/pdf/de-novo-synthesis-of-gem-dialkyl-chlorophyll-analogues-for-47xs8jxxeo.pdf

De Novo Synthesis of Gem-Dialkyl Chlorophyll Analogues for Probing and Emulating Our Green World

Physico-chemical characterization of nanocapsule polymeric wall using fluorescent benzazole probes.

Nanoconfined liquids are of interest because of both their fundamental properties and their potential utility in an array of applications. The structure and dynamics of the liquid can be dramatically impacted by the geometrical constraints and the interactions with the interface. Understanding the molecular-level origins of these changes and how they are determined by the characteristics of the confining framework is the subject of ongoing experimental and theoretical studies. The progress and remaining challenges in these efforts are reviewed in the context of solvation dynamics and proton transfer reactions, processes that are strongly affected by nanoscale confinement.

Solvation Dynamics and Proton Transfer in Nanoconfined Liquids

We have investigated the dynamics and mechanistic details of the interaction between bovine serum albumin (BSA) and allylamine-capped silicon quantum dots (Si QDs) by means of fluorescence spectroscopy, circular dichroism (CD), and FTIR spectroscopy. The intrinsic fluorescence of BSA gets quenched in the presence of Si QDs due to ground-state complex formation. The binding stoichiometry and various thermodynamic parameters have been evaluated by using the van't Hoff equation. It has been observed that the association process is driven by a favourable negative enthalpy change with an unfavorable negative entropy change. These results have been explained by considering specific hydrogen bonding interactions between amine moieties (–NH2) of Si QDs and carboxylate groups (–COO−) of aspartate (Asp) and glutamate (Glu) residues of BSA. Circular dichroism (CD) and FTIR spectroscopy revealed nominal changes in the secondary structure of the adsorbed proteins due to partial unfolding of the native protein upon surface adsorption while the overall tertiary structure remains close to that of the native state.

Spectroscopic investigation of interaction between bovine serum albumin and amine-functionalized silicon quantum dots

A supramolecular fluorophore, 1,3,5-tris(4′-aminophenyl)benzene (TAPB), selectively senses polynitroaromatic compounds (PNAC), viz. 2,4,6-trinitrotoluene (TNT), 2,4-dinitrotoluene (DNT), picric acid (PA), m-dinitrobenzene (m-DNB) and p-dinitrobenzene (p-DNB) through donor–acceptor complexation. Steady-state and time resolved fluorescence measurements indicate predominantly static quenching of the TAPB fluorophore with TNT, DNT, m-DNB and p-DNB. In the case of PA, a new emissive band with a marginally longer lifetime emerges due to complex formation with TAPB. The selectivity of sensing action is rationalized through computation of HOMO and LUMO energies for both the fluorophore and the analytes using the M06-2X/6-311+G(d,p) level of theory. Practical utility of the fluorophore has also been demonstrated with TNT and DNT vapour.

Selective fluorescence sensing of polynitroaromatic explosives using triaminophenylbenzene scaffolds

Excited-state proton transfer (ESPT) of 2-(2'-pyridyl)benzimidazole (2PBI) in reverse micelles has been studied by steady-state and time-resolved fluorescence spectroscopy. The nanometer sized water pool in the n-heptane/Aerosol OT (AOT)/water microemulsion is found to promote tautomer emission of this probe, as is evident from the emergence of a Stokes shifted band at 450 nm at the expense of the normal emission band on increasing the water content of the system. In the nonaquous microemulsion with a methanol core, the normal emission is quenched but no tautomer emission is obtained. With an acetonitrile core, there is no change in emission properties. Similarly, there is no evidence of ESPT in Triton X-100 reverse micelles. This indicates the requirement of ESPT to occur in microheterogeneous media; the medium should be a ternary system comprised of water and a hydrophobic phase separated by a negatively charged interface. In the microemulsions with an aqueous core, the fluorescence decays of 2PBI at the red end exhibit rise times of 0.8 ns and the time-resolved area-normalized emission spectra (TRANES) exhibit an isoemissive point, indicating slow dynamics of the two-state ESPT of 2PBI in aqueous AOT reverse micelles. The origin of the selective enhancement in AOT microemulsions as well as the slow dynamics is explored using fluorescence spectroscopic techniques, with support from quantum chemical calculation.

Excited-state proton transfer of 2-(2'-pyridyl)benzimidazole in microemulsions: selective enhancement and slow dynamics in aerosol OT reverse micelles with an aqueous core.

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Excited-state proton transfer of 2-(2'-pyridyl)benzimidazole in microemulsions: selective enhancement and slow dynamics in aerosol OT reverse micelles with an aqueous core.