COOPERATIVE ULTRAFAST NONLINEAR-OPTICAL RESPONSE OF MOLECULAR NANOSTRUCTURES

The stationary nonlinear reflection and the time resolved four wave mixing signal from a molecular monolayer are calculated using Green function techniques. Cooperative resonant nonlinear response found in small aggregates suggests the existence of coherence size of order of optical wavelength. A new peak in the nonlinear reflection spectrum is predicted, which is missed by the local field approximation. For an infinite two dimensional molecular monolayer with transition dipole moments in the lattice plane, the momentum-dependent two exciton decay rate is found to be larger than the sum of the single exciton radiative decay rates, as predicted by the local field approximation.