On the spectral shape of the structural relaxation in supercooled liquids

Structural relaxation in supercooled liquids is non-exponential. In susceptibility representation, χ″(ν), the spectral shape of the structural relaxation is observed as an asymmetrically broadened peak with a ν1 low- and ν-β high-frequency behavior. In this perspective article, we discuss common notions, recent results, and open questions regarding the spectral shape of the structural relaxation. In particular, we focus on the observation that a high-frequency behavior of ν-1/2 appears to be a generic feature in a broad range of supercooled liquids. Moreover, we review extensive evidence that contributions from orientational cross-correlations can lead to deviations from the generic spectral shape in certain substances, in particular in dielectric loss spectra. In addition, intramolecular dynamics can contribute significantly to the spectral shape in substances containing more complex and flexible molecules. Finally, we discuss the open questions regarding potential physical origins of the generic ν-1/2 behavior and the evolution of the spectral shape toward higher temperatures.

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Publication Details

Journal
The Journal of Chemical Physics
Published
2025-03-26
DOI
https://doi.org/10.1063/5.0254534
Citations
16
Primary Topic
Material Dynamics and Properties
Type
article
Field-Weighted Citation Impact
8.28

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article

On the spectral shape of the structural relaxation in supercooled liquids

Rolf Zeißler, Jan Philipp Gabriel, Till Böhmer, Thomas Blochowicz et al.
16 citations
The Journal of Chemical Physics
Material Dynamics and Properties
8.28
article

On the spectral shape of the structural relaxation in supercooled liquids

Rolf Zeißler, Jan Philipp Gabriel, Till Böhmer, Thomas Blochowicz, Florian Pabst
article en
16 citations

Abstract

Structural relaxation in supercooled liquids is non-exponential. In susceptibility representation, χ″(ν), the spectral shape of the structural relaxation is observed as an asymmetrically broadened peak with a ν1 low- and ν-β high-frequency behavior. In this perspective article, we discuss common notions, recent results, and open questions regarding the spectral shape of the structural relaxation. In particular, we focus on the observation that a high-frequency behavior of ν-1/2 appears to be a generic feature in a broad range of supercooled liquids. Moreover, we review extensive evidence that contributions from orientational cross-correlations can lead to deviations from the generic spectral shape in certain substances, in particular in dielectric loss spectra. In addition, intramolecular dynamics can contribute significantly to the spectral shape in substances containing more complex and flexible molecules. Finally, we discuss the open questions regarding potential physical origins of the generic ν-1/2 behavior and the evolution of the spectral shape toward higher temperatures.

The Journal of Chemical PhysicsVol. 162(12)
Roskilde University (DK), Scuola Internazionale Superiore di Studi Avanzati (IT), Deutsches Zentrum für Luft- und Raumfahrt e. V. (DLR) (DE), Technische Universität Darmstadt (DE), Yukhnovskii Institute for Condensed Matter Physics of the National Academy of Sciences of Ukraine (UA)
Deutsche Forschungsgemeinschaft
Openalex Percentile: Top 2%
Material Dynamics and Properties
8.28
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