arXiv subjects

J. Knoester

Publications and source records attributed to J. Knoester.

At least 19 recordsLinked to original sources

arXiv2018

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.

cond-mat.mes-hall↗

arXiv2014

One-dimensional excitonic systems with diagonal Lévy disorder: A detailed study of the absorption spectra and the disorder scaling of localization length

We present a detailed study of the effects of Lévy $α$-stable disorder distributions on the optical and localization properties of excitonic systems. These distributions are a generalization of commonly studied Gaussian randomness ($α= 2$). However, the more general case ($α< 2$) 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 Lévy $α$-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.

cond-mat.dis-nn↗

arXiv2013

Bistable optical response of nanoparticle heterodimer: Mechanism, phase diagram, and switching time

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 $G_\mathrm{I} = 8Γ$, whereas at $G_\mathrm{I} = 0$, the critical value of $G_\mathrm{R} = 4Γ$, where $Γ$ 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 $Δ$, 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.

cond-mat.mtrl-sci↗

arXiv2012

Response to the Comment on "Excitons in Molecular Aggregates with Lévy Disorder: Anomalous Localization and Exchange Broadening of Optical Spectra"

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 α<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 σ values.

cond-mat.dis-nn↗

arXiv2011

Manipulating optical signals at sub-wavelength scale by planar arrays of metallic nanospheres: Towards plasmonic interference devices

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.

cond-mat.mes-hall↗

arXiv2010

Quest for Order in Chaos: Hidden Repulsive Level Statistics in Disordered Quantum Nanoaggregates

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.

cond-mat.dis-nn↗

arXiv2010

Excitons in Molecular Aggregates with Lévy 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 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.

cond-mat.dis-nn↗

arXiv2009

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.

cond-mat.dis-nn↗

arXiv2007

Thermal effects in exciton harvesting in biased one-dimensional systems

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.

cond-mat.dis-nn↗

arXiv2007

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.

cond-mat.dis-nn↗

arXiv2007

Intrinsic optical bistability of thin films of linear molecular aggregates: The one-exciton approximation

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.

cond-mat.dis-nn↗

arXiv2007

Selection of dominant multi-exciton transitions in disordered linear J-aggregates

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.

cond-mat.dis-nn↗

arXiv2007

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

cond-mat.dis-nn↗

arXiv2006

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, which involves the initial excitation condition.

cond-mat.dis-nn↗

arXiv2006

Exciton Dephasing and Thermal Line Broadening in Molecular Aggregates

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.

cond-mat.dis-nn↗

arXiv2005

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 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.

cond-mat.other↗

arXiv2005

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 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)].

cond-mat.other↗

arXiv2004

Optical Spectra and Localization of Excitons in Inhomogeneous Helical Cylindrical Aggregates

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.

cond-mat.dis-nn↗