Publications

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Biological imaging and assay technologies rely on fluorescent organic dyes as reporters for a number of interesting targets and processes. However, limitations of organic dyes such as small Stokes shifts, spectral overlap of emission signals with native biological fluorescence background, and photobleaching have all inhibited the development of highly sensitive assays. To overcome the limitations of organic dyes for bioassays, we propose to develop lanthanide-based luminescent dyes and demonstrate them for molecular reporting applications. This relatively new family of dyes was selected for their attractive spectral and chemical properties. Luminescence is imparted by the lanthanide atom and allows for relatively simple chemical structures that can be tailored to the application. The photophysical properties offer unique features such as narrow and non-overlapping emission bands, long luminescent lifetimes, and long wavelength emission, which enable significant sensitivity improvements over organic dyes through spectral and temporal gating of the luminescent signal.Growth in this field has been hindered due to the necessary advanced synthetic chemistry techniques and access to experts in biological assay development. Our strategy for the development of a new lanthanide-based fluorescent reporter system is based on chelation of the lanthanide metal center using absorbing chromophores. Our first strategy involves "Click" chemistry to develop 3-fold symmetric chelators and the other involves use of a new class of tetrapyrrole ligands called corroles. This two-pronged approach is geared towards the optimization of chromophores to enhance light output.

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Metal-Organic Frameworks (MOFs) are nanoporous materials with tunable pore sizes that can accommodate and stabilize small molecules. Because of their long-range order and wellunderstood pore environment, the nano-confinement of donoracceptor materials within MOFs offers a new methodology for creating uniform phase-segregated donor-acceptor interfaces. Phase segregation and the photo-physical effects of confining α,ω-Dihexylsexithiophene (DH-6T) and [6,6]-phenyl-C61-butyric acid methyl ester (PCBM) in several MOFs and the potential role of the MOF in creating a nano-heterojunction for organic photovoltaics are discussed. We demonstrate infiltration of both molecules into MOF pores and use luminescence and absorption spectroscopies to characterize the MOF-guest energy transfer processes. Comparison with density functional theory allows us to determine the energetics and band alignment within the MOF. The results demonstrate the utility of MOFs as scaffolds for sub-nanoscale ordering of donor and acceptor species within a highly uniform environment, allowing both the interaction and separation distance to be much more controlled than in the classical bulk heterojunction. © The Electrochemical Society.

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