The physics of aggregates of polar and polarizable donor-acceptor dyes is discussed, extending a previous model to account for the coupling of electronic and vibrational degrees of freedom. Fully exploiting...
Delivery of hydrophobic materials
in biological systems, for example,
contrast agents or drugs, is an obdurate challenge, severely restricting
the use of materials with otherwise advantageous properties. The synthesis
and characterization of a highly stable and water-soluble nanovesicle,
referred to as a quatsome (QS, vesicle prepared from cholesterol and
amphiphilic quaternary amines), that allowed the nanostructuration
of a nonwater soluble fluorene-based probe are reported. Photophysical
properties of fluorenyl–quatsome nanovesicles were investigated
via ultraviolet–visible absorption and fluorescence spectroscopy
in various solvents. Colloidal stability and morphology of the nanostructured
fluorescent probes were studied via cryogenic transmission electronic
microscopy, revealing a “patchy” quatsome vascular morphology.
As an example of the utility of these fluorescent nanoprobes, examination
of cellular distribution was evaluated in HCT 116 (an epithelial colorectal
carcinoma cell line) and COS-7 (an African green monkey kidney cell
line) cell lines, demonstrating the selective localization of C-QS and M-QS vesicles in lysosomes with high
Pearson’s colocalization coefficient, where C-QS and M-QS refer to quatsomes prepared with hexadecyltrimethylammonium
bromide or tetradecyldimethylbenzylammonium chloride, respectively.
Further experiments demonstrated their use in time-dependent lysosomal
tracking.
A multiscale approach to the dynamics of resonant energy transfer is presented, combining DFT and TD-DFT results on the energy donor (D) and acceptor (A) moieties with an extensive equilibrium and non-equilibrium molecular dynamics (MD) analysis of a bound D-A pair in solution to build a coarse-grained kinetic model. We demonstrate that a thorough MD study is needed to properly address RET: the enormous configuration space visited by the system cannot be reliably sampled accounting only for a few representative configurations. Moreover, the conformational motion of the RET pair, occurring in a similar timescale as the RET process itself, leads to a sizable increase of the overall process efficiency.
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