Abstract
The microscopic second-order and third-order optical susceptibilities for conjugated molecular structures with real population of the Sn electronic excited state have been examined in detail and found to be generally enhanced by orders of magnitude compared to and for systems that occupy the ground electronic state S0. The enhancement mechanisms for excited-state nonlinear-optical processes will be discussed based on electron correlation theory of nonlinear-optical processes, which has been proven successful in explaining the ground-state susceptibilities and for conjugated structures.
© 1991 Optical Society of America
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