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By employing random walk an analytic theory for the dissociation of singlet excitons in a random organic solid, for instance, a conjugated polymer, has been developed. At variance of conventional three-dimensional Onsager theory, it is assumed that an exciton with finite lifetime can first transfer endothermically an electron to an adjacent site, thereby generating a charge transfer state whose energy is above the energy of that of the initial exciton. In a second step the latter can fully dissociate in accordance with Onsager’s concept Brownian motion. The results indicate that, depending of the energy required for the first jump, the first jump contributes significantly to the field dependence of the dissociation yield. Disorder weakens the temperature dependence of the yield dramatically and precludes extracting information on the exciton binding energy from it. [ABSTRACT FROM AUTHOR]

The delayed luminescence and phosphorescence of ladder-type methyl-poly(para-phenylene) (MeLPPP) doped with benzil at a concentration of 20% by weight has been measured. The introduction of benzil leads to a dramatic reduction of the polymer singlet emission. At the same time, a new band with maximum at 611 nm appears, corresponding to the phosphorescence of MeLPPP. The phosphorescence decay on the short time scale is close to an exponential law with a time decay of 15 ms. This indicates that benzil can efficiently sensitize the phosphorescence of the polymer. In addition, a broad and featureless emission is observed in the delayed luminescence spectra of benzil-doped MeLPPP, which is attributed to an exciplex formed between the polymer host and the dopant. We further observe that the delayed fluorescence is enhanced by the addition of benzil. It is concluded that the delayed fluorescence of benzil-doped MeLPPP is mainly due to the annihilation of triplet excitons on the polymer. Finally, efficient triplet-triplet energy transfer from the benzil-doped polymer to the red-emitting phosphorescent dye Pt(II)octaethylporphyrin is established. © 2004 American Institute of Physics. [ABSTRACT FROM AUTHOR]

Stationary photoconduction in either a phenyl-substituted poly-phenylenevinylene copolymer (PhPPV) or an alkylated hexa-peri-hexabenzocoronene (HBC) doped by perylenediimide (PdI) at a broad range of dopant concentrations has been measured and compared to previous results on PhPPV doped by trinitrofluorenone (TNF). At moderate concentration, the yield of the photogeneration is virtually invariant regardless of the system and blend ratio because practically every primary excitation dissociates at a donor-acceptor site and the subsequent escape from the coulombic potential is virtually system-independent. At dopant concentrations >10% the yield of that escape process increases by two to three orders of magnitude. [ABSTRACT FROM AUTHOR]

The properties of light-emitting diodes based on the electrophorescent platinum-porphyrin dye PtOEP blended into a ladder-type poly(para-phenylene) (LPPP) polymer host are presented. Due to the small difference between the highest occupied molecular orbital (HOMO) levels of the guest and the host, the operating voltage of single layer devices is almost independent of the dopant concentration in clear contrast to what has been observed in the case of wide-band gap host polymers. However, the efficiency and the color purity of these single-layer devices is quite poor, which can be attributed to the weak trapping of carriers on the phosphorescent dye. Incorporating an electron-transporting/hole-blocking layer greatly increases the efficiency of the devices but at the same time emission from the host becomes more significant. Adding a hole-transporting/ electron-blocking layer further increases the efficiency of the devices. Pure red emission is, however, only obtained if the HOMO of the hole-transporting layer is well above that of the LPPP host. This effect is interpreted in terms of a direct injection of holes from the hole-transporting layer into the HOMO level of the dopant. Further, prompt fluorescence and phosphorescence studies indicate that energy transfer from LPPP singlet excitons contributes to the emission from the dopant, but that the efficiency of singlet exciton transfer is too small to explain the almost complete absence of host emission in the electroluminescence spectra of single- and three-layer devices. [ABSTRACT FROM AUTHOR]

We present a comprehensive experimental and computational study on fs-relaxational dynamics of optical excitations in the conjugated polymer poly(p-phenylenevinylene) (PPV) under selective excitation tuning conditions into the long-wavelength, low-vibrational S[sup v=0, sub 1]-density-of-states (DOS). The dependence of single-wavelength luminescence kinetics and time-windowed spectral transients on distinct, initial excitation boundaries at 1.4 K and at room temperature was measured applying the luminescence up-conversion technique. The typical energy-dispersive intra-DOS energy transfer was simulated by a combination of static Monte Carlo method with a dynamical algorithm for solving the energy-space transport Master-Equation in population-space. For various, selective excitations that give rise to specific S[sub l]-population distributions in distinct spatial and energetic subspaces inside the DOS, simulations confirm the experimental results and show that the subsequent, energy-dissipative, multilevel relaxation is hierarchically constrained, and reveals a pronounced site-energy memory effect with a migration-threshold, characteristic of the (dressed) excitation dynamics in the disordered PPV many-body system. [ABSTRACT FROM AUTHOR]

The question of the origin of delayed fluorescence from a phenyl-substituted poly(p-phenylenevinylene)-type copolymer (Ph-PPV) is addressed. Two origins have to be considered, i.e., triplet-triplet annihilation and recombination of geminate electron-hole pairs. Ph-PPV is investigated in the form of two different samples, namely diluted in 2-methyltetrahydrofuran (MTHF) glass at 80 K and as a thin film of optical density of 0.6. It will be shown that in the diluted solution, delayed fluorescence is due to triplet-triplet annihilation and in the thin film, it is due to geminate pair recombination. The assignment of delayed fluorescence to geminate pair recombination in the thin film could be made due to delayed fluorescence experiments under applying an electric field of 2 × 10[SUP6] V/cm. The delayed fluorescence is strongly influenced by the electric field which is a sign that charged species, i.e., geminate electron-hole pairs, are involved in the process of delayed fluorescence. [ABSTRACT FROM AUTHOR]

The effect of permanent dipoles on the density-of-states (DOS) function of an array of hopping sites is examined by summing the contributions of individual dipoles to the total potential at a given site. For relative dipolar site concentrations >=0.1, the DOS function is of Gaussian shape. At lower concentrations, it approaches a Lorentzian. Good agreement with literature data on the dipolar contribution to the DOS function for hole transport in molecularly doped polymers and molecular glasses differing with regard to dipole moment and concentration of dipolar moieties is found. [ABSTRACT FROM AUTHOR]

The field and temperature dependencies of the hole mobility of 1,1-bis(di-4-tolylaminophenyl)cyclohexane (TAPC) doped polystyrene have been measured and compared to results obtained for the TAPC doped polycarbonate and pure TAPC. The results are described by the disorder formalism, due to Bässler and co-workers. The mobility of TAPC doped polystyrene is approximately 100-fold greater than that observed for TAPC doped polycarbonate. This effect is interpreted in terms of (1) the elimination of random dipolar fields due to static dipole moments of the polycarbonate that affect the energetic disorder, and (2) improved electronic intermolecular coupling with a concomitant reduction of positional disorder. [ABSTRACT FROM AUTHOR]