are most relevant to organic light-emitting diodes (OLEDs), the diffusion contribution is in general quite small. Under these weak-diffusion conditions, the absolute diffusion contribution to the TTA-induced efficiency loss can be understood quantitatively using a capture radius formalism. The effective guest-guest diffusion coefficient that follows from the TTA simulations, using the capture radius formalism, agrees well with the diffusion coefficient that follows from direct KMC diffusion simulations. The simulations reveal that the diffusion coefficient is strongly affected by the randomness of the distribution of guest molecule locations.
关键词： OLEDs,photoluminescence,kinetic Monte Carlo simulations,Dexter transfer,organic semiconductors,triplet-triplet annihilation,exciton diffusion,host-guest systems,F?rster transfer
更新于2025-09-23 15:23:52
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Suppressed Triplet Exciton Diffusion Due to Small Orbital Overlap as a Key Design Factor for Ultralong-Lived Room-Temperature Phosphorescence in Molecular Crystals
摘要： Persistent room-temperature phosphorescence (RTP) under ambient conditions is attracting attention due to its strong potential for applications in bioimaging, sensing, or optical recording. Molecular packing leading to a rigid crystalline structure that minimizes nonradiative pathways from triplet state is often investigated for efficient RTP. However, for complex conjugated systems a key strategy to suppress the nonradiative deactivation is not found yet. Here, the origin of small rates of a nonradiative decay process from triplet states of conjugated molecular crystals showing RTP is reported. Optical microscopy analysis showed that, despite a favorable molecular stacking, an aromatic crystal with strong RTP is characterized by small diffusion length and small values of the diffusion coefficient of triplet excitons. Quantum chemical calculations reveal a large overlap between the lowest unoccupied molecular orbitals but very small overlap between the highest occupied molecular orbitals (HOMOs). Inefficient electron exchange caused by the small overlap of HOMOs prevents triplet excitons from diffusing over long distances and consequently from quenching at defect sites inside the crystal or at the crystal surface. These results will allow design of comprehensive molecular structures to obtain molecular solids with more efficient RTP.
关键词： suppressed nonradiative rate,persistent room-temperature phosphorescence,triplet exciton diffusion,molecular orbital overlap,fluorescence microscopy
更新于2025-09-23 15:23:52
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Novel strategy to improve the efficiency roll-off at high luminance and operational lifetime of hybrid white OLEDs via employing an assistant layer with triplet-triplet annihilation up-conversion characteristics
摘要： The efficiency roll-off at high luminance and operational lifetime remain a major challenge before the wide applications of white organic light-emitting diodes (WOLEDs) technology. Here we present a novel strategy to improve the efficiency roll-off at high luminance and operational lifetime by employing an assistant layer with triplet-triplet annihilation (TTA) up-conversion characteristics in emitters. It can be seen that at high luminance, the partial triplet energies in emitters will transfer to the TTA assistant layer and finally lead to the TTA emission, which reduces the exciton quenching at high luminance. Therefore, not only the efficiency roll-off, but also the operational lifetime are greatly improved. The resulting hybrid WOLEDs exhibited the maximum forward-viewing external quantum efficiency and power efficiency of 23.6% and 68.8 lm W?1, and they only dropped to 18.3% and 38.1 lm W?1 at 1000 cd m?2 and 17.1% and 25.9 lm W?1 at 5000 cd m?2, which are significantly higher than 10.5% and 17.9 lm W?1 at 5000 cd m?2 of WOLEDs without TTA assistant layer. Furthermore, the operational half-lifetime of the resulting hybrid WOLEDs also reached 600 hours at the luminance of 1000 cd m?2, which is nearly two-fold longer than that of the reference WOLEDs.
关键词： exciton diffusion,triplet-triplet annihilation up-conversion,Efficiency roll-off,white organic light-emitting diodes,lifetime
更新于2025-09-23 15:21:01
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Measurement and Theoretical Interpretation of Exciton Diffusion as a Function of Intermolecular Separation for Squaraines Targeted for Bulk Heterojunction Solar Cells
摘要： The efficiency of bulk heterojunction (BHJ) organic photovoltaic (OPV) devices depends significantly upon absorption of photons and the migration of the photogenerated excited state to the heterojunction interface between the electron donor and electron acceptor. Within anilino-squaraine, molecules known for their successful use in the active layer of OPV devices, electronic aggregation strongly influences the absorption spectrum, energy transfer (EnT), and exciton migration to this heterojunction interface. Therefore, the long-range transition dipole coupling and the relative populations of the associated excited states dictate the general effectiveness of these materials in optoelectronic devices. This work presents subpicosecond transient absorption (TA) data that probe the excited-state photophysics of samples with a continuum of intermolecular separation, from monomers in solution to high-concentration solid solution thin films analogous to OPV active layers. EnT times are calculated for each squaraine concentration, and pump-power dependence provides evidence for significant EnT despite a high preponderance of H-aggregation. Theoretical modeling of essential states supports the interpretation from TA spectra that excited states relax into more tightly packed H-aggregates. This work prompts further questions regarding a far-reaching mechanistic EnT bottleneck for molecular and polymeric BHJ devices.
关键词： H-aggregation,squaraine,organic photovoltaic,bulk heterojunction,exciton diffusion,energy transfer
更新于2025-09-23 15:19:57
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Evaluation of exciton diffusion length in highly oriented fullerene films of fullerene/p-Si(100) hybrid solar cells
摘要： Highly oriented fullerene (C60) films on p-Si (100) substrates were fabricated to evaluate the crystallinity dependent exciton diffusion length of C60 (LC60). The crystal structure of the C60 films was examined using grazing incidence X-ray diffraction (GIXD). The results of an in-plane rocking scan and a pole figure suggested that a 12-fold-symmetry crystal was grown with the C60(111) surface interfaced to the Si(100) substrate. The photovoltaic characteristics of the oriented C60/p-Si(100) hybrid solar cells were evaluated. A masking effect was clearly evident in the incident photon-to-current conversion efficiency (IPCE) spectra. LC60 was evaluated using both experimental IPCE spectra and that produced by one-dimensional-optical simulation. It was concluded that LC60 for highly oriented C60 was 60 nm, which was longer than that of disordered C60 films.
关键词： crystal growth,hybrid solar cells,fullerene (C60),exciton diffusion length,grazing incidence X-ray diffraction (GIXD),masking effect
更新于2025-09-11 14:15:04
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Applied Nanophotonics || Energy transfer processes
摘要： In this chapter, we introduce the general phenomenon of excitation energy transfer, explain radiative and nonradiative types of energy transfer, and derive the basic processes of energy transfer. We look at the F?rster resonance energy transfer (FRET) in particular. We also describe Dexter energy transfer, charge transfer, exciton diffusion, and exciton dissociation. Finally, we summarize the modifications of FRET when using nanostructures with mixed dimensionalities and in different assemblies.
关键词： F?rster resonance energy transfer,nanostructures,FRET,charge transfer,exciton diffusion,energy transfer,Dexter energy transfer,exciton dissociation
更新于2025-09-10 09:29:36