Nonperturbative susceptibility of a three-level system interacting with a monochromatic field

Kavanaugh, Theresa C.; Silbey, Robert J.
May 1992
Journal of Chemical Physics;5/1/1992, Vol. 96 Issue 9, p6443
Academic Journal
We derive an exact, intensity-dependent expression for the susceptibility of a three-level system interacting with one monochromatic electric field. This expression, once expanded, is equivalent to the usual perturbative series χ=χ(1)+χ(3)E2+··· within the rotating wave approximation. We consider two types of resonant processes: one- and two-photon resonances corresponding to the intensity-dependent susceptibility χ(3)(-ω;ω,-ω,ω), and one-, two-, and three-photon resonances corresponding to χ(3)(-3ω;ω,ω,ω). As an example of current interest, we use a model three-level system that mimics the excited electronic states of typical nonlinear optical polymers and show that near resonance, successive terms in the perturbative series approach the same order of magnitude for experimentally realizable fields.


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