Subsurface oxygen in oxide-derived copper catalysts significantly influences CO$_2$ activation. However, its effect on the molecular charging process, the key to forming the CO$_2^{δ-}$ intermediate, remains poorly understood. We employ many-body perturbation theory to investigate the impact of the structural factors induced by the subsurface oxygen on charged activation of CO$_2$. By computing the molecular single-particle state energy of the electron-accepting orbital ($σ*$) on Cu (111) surface, we examined how this molecular quasi-particle (QP) energy changes with varied vicinity of adsorption and multiple subsurface oxygen configuration. We demonstrate that subsurface oxygen impairs CO$_2$ charging, with its presence and density being influential factors. The non-local potential proves substantial for accurate excitation energy predictions yet is not sensitive to minor atomic structural changes. More importantly, state delocalization and hybridization are critical for determining QP energy. These insights are enlightening for designing atomic architectures to optimize catalytic performance on modified surfaces.
State Key Laboratory of Silicon and Advanced Semiconductor Materials and Center of Electron Microscopy, School of Materials Science and Engineering, Zhejiang University（浙江大学材料科学与工程学院）；Yusuf Hamied Department of Chemistry, University of Cambridge（剑桥大学化学系）；Institute of Fundamental and Transdisciplinary Research, Zhejiang University（浙江大学基础与交叉研究院）；Zhejiang Key Laboratory of Low-Carbon Synthesis of Value-Added Chemicals（斯科尔科沃科学技术研究所）；Skolkovo Institute of Science and Technology
Charge Localization Dynamics induced by Oxygen Vacancies on the Titania TiO$_2$(110) Surface
用{ \it ab initio}分子动力学研究了氧空位在$\mathrm{TiO_{2}(110)}$金红石表面产生F-心的动力学。这些模拟揭示了一个真正复杂的，随时间变化的行为波动的电子局域拓扑结构的附近的氧空位。虽然两个多余的电子被发现优先填充的第二次表面层，他们偶尔访问表面网站，也第三次表面层。过量电荷的这种动力学行为解释了迄今为止理论发现和实验数据的相互矛盾的解释。
Anomalous Subsurface Vacancy Stabilization Dictated by Geometry-Electronic Decoupling on Metal Surfaces
State Key Laboratory of Materials for Integrated Circuits Shanghai Institute of Microsystem and Information Technology Chinese Academy of Sciences（集成电路材料国家重点实验室 上海微系统与信息技术研究所 中国科学院）
Near-surface Defects Break Symmetry in Water Adsorption on CeO$_{2-x}$(111)
National Institute for Materials Science (NIMS)（物质材料研究机构）；Departamento de Física Teórica de la Materia Condensada, Universidad Autónoma de Madrid（马德里自治大学凝聚态理论物理系）；Instituto de Catálisis y Petroleoquímica (CSIC)（催化与石油化工研究所（西班牙国家研究委员会））；Condensed Matter Physics Center (IFIMAC), Universidad Autónoma de Madrid（马德里自治大学凝聚态物理中心）；Graduate School of Engineering Science, Osaka University（大阪大学工学研究科）
From Bulk to Surface: Structure and Dynamics of Amorphous Alumina from Deep Potential Molecular Dynamics
Princeton University（普林斯顿大学）；Shell International Exploration & Production Inc.（壳牌国际勘探与生产有限公司）；Shell India Markets Pvt., Ltd.（壳牌印度市场私人有限公司）；Shell Information Technology International Inc.（壳牌信息技术国际有限公司）
