Li Junhong, Guo Hua, Li Jun
School of Chemistry and Chemical Engineering and Chongqing Key Laboratory of Chemical Theory and Mechanism, Chongqing University, Chongqing 401331, China.
Department of Chemistry and Chemical Biology, Center for Computational Chemistry, University of New Mexico, Albuquerque, New Mexico 87131, United States.
J Phys Chem Lett. 2024 Jun 6;15(22):5824-5830. doi: 10.1021/acs.jpclett.4c00994. Epub 2024 May 24.
Motivated by recent experimental work by the Neumark group, we present here an all-atom molecular dynamics study of Ne scattering from a dodecane liquid surface with the objective of elucidating the fundamental aspects of gas-liquid dynamics. Using a fine-tuned force field, the GPU-accelerated simulations reproduced semiquantitatively the energy- and angle-resolved experimental results. The branching ratio between the impulsive scattering (IS) and thermal desorption (TD) channels exhibits a clear correlation with the incidence energy () and angle. Ne atoms with lower values are more likely to be trapped, yielding an increased TD ratio. For a given , a large incidence angle led to a higher IS ratio. The energy transfer between Ne atoms and liquid dodecane was found to be more sensitive to the deflection angle than to the incidence or reflection angle. With an increasing deflection angle, the fractional energy loss increases, suggesting that more kinetic energy is transferred to the liquid.
受纽马克小组近期实验工作的启发，我们在此展示了一项关于氖从十二烷液体表面散射的全原子分子动力学研究，目的是阐明气液动力学的基本方面。使用经过微调的力场，GPU加速模拟半定量地再现了能量和角度分辨的实验结果。脉冲散射（IS）和热脱附（TD）通道之间的分支比与入射能量（）和角度呈现出明显的相关性。较低值的氖原子更有可能被俘获，从而导致TD比率增加。对于给定的，大入射角导致更高的IS比率。发现氖原子与液态十二烷之间的能量转移对偏转角比对入射角或反射角更敏感。随着偏转角的增加，能量损失分数增加，这表明更多的动能转移到了液体中。
