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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 PRB

We present a detailed study of the effects of L\'evy $\alpha$-stable disorder distributions on the optical and localization properties of excitonic systems. These distributions are a generalization of commonly studied Gaussian randomness ($\alpha = 2$). However, the more general case ($\alpha < 2$) includes also heavy-tailed behavior with a divergent second moment. These types of distributions give rise to novel effects, such as exchange broadening of the absorption spectra and anomalous localization of the excitonic states, which has been found in various excitonic systems. We provide a thorough examination of the localization behavior and the absorption spectra of excitons in chains with L\'evy $\alpha$-stable diagonal disorder. Several regimes are considered in detail: (i) weak disorder and small systems, where finite size effects become significant; (ii) intermediate disorder and/or larger systems for which exciton states around the exciton band edge spread over a number of monomers, and (iii) strong disorder where the exciton wave functions resemble the individual molecular states. We propose analytical approaches to describe the disorder scaling of relevant quantities for these three regimes of localization, which match excellently with numerical results. We also show the appearance of short localization segments caused by outliers (monomers having transition energies larger than the exciton band width). Such states give rise to an additional structure in the absorption spectrum, density of states, and in the nontrivial disorder scaling of the absorption band width.

In previous work, we have predicted novel effects, such as exchange broadening, anomalous scaling of the localization length and a blue shift of the absorption spectrum with increasing disorder strength, for static disorder models described by stable distributions with stability index {\alpha}<1. The main points of the Comment are that the outliers introduced by heavy tails in the disorder distribution (i) do not lead to deviations from the conventional scaling law for the half width at half maximum (HWHM) of the absorption spectrum and (ii) do not lead to non-universality of the distribution of localization lengths. We show below that the findings reported by us in the Letter are correct and that the wrong conclusions of the Comment arise from focusing on small {\sigma} values., Comment: Based on our response submitted to Physical Review Letters on January 20, 2012. We now also take into account the modifications made to the Comment upon resubmission of the Comment. The Reply has been accepted in Physical Review Letters

We conduct a theoretical study of the bistable optical response of a nanoparticle heterodimer comprised of a closely spaced semiconductor quantum dot and metal nanoparticle. The bistable nature of the response results from the interplay between the quantum dot's optical nonlinearity and its self-action (feedback) originating from the presence of the metal nanoparticle. We show that the feedback is governed by a complex valued coupling parameter $G$. Both the real and imaginary parts of $G$ ($G_\mathrm{R}$ and $G_\mathrm{I}$) play an important role in the occurrence of bistability, which is manifested in an S-shaped dependence of the quantum dot excited state population on the intensity of the external field, and hysteresis of the population. From our calculations, we find that at $G_\mathrm{R} = 0$, the critical value for bistability to occur is $G_\mathrm{I} = 8\Gamma$, whereas at $G_\mathrm{I} = 0$, the critical value of $G_\mathrm{R} = 4\Gamma$, where $\Gamma$ is the polarization dephasing rate. Thus, there exist two different (limiting) mechanisms of bistability, depending on whether $G_\mathrm{R}$ is much larger or much smaller than $G_\mathrm{I}$. We also calculate the bistability phase diagram within the system's parameter space: spanned by $G_\mathrm{R}$, $G_\mathrm{I}$ and $\Delta$, the latter being the detuning between the driving frequency and the transition frequency of the quantum dot. Additionally, switching times from the lower stable branch to the upper one (and {\it vise versa}) are calculated as a function of the intensity of the driving field. We show that the conditions for bistability to occur can be realized, for example, for a heterodimer comprised of a closely spaced CdSe (or CdSe/ZnSe) quantum dot and a gold nanosphere., Comment: 9 pages, 6 figures

We show that interference can be the principle of operation of an all-optical switch and other nanoscale plasmonic interference devices (PIDs). The optical response of two types of planar plasmonic waveguides is studied theoretically: bent chains and Y-shaped configurations of closely-spaced metallic nanospheres. We study symmetric Y-shape arrays as an example of an all-optical switch and demonstrate that effective phase- and amplitude-sensitive control of the output signal can be achieved due to interference effects., Comment: 4 pages, 5 figures, reported at The 2nd European Topical Meeting on Nanophotonics and Metamaterials (Nanometa), Seefeld, Austria, January 5-9, 2009

The local distribution of exciton levels in disordered cyanine-dye-based molecular nano-aggregates has been elucidated using fluorescence line narrowing spectroscopy. The observation of a Wigner-Dyson-type level spacing distribution provides direct evidence of the existence of level repulsion of strongly overlapping states in the molecular wires, which is important for the understanding of the level statistics, and therefore the `functional properties, of a large variety of nano-confined systems., Comment: 6 pages, 5 figures

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.

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. B

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 Physics

The study of energy harvesting in chain-like structures is important due to its relevance to a variety of interesting physical systems. Harvesting is understood as the combination of exciton transport through intra-band exciton relaxation (via scattering on phonon modes) and subsequent quenching by a trap. Previously, we have shown that in the low temperature limit different harvesting scenarios as a function of the applied bias strength (slope of the energy gradient towards the trap) are possible \cite{Vlaming07}. This paper generalizes the results for both homogeneous and disordered chains to nonzero temperatures. We show that thermal effects are appreciable only for low bias strengths, particularly so in disordered systems, and lead to faster harvesting., Comment: 8 pages, 2 fugures, to appear in Journal of Luminescence

We perform a theoretical study of the nonlinear optical response of an ultrathin film consisting of oriented linear aggregates. A single aggregate is described by a Frenkel exciton Hamiltonian with uncorrelated on-site disorder. The exciton wave functions and energies are found exactly by numerically diagonalizing the Hamiltonian. The principal restriction we impose is that only the optical transitions between the ground state and optically dominant states of the one-exciton manifold are considered, whereas transitions to other states, including those of higher exciton manifolds, are neglected. The optical dynamics of the system is treated within the framework of truncated optical Maxwell-Bloch equations in which the electric polarization is calculated by using a joint distribution of the transition frequency and the transition dipole moment of the optically dominant states. This function contains all the statistical information about these two quantities that govern the optical response, and is obtained numerically by sampling many disorder realizations. We derive a steady-state equation that establishes a relationship between the output and input intensities of the electric field and show that within a certain range of the parameter space this equation exhibits a three-valued solution for the output field. A time-domain analysis is employed to investigate the stability of different branches of the three-valued solutions and to get insight into switching times. We discuss the possibility to experimentally verify the bistable behavior., Comment: 13 two-column pages, 8 figures, accepted to the Journal of Chemical Physics

We show that the third-order optical response of disordered linear J-aggregates can be calculated by considering only a limited number of transitions between (multi-) exciton states. We calculate the pump-probe absorption spectrum resulting from the truncated set of transitions and show that, apart from the blue wing of the induced absorption peak, it agrees well with the exact spectrum., Comment: 8 pages, 2 figures, accepted to Journal of Luminescence

We argue that the time-resolved spectrum of selectively-excited resonance fluorescence at low temperature provides a tool for probing the quantum-mechanical level repulsion in the Lifshits tail of the electronic density of states in a wide variety of disordered materials. The technique, based on detecting the fast growth of a fluorescence peak that is red-shifted relative to the excitation frequency, is demonstrated explicitly by simulations on linear Frenkel exciton chains., Comment: 4 pages, 4 figures, to appear in Phys. Rev. Lett

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 figures

Using a model of Frenkel excitons coupled to a bath of acoustic phonons in the host medium, we study the temperature dependence of the dephasing rates and homogeneous line width in linear molecular aggregates. The model includes localization by disorder and predicts a power-law thermal scaling of the effective homogeneous line width. The theory gives excellent agreement with temperature dependent absorption and hole-burning experiments on aggregates of the dye pseudoisocyanine., Comment: 11 pages, 3 PostScript figures

We study the temperature-dependent dephasing rate of excitons in chains of chromophores, accounting for scattering on static disorder as well as acoustic phonons in the host matrix. From this we find a powerlaw temperature dependence of the absorption line width, in excellent quantitative agreement with experiments on dye aggregates. We also propose a relation between the line width and the exciton coherence length imposed by the phonons. The results indicate that the much debated steep rise of the fluorescence lifetime of pseudo-isocyanine aggregates above 40 K results from the fact that this coherence length drops below the localization length imposed by static disorder., Comment: 4 pages, 2 figures

We theoretically study the temperature dependence of the J-band width in disordered linear molecular aggregates, caused by dephasing of the exciton states due to scattering on vibrations of the host matrix. In particular, we consider inelastic one- and two-phonon scattering between different exciton states (energy-relaxation-induced dephasing), as well as elastic two-phonon scattering of the excitons (pure dephasing). The exciton states follow from numerical diagonalization of a Frenkel Hamiltonian with diagonal disorder; the scattering rates between them are obtained using the Fermi Golden Rule. A Debye-like model for the one- and two-phonon spectral densities is used in the calculations. We find that, owing to the disorder, the dephasing rates of the individual exciton states are distributed over a wide range of values. We also demonstrate that the dominant channel of two-phonon scattering is not the elastic one, as is often tacitly assumed, but rather comes from a similar two-phonon inelastic scattering process. In order to study the temperature dependence of the J-band width, we simulate the absorption spectrum, accounting for the dephasing induced broadening of the exciton states. We find a power-law (T^p) temperature scaling of the effective homogeneous width, with an exponent p that depends on the shape of the spectral density of host vibrations. In particular, for a Debye model of vibrations, we find p ~ 4, which is in good agreement with experimental data on J-aggregates of pseudoisocyanine [J. Phys. Chem. A 101, 7977 (1997)]., Comment: 14 pages, 7 figures

We study the linear optical properties of helical cylindrical molecular aggregates accounting for the effects of static diagonal disorder. Absorption, linear dichroism, and circular dichroism spectra are presented, calculated using brute force numerical simulations and a modified version of the coherent potential approximation that accounts for finite size effects. Excellent agreement between both approaches is found. It is also shown that the inclusion of disorder results in a better agreement between calculated and measured spectra for the chlorosomes of green bacteria as compared to our previous report, where we restricted ourselves to homogeneous cylinders [J. Phys. Chem. B 106, 11474 (2002)]. We also investigate the localization properties of the excitons responsible for the optical response. By analyzing an autocorrelation function of the exciton wave function, we find a strongly anisotropic localization behavior, closely following the properties of chiral wave functions which previously have been found for homogenoeus helical cylinders [J. Chem. Phys. 121, 946 (2004)]. It is shown that the circular dichroism spectrum may still show a strong dependence on the cylinder length, even when the exciton wave function is localized in a region small compared to the cylinder's size., Comment: 14 pages, 7 figures, submitted to J. Chem. Phys

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 figures

We model the optical dynamics in linear Frenkel exciton systems governed by scattering on static disorder and lattice vibrations, and calculate the temperature dependent fluorescence spectrum and lifetime. The fluorescence Stokes shift shows a nonmonotonic behavior with temperature, which derives from the interplay of the local band-edge level structure and thermal equilibration. The model yields excellent fits to experiments performed on linear dye aggregates., Comment: 4 pages, 3 figures

We present results of numerical simulations of the kinetics of exciton-exciton annihilation of weakly localized one-dimensional Frenkel excitons at low temperatures. We find that the kinetics is represented by two well-distinguished components: a fast short-time decay and a very slow long-time tail. The former arises from excitons that initially reside in states belonging to the same localization segment of the chain, while the slow component is caused by excitons created on different localization segments. We show that the usual bi-molecular theory fails in the description of the behavior found. We also present a qualitative analytical explanation of the non-exponential behavior observed in both the short- and the long-time decay components., Comment: Published in J. Chem. Phys. 114, 1 April (2001)

We argue that in the quarter-filled ladder compound NaV_2O_5 the quasi-one-dimensional spin system is strongly coupled to a low-energy antiferroelectric mode of the excitonic type. This mode results from the interplay between the electron hopping along the rungs of the vanadium two-leg ladders and the Coulomb repulsion between electrons. The charge ordering observed in sodium vanadate at T_c = 34K corresponds to the softening of the antiferroelectric mode. We consider the spin-isospin model, which describes the spin and low-energy charge degrees of freedom in sodium vanadate. Within this model we explain the observed anomalous temperature-dependence of the dielectric susceptibility at T_c and the midinfrared absorption continuum. We identify the broad structure in the low-energy optical absorption spectrum of NaV_2O_5 with the continuum formed by two spinons and one low-energy charge excitation., Comment: 30 pages, 12 figures, submitted to Phys. Rev. B

We study the effects of weak off-diagonal disorder on Peierls systems with a doubly degenerate ground state. We show that for these systems disorder in the electron hopping amplitudes induces a finite density of solitons in the minimal-energy lattice configuration of a single chain. These disorder-induced dimerization kinks are neutral and have spin 1/2. Using a continuum model for the Peierls chain and treating the lattice classically, we analytically calculate the average free energy and density of kinks. We compare these results to numerical calculations for a discrete model and discuss the implications of the kinks for the optical and magnetic properties of the conjugated polymer trans-polyacetylene., Comment: 28 pages, revtex, 5 Postscript figures, to appear in Phys. Rev. B