Pulsed magnetic field generation system for laser-plasma research.

An up to 15 T pulsed magnetic field generator in a volume of a few cubic centimeters has been developed for experiments with magnetized laser plasma. The magnetic field is created by a pair of coils placed in a sealed reservoir with liquid nitrogen, installed in a vacuum chamber with a laser target. The bearing body provides the mechanical strength of the system both in the case of co-directional and oppositely connected coils. The configuration of the housing allows laser radiation to be introduced into the working area between the coils in a wide range of directions and focusing angles, places targets away from the symmetry axis of the magnetic system, and irradiates several targets simultaneously.

Signature of anomalous exciton localization in the optical response of self-assembled organic nanotubes.

We show that the disorder scaling of the low-temperature optical absorption linewidth of tubular molecular assemblies sharply contrasts with that known for one-dimensional aggregates. The difference can be explained by an anomalous localization of excitons, which arises from the combination of long-range intermolecular interactions and the tube's higher-dimensional geometry. As a result, the exciton density of states near the band bottom drops to zero, leading to a strong suppression of exciton localization. Our results explain the strong linear dichroism and weak exciton-exciton scattering in tubular J aggregates observed in experiments and suggest that for nanoscale wirelike applications a tubular shape is to be preferred over a truly one-dimensional chain.

Subdiffusive exciton motion in systems with heavy-tailed disorder.

We study the transport of collective excitations (Frenkel excitons) in systems with static disorder in the transition energies, not limiting ourselves to Gaussian transition energy distributions. Instead, we generalize this model to the wider class of Lévy stable distributions, characterized by heavy tails. Phonon-assisted scattering of excitons, localized by the disorder, leads to thermally activated exciton motion. The time evolution of the second moment of the exciton distribution is shown to be sublinear, thus indicating that the exciton dynamics in such systems is not diffusive, but rather subdiffusive instead. The heavier the tail in the transition energy distribution is, the larger are the deviations from the diffusive regime. This from fluctuations of site energies larger than the exciton band width (outliers). We show that the occurrence of subdiffusive transport for heavy-tailed disorder distributions can be understood from the scattering rate distributions, which possess a (second) peak at zero scattering rate.

Optical nanoantennas with tunable radiation patterns.

We address new optical nanoantenna systems with tunable highly directional radiation patterns. The antenna comprises a regular linear array of metal nanoparticles in the proximity of an interface with high dielectric contrast. We show that the radiation pattern of the system can be controlled by changing parameters of the excitation, such as the polarization and/or incidence angles. In the case of excitation under the total reflection condition, the system operates as a nanoscopic source of radiation, converting the macroscopic incident plane wavefront into a narrow beam of light with adjustable characteristics. We derive also simple analytical formulas which give an excellent description of the radiation pattern and provide a useful tool for analysis and antenna design.

Excitons in molecular aggregates with Lévy-type disorder: anomalous localization and exchange broadening of optical spectra.

We predict the existence of exchange broadening of optical line shapes 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 Lévy 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.

Effects of the environment on the electric conductivity of double-stranded DNA molecules.

We present a theoretical analysis of the effects of the environment on charge transport in double-stranded synthetic poly(G)-poly(C) DNA molecules attached to two ideal leads. Coupling of the DNA to the environment results in two effects: (i) localization of carrier functions due to static disorder and (ii) phonon-induced scattering of the carriers between the localized states, resulting in hopping conductivity. A nonlinear Pauli master equation for populations of localized states is used to describe the hopping transport and calculate the electric current as a function of the applied bias. We demonstrate that, although the electronic gap in the density of states shrinks as the disorder increases, the voltage gap in the I-V characteristics becomes wider. A simple physical explanation of this effect is provided.

Frequency-controlled localization of optical signals in graded plasmonic chains.

We study theoretically the optical response of graded linear arrays of noble metal nanospheres in which the center-to-center distances and/or the radii of the spheres change linearly along the chain. A strong asymmetry of the system response with respect to the direction of incidence of the incoming light is revealed. We show that for light propagating from smaller to larger spheres the optical signal can be localized in a controlled way at an arbitrary subset of a few neighboring spheres by adjusting the wavelength of the incoming field. This opens new opportunities to control the flow of electromagnetic energy at the nanometer scale.

Scaling and universality in the optics of disordered exciton chains.

The joint probability distribution of exciton energies and transition dipole moments determines a variety of optical observables in disordered exciton systems. We demonstrate numerically that this distribution obeys a one-parameter scaling, originating from the fact that both the energy and the dipole moment are determined by the number of coherently bound molecules. A universal underlying distribution is found, which is identical for uncorrelated Gaussian disorder in the molecular transition energies or in the intermolecular transfer interactions. The universality breaks down for disorder in the transfer interactions resulting from variations in the molecular positions. We suggest the possibility to probe the joint distribution by means of single-molecule spectroscopy.

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.

Probing quantum-mechanical level repulsion in disordered systems by means of time-resolved selectively excited resonance fluorescence.

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 redshifted relative to the excitation frequency, is demonstrated explicitly by simulations on linear Frenkel exciton chains.

Temperature-dependent relaxation of excitons in tubular molecular aggregates: Fluorescence decay and stokes shift.

We report temperature-dependent steady-state and time-resolved fluorescence studies to probe the exciton dynamics in double-wall tubular J-aggregates formed by self-assembly of the dye 3,3'-bis(3-sulfopropyl)-5,5',6,6'-tetrachloro-1,1'-dioctylbenzimidacarbocyanine. We focus on the lowest energy fluorescence band, originating from the inner cylindrical wall. At low temperatures, the experiments reveal a nonexponential decay of the fluorescence, with a typical time scale that depends on the emission wavelength. At these temperatures we also find a dynamic Stokes shift of the fluorescence spectrum and its nonmonotonic dependence on temperature under steady-state conditions. All these data indicate that below about 20 K the excitons in the lowest fluorescence band do not reach thermal equilibrium before emission occurs, while above about 60 K thermalization on this time scale is complete. By comparing the two lowest fluorescence bands, we also find indications for fast energy transfer from the outer to the inner wall. We show that the Frenkel exciton model with diagonal disorder, which previously has been proposed to explain the absorption and linear dichroism spectra of these aggregates, yields a quantitative explanation to the observed dynamics. To this end, we extend the model to account for weak phonon-induced scattering of the localized exciton states; the spectral dynamics are then described by solving a Pauli master equation for the exciton populations.

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 Förster 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 Förster 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 that involves the initial excitation condition. Our results suggest that the best way of determining this transfer rate between two J-aggregates is to measure the fluorescence kinetics of the acceptor J-band after resonant excitation of the donor J-band.

Decoherence of excitons in multichromophore systems: thermal line broadening and destruction of superradiant emission.

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 power-law temperature dependence of the absorption linewidth, in excellent quantitative agreement with experiments on dye aggregates. We also propose a relation between the linewidth and the exciton coherence length imposed by the phonons. The results indicate that the much debated steep rise of the fluorescence lifetime of pseudoisocyanine aggregates above 40 K results from the fact that this coherence length drops below the localization length imposed by static disorder.

Thermal broadening of the J-band in disordered linear molecular aggregates: a theoretical study.

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 scatterings between different exciton states (energy-relaxation-induced dephasing), as well as the elastic two-phonon scattering of the excitons (pure dephasing). The exciton states follow from numerical diagonalization of a Frenkel exciton Hamiltonian with diagonal disorder; the scattering rates between them are obtained using the Fermi golden rule. A Debye-type 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 the host vibrations. In particular, for a Debye model of vibrations, we find p approximately 4, which is in good agreement with the experimental data on J aggregates of pseudoisocyanine [I. Renge and U. P. Wild, J. Phys. Chem. A, 101, 7977 (1997)].

Low-temperature dynamics of weakly localized Frenkel excitons in disordered linear 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 nonequilibrium of the subsystem of localized Frenkel excitons on the time scale of the emission process, and different excitation conditions (resonant or nonresonant). 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 nonmonotonic 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 intraband 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.

Temperature dependent fluorescence in disordered Frenkel chains: interplay of equilibration and local band-edge level structure.

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.

Bloch-like oscillations in a one-dimensional lattice with long-range correlated disorder.

We study the dynamics of an electron subjected to a uniform electric field within a tight-binding model with long-range-correlated diagonal disorder. The random distribution of site energies is assumed to have a power spectrum S(k) approximately 1/k(alpha) with alpha>0. de Moura and Lyra [Phys. Rev. Lett. 81, 3735 (1998)]] predicted that this model supports a phase of delocalized states at the band center, separated from localized states by two mobility edges, provided alpha>2. We find clear signatures of Bloch-like oscillations of an initial Gaussian wave packet between the two mobility edges and determine the bandwidth of extended states, in perfect agreement with the zero-field prediction.

Anderson transition in low-dimensional disordered systems driven by long-range nonrandom hopping.

The single-parameter scaling hypothesis predicts the absence of delocalized states for noninteracting quasiparticles in low-dimensional disordered systems. We show analytically, using a supersymmetric method combined with a renormalization group analysis, as well as numerically that extended states may occur in the one- and two-dimensional Anderson model with a nonrandom hopping falling off as some power of the distance between sites. The different size scaling of the bare level spacing and the renormalized magnitude of the disorder seen by the quasiparticles finally results in the delocalization of states at one of the band edges of the quasiparticle energy spectrum.