Surface properties of water ice at 150-191 K studied by elastic helium scattering.
A highly surface sensitive technique based on elastic scattering of low-energy helium atoms has been used to probe the conditions in the topmost molecular layer on ice in the temperature range of 150-191 K. The elastically scattered intensity decreased slowly as the temperature was increased to about 180 K, followed by a rapid decrease at higher temperatures. An effective surface Debye temperature of 185+/-10 K was calculated from the data below 180 K. The changes in the ice surface above 180 K are interpreted as the onset of an anomalous enhancement of the mean square vibrational amplitude for the surface molecules and/or the onset of a limited amount of disorder in the ice surface. The interpretation is consistent with earlier experimental studies and molecular dynamics simulations. The observed changes above 180 K can be considered as the first sign of increased mobility of water molecules in the ice surface, which ultimately leads to the formation of a quasiliquid layer at higher temperatures. A small shift and broadening of the specular peak was also observed in the range of 150-180 K and the effect is explained by the inherent corrugation of the crystalline ice surface. The peak shift became more pronounced with increasing temperature, which indicates that surface corrugation increases as the temperature approaches 180 K. The results have implications for the properties and surface chemistry of atmospheric ice particles, and may contribute to the understanding of solvent effects on the internal molecular motion of hydrated proteins and other organic structures such as DNA.
Suter
Martina T
MT
Department of Chemistry, Atmospheric Science, Göteborg University, SE-412 96 Göteborg, Sweden.
Andersson
Patrik U
PU
Pettersson
Jan B C
JB