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Communication: Temperature derivative of the dielectric constant gives access to multipoint correlations in polar liquids
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28.Note that the four-point time correlation function is given as χ4(t) ∝ T2χT(t) (Ref. 20). From Fig. 2, χ4(0) decreases when the temperature is lowered toward the glass transition temperature.
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Fluctuations of the dipole moment of a macroscopic dielectric sample are induced by thermal motions. The variance of the sample dipole moment, characterizing the extent of thermal fluctuations, is a decaying function of temperature for many polar liquids. This result is inconsistent with the Nyquist (fluctuation-dissipation) theorem predicting the variance of a macroscopic property to grow linearly with temperature. The reason for a qualitatively different behavior is in strong multi-particle correlations of dipolar orientations. An equation connecting the temperature slope of the dielectric constant to a static three-point correlation function is derived. When applied to experimental data for polar and hydrogen-bonding liquids at normal conditions, the three-point correlations of different liquids fall on a single master curve as a function of the dielectric constant. Static three-point correlation functions can potentially reflect the growing spatial correlation length on approach to the glass transition. However, the measuredtemperature slope of the dielectric constant of glycerol does not indicate a change in such a lengthscale.
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