Supermolecular chromophores and new conjugated organic materials can be prepared from ethyne-elaborated porphyrin synthons through the utilization of metal-mediated cross-coupling methodologies.  Examples of such neoteric chromophores include species that combine porphyrin-derived pigments with strong (polypyridyl)metal-based oscillators; these structures manifest exceptional electronic interactions between the component pigments.  These assemblies show the efficacy of coupled oscillator photophysics to delineate new classes of optoelectronic materials that exhibit unusual excited-state dynamics and manifest exceptional nonlinear responses.  Modifying the nature of excitonic and electronic interactions between the component oscillators of these systems elaborates chromophores that manifest extraordinarily large hyperpolarizabilities, precisely tuned depolarization ratios, and exceptional, low energy electronically excited triplet states.  The electronically excited triplet states of these species can be further manipulated to provide extraordinary absorptivity over the 0.75 � 1.75 mm wavelength domain of the NIR and lifetimes that exceed several microseconds.  The combination of these exceptional properties enables exploitation of these supermolecular chromophores in waveguides and optical limiters, as well as sensitizers for NIR-to-visible fluorescence upconversion via triplet- triplet annihilation (TTA) photochemistry.

Coupled-oscillator photophysics and the elaboration of chromophores having exceptional nonlinear optical properties

245th National Meeting (2013)

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