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一种用于在超高真空下研究液膜和过冷液膜的纳秒脉冲激光加热系统。

A nanosecond pulsed laser heating system for studying liquid and supercooled liquid films in ultrahigh vacuum.

作者信息

Xu Yuntao, Dibble Collin J, Petrik Nikolay G, Smith R Scott, Joly Alan G, Tonkyn Russell G, Kay Bruce D, Kimmel Greg A

机构信息

Physical Sciences Division, Pacific Northwest National Laboratory, P.O. Box 999, Richland, Washington 99352, USA.

出版信息

J Chem Phys. 2016 Apr 28;144(16):164201. doi: 10.1063/1.4947304.

Abstract

A pulsed laser heating system has been developed that enables investigations of the dynamics and kinetics of nanoscale liquid films and liquid/solid interfaces on the nanosecond time scale in ultrahigh vacuum (UHV). Details of the design, implementation, and characterization of a nanosecond pulsed laser system for transiently heating nanoscale films are described. Nanosecond pulses from a Nd:YAG laser are used to rapidly heat thin films of adsorbed water or other volatile materials on a clean, well-characterized Pt(111) crystal in UHV. Heating rates of ∼10(10) K/s for temperature increases of ∼100-200 K are obtained. Subsequent rapid cooling (∼5 × 10(9) K/s) quenches the film, permitting in-situ, post-heating analysis using a variety of surface science techniques. Lateral variations in the laser pulse energy are ∼±2.7% leading to a temperature uncertainty of ∼±4.4 K for a temperature jump of 200 K. Initial experiments with the apparatus demonstrate that crystalline ice films initially held at 90 K can be rapidly transformed into liquid water films with T > 273 K. No discernable recrystallization occurs during the rapid cooling back to cryogenic temperatures. In contrast, amorphous solid water films heated below the melting point rapidly crystallize. The nanosecond pulsed laser heating system can prepare nanoscale liquid and supercooled liquid films that persist for nanoseconds per heat pulse in an UHV environment, enabling experimental studies of a wide range of phenomena in liquids and at liquid/solid interfaces.

摘要

已开发出一种脉冲激光加热系统,该系统能够在超高真空(UHV)环境下,在纳秒时间尺度上研究纳米级液膜以及液/固界面的动力学和动力学过程。本文描述了用于瞬态加热纳米级薄膜的纳秒脉冲激光系统的设计、实施和特性。来自Nd:YAG激光器的纳秒脉冲用于在超高真空环境下快速加热清洁且特性良好的Pt(111)晶体上吸附的水或其他挥发性材料的薄膜。对于约100 - 200 K的温度升高,可获得约10(10) K/s的加热速率。随后的快速冷却(约5×10(9) K/s)使薄膜淬火,从而允许使用各种表面科学技术进行原位加热后分析。激光脉冲能量的横向变化约为±2.7%,对于200 K的温度跃升,导致温度不确定性约为±4.4 K。该装置的初步实验表明,最初保持在90 K的结晶冰膜可迅速转变为温度T > 273 K的液态水膜。在快速冷却回低温的过程中未发生可察觉的再结晶现象。相比之下,加热至熔点以下的非晶态固态水膜会迅速结晶。纳秒脉冲激光加热系统可在超高真空环境下制备每个加热脉冲持续纳秒的纳米级液体和过冷液体薄膜,从而能够对液体以及液/固界面的广泛现象进行实验研究。

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