论文标题
H原子在Pt上表面扩散的原子共振隧道（111）
Atomic Resonant Tunneling in the Surface Diffusion of H Atoms on Pt(111)
论文作者
论文摘要
氢（H）原子的量子运动在凝结相材料的动力学和功能以及生物系统中起重要作用。在这项工作中，基于转移矩阵方法和第一原理计算，我们研究了pt（111）表面上H原子的动力学，并数值计算H跨表面电势场的H传递的量子概率。沿许多扩散途径证明了原子共振隧道（ART）。由于谐振隧道，预测在低温下沿特定路径的H扩散的异常转移速率。由于量子隧穿而显着降低了有效的屏障，并随着特定区域内的温度单调降低。对于适用Arrhenius类型关系的屏障横断过程，我们显示了非零的低温速率恒定限制的存在，这表明在低温条件下H-volved反应的非平凡活性。
The quantum motions of hydrogen (H) atoms play an important role in the dynamical properties and functionalities of condensed phase materials as well as biological systems. In this work, based on the transfer matrix method and first-principles calculations, we study the dynamics of H atoms on Pt(111) surface and numerically calculate the quantum probability of H transferring across the surface potential fields. Atomic resonant tunneling (ART) is demonstrated along a number of diffusion pathways. Owing to resonant tunneling, anomalous rate of transfer is predicted for H diffusion along certain path at low temperatures.The role of nuclear quantum effects (NQEs) on the surface reactions involving H is investigated, by analyzing the probabilities of barrier-crossing. The effective barrier is significantly reduced due to quantum tunneling, and decreases monotonically with temperature within a certain region. For barrier-crossing processes where the Arrhenius type relation applies, we show the existence of a nonzero low-temperature limit of rate constant, which indicates the nontrivial activity of H-involved reactions at cryogenic conditions.
