DOI: 10.1063/1.460990. A possible molecular structural indicator of the liquid

A possible molecular structural indicator of the liquid–glass transition

10.1063/1.460990

Crossref journal-article

AIP Publishing

The Journal of Chemical Physics (317)

Abstract

In studying the VH depolarized Rayleigh light-scattering spectrum of orthoterphenyl we have separated an ‘‘intermediate’’ line with almost temperature-independent halfwidth of 50 GHz from both the narrower rotational line with strongly temperature-dependent halfwidth and the broader base line associated with short-range overlap interactions. The integrated intensity IVH of the intermediate line decreases by a factor of 25 as the temperature decreases over a range for which the viscosity increases by 11 orders of magnitude. It appears that the extrapolated value of (IVH/ρ2)1/2 for this line vanishes as T→T0, where ρ is the density and T0 is the ideal liquid–glass transition temperature established by fitting a Vogel–Fulcher relation to the viscosity. We associate this intermediate line with dipole–induced-dipole interactions; its intensity is then given by an equal-time correlation function involving two-, three-, and four-body interactions. Because dipole interactions are quite long range, this correlation function may be a good probe of local molecular order, and IVH may thus be a good molecular structural (thermodynamic) indicator (order parameter) of the liquid–glass transition, the first such indicator identified.

Bibliography

Kivelson, D., Steffen, W., Meier, G., & Patkowski, A. (1991). A possible molecular structural indicator of the liquidâglass transition. The Journal of Chemical Physics, 95(3), 1943â1949.

Authors 4

Daniel Kivelson (first)
Werner Steffen (additional)
Gerhard Meier (additional)
Adam Patkowski (additional)

References 32 Referenced 23

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Dates

Type	When
Created	23 years ago (July 26, 2002, 8:38 a.m.)
Deposited	1 year, 6 months ago (Feb. 10, 2024, 8:05 a.m.)
Indexed	1 year, 6 months ago (Feb. 11, 2024, 3:34 a.m.)
Issued	34 years ago (Aug. 1, 1991)
Published	34 years ago (Aug. 1, 1991)
Published Print	34 years ago (Aug. 1, 1991)

Funders 0

None

BibTeX

@article{Kivelson_1991, title={A possible molecular structural indicator of the liquid–glass transition}, volume={95}, ISSN={1089-7690}, url={http://dx.doi.org/10.1063/1.460990}, DOI={10.1063/1.460990}, number={3}, journal={The Journal of Chemical Physics}, publisher={AIP Publishing}, author={Kivelson, Daniel and Steffen, Werner and Meier, Gerhard and Patkowski, Adam}, year={1991}, month=aug, pages={1943–1949} }

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  "abstract": "<jats:p>In studying the VH depolarized Rayleigh light-scattering spectrum of orthoterphenyl we have separated an \u2018\u2018intermediate\u2019\u2019 line with almost temperature-independent halfwidth of 50 GHz from both the narrower rotational line with strongly temperature-dependent halfwidth and the broader base line associated with short-range overlap interactions. The integrated intensity IVH of the intermediate line decreases by a factor of 25 as the temperature decreases over a range for which the viscosity increases by 11 orders of magnitude. It appears that the extrapolated value of (IVH/\u03c12)1/2 for this line vanishes as T\u2192T0, where \u03c1 is the density and T0 is the ideal liquid\u2013glass transition temperature established by fitting a Vogel\u2013Fulcher relation to the viscosity. We associate this intermediate line with dipole\u2013induced-dipole interactions; its intensity is then given by an equal-time correlation function involving two-, three-, and four-body interactions. Because dipole interactions are quite long range, this correlation function may be a good probe of local molecular order, and IVH may thus be a good molecular structural (thermodynamic) indicator (order parameter) of the liquid\u2013glass transition, the first such indicator identified.</jats:p>",
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