Excitation energy transfer between closely spaced multichromophoric systems: Effects of band mixing and intraband relaxation

We theoretically analyze the excitation energy transfer between two closely spaced linear molecular J-aggregates, whose excited states are Frenkel excitons. The aggregate with the higher (lower) exciton band edge energy is considered as the donor (acceptor). The celebrated theory of F\"orster resonance energy transfer (FRET), which relates the transfer rate to the overlap integral of optical spectra, fails in this situation. We point out that in addition to the well-known fact that the point-dipole approximation breaks down (enabling energy transfer between optically forbidden states), also the perturbative treatment of the electronic interactions between donor and acceptor system, which underlies the F\"orster approach, in general loses its validity due to overlap of the exciton bands. We therefore propose a nonperturbative method, in which donor and acceptor bands are mixed and the energy transfer is described in terms of a phonon-assisted energy relaxation process between the two new (renormalized) bands. The validity of the conventional perturbative approach is investigated by comparing to the nonperturbative one; in general this validity improves for lower temperature and larger distances (weaker interactions) between the aggregates. We also demonstrate that the interference between intraband relaxation and energy transfer renders the proper definition of the transfer rate and its evaluation from experiment a complicated issue, which involves the initial excitation condition.Comment: 13 pages, 6 PostScript figure

Low-temperature dynamics of weakly localized Frenkel excitons in disordered linar chains

We calculate the temperature dependence of the fluorescence Stokes shift and the fluorescence decay time in linear Frenkel exciton systems resulting from the thermal redistribution of exciton population over the band states. The following factors, relevant to common experimental conditions, are accounted for in our kinetic model: (weak) localization of the exciton states by static disorder, coupling of the localized excitons to vibrations in the host medium, a possible non-equilibrium of the subsystem of localized Frenkel excitons on the time scale of the emission process, and different excitation conditions (resonant or non resonant). A Pauli master equation, with microscopically calculated transition rates, is used to describe the redistribution of the exciton population over the manifold of localized exciton states. We find a counterintuitive non-monotonic temperature dependence of the Stokes shift. In addition, we show that depending on experimental conditions, the observed fluorescence decay time may be determined by vibration-induced intra-band relaxation, rather than radiative relaxation to the ground state. The model considered has relevance to a wide variety of materials, such as linear molecular aggregates, conjugated polymers, and polysilanes.Comment: 15 pages, 8 figure

Trapping time statistics and efficiency of transport of optical excitations in dendrimers

We theoretically study the trapping time distribution and the efficiency of the excitation energy transport in dendritic systems. Trapping of excitations, created at the periphery of the dendrimer, on a trap located at its core, is used as a probe of the efficiency of the energy transport across the dendrimer. The transport process is treated as incoherent hopping of excitations between nearest-neighbor dendrimer units and is described using a rate equation. We account for radiative and non-radiative decay of the excitations while diffusing across the dendrimer. We derive exact expressions for the Laplace transform of the trapping time distribution and the efficiency of trapping and analyze those for various realizations of the energy bias, number of dendrimer generations, and relative rates for decay and hopping. We show that the essential parameter that governs the trapping efficiency, is the product of the on-site excitation decay rate and the trapping time (mean first passage time) in the absence of decay.Comment: 26 pages, 6 figure

Time-dependent transport of a localized surface plasmon through a linear array of metal nanoparticles: Precursor and normal mode contributions

We theoretically investigate the time-dependent transport of a localized surface plasmon excitation through a linear array of identical and equidistantly spaced metal nanoparticles. Two different signals propagating through the array are found: one traveling with the group velocity of the surface plasmon polaritons of the system and damped exponentially, and the other running with the speed of light and decaying in a power-~law fashion, as $x^{-1}$ and $x^{-2}$ for the transversal and longitudinal polarizations, respectively. The latter resembles the Sommerfeld-Brillouin forerunner and has not been identified in previous studies. The contribution of this signal dominates the plasmon transport at large distances. In addition, even though this signal is spread in the propagation direction and has the lateral dimension larger than the wavelength, the field profile close to the chain axis does not change with distance, indicating that this part of the signal is confined to the array.Comment: 13 pages, 10 figures, to be published in PR

Phenomenology of current-skyrmion interactions in thin films with perpendicular magnetic anisotropy

We study skyrmions in magnetic thin films with structural inversion asymmetry perpendicular to the film plane. We determine the magnetization texture of a single skyrmion and its dependence on the strength of the Dzyaloshinskii-Moriya interaction relative to the magnetostatic energy. Furthermore, we construct a phenomenological model that describes the interaction between the motion of skyrmions and electric currents to lowest order in spin-orbit coupling. We estimate the experimental verifiable velocities for current-driven motion of skyrmion textures based on available results obtained from domain walls dynamics

Localization properties of one-dimensional Frenkel excitons: Gaussian versus Lorentzian diagonal disorder

We compare localization properties of one-dimensional Frenkel excitons with Gaussian and Lorentzian uncorrelated diagonal disorder. We focus on the states of the Lifshits tail, which dominate the optical response and low-temperature energy transport in molecular J-aggregates. The absence of exchange narrowing in chains with Lorentzian disorder is shown to manifest itself in the disorder scaling of the localization length distribution. Also, we show that the local exciton level structure of the Lifshits tail differs substantially for these two types of disorder: In addition to the singlets and doublets of localized states near the bare band edge, strongly resembling those found for Gaussian disorder, for Lorentzian disorder two other types of states are found in this energy region as well, namely multiplets of three or four states localized on the same chain segment and isolated states localized on short segments. Finally, below the Lifshits tail, Lorentzian disorder induces strongly localized exciton states, centered around low energy sites, with localization properties that strongly depend on energy. For Gaussian disorder with a magnitude that does not exceed the exciton bandwidth, the likelihood to find such very deep states is exponentially small.Comment: 9 two-column pages, 4 figures, to appear in Phys. Rev.

Tailoring optical response of a hybrid comprising a quantum dimer emitter strongly coupled to a metal nanoparticle

We study theoretically the optical response of a nanohybrid comprising a symmetric quantum dimer emitter coupled to a metal nanoparticle (MNP). The interactions between the exitonic transitions in the dimer and the plasmons in the MNP lead to novel effects in the composite's input-output characteristics for the light intensity and the absorption spectrum, which we study in the linear and nonlinear regimes. We fnd that the exciton-plasmon hybridization leads to optical bistability and hysteresis for the one-exciton transition and enhancement of excitation for the two-exciton transition. The latter leads to a signifcant decrease of the field strength needed to saturate the system. In the linear regime, the absortion spectrum has a dispersive (Fano-like) line shape. The spectral position and shape of this spectrum depend on the detuning of the dimer's one-exciton resonance relative to the plasmon resonance. Upon increasing the applied field intensity to the nonlinear regime, the Fano-like singularities in the absorption spectra are smeared and they disappear due to the saturation of the dimer, which leads to the MNP dominating the spectrum. The above effects, for which we provide physical explanations, allow one to tailor the Fano-like shape of the absorption spectrum, by changing either the detuning or the input power

Excitons in Molecular Aggregates with L\'evy Disorder: Anomalous Localization and Exchange Broadening of Optical Spectra

We predict the existence of exchange broadening of optical lineshapes in disordered molecular aggregates and a nonuniversal disorder scaling of the localization characteristics of the collective electronic excitations (excitons). These phenomena occur for heavy-tailed L\'evy disorder distributions with divergent second moments - distributions that play a role in many branches of physics. Our results sharply contrast with aggregate models commonly analyzed, where the second moment is finite. They bear a relevance for other types of collective excitations as well

Plasmon-assisted two-photon Rabi oscillations in a semiconductor quantum dot -- metal nanoparticle heterodimer

Tho-photon Rabi oscillations hold potential for quantum computing and quantum information processing, because during a Rabi cycle a pair of entangled photons may be created. We theoretically investigate the onset of this phenomenon in a heterodimer comprising a semiconductor quantum dot strongly coupled to a metal nanoparticle. Two-photon Rabi oscillations in this system occur due to a coherent two-photon process involving the ground-to-biexciton transition in the quantum dot. The presence of a metal nanoparticle nearby the quantum dot results in a self-action of the quantum dot via the metal nanoparticle, because the polatization state of the latter depends on the quantum state of the former. The interparticle interaction gives rise to two principal effects: (i) - enhancement of the external field amplitude and (ii) - renormalization of the quantum dot's resonance frequencies and relaxation rates of the off-diagonal density matrix elements, both depending on the populations of the quantum dot's levels. Here, we focus on the first effect, which results in interesting new features, in particular, in an increased number of Rabi cycles per pulse as compared to an isolated quantum dot and subsequent growth of the number of entangled photon pairs per pulse. We also discuss the destructive role of radiative decay of the excitonic states on two-photon Rabi oscillations for both an isolated quantum dot and a heterodimer.Comment: 11 pages, 19 figure