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Title: The dielectric response of phenothiazine‑based glass‑formers with different molecular complexity
Authors: Rams-Baron, Marzena
Jędrzejowska, A.
Jurkiewicz, Karolina
Matussek, Marek
Musiał, M.
Paluch, M.
Keywords: glass; Debye process; phenothiazine
Issue Date: 2021
Citation: Scientific Reports, 2021, Vol. 1, art. no. 15816
Abstract: We examined a series of structurally related glass-forming liquids in which a phenothiazine-based tricyclic core (PTZ) was modified by attaching n-alkyl chains of different lengths (n = 4, 8, 10). We systematically disentangled the impact of chemical structure modification on the intermolecular organization and molecular dynamics probed by broadband dielectric spectroscopy (BDS). X-ray diffraction (XRD) patterns evidenced that all PTZ-derivatives are not ‘ordinary’ liquids and form nanoscale clusters. The chain length has a decisive impact on properties, exerting a plasticizing effect on the dynamics. Its elongation decreases glass transition temperature with slight impact on fragility. The increase in the medium-range order was manifested as a broadening of the dielectric loss peak reflected in the lower value of stretching parameter βKWW. A disagreement with the behavior observed for non-associating liquids was found as a deviation from the anti-correlation between the value of βKWW and the relaxation strength of the α-process. Besides, to explain the broadening of loss peak in PTZ with the longest (decyl) chain a slow Debye process was postulated. In contrast, the sample with the shortest alkyl chain and a less complex structure with predominant supramolecular assembly through π–π stacking exhibits no clear Debye-mode fingerprints. The possible reasons are also discussed.
DOI: 10.1038/s41598-021-95127-y
ISSN: 2045-2322
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