Spin-Forster transfer in optically excited quantum dots

The mechanisms of energy and spin transfer in quantum dot pairs coupled via the Coulomb interaction are studied. Exciton transfer can be resonant or phonon-assisted. In both cases, the transfer rates strongly depend on the resonance conditions. The spin selection rules in the transfer process come from the exchange and spin-orbit interactions. The character of energy dissipation in spin transfer is different than that in the traditional spin currents. The spin-dependent photon cross-correlation functions reflect the exciton transfer process. In addition, a mathematical method to calculate F\"orster transfer in crystalline nanostructures beyond the dipole-dipole approximation is described.Comment: 22 pages, 10 figures, Phys. Rev. B, in pres

Nonmonotonic energy harvesting efficiency in biased exciton chains

We theoretically study the efficiency of energy harvesting in linear exciton chains with an energy bias, where the initial excitation is taking place at the high-energy end of the chain and the energy is harvested (trapped) at the other end. The efficiency is characterized by means of the average time for the exciton to be trapped after the initial excitation. The exciton transport is treated as the intraband energy relaxation over the states obtained by numerically diagonalizing the Frenkel Hamiltonian that corresponds to the biased chain. The relevant intraband scattering rates are obtained from a linear exciton-phonon interaction. Numerical solution of the Pauli master equation that describes the relaxation and trapping processes, reveals a complicated interplay of factors that determine the overall harvesting efficiency. Specifically, if the trapping step is slower than or comparable to the intraband relaxation, this efficiency shows a nonmonotonic dependence on the bias: it first increases when introducing a bias, reaches a maximum at an optimal bias value, and then decreases again because of dynamic (Bloch) localization of the exciton states. Effects of on-site (diagonal) disorder, leading to Anderson localization, are addressed as well.Comment: 9 pages, 6 figures, to appear in Journal of Chemical Physic

Optical properties of coupled metal-semiconductor and metal-molecule nanocrystal complexes: the role of multipole effects

We investigate theoretically the effects of interaction between an optical dipole (semiconductor quantum dot or molecule) and metal nanoparticles. The calculated absorption spectra of hybrid structures demonstrate strong effects of interference coming from the exciton-plasmon coupling. In particular, the absorption spectra acquire characteristic asymmetric lineshapes and strong anti-resonances. We present here an exact solution of the problem beyond the dipole approximation and find that the multipole treatment of the interaction is crucial for the understanding of strongly-interacting exciton-plasmon nano-systems. Interestingly, the visibility of the exciton resonance becomes greatly enhanced for small inter-particle distances due to the interference phenomenon, multipole effects, and electromagnetic enhancement. We find that the destructive interference is particularly strong. Using our exact theory, we show that the interference effects can be observed experimentally even in the exciting systems at room temperature.Comment: 9 page

Exactly soluble model of resonant energy transfer between molecules

F\"orster's theory of resonant energy transfer (FRET) predicts the strength and range of exciton transport between separated molecules. We introduce an exactly soluble model for FRET which reproduces F\"orster's results as well as incorporating quantum coherence effects. As an application the model is used to analyze a system composed of quantum dots and the protein bacteriorhodopsin.Comment: 10 pages, 2 figure

Theory of Exciton Migration and Field-Induced Dissociation in Conjugated Polymers

The interplay of migration, recombination, and dissociation of excitons in disordered media is studied theoretically in the low temperature regime. An exact expression for the photoluminescence spectrum is obtained. The theory is applied to describe the electric field-induced photoluminescence-quenching experiments by Kersting et al. [Phys. Rev. Lett. 73, 1440 (1994)] and Deussen et al. [Synth. Met. 73, 123 (1995)] on conjugated polymer systems. Good agreement with experiment is obtained using an on-chain dissociation mechanism, which implies a separation of the electron-hole pair along the polymer chain.Comment: 4 pages, RevTeX, 2 Postscript figure

Theory of Electric Field-Induced Photoluminescence Quenching in Disordered Molecular Solids

The dynamics of excitons in disordered molecular solids is studied theoretically, taking into account migration between different sites, recombination, and dissociation into free charge carriers in the presence of an electric field. The theory is applied to interpret the results of electric field-induced photoluminescence (PL) quenching experiments on molecularly doped polymers by Deussen et al. [Chem. Phys. 207, 147 (1996)]. Using an intermolecular dissociation mechanism, the dependence of the PL quenching on the electric field strength and the dopant concentration, and the time evolution of the transient PL quenching can be well described. The results constitute additional proof of the distinct exciton dissociation mechanisms in conjugated polymer blends and molecularly doped polymers.Comment: 4 pages RevTeX, 3 Postscript figure

Theory of plasmon-enhanced Foerster energy transfer in optically-excited semiconductor and metal nanoparticles

We describe the process of Foerster transfer between semiconductor nanoparticles in the presence of a metal subsystem (metal nanocrystals). In the presence of metal nanocrystals, the Foerster process can become faster and more long-range. The enhancement of Foerster transfer occurs due to the effect of plasmon-assisted amplification of electric fields inside the nanoscale assembly. Simultaneously, metal nanocrystals lead to an increase of energy losses during the Foerster transfer process. We derive convenient equations for the energy transfer rates, photoluminescence intensities, and energy dissipation rates in the please of plasmon resonances. Because of strong dissipation due to the metal, an experimental observation of plasmon-enhanced Foerster transfer requires special conditions. As possible experimental methods, we consider cw- and time-resolved photoluminescence studies and describe the conditions to observe plasmon-enhanced transfer. In particular, we show that the photoluminescence spectra should be carefully analyzed since the plasmon-enhanced Foerster effect can appear together with strong exciton energy dissipation. Our results can be applied to a variety of experimental nanoscale systems.Comment: 60 page

Ge-modified Si(100) substrates for the growth of 3C-SiC (100)

An alternative route to improve the epitaxial growth of 3C-SiC (100) on Si(100) was developed. It consists in covering the silicon wafers with germanium prior to the carbonization step of the silicon substrate. Transmission electron microscopy and μ -Raman investigations revealed an improvement in the residual strain and crystalline quality of the grown 3C-SiC layers comparable to or better than in the case of 3C-SiC grown on silicon on insulator substrates. These beneficial effects were reached by using a Ge coverage in the range of 0.5-1 monolayer