archives@tulane.edu / Translational research pertains to the areas of scientific exploration and innovation that engenders short-term positive impact on human life and well-being. Toward that end, research of advanced, synthetic polymers present significant translational potential for accessing tailor-made biomaterials of targeted therapeutic functionality. In the present study, the application of amphiphilic polymers as soluble carriers for drug delivery is explored, specifically considering the effect of non-linear polymer architecture in directing physiochemical and therapeutic material performance. To systematically explore structure-property contributions arising from location and extent of polymer branching, a series of lipophile-functionalized poly(ethylene glycol) (PEG) linear-/star-dendrimer hybrids was synthesized. Here, amphiphile topology was controlled by varying the number of branching motifs incorporated at either the polymer core (one-, two- and four-arm PEG) and/or the polar/non-polar interface (peripheral dendritic generations 0 to 2). Material characterization by matrix-assisted laser desorption/ionization time-of-flight mass spectroscopy (MALDI-TOF MS), gel permeation chromatography (GPC) and nuclear magnetic resonance (NMR) analysis confirm the well-defined structural and chemical purity of the derived polymer library. As such, the effects of branching location (core versus peripheral) on amphiphilic, reverse micelle self-assembly behavior could be directly probed towards application in carrier-mediated transdermal drug delivery. Physiochemical parameters under investigation include reverse micelle dimensions, stability and payload capacity, with observed architecture-dependent, structure-property contributions further assessed by in vitro transdermal permeation studies. Finally, to demonstrate translational research value, the clinical significance and applications of non-linear polymer carriers in transdermal drug administration is explored. / 1 / Karolina Kosakowska

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Cyclophanes are a family of bridged cyclic aromatic compounds that have found extensive applications in host-guest chemistry, molecular recognition, biomimetics and most recently as precursors in ring-opening polymerizations.;This research presents the synthesis of several novel cyclic arylene ether oligomers, based on 1,3-bis(4-fluorobenzoyl) benzene and 3,3{dollar}\sp\prime{dollar}-methylene diphenol and 3,3{dollar}\sp\prime{dollar}-(ethylene dioxy) diphenol, and their characterization by LC-MS/MS, 1-D {dollar}\sp1{dollar}H-NMR and x-ray crystallography. Electrospray ionization (ES) along with MS/MS was used to characterize cyclic oligomers of molecular weight up to 1600 Da. The thermal properties of these cyclic oligomers were studied by differential scanning calorimetery (DSC) and thermal gravimetric analysis (TGA).;These cyclic oligomers were synthesized in high yield by regulating the reaction time, concentration, temperature and solvent systems. The relevance of reaction conditions was investigated by selected reaction monitoring (SRM).;Molecular dynamics and potential energy calculations were also carried out to understand the molecular characteristics of the bisphenols that lead to the formation of these cyclic species. Furthermore, the molecular modeling studies assisted in predicting the conformations of the small macrocyclic rings. The predicted structures indicted the cavity size and the relative orientation of the oxygen atoms.

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