Publications by authors named "Andrew D Shaller"

The fluorescence brightness of a molecular probe determines whether it can be effectively measured and its water solubility dictates if it can be applied in real-world biological systems. However, molecules brighter than the most efficient fluorescent dyes or particles brighter than quantum dots are hard to come by, especially when they must also be soluble in water. In this report, chromophoric phosphoramidites are used in a solid-state synthesis to construct functional dendrimers.

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Controlled syntheses give unique block oligomers with alternating flexible ethylene glycol and rigid perylenetetracarboxylic diimide (PDI) units. The number of rigid units vary from n=1 to 10. PDI units were stitched together by using efficient phosphoramidite chemistry.

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In this communication, we report a synthesis of anisotropic colloidal superparticles (SPs) from CdSe/CdS semiconductor nanorods. These anisotropic SPs are cylindrical disks or stacked-disk arrays. We attribute the major driving forces controlling the SP shape to interparticle interactions between nanorods and solvophobic interactions between a superparticle and its surrounding solvent.

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Polymeric fluorescent nanoparticles with covalently embedded perylene fluorophores were developed by facile synthesis strategy and their advanced features of extremely high fluorescence intensity, non-photoblinking and excellent photostability were experimentally confirmed at the single nanoparticle level.

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Unique perylene diastereomeric linear and cyclic dimers were synthesized from twisted perylene monomers, revealing that pi-stacking stereoisomerism imparted specific intermolecular self-assembly and intramolecular folding. Only the homochiral twisted tetrachloroperylene monomers cyclized via a cooperative reaction, forming the homochiral diastereomers. The heterochiral tetrachloroperylene monomers proceeded through a stepwise reaction and yielded a linear heterochiral dimer, which equilibrated with the linear homochiral dimers.

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Single molecule fluorescence spectroscopy has been used to probe architecturally diverse and unique model oligomers containing exactly two or four perylene tetracarboxylic diimide (PTDI) units: linear foldamers lin2 and lin4, monocyclic complement cyc2, and concatenated foldable rings cat4. Linear, cyclic, and concatenated foldamers reveal that photoabsorption and excitation induces unfolding and refolding, generating colorful spectral switching from one spectral type to another. Foldamer architectures dictate the unfolding and refolding processes, and hence the spectral dynamics.

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