Abstract
As a result of fundamental progress in the field of nonlinear optics, the microscopic origin and mechanism for nonresonant second order and third order optical processes originating from the So ground electronic state of conjugated structures are fairly well understood, especially in terms of highly correlated virtual excitations that are accurately described by electron correlation theory for low dimensional systems. In finite systems, the theoretical description is in excellent agreement with experimental measurements of the magnitude, sign, and dispersion of the microscopic second order ßijk S 0(-ω3;ω1,ω2) and third order γijkl S 0(-ω4;ω1,ω2,ω3) optical susceptibilities[1]–[4]. Based on this understanding, the microscopic description can be naturally developed to consider nonlinear optical processes originating not only from the ground state but also from real population of an optically pumped excited state S n.
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References
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Zhou, Q.L., Heflin, J.R., Wong, K.Y., Zamani-Khamiri, O., Garito, A.F. (1991). Excited State Nonlinear Optics. In: Messier, J., Kajzar, F., Prasad, P. (eds) Organic Molecules for Nonlinear Optics and Photonics. NATO ASI Series, vol 194. Springer, Dordrecht. https://doi.org/10.1007/978-94-011-3370-8_18
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DOI: https://doi.org/10.1007/978-94-011-3370-8_18
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