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首页> 外文期刊>The journal of physical chemistry, A. Molecules, spectroscopy, kinetics, environment, & general theory >Crystallization kinetics and excess free energy of H_2O and D_2O nanoscale films of amorphous solid water
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Crystallization kinetics and excess free energy of H_2O and D_2O nanoscale films of amorphous solid water

机译：非晶态固体水H_2O和D_2O纳米薄膜的结晶动力学和过量自由能

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摘要

Temperature-programmed desorption (TPD) and reflection absorption infrared spectroscopy (RAIRS) are used to investigate the crystallization kinetics and measure the excess free energy of metastable amorphous solid water films (ASW) of H_2O and D_2O grown using molecular beams. The desorption rates from the amorphous and crystalline phases of ASW are distinct, and as such, crystallization manifests can be observed in the TPD spectrum. The crystallization kinetics were studied by varying the TPD heating rate from 0.001 to 3 K/s. A coupled desorption-crystallization kinetic model accurately simulates the desorption spectra and accurately predicts the observed temperature shifts in the crystallization. Isothermal crystallization studies using RAIRS are in agreement with the TPD results. Furthermore, highly sensitive measurements of the desorption rates were used to determine the excess free energy of ASW near 150 K. The excess entropy obtained from these data is consistent with there being a thermodynamic continuity between ASW and supercooled liquid water.
机译：使用程序升温脱附（TPD）和反射吸收红外光谱（RAIRS）来研究结晶动力学并测量使用分子束生长的H_2O和D_2O的亚稳非晶固体水膜（ASW）的过量自由能。 ASW的非晶相和结晶相的解吸速率截然不同，因此可以在TPD光谱中观察到结晶现象。通过将TPD加热速率从0.001更改为3 K / s，研究了结晶动力学。耦合的解吸-结晶动力学模型可以精确地模拟解吸光谱并准确预测观察到的结晶温度变化。使用RAIRS进行的等温结晶研究与TPD结果一致。此外，使用高灵敏度的解吸速率测量值来确定150 K附近ASW的过量自由能。从这些数据中获得的过量熵与ASW和过冷液态水之间的热力学连续性是一致的。

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