Linear optical properties of one-dimensional Frenkel exciton systems with intersite energy correlations

We analyze the effects of intersite energy correlations on the linear optical properties of one-dimensional disordered Frenkel exciton systems. The absorption line width and the factor of radiative rate enhancement are studied as a function of the correlation length of the disorder. The absorption line width monotonously approaches the seeding degree of disorder on increasing the correlation length. On the contrary, the factor of radiative rate enhancement shows a non-monotonous trend, indicating a complicated scenario of the exciton localization in correlated systems. The concept of coherently bound molecules is exploited to explain the numerical results, showing good agreement with theory. Some recent experiments are discussed in the light of the present theory.Comment: 18 pages, 3 figues, REVTeX, to appear in Physical Review

Statistics of low-energy levels of a one-dimensional weakly localized Frenkel exciton: A numerical study

Numerical study of the one-dimensional Frenkel Hamiltonian with on-site randomness is carried out. We focus on the statistics of the energy levels near the lower exciton band edge, i. e. those determining optical response. We found that the distribution of the energy spacing between the states that are well localized at the same segment is characterized by non-zero mean, i.e. these states undergo repulsion. This repulsion results in a local discrete energy structure of a localized Frenkel exciton. On the contrary, the energy spacing distribution for weakly overlapping local ground states (the states with no nodes within their localization segments) that are localized at different segments has zero mean and shows almost no repulsion. The typical width of the latter distribution is of the same order as the typical spacing in the local discrete energy structure, so that this local structure is hidden; it does not reveal itself neither in the density of states nor in the linear absorption spectra. However, this structure affects the two-exciton transitions involving the states of the same segment and can be observed by the pump-probe spectroscopy. We analyze also the disorder degree scaling of the first and second momenta of the distributions.Comment: 10 pages, 6 figure