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 q
uantum dots 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 $G_mathrm{I} = 8Gamma$, whereas at $G_mathrm{I} = 0$, the critical value of $G_mathrm{R} = 4Gamma$, 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 systems 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.
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 e
vidence 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.
We present a theoretical analysis of the environment effects 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 o
f carrier functions due to the static disorder and (ii) phonon-induced scattering of the carrier between these 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. Simple physical explanation of this effect is provided.
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 scatte
ring 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.
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 effi
ciency 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.
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 func
tions 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.
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.
