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Predicting Nonlinear Optical Properties of Delocalized Charge States in Polyenylic Chromophores and Dendrimers

  • C. Dirk (a1), C. Spangler (a2), L. Madrigal (a2) and E. H. Elandaloussi (a2)

Abstract

Over the past several years there has been continuing interest in the design of highly conjugated monomers, oligomers and polymers for a variety of photonics applications dependent on a nonlinear response to intense laser radiation. Materials design criteria for these various applications depend on accurate structure-property relationships, and while these relationships can best be determined experimentally, computational approaches that can accurately predict trends in series are extremely useful in establishing target molecules having the desired photonic properties. We have recently reviewed the relationship between incorporation of polaronic or bipolaronic charge states in oligomeric or polymeric conjugation sequences' and enhanced third-order optical nonlinearity, particularly for finite-length polyenes. In this presentation we will focus on how these charge states can be stabilized by electron-donating substituents in dithienylpolyenes, and in model dendrimers based on bis(diphenylamino)stilbene repeat units, and illustrate why these criteria are important for the design of new optical limiting chromophores.

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