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Excited State Enhancement of Nonlinear Optical Properties

D.C. Rodenberger, J.R. Heflin and A.F. Garito,

In the search for efficient materials for all-optical photonic devices based on the third order optical susceptibility X(3), organic and polymeric materials are being intensely investigated because nonresonant virtual excitation of the delocalized π-electron systems of these materials can result in large ultrafast nonlinear optical responses with minimal background absorption. We have recently shown through theoretical and experimental studies that x(3)(-ω4;ω1,ω2,ω3) can be increased by orders of magnitude over the normally observed ground state values by population of electronic excited states.