从头原理Newns-Anderson哈密顿量构造用于金属表面化学吸附氢
First-principles Newns-Anderson Hamiltonian Construction for Chemisorbed Hydrogen at Metal Surfaces
AI总结：
本文提出从头原理方法构造Newns-Anderson哈密顿量，用于研究金属表面化学吸附氢的电子耦合与吸附特性。
摘要：
Newns-Anderson哈密顿量被广泛用于描述气体-固体界面的吸附，但其构造通常依赖于简化假设，如耦合常数恒定和宽带极限近似。本文提出了一种从头原理的方法，通过将投影算子对易化应用于由Kohn-Sham密度泛函理论计算得到的哈密顿矩阵，来构造Newns-Anderson哈密顿量。我们展示了该方法用于化学吸附氢在三种面心立方金属(111)表面（Al、Cu和Pt）上的应用。为验证吸附氢与金属表面之间的电子耦合，我们从构造的Newns-Anderson哈密顿量中计算了投影态密度、电子隧道寿命和振动寿命，并发现与参考计算结果有良好一致。对化学吸附函数的分析表明，宽带极限近似对H/Al(111)有效，但对H/Cu(111)和H/Pt(111)的适用性有限。
英文摘要：
The Newns-Anderson Hamiltonian is widely used to describe adsorption at gas-solid interfaces, yet its construction typically relies on simplifying assumptions such as constant coupling and the wideband limit approximation. Here, we present a first-principles approach to construct Newns-Anderson Hamiltonians by applying projection operator diabatisation to Hamiltonian matrices obtained from Kohn-Sham density functional theory calculations. We demonstrate this method for chemisorbed hydrogen on three fcc metal(111) surfaces: Al, Cu, and Pt. To validate the electronic coupling between adsorbed hydrogen and the metal surface, we compute the projected density of states, electronic tunnelling lifetimes, and vibrational lifetimes from the constructed Newns-Anderson Hamiltonians and find good agreement with reference calculations. Analysis of the chemisorption function reveals that the wideband limit approximation is valid for H/Al(111) but has limited applicability for H/Cu(111) and H/Pt(111).
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