Böhmer, Till ; Gabriel, Jan Philipp ; Zeißler, Rolf ; Richter, Timo ; Blochowicz, Thomas (2022)
Glassy dynamics in polyalcohols: intermolecular simplicity vs. intramolecular complexity.
In: Physical Chemistry Chemical Physics, 24 (30)
doi: 10.1039/D2CP01969H
Artikel, Bibliographie
Kurzbeschreibung (Abstract)
Using depolarized light scattering, we have recently shown that structural relaxation in a broad range of supercooled liquids follows, to good approximation, a generic line shape with high-frequency power law . We now continue this study by investigating a systematic series of polyalcohols (PAs), frequently used as model-systems in glass-science, , because the width of their respective dielectric loss spectra varies strongly along the series. Our results reveal that the microscopic origin of the observed relaxation behavior varies significantly between different PAs: while short-chained PAs like glycerol rotate as more or less rigid entities and their light scattering spectra follow the generic shape, long-chained PAs like sorbitol display pronounced intramolecular dynamic contributions on the time scale of structural relaxation, leading to systematic deviations from the generic shape. Based on these findings we discuss an important limitation for observing the generic shape in a supercooled liquid: the dynamics that is probed needs to reflect the intermolecular dynamic heterogeneity, and must not be superimposed by effects of intramolecular dynamic heterogeneity.
| Typ des Eintrags: | Artikel |
|---|---|
| Erschienen: | 2022 |
| Autor(en): | Böhmer, Till ; Gabriel, Jan Philipp ; Zeißler, Rolf ; Richter, Timo ; Blochowicz, Thomas |
| Art des Eintrags: | Bibliographie |
| Titel: | Glassy dynamics in polyalcohols: intermolecular simplicity vs. intramolecular complexity |
| Sprache: | Englisch |
| Publikationsjahr: | 18 Juli 2022 |
| Verlag: | Royal Society of Chemistry |
| Titel der Zeitschrift, Zeitung oder Schriftenreihe: | Physical Chemistry Chemical Physics |
| Jahrgang/Volume einer Zeitschrift: | 24 |
| (Heft-)Nummer: | 30 |
| DOI: | 10.1039/D2CP01969H |
| Kurzbeschreibung (Abstract): | Using depolarized light scattering, we have recently shown that structural relaxation in a broad range of supercooled liquids follows, to good approximation, a generic line shape with high-frequency power law . We now continue this study by investigating a systematic series of polyalcohols (PAs), frequently used as model-systems in glass-science, , because the width of their respective dielectric loss spectra varies strongly along the series. Our results reveal that the microscopic origin of the observed relaxation behavior varies significantly between different PAs: while short-chained PAs like glycerol rotate as more or less rigid entities and their light scattering spectra follow the generic shape, long-chained PAs like sorbitol display pronounced intramolecular dynamic contributions on the time scale of structural relaxation, leading to systematic deviations from the generic shape. Based on these findings we discuss an important limitation for observing the generic shape in a supercooled liquid: the dynamics that is probed needs to reflect the intermolecular dynamic heterogeneity, and must not be superimposed by effects of intramolecular dynamic heterogeneity. |
| ID-Nummer: | pmid:35880532 |
| Fachbereich(e)/-gebiet(e): | 05 Fachbereich Physik 05 Fachbereich Physik > Institut für Festkörperphysik (2021 umbenannt in Institut für Physik Kondensierter Materie (IPKM)) 05 Fachbereich Physik > Institut für Festkörperphysik (2021 umbenannt in Institut für Physik Kondensierter Materie (IPKM)) > Struktur und Dynamik amorpher Systeme |
| Hinterlegungsdatum: | 25 Aug 2022 08:31 |
| Letzte Änderung: | 17 Nov 2022 11:23 |
| PPN: | 501727035 |
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