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Depolarized Dynamic Light Scattering and Dielectric Spectroscopy: Two Perspectives on Molecular Reorientation in Supercooled Liquids

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The Scaling of Relaxation Processes

Part of the book series: Advances in Dielectrics ((ADVDIELECT))

Abstract

Broadband dielectric spectroscopy (BDS) can be considered the standard and most widespread method to experimentally access molecular reorientation in supercooled liquids, as it covers a range of time constants from sub picoseconds corresponding to the highly fluid liquid to several thousand seconds below the glass transition temperature. In a similar fashion, depolarized dynamic light scattering (DLS) is able to probe molecular reorientation. A comparable range of time scales is covered by combining Tandem Fabry Perot Interferometry (TFPI) and Photon Correlation Spectroscopy (PCS) with recent multispeckle techniques allowing to access even the non-ergodic regime below \(T_g\). Thus, DLS represents an alternative route to cover the full range of glassy dynamics. Moreover, due to the fact that both methods couple to different molecular properties, extra information in particular on the motional mechanism behind a certain dynamic process can be obtained by comparing experimental data from both techniques. In the present work we explore this approach for several examples, including ionic liquids and monohydroxy alcohols, and discuss the implications for different relaxation processes. For instance in the case of supercooled ionic liquids, i.e., molten salts, which are liquid at room temperature, the combination of both techniques allows to unambiguously disentangle the contribution of molecular reorientation from other polarization features that often mask reorientation in the dielectric spectra, and a detailed analysis reveals indications for a crossover in the motional mechanism involved in the \(\alpha \)-relaxation. In monohydroxy alcohols we discuss the appearance of the Johari-Goldstein \(\beta \)-process in both techniques and what the observations imply for the underlying motional mechansim. Furthermore, we consider the Debye relaxation, which is frequently observed in the dielectric spectra of monoalcohols and is usually ascribed to transient supramolecular structures. Here, such a comparison of data reveals molecular details about the conditions under which the supramolecular structures are formed.

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Acknowledgements

We cordially thank Ernst Rößler, Bayreuth, for providing the data on 1-propanol from Refs. [54, 55] and for making the dielectric time domain setup and the Tandem Fabry-Perot interferometer available to us. We are grateful to Catalin Gainaru, Dortmund, for stimulating discussions about alcohols and ionic liquids. Financial support by the Deutsche Forschungsgemeinschaft under Grant No. BL 923/1 and within FOR 1583 under Grant No. BL 1192/1 is gratefully acknowledged.

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  1. Institute of Condensed Matter Physics, Hochschulstr. 6, 64289, Darmstadt, Germany

    J. Gabriel, F. Pabst, A. Helbling, T. Böhmer & T. Blochowicz

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  1. Molekülphysik, Peter-Debye-Institut für Physik der weichen Materie, Universität Leipzig, Leipzig, Germany

    Friedrich Kremer

  2. Institut für Physik, Universität Augsburg, Augsburg, Germany

    Alois Loidl

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Gabriel, J., Pabst, F., Helbling, A., Böhmer, T., Blochowicz, T. (2018). Depolarized Dynamic Light Scattering and Dielectric Spectroscopy: Two Perspectives on Molecular Reorientation in Supercooled Liquids. In: Kremer, F., Loidl, A. (eds) The Scaling of Relaxation Processes. Advances in Dielectrics. Springer, Cham. https://doi.org/10.1007/978-3-319-72706-6_7

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