催化剂存在下的分子离解：将键断裂解释为量子动力学相变
Molecular dissociation in presence of catalysts: Interpreting bond breaking as a quantum dynamical phase transition
摘要：
在这项工作中，我们表明，在金属催化剂的d-带的存在下的分子化学键的形成和解离可以被描述为量子动力学相变（QDPT）。这与DFT计算预测的分子断裂时某些可观测量的突然跳跃一致。根据我们的模型，这种现象的出现是因为催化剂提供了一个非厄米哈密顿量。我们发现，当分子接近表面时，发生在H2的Heyrovsky反应中，成键H2轨道有一个平滑的交叉成键分子轨道与最近的H轨道和表面金属d-状态。反键态也是如此。同时，在d带的连续谱中出现了两个共振峰，它们与第二金属层上最远的H原子和d态之间的成键和反键轨道有关.它们向能带中心移动，在那里它们坍缩成纯金属共振和几乎孤立的H轨道。这种现象构成了一个引人注目的例子，非平凡的物理学，使当一个处理非厄米哈密顿超出通常的宽带近似。
英文摘要：
In this work we show that the molecular chemical bond formation and dissociation in presence of the d-band of a metal catalyst can be described as a Quantum Dynamical Phase Transition (QDPT). This agree with DFT calculations that predict sudden jumps in some observables as the molecule breaks. According to our model this phenomenon emerges because the catalyst provides for a non- Hermitian Hamiltonian. We show that when the molecule approaches the surface, as occurs in the Heyrovsky reaction of H 2, the bonding H 2 orbital has a smooth crossover into a bonding molecular orbital built with the closest H orbital and the surface metal d-states. The same occurs for the antibonding state. Meanwhile, two resonances appear within the continuous spectrum of the d- band which are associated with bonding and antibonding orbitals between the furthest H atom and the d-states at the second metallic layer. These move towards the band center where they collapse into a pure metallic resonance and an almost isolated H orbital. This phenomenon constitutes a striking example of the non-trivial physics enabled when one deals with non-Hermitian Hamiltonian beyond the usual wide band approximation.
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