Abstract
Solubilized poly(3-alkylthiophene)s are known to self-assemble into well-ordered supramolecular aggregates upon lowering the solvent quality. This supramolecular organization largely determines the optical and electronic properties of these polymers. However, despite numerous studies the exact mechanism and kinetics of the aggregation process and the role of external stimuli are still poorly understood. Classical characterization techniques such as electronic spectroscopy, dynamic light scattering, and diffraction-based techniques have not been able to provide a full understanding. Here we use second-harmonic scattering (SHS) and third-harmonic scattering (THS) techniques to investigate this supramolecular aggregation mechanism. Our results indicate that the actual supramolecular aggregation is preceded by the formation of structured polymer-solvent clusters consistent with a nonclassical crystallization pathway.
Highlights
Solubilized poly(3-alkylthiophene)s are known to self-assemble into well-ordered supramolecular aggregates upon lowering the solvent quality
The appearance of clusters can be detected with standard techniques such as static and dynamic light scattering (SLS and DLS) since they often emerge in relatively high concentrations due to their thermodynamicstability
We first characterized the regioregular poly(3-alkyltiophene) (P3AT) (Fig. 1) supramolecular aggregation process using a combination of UV/Vis and circular dichroism (CD)
Summary
Solubilized poly(3-alkylthiophene)s are known to self-assemble into well-ordered supramolecular aggregates upon lowering the solvent quality. By combining nonlinear light scattering with dynamic light scattering (DLS) and electronic spectroscopy techniques, we are able to study aggregation processes in a regioregular P3AT (semi-)microcrystalline phase in situ, and provide experimental evidence for the role of structured clusters in the supramolecular organization of these systems.
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