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.Comment: 14 pages, 7 figures, submitted to J. Chem. Phy

Microscopic derivation of Frenkel excitons in second quantization

Starting from the microscopic hamiltonian describing free electrons in a periodic lattice, we derive the hamiltonian appropriate to Frenkel excitons. This is done through a grouping of terms different from the one leading to Wannier excitons. This grouping makes appearing the atomic states as a relevant basis to describe Frenkel excitons in the second quantization. Using them, we derive the Frenkel exciton creation operators as well as the commutators which rule these operators and which make the Frenkel excitons differing from elementary bosons. The main goal of the present paper is to provide the necessary grounds for future works on Frenkel exciton many-body effects, with the composite nature of these particles treated exactly through a procedure similar to the one we have recently developed for Wannier excitons.Comment: 16 pages, 4 figure

Role of anisotropy in the F\"orster energy transfer from a semiconductor quantum well to an organic crystalline overlayer

We consider the non-radiative resonant energy transfer from a two-dimensional Wannier exciton (donor) to a Frenkel exciton of a molecular crystal overlayer (acceptor). We characterize the effect of the optical anisotropy of the organic subsystem on this process. Using realistic values of material parameters, we show that it is possible to change the transfer rate within typically a factor of two depending on the orientation of the crystalline overlayer. The resonant matching of donor and acceptor energies is also partly tunable via the organic crystal orientation.Comment: 6 pages, 8 figure

Biphonons in the Klein-Gordon lattice

A numerical approach is proposed for studying the quantum optical modes in the Klein-Gordon lattices where the energy contribution of the atomic displacements is non-quadratic. The features of the biphonon excitations are investigated in detail for different non-quadratic contributions to the Hamiltonian. The results are extended to multi-phonon bound states.Comment: Comments and suggestions are welcom

Strong and weak coupling limits in optics of quantum well excitons

A transition between the strong (coherent) and weak (incoherent) coupling limits of resonant interaction between quantum well (QW) excitons and bulk photons is analyzed and quantified as a function of the incoherent damping rate caused by exciton-phonon and exciton-exciton scattering. For confined QW polaritons, a second, anomalous, damping-induced dispersion branch arises and develops with increasing damping. In this case, the strong-weak coupling transition is attributed to a critical damping rate, when the intersection of the normal and damping-induced dispersion branches occurs. For the radiative states of QW excitons, i.e., for radiative QW polaritons, the transition is described as a qualitative change of the photoluminescence spectrum at grazing angles along the QW structure. Furthermore, we show that the radiative corrections to the QW exciton states with in-plane wavevector approaching the photon cone are universally scaled by an energy parameter rather than diverge. The strong-weak coupling transition rates are also proportional to the same energy parameter. The numerical evaluations are given for a GaAs single quantum well with realistic parameters.Comment: Published in Physical Review B. 29 pages, 12 figure

Tunable exciton interactions in optical lattices with polar molecules

Rotational excitation of polar molecules trapped in an optical lattice gives rise to rotational excitons. Here we show that non-linear interactions of such excitons can be controlled by an electric field. The exciton--exciton interactions can be tuned to induce exciton pairing, leading to the formation of biexcitons. Tunable non-linear interactions between excitons can be used for many applications ranging from the controlled preparation of entangled quasiparticles to the study of polaron interactions and the effects of non-linear interactions on quantum energy transport in molecular aggregates.Comment: Some typos have been corrected in this versio

Comment on "Effects of spatial dispersion on electromagnetic surface modes and on modes associated with a gap between two half spaces"

Recently Bo E. Sernelius [Phys. Rev. B {\bf 71}, 235114 (2005)] investigated the effects of spatial dispersion on the thermal Casimir force between two metal half spaces. He claims that incorporating spatial dispersion results in a negligible contribution from the transverse electric mode at zero frequency as compared to the transverse magnetic mode. We demonstrate that this conclusion is not reliable because, when applied to the Casimir effect, the approximate description of spatial dispersion used is unjustified.Comment: 9 pages, minor corrections in accordance with the journal publication have been mad

Ultra-short solitons and kinetic effects in nonlinear metamaterials

We present a stability analysis of a modified nonlinear Schroedinger equation describing the propagation of ultra-short pulses in negative refractive index media. Moreover, using methods of quantum statistics, we derive a kinetic equation for the pulses, making it possible to analyze and describe partial coherence in metamaterials. It is shown that a novel short pulse soliton, which is found analytically, can propagate in the medium.Comment: 6 pages, 2 figures, to appear in Phys. Rev.