Energy relaxation dynamics and universal scaling laws in organic light emitting diodes

dc.creatorKarabunarliev, S.
dc.creatorBittner, Eric R.
dc.date2002-06-03
dc.date2003-02-11
dc.date.accessioned2026-07-07T02:45:43Z
dc.date.available2026-07-07T02:45:43Z
dc.descriptionElectron-hole (e-h) capture in luminescent conjugated polymers (LCPs) is modeled by the dissipative dynamics of a multilevel electronic system coupled to a phonon bath. Electroinjected e-h pairs are simulated by a mixed quantum state, which relaxes via phonon-driven internal conversions to low-lying charge-transfer (CT) and excitonic (XT) states. The underlying two-band polymer model reflects PPV and spans monoexcited configuration interaction singlets (S) and triplets (T), coupled to Franck-Condon active C=C stretches and ring-torsions. Focusing entirely upon long PPV chains, we consider the recombination kinetics of an initially separated CT pair. Our model calculations indicated that S and T recombination proceeds according to a branched, two-step mechanism dictated by near e-h symmetry. The initial relaxation occurs rapidly with nearly half of the population going into excitons ($S_{XT}$ or $T_{XT}$), while the remaining portion remains locked in metastable CT states. While formation rates of $S_{CT}$ and $T_{CT}$ are nearly equal, $S_{XT}$ is formed about twice as fast $T_{XT}$ in concurrence with experimental observations of these systems. Furthermore, breaking e-h symmetry suppresses the XT to CT branching ratio for triplets and opens a slow CT$\to$ XT conversion channel exclusively for singlets due to dipole-dipole interactions between geminate and non-geminate configurations. Finally, our calculations yield a remarkable linear relation between chain length and singlet/triplet branching ratio which can be explained in terms of the binding energies of the respective final excitonic states and the scaling of singlet-triplet energy gap with chain length.
dc.descriptionFor IJQC-Sanibel Quantum Chemistry Symposium, 2003
dc.identifierhttps://arxiv.org/abs/cond-mat/0206015
dc.identifierhttp://arxiv.org/abs/cond-mat/0206015
dc.identifier.urihttp://salesiana.dossiersoluciones.com/handle/123456789/19402
dc.subjectMaterials Science
dc.titleEnergy relaxation dynamics and universal scaling laws in organic light emitting diodes
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