PIETRO CICUTA, ALBERTO VAILATI, M. Giglio
Università di Milano
Equilibrium and nonequilibrium fluctuations at the interface between two
fluid phases
We have investigated the concentration fluctuations at the interface between
two liquid phases. The sample investigated is a binary mixture prepared at
its critical consolution concentration, and kept below its critical
temperature, so that it is separated into two phases. The experimental
technique used is small angle static light scattering, an unusual technique
to study interfacial fluctuations.
We have investigated both the equilibrium interfacial fluctuations at a
fixed temperature, and the nonequilibrium ones during the transient
following a sudden increase of the temperature. The nonequilibrium condition
is obtained by suddenly raising the temperature below its critical value, so
that the binary mixture is still separated into two phases, and a very slow
partial diffusive remixing of the two phases occurs. The scattered light
contains two contributions. One is due to the interfacial fluctuations, and
the other is due to the fluctuations in the bulk phases. At equilibrium
light is mainly scattered from the capillary waves at the interface between
the two phases, and the well known q^(-2) spectrum is observed. We show
that during the transient the capillary waves contribution to the scattered
light is superimposed to a q^(-4) term due to nonequilibrium fluctuations in
the bulk phases. The light scattering data allow us to show for the first
time that the interface is preserved during the diffusive remixing of the
bulk phases. Moreover, the surface tension and concentration difference
across the interface attain almost instantaneously their equilibrium values.
We also show for the first time that giant fluctuations are present in the
bulk phases during the transient following the fast rearrangement of the
interface, and their contribution to the scattered light is even larger than
that associated to capillary waves. During the diffusive remixing, the
presence of a macroscopic concentration gradient makes spontaneous velocity
fluctuations of the fluid in the vertical direction give rise to
nonequilibrium concentration fluctuations.
We have developed a fluctuating hydrodynamics treatment of the fluctuations
which, together with a mean field description of the macroscopic state of
the system, provides a satisfactory description of the experimental
results.