Exciton transfer between localized states in ZnO quantum well structures

The dynamics of photocreated excitons in a CdZnO/MgZnO quantum well (QW) was studied by comparing the experimental photoluminescence (PL) data with the results of Monte Carlo simulations of the exciton hopping. The temperature-dependent PL linewidth was found to be in reasonable agreement with the model of exciton hopping, with an additional inhomogeneous broadening (Γ) accounted for. The simulation analysis revealed fluctuations of the band potential to be 20 meV with an additional inhomogeneous broadening of , and a crossover from a non-thermalized to thermalized exciton energy distribution at about 100 K. In addition, a Bose–Einstein distribution like temperature dependence of the exciton energy in the wells was extracted using the data on the PL peak position.     

Triplet exciton diffusion and phosphorescence quenching in iridium(III)-centered dendrimers

A study of triplet-triplet exciton annihilation and nonradiative decay in films of iridium(III)-centered phosphorescent dendrimers is reported. The average separation of the chromophore was tuned by the molecular structure and also by blending with a host material. It was found that triplet exciton hopping is controlled by electron exchange interactions and can be over 600 times faster than phosphorescence quenching. Nonradiative decay occurs by weak dipole-dipole interactions and is independent of exciton diffusion, except in very thin films (<20 nm) where surface quenching dominates the decay.     

Time-resolved luminescence quenching in thin films of perylene-tetracarboxylic-dianhydride

We present luminescence quenching experiments and determine the exciton diffusion length in polycrystalline thin films of PTCDA (perylene-3,4,9,10-tetracarboxylic-dianhydride). From an analysis of time-resolved experiments, we can distinguish between exciton transport during an ultra-fast initial relaxation phase and transport in the long-living emitting states. The temperature dependence of the exciton diffusion constant in the emitting states indicates thermally activated hopping.     

Localized exciton dynamics in AlInGaN alloy

Carrier recombination dynamics in AlInGaN alloy has been studied by photoluminescence (PL) and time-resolved PL (TRPL) at various temperatures. The fast red-shift of PL peak energy is observed and well fitted by a physical model considering the thermal activation and transfer processes. This result provides evidence for the exciton localization in the quantum dot (QD)-like potentials in our AlInGaN alloy. The TRPL signals are found to be described by a stretched exponential function of exp[(−t/τ)^β], indicating the presence of a significant disorder in the material. The disorder is attributed to a randomly distributed QDs or clusters caused by indium fluctuations. By studying the dependence of the dispersive exponent β on temperature and emission energy, we suggest that the exciton hopping dominate the diffusion of carriers localized in the disordered QDs. Furthermore, the localized states are found to have 0D density of states up to 250 K, since the radiative lifetime remains almost unchanged with increasing temperature.     

The influence of exciton motion on spin-resonance absorption

We use a stochastic model for the exciton motion which comprises both the coherent and the incoherent motion. The incoherent part is taken care of by a stochastic process which allows the local excitation energy and the transition matrix element to fluctuate by means of a Markovian process. The interaction between the spins and their surroundings is described by the usual spin-Hamiltonian which is, however, simplified to a spin 1/2 particle (instead of the triplet state). In the present paper we solve exactly the two limiting cases of completely coherent and incoherent motion (for two molecules). In the incoherent case the influence of the exchange interaction integral is taken into account by perturbation theory. We find expressions which are immediately comparable with ESR-experimental data. This comparison and additional information derived from optical absorption measurements allow us to determine all free parameters of our model uniquely. In particular, the fluctuations of the exchange interaction integral (with strength γ₁) play an important role. From these parameters we may furthermore calculate the correlation time of the proton spin resonance in agreement with experimental data. The results show clearly that at room temperature in anthracene crystals the exciton undergoes a hopping process.     

Exciton condensation in coupled quantum wells

Bound electron-hole pairs—excitons—are Bose particles with small mass. Exciton Bose-Einstein condensation is expected to occur at a few degrees Kelvin—a temperature many orders of magnitude higher than for atoms. Experimentally, an exciton temperature well below 1 K is achieved in coupled quantum well (CQW) semiconductor nanostructures. In this contribution, we review briefly experiments that signal exciton condensation in CQWs: a strong enhancement of the indirect exciton mobility consistent with the onset of exciton superfluidity, a strong enhancement of the radiative decay rate of the indirect excitons consistent with exciton condensate superradiance, strong fluctuations of the indirect exciton emission consistent with critical fluctuations near the phase transition, and a strong enhancement of the exciton scattering rate with increasing concentration of the indirect excitons revealing bosonic stimulation of exciton scattering. Novel experiments with exciton condensation in potential traps, pattern formation in exciton system and macroscopically ordered exciton state will also be reviewed briefly.     

Effect of localized-exciton energy relaxation on the emission spectrum of ZnS-ZnSe single quantum wells

A study is reported on the dependence of exciton photoluminescence spectra of ZnS-ZnSe quantum wells with different localization-center concentrations on the excitation intensity and temperature. The shape of the experimental low-temperature photoluminescence band is shown to agree well with that calculated in a model of exciton hopping to the nearest localization center and in one that takes into account transitions of a localized exciton to all centers in its local environment. The parameters characterizing localized excitons in these quantum structures of a submonolayer thickness have been determined.     

Coherent and incoherent exciton motion in the framework of the continuous time random walk

We derive the hopping time distribution functions of the continuous time random walk theory starting from an exact kernel for one-dimensional exciton motion. The derivation is based on exact relations between the kernel and the hopping time distribution functions.     

Exact Propagators for Exciton Motion on a Chain with Alternating Site Energies or Intersite Interactions

The exciton motion on a chain with alternating site energies (model A) or intersite interactions (model B) is studied analytically. Exact solutions for the amplitude propagators in two systems are obtained explicitly, from which the effects of the site-energy mismatch and the hopping disturbance on the diffusing behavior of the moving exciton are displayed. The symmetry properties for the amplitude propagators in the real space are also given.     

An exactly solvable model for coherent and incoherent exciton motion

We treat the motion of a Frenkel exciton using a Hamiltonian which comprises a completely coherent part and a fluctuating part which describes both fluctuations of the energy of a localized exciton and fluctuations of the transition matrix elements between different lattice sites. Under the assumption that the fluctuating forces are Markoffian and Gaussian we derive exactly a density matrix equation which can be solved by a Green's function method.     

Sensitive linear response of an electron-hole superfluid in a periodic potential

We consider excitons in a two-dimensional periodic potential and study the linear response of the excitonic superfluid to an electromagnetic wave at low and high densities. It turns out that the static structure factor for small wavevectors is very sensitive to a change of density and temperature. It is a consequence of the fact that thermal fluctuations play a crucial role at small wavevectors, since exchanging the order of the two limits, zero temperature and vanishing wavevector, leads to different results for the structure factor. This effect could be used for high accuracy measurements in the superfluid exciton phase, which might be realized by a gated electron-hole gas, for instance, in coupled quantum wells or double layer materials. The transition of the exciton system from the superfluid state to a non-superfluid state and its manifestation by light scattering are discussed.     

A theory of exciton dynamics with a percolation threshold

Mode-coupling methods are used to obtain an integral equation for the exciton diffusion constant in isotopically mixed crystals. Numerical solutions are obtained for nearest neighbor hopping in one- and two-dimensional square lattices. These solutions exhibit percolation thresholds.Supported by NSF Grant CHE78-09704.     

Exciton and biexciton fine structure in single elongated islands grown on a vicinal surface

We report a microphotoluminescence study of the exciton and the biexciton localized in very elongated islands formed by well-width fluctuations in a thin CdTe/CdMgTe quantum well grown on a vicinal surface. The electron-hole exchange interaction in a local reduced symmetry splits the exciton states. The resulting transitions are linearly polarized along the two orthogonal principal axes of the island. The valence band mixing induced by the elongated shape of the potential leads to a strong polarization anisotropy and to the observation of dark exciton states under magnetic field. The biexciton-exciton transition reproduces all the fine structure of the exciton state including the transition of the biexciton to the dark exciton state.     

Optical excitations in hexagonal nanonetwork materials

Optical excitations in hexagonal nanonetwork materials, for example, Boron-Nitride (BN) sheets and nanotubes, are investigated theoretically. Exciton dipoles directed from the B site to the N site are considered along the BN bond. When the exciton hopping integral is restricted to the nearest neighbors, two flat bands of excitons appear. The symmetry of these exciton bands is optically forbidden. Possible relations to experiment are discussed.     

Resonant Rayleigh scattering from excitons in CdxZn1−xTe:ZnTe quantum wells: measurement of homogeneous linewidths

The technique of resonant Rayleigh scattering is used to determine the homogeneous linewidth across the inhomogeneously broadened exciton resonance in a Cd_0.25Zn_0.75Te/ZnTe multiple quantum well structure. An order of magnitude increase of the Rayleigh scattering signal over background is observed on tuning a narrow-band laser through the exciton resonance at low temperatures. Spectral and temporal measurements show the effect to be a true scattering process rather than luminescence. The interface and alloy fluctuations in the quantum well give rise to spatial fluctuations in the dielectric response of the system while the large exciton resonance causes strong enhancement of scattering. The homogeneous linewidth was calculated across the exciton resonance. The technique is compared with the dephasing and hole-burning techniques more commonly used in homogeneous linewidth measurements.     

Transport and recombination in organic light-emitting diodes studied by electrically detected magnetic resonance

We have used electrically detected magnetic resonance (EDMR) to study a series of multilayer organic devices based on aluminum (III) 8-hydroxyquinoline (Alq₃). These devices were designed to identify the microscopic origin of different spin-dependent processes, i.e. hopping and exciton formation. The EDMR signal in organic light-emitting diodes (OLEDs) based on Alq₃ is only observed when the device is electroluminescent and is assigned to spin-dependent exciton formation. It can be decomposed in at least two Gaussians: one with peak-to-peak line ( ΔH_PP) of 1.6 mT and another with ΔH_PP of 2.0 to 3.4 mT, depending on bias and temperature. The g-factors of the two components are barely distinguishable and close to 2.003. The broad line is attributed to the resonance in Alq₃ anions, while the other line is attributed to cationic states. These attributions are supported by line shape and its electrical-field dependence of unipolar Alq₃-based diodes, where hopping process related to dication and dianion formation is observed. In these unipolar devices, it is shown that the signal coming from spin-dependent hopping occurs close to organic semiconductor/metal interfaces. The sign of the magnetic-resonance-induced conductivity change is dominated by charge injection rather than charge mobility. Our results indicate that the probability of singlet exciton formation in our OLEDs is smaller than 25%.     

Ultrafast relaxation in quasi-one-dimensional organic molecular crystals

We present a comprehensive study of ultrafast relaxation properties of optical excitations in thin films of quasi-1D stacked organic materials PTCDA (3,4,9,10-perylenetetracarboxylic dianhydride) and MePTCDI (N,N'-dimethylperylene-3,4,9,10-dicarboximide) over five decades of time. Pump-probe experiments reveal excitonic intraband relaxation time constants of 65 fs for MePTCDI and 100 fs for PTCDA. The initial time-resolved luminescence anisotropy is consistent with the exciton model of Davydov-split states. The subsequent decay of the anisotropy can be explained with a thermally activated exciton hopping process. A full understanding of the pump-probe experiments calls for an explanation beyond the models presently available.     

Statistical properties of Lyapunov exponents and of quantum conductance of random systems in the regime of hopping transport

The statistics of the zero-temperature conductance and the Lyapunov exponents of one-, two- and three-dimensional disordered systems in the regime of strong localization is studied numerically. In one dimension, the origin of the universality of the moments of the conductance is explained. The relation between the most probable value of the conductance and its configurational average is discussed. The relative fluctuations of the conductance (and of the resistance) are shown to grow exponentially with the system length. In higher dimensions the conductance is almost entirely determined by the smallest of the Lyapunov exponents. The statistics of the conductance is therefore the same as in the one dimensional case. A model is proposed for the treatment of the fluctuations in hopping transport at finite temperatures. An exponential dependence of the relative fluctuations of the conductance/resistance on the temperature is predicted, log (δg/g) ∞ T^?a with α = 1/(d+1). It is concluded that the presently available experimental data on the temperature dependence of the conductance fluctuations in the hopping regime can be understood by replacing the system size in the zerotemperature result for the fluctuations of the conductance by the hopping length.     

Energy Transfer and Trapping in Rigid Solutions of Aromatic Polymers

Energy transfer by excitons is now well established in films and solutions of aromatic polymers. Excitons in disordered systems can be considered as electronically excited states, which are transferred between the light absorbing groups in a random hopping process (the same is true in molecular crystals if, because of thermal vibrations, the coherence length of the exciton waves approaches the lattice constant and consequently the band model of the excitons breaks down).