当前位置: X-MOL 学术Phys. Rev. Lett. › 论文详情
Our official English website, www.x-mol.net, welcomes your feedback! (Note: you will need to create a separate account there.)
Ab InitioApproach for Thermodynamic Surface Phases with Full Consideration of Anharmonic Effects: The Example of Hydrogen at Si(100)
Physical Review Letters ( IF 8.6 ) Pub Date : 2022-06-17 , DOI: 10.1103/physrevlett.128.246101
Yuanyuan Zhou 1 , Chunye Zhu 1, 2 , Matthias Scheffler 1 , Luca M Ghiringhelli 1
Affiliation  

A reliable description of surfaces structures in a reactive environment is crucial to understand materials’ functions. We present a first-principles theory of replica-exchange grand-canonical-ensemble molecular dynamics and apply it to evaluate phase equilibria of surfaces in a reactive gas-phase environment. We identify the different surface phases and locate phase boundaries including triple and critical points. The approach is demonstrated by addressing open questions for the Si(100) surface in contact with a hydrogen atmosphere. In the range from 300 to 1000 K, we find 25 distinct thermodynamically stable surface phases, for which we also provide microscopic descriptions. Most of the identified phases, including few order-disorder phase transitions, have not yet been observed experimentally. Furthermore, we show that the dynamic Si-Si bonds forming and breaking is the driving force behind the phase transition between 3×1 and 2×1 adsorption patterns.

中文翻译:

充分考虑非谐效应的热力学表面相的从头算方法:Si(100) 处的氢示例

反应环境中表面结构的可靠描述对于理解材料的功能至关重要。我们提出了复制交换大规范系综分子动力学的第一性原理理论,并将其应用于评估反应气相环境中表面的相平衡。我们识别不同的表面相并定位相边界,包括三重点和临界点。该方法通过解决与氢气氛接触的 Si(100) 表面的开放性问题来证明。在 300 到 1000 K 的范围内,我们发现了 25 种不同的热力学稳定表面相,我们还提供了微观描述。大多数已确定的相,包括少数有序-无序相变,尚未通过实验观察到。此外,3×12×1吸附模式。
更新日期:2022-06-17
down
wechat
bug