Abstract
Recent many-electron calculations1–3 of the nonlinear optical properties of organic conjugated linear and cyclic chains have now demonstrated the dominant role of electron correlation in this important class of molecular structure. The microscopic third-order susceptibility γijkl(−ω4;ω1,ω2,ω3) in centrosymmetric polyenes, for example, has major contributions resulting from virtual transitions to energetically high lying strongly correlated two-photon π-electron states.
© 1990 Optical Society of America
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