Why do we need three levels to understand the molecular optical response?

Javier Perez-Moreno; Koen Clays; Mark G. Kuzyk

doi:10.1117/12.893477

7 September 2011 Why do we need three levels to understand the molecular optical response?

Javier Perez-Moreno, Koen Clays, Mark G. Kuzyk

Proceedings Volume 8113, Linear and Nonlinear Optics of Organic Materials XI; 81130L (2011) https://doi.org/10.1117/12.893477
Event: SPIE Photonic Devices + Applications, 2011, San Diego, California, United States

Abstract

Traditionally, the nonlinear optical response at the molecular level has been modeled using the two-level approximation, under the assumption that the behavior of the exact sum-over-states (SOS) expressions for the molecular polarizabilities is well represented by the contribution of only two levels. We show how, a rigorous application of the Thomas-Kuhn sum-rules over the SOS expression for the diagonal component of the first-hyperpolarziability proves that the two-level approximation is unphysical. In addition, we indicate how the contributions of potentially infinite number of states to the SOS expressions for the first-hyperpolarizability are well represented by the contributions of a generic three-level system. This explains why the analysis of the three-level model in conjugation with the sum rules has lead to successful paradigms for the optimization of organic chromophores.

Citation Download Citation

Javier Perez-Moreno, Koen Clays, and Mark G. Kuzyk "Why do we need three levels to understand the molecular optical response?", Proc. SPIE 8113, Linear and Nonlinear Optics of Organic Materials XI, 81130L (7 September 2011); https://doi.org/10.1117/12.893477

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