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.Comment: 8 pages, 2 figures, accepted to Journal of Luminescenc

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.

Mode Softening, Ferroelectric Transition, and Tunable Photonic Band Structures in a Point-Dipole Crystal

We study the photonic band structure of cubic crystals of point dipoles. It is shown that in contrast to earlier claims these systems cannot have an omnidirectional photonic band gap. For sufficiently large plasma frequencies, however, they exhibit softening of photonic bands, leading to (anti)ferroelectric ordering of the dipoles and the possibility to open and tune directional band gaps by external electric fields. The model studied may be realized through lattices of quantum dots.