Abstract
The third-order nonlinear response function and optical susceptibility χ(3) of polyatomic molecules and molecular aggregates in condensed phases are analyzed. Our expression for χ(3), derived using Liouville space Green's function techniques, contains contributions from excitons as well as biexcitons. The scaling of χ(3) with aggregate size and its dependence on the laser detuning and homogeneous and inhomogeneous dephasing rates are analyzed. Applications are made to phase conjugate degenerate four-wave mixing and pumpprobe spectroscopy.
© 1990 Optical Society of America
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