Cm. Roland et Kl. Ngai, SHORT-TIME VISCOUS AND DENSITY RELAXATION IN GLYCEROL AND ORTHO-TERPHENYL, The Journal of chemical physics, 106(3), 1997, pp. 1187-1190
Coupling model analyses of short-time relaxation data of glycerol from
quasielastic neutron scattering and ortho-terphenyl (OTP) by molecula
r dynamic simulation are shown to account for both the time dependence
of the correlation function and its temperature dependence. The latte
r is expressible over a limited temperature range as an Arrhenius rela
tion with an apparent activation energy for the fast alpha-relaxation
process, with E(A) = 6.2 and 3.9 kcal/mol for glycerol and OTP, respec
tively. The viscosities of these glass formers have also been measured
up to temperatures sufficiently high that the mean viscosity relaxati
on time, [tau(n)(T)], becomes short, approaching the crossover time, t
(c) approximate to 2 ps, of the coupling model. When this condition is
realized, [tau(n)(T)] becomes comparable to tau(D)(T) in both magnitu
de and temperature dependence. Hence, the asymptotic high temperature
activation energy of [tau(eta)(T)] approximately equals the apparent a
ctivation energy of tau(D). The experimental data, supporting this con
nection between macroscopic variables such as viscosity and microscopi
c dynamics from neutron scattering and molecular dynamics simulation,
indicate the significance of the fast cr-relaxation process in both fr
agile and strong liquids.