AI 中文总结
该研究提出QC-DFET量子计算密度泛函嵌入框架，将表面反应活性空间映射为量子比特哈密顿量，在Cu(111)上验证其可准确模拟多种表面反应，确立嵌入式量子计算为关联表面反应能量学的实用途径。
AI 中文摘要
催化界面的预测模拟需要关联电子结构处理方法，该方法需描述局域化学转化，同时保留扩展金属环境的影响。我们提出QC-DFET，一种量子计算密度泛函嵌入框架，可将表面反应活性空间映射为紧凑的、感知环境的量子比特哈密顿量。反应一致的活性空间协议保持轨道沿反应坐标的连续性，而基于Zuchongzhi超导量子处理器测量的量子选择组态相互作用，以及强收缩微扰理论，可捕获静态和动态关联。在Cu(111)上，QC-DFET处理高达28量子比特的活性空间，并通过一系列实验约束的表面化学挑战得到验证：H2解离/脱附测试平衡了键断裂与复合势垒，CO吸附测试体现了位点选择性与金属-吸附质键合，甲酸盐氢化测试对比了具有不同动力学和热力学特征的竞争氢化分支。在这些案例中，QC-DFET重现了双向H2势垒，恢复了观测到的CO顶位偏好及吸附强度，并调和了实验基准的H2COO*逆势垒与较低的HCOOH*前向势垒。这些结果确立了嵌入式量子计算作为关联表面反应能量学的实用途径。
英文摘要
Predictive simulations of catalytic interfaces require correlated electronic-structure treatments that describe localized chemical transformations while retaining the influence of the extended metallic environment. We introduce QC-DFET, a quantum-computing density-functional embedding framework that maps surface-reaction active spaces to compact, environment-aware qubit Hamiltonians. A reaction-consistent active-space protocol preserves orbital continuity along reaction coordinates, while quantum-selected configuration interaction based on measurements from the Zuchongzhi superconducting quantum processor and strongly contracted perturbation theory capture static and dynamic correlation. On Cu(111), QC-DFET treats active spaces up to 28 qubits and is validated through a hierarchy of experimentally constrained surface-chemistry challenges. H2 dissociation/desorption tests balanced bond breaking and recombination barriers, CO adsorption tests site selectivity and metal-adsorbate bonding, and formate hydrogenation tests competing hydrogenation branches with different kinetic and thermodynamic signatures. Across these cases, QC-DFET reproduces bidirectional H2 barriers, recovers the observed top-site preference and adsorption strength of CO, and reconciles the experimentally benchmarked H2COO* reverse barrier with the lower forward barrier to HCOOH*. These results establish embedded quantum computing as a practical route to correlated surface-reaction energetics.
