The variation of the dynamic susceptibility along an isochrone

Abstract

Koperwas {\it et al.} showed in a recent paper, Phys. Rev. Lett. {\bf 111}, 125701 (2013), that the dynamic susceptibility $χ_4$ as estimated by dielectric measurements for certain glass-forming liquids decreases substantially with increasing pressure along a curve of constant relaxation time. This observation is at odds with other measures of dynamics being invariant and seems to pose a problem for theories of glass formation. We show that this variation is in fact consistent with predictions for liquids with hidden scale invariance: measures of dynamics at constant volume are invariant along isochrones, called isomorphs in such liquids, but contributions to fluctuations from long-wavelength fluctuations can vary. This is related to the known non-invariance of the isothermal bulk modulus. Considering the version of $χ_4$ defined for the NVT ensemble, data from simulations of a binary Lennard-Jones liquid show in fact a slight increase with increasing density. This is a true departure from the formal invariance expected for this quantity.