SUNCAT Center for Interface Science and Catalysis, SLAC National Accelerator Laboratory, Menlo Park, CA 94025, USA.
Sci Rep. 2013;3:1074. doi: 10.1038/srep01074. Epub 2013 Jan 15.
The structure of thin-film water on a BaF(2)(111) surface under ambient conditions was studied using x-ray absorption spectroscopy from ambient to supercooled temperatures at relative humidity up to 95%. No hexagonal ice-like structure was observed in spite of the expected templating effect of the lattice-matched (111) surface. The oxygen K-edge x-ray absorption spectrum of liquid thin-film water on BaF(2) exhibits, at all temperatures, a strong resemblance to that of high-density phases for which the observed spectroscopic features correlate linearly with the density. Surprisingly, the highly compressed, high-density thin-film liquid water is found to be stable from ambient (300 K) to supercooled (259 K) temperatures, although a lower-density liquid would be expected at supercooled conditions. Molecular dynamics simulations indicate that the first layer water on BaF(2)(111) is indeed in a unique local structure that resembles high-density water, with a strongly collapsed second coordination shell.
在环境条件下,使用 X 射线吸收光谱法研究了 BaF(2)(111)表面上的薄水膜结构,相对湿度高达 95%,温度从环境温度降至过冷温度。尽管晶格匹配的 (111)表面具有预期的模板效应,但未观察到类似六方冰的结构。在所有温度下,BaF(2)上薄水膜的液态氧 K 边 X 射线吸收光谱与高密度相非常相似,其中观察到的光谱特征与密度呈线性相关。令人惊讶的是,尽管在过冷条件下应该存在低密度液体,但高度压缩的高密度薄水膜液体被发现从环境温度(300 K)到过冷温度(259 K)都是稳定的。分子动力学模拟表明,BaF(2)(111)上的第一层水确实具有独特的局部结构,类似于高密度水,具有强烈塌陷的第二配位壳。