Abstract
Nonlinear-optical processes based on the localized response of individual atoms to strong applied optical fields are well known. In addition, strong nonlinearities have been demonstrated in recent years for delocalized excitations in organic molecules and artificial structures like quantum wells and superlattices. Here, however, we present observations and theory of a novel delocalized mechanism for nonlinear optics due to cooperative population dynamics in the excited states of rare-earth solids. Cooperative nonlinearities are shown to exhibit unusual features, such as threshold incident intensity, and are expected to exhibit temporal oscillations1 and intrinsic chaotic behavior in strong coupling limits.2
© 1991 Optical Society of America
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