Final Generalization of the Three Coupled Oscillator Model in the Crystal Optical Activity

In this paper we generalize the quantum mechanical model of three coupled oscillators because of its usage in the crystal optical activity. Using this model we can include the influence of all essential couplings between single oscillators which represent the molecules or atoms of optically active crystals belonging for example to the space groups of symmetry D(3,4) or D(3,6). The single oscillators are damped and therefore we can include both parts of the optical activity - optical rotatory dispersion and circular dichroism - into computations. We present more universal formulas for description of the above mentioned parts.Comment: 12 pages, LaTeX 2.0.

Frenkel Excitons in Random Systems With Correlated Gaussian Disorder

Optical absorption spectra of Frenkel excitons in random one-dimensional systems are presented. Two models of inhomogeneous broadening, arising from a Gaussian distribution of on-site energies, are considered. In one case the on-site energies are uncorrelated variables whereas in the second model the on-site energies are pairwise correlated (dimers). We observe a red shift and a broadening of the absorption line on increasing the width of the Gaussian distribution. In the two cases we find that the shift is the same, within our numerical accuracy, whereas the broadening is larger when dimers are introduced. The increase of the width of the Gaussian distribution leads to larger differences between uncorrelated and correlated disordered models. We suggest that this higher broadening is due to stronger scattering effects from dimers.Comment: 9 pages, REVTeX 3.0, 3 ps figures. To appear in Physical Review

Time-domain chirally-sensitive three-pulse coherent probes of vibrational excitons in proteins

The third order optical response of bosonic excitons is calculated using the Green's function solution of the Nonlinear Exciton Equations (NEE) which establish a quasiparticle-scattering mechanism for optical nonlinearities. Both time ordered and non ordered forms of the response function which represent time and frequency domain techniques, respectively, are derived. New components of the response tensor are predicted for isotropic ensembles of periodic chiral structures to first order in the optical wavevector. The nonlocal nonlinear response function is calculated in momentum space, where the finite exciton-exciton interaction length greatly reduces the computational effort. Applications are made to coupled anharmonic vibrations in the amide I infrared band of peptides. Chirally-sensitive and non sensitive signals for alpha helices and antiparallel beta sheets are compared.Comment: 26 pages, 6 figure

Fluorescence decay in aperiodic Frenkel lattices

We study motion and capture of excitons in self-similar linear systems in which interstitial traps are arranged according to an aperiodic sequence, focusing our attention on Fibonacci and Thue-Morse systems as canonical examples. The decay of the fluorescence intensity following a broadband pulse excitation is evaluated by solving the microscopic equations of motion of the Frenkel exciton problem. We find that the average decay is exponential and depends only on the concentration of traps and the trapping rate. In addition, we observe small-amplitude oscillations coming from the coupling between the low-lying mode and a few high-lying modes through the topology of the lattice. These oscillations are characteristic of each particular arrangement of traps and they are directly related to the Fourier transform of the underlying lattice. Our predictions can be then used to determine experimentally the ordering of traps.Comment: REVTeX 3.0 + 3PostScript Figures + epsf.sty (uuencoded). To appear in Physical Review