Observation of surface layering in a nonmetallic liquid.pdfVIP

Observation of surface layering in a nonmetallic liquid Haiding Mo,1 Guennadi Evmenenko,1 Sumit Kewalramani,1 Kyungil Kim,1 Steven N. Ehrlich2 and Pulak Dutta1 1Department of Physics Astronomy, Northwestern University, Evanston, IL 60208 USA 2National Synchrotron Light Source, Brookhaven National Laboratory, Upton, NY 11973 USA 68.10.-m, 68.15.+e, 68.35.Ct Oscillatory density profiles (layers) have previously been observed at the free surfaces of liquid metals, but not in other isotropic liquids. We have used x-ray reflectivity to study a molecular liquid, tetrakis(2-ethylhexoxy)silane. When cooled to T/Tc≈0.25 (well above the freezing point for this liquid), density oscillations appear at the surface. Lateral order within the layers is liquid-like. Our results confirm theoretical predictions that a surface- layered state will appear even in dielectric liquids at sufficiently low temperatures, if not preempted by freezing. -2- Until recently, the structure of a liquid surface was thought to be well understood:1 the density changes monotonically from the density of the liquid to that of the vapor. However, Rice et al.2 predicted in 1973 that there would be density oscillations (layers) at liquid metal surfaces. This theory assigned an essential role to the electron gas in causing an abrupt transition between the conducting liquid and nonconducting vapor, resulting in an effective wall potential. Starting in 1995, X-ray scattering experiments have established that such smectic-like order does exist near the surfaces of a number of liquid metals and metallic alloys.3-7 (This phenomenon is distinct from surface freezing,8 which is a pretransition effect seen in certain liquids only just above the bulk freezing point, and where the surface layer is frozen, i.e. laterally ordered.) There have also been many X-ray studies of the surface profiles of classical dielectric liquids, including alkanes,9 ethanol,10 toluene,11 polymers and poly