Abstract
Virtual π-electron excitations occuring on individual molecular, or polymer chain, sites are responsible for large, ultrafast nonresonant second order βjjk(-ω3;ω1,ω2) and third order γijKl(−ω4;ω1,ω2ω3) noniinear optical susceptibilities of organic conjugated linear chains. It has now been clearly demonstrated that the proper description of βijk in such conjugated structures, as well as resonant one-photon and two-photon processes in finite polyenes, requires account of the electron-electron interaction and resulting electron correlation.1 We present the results of a series of calculations of βijk and γijkl of conjugated linear chains in which the π-electronic states are determined by singly and doubly-excited configuration interaction of the π-electron molecular orbitals obtained from an all-valence electron self-consistent field molecular orbital description of the ground state. Thus, the many- electron nature of the virtual electronic excitations is carefully considered.2,3
© 1988 Optical Society of America
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