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Journal of Chemical Physics / Volume 131 / Issue 20 / COMMUNICATIONS
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J. Chem. Phys. 131, 201101 (2009); http://dx.doi.org/10.1063/1.3265862 (4 pages)

Universal nonexponential relaxation: Complex dynamics in simple liquids

David A. Turton and Klaas Wynne

Department of Physics, SUPA, University of Strathclyde, Glasgow G4 0NG, United Kingdom

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(Received 29 September 2009; accepted 29 October 2009; published online 30 November 2009)

The dynamics of the noble-gas liquids underlies that of all liquids making them an important prototypical model system. Using optical Kerr-effect spectroscopy we show that for argon, krypton, and xenon, both the librational and diffusional contributions to the spectrum are surprisingly complex. The diffusional relaxation appears as a stretched-exponential, such as widely found in studies of structured (e.g., glass-forming) liquids and as predicted by mode-coupling theory. We show that this behavior is remarkably similar to that measured in water and suggest that it is a fundamental or universal property.

© 2009 American Institute of Physics

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KEYWORDS and PACS

Keywords

argon, diffusion, krypton, librational states, liquid structure, liquid theory, optical Kerr effect, vibrational modes, xenon

PACS

ARTICLE DATA

Digital Object Identifier
http://dx.doi.org/10.1063/1.3265862

PUBLICATION DATA

ISSN

0021-9606 (print)  
1089-7690 (online)

Publisher

$abstract.society.value is a Member of CrossRef American Institute of Physics

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Figures (4) Tables (1)

Figures (click on thumbnails to view enlargements)

FIG.1
Time-domain OKE data for argon (purple), krypton (green), and xenon (orange) displayed on logarithmic axes. Although the intensity units are arbitrary, the relative intensities are as measured and reflect the relative magnitude of the atomic polarizabilities. The data were measured, in each case, within 1 K of the triple point (see Table 1). The instantaneous response is shown (dashed) and the two inflexions, for xenon, are marked ×. The nonexponential relaxation is apparent when compared with the exponential (Debye) function. Inset: detail on linear axes of the OKE data for crystalline xenon at 158 K (blue), compared with the liquid phase (orange).

FIG.1 Download High Resolution Image (.zip file) | Export Figure to PowerPoint

FIG.2
Detail of the OKE data and fit for xenon. Up to ∼ 5 ps, the data (dots) are indistinguishable from the fit (red). Also shown are the stretched-exponential function S [Eq. ( 1 )) (dashed)] and the pair of DHOs. Above are the fit residuals, which show that the fit is generally within the noise of the data. Very similar fits were obtained for argon and krypton, and the fit parameters for each liquid are shown in Table 1.

FIG.2 Download High Resolution Image (.zip file) | Export Figure to PowerPoint

FIG.3
The imaginary part of the OKE spectrum on logarithmic axes for xenon. The data (dots) are indistinguishable from the fit (red). The components of the fit are the Fourier transform of the stretched-exponential function S [Eq. ( 1 )], (dashed), and the DHOs. Also shown is the spectrum of the solid xenon at 158 K (blue).

FIG.3 Download High Resolution Image (.zip file) | Export Figure to PowerPoint

FIG.4
Detail of the data for argon, krypton, and xenon with the amplitude and time axes for krypton and xenon rescaled to show the universal scaling. The inset table gives the scaling factors relative to argon. Nα2 is, for comparison, an approximate amplitude factor based on the atomic polarizability (see text for details). Also shown are our OKE data for water for which the time-amplitude scaling applies only to the final diffusive decay due to the very different librational behavior of the strongly interacting liquid. These data were measured at an earlier date so the amplitude scaling cannot be compared.

FIG.4 Download High Resolution Image (.zip file) | Export Figure to PowerPoint

Tables

Table I. Fit parameters for argon, krypton, and xenon.

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