Journal
LANGMUIR
Volume 27, Issue 4, Pages 1513-1523Publisher
AMER CHEMICAL SOC
DOI: 10.1021/la104276y
Keywords
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Funding
- European Union [MRTN-CT-2006-035810, PITN-GA-2008-215399]
- CNR [commessa PM.P04.010]
- INSTM
- Belgian National Research Foundation (through FRFC) [2.4.625.08, 2.4.550.09, 2.4.617.07.F, F.4.505.10.F]
- Loterie Nationale
- Region Wallonne through the SOL WATT [850551]
- Belgian French Community [09/14-023]
- University of Namur
- University of Trieste
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The ability of two complementary molecular modules bearing H-bonding uracilic and 2,6-(diacetylamino)pyridyl moieties to self-assemble and self-organize into submicrometer morphologies has been investigated by means of spectroscopic, thermogravimetric, and microscopic methods. Using uracilic N-3-BOC-protected modules, it has been possible to thermally trigger the self-assembly/self-organization process of the two molecular modules, inducing the formation of objects on a mica surface that exhibit crater-like morphology and a very homogeneous size distribution. Confirmation of the presence of the hydrogen-bonding-driven self-assembly/self-organization process in solution was obtained by variable-temperature (VT) steady-state UV-vis absorption and emission measurements. The variation of the geometric and spatial features of the morphologies was monitored at different T by means of atomic force microscopy (AFM) and was interpreted by a nonequilibrium diffusion model for two chemical species in solution. The formation of nanostructures turned out to be affected by the solid substrate (molecular interactions at a solid-liquid interface), by the matter-momentum transport in solution (solute diffusivity D-0 and solvent kinematic viscosity nu), and the thermally dependent cleavage reaction of the BOC functions (T-dependent differential weight loss, theta = theta(T)) in a T interval extrapolated to similar to 60 K. A scaling function, f = T(nu D-0, nu/D-0, theta), relying on the onset condition of a concentration-driven thermosolutal instability has been established to simulate the T-dependent behavior of the structural dimension (i.e., height and radius) of the self-organized nanostructures as < h > approximate to f(T) and < r > approximate to 1/f (T).
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