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Equations of motion for the nonlinear optical response of arbitrary-size molecular aggregates are derived. The relative role of intramolecular and intermolecular (two-exciton) nonlinearities and the cooperative enhancement induced by the latter are analyzed. A crossover from N^2 to scaling of the nonlinear polarizability is predicted as the aggregate dimension becomes comparable to the optical wavelength, N being the aggregate size. The limitations of the local-field approximation are demonstrated.
Spano et al. (Mon,) studied this question.
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