Structure−Property Relationships in Third-Order Nonlinear Optical Chromophores

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Abstract

Scientists have sought for over two decades to incorporate the necessary attributes of transparency, stability, and high nonlinear susceptibilities into optimized organic or organometallic chromophores for third-order nonlinear optical (NLO) applications. These investigations have provided an ever-expanding understanding of structure−function relationships for the second hyperpolarizability γ and the bulk third-order nonlinear optical susceptibility χ(3) in organic materials, which are reviewed herein. Contributing to this understanding are the studies of the third-order NLO properties displayed by an array of structurally related organic chromophores based on the conjugated carbon skeletons of hex-3-ene-1,5-diynes (1,2-diethynylethenes, DEEs) and 3,4-diethynylhex-3-ene-1,5-diynes (tetraethynylethenes, TEEs). A comprehensive series of donor (D) and/or acceptor (A) substituted derivatives of DEEs and TEEs has been measured by third-harmonic generation (THG) experiments, and the investigations on these one- and two-dimensionally conjugated chromophores have provided fundamental insight into routes leading to enhanced optical nonlinearities. The molecular characteristics identified to impact the second hyperpolarizability γ include conjugation length, heteroaromatic conjugation, degree of D/A substitution, cis, trans, and geminal D/A conjugation, and molecular asymmetry. A comparison of NLO properties for small molecular systems to those of a number of larger oligomers based on the DEE and TEE framework is also presented.

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