论文标题

模拟催化剂引起的Heyrovsky反应的量子动态相变,具有不同的环境模型

Simulating a Catalyst induced Quantum Dynamical Phase Transition of a Heyrovsky reaction with different models for the environment

论文作者

Lozano-Negro, Fabricio S., Ferreyra-Ortega, Marcos A., Bendersky, Denise, Fernández-Alcázar, Lucas, Pastawski, Horacio M.

论文摘要

Through an appropriate election of the molecular orbital basis, we show analytically that the molecular dissociation occurring in a Heyrovsky reaction can be interpreted as a Quantum Dynamical Phase Transition, i.e., an analytical discontinuity in the molecular energy spectrum induced by the catalyst.金属底物扮演着在Adatom上产生能量不确定性的环境的作用。在量子封闭系统中,这种扩展会导致不可能的关键行为。 We use suitable approximations on symmetry, together with both Lanczos and canonical transformations, to give analytical estimates for the critical parameters of molecular dissociation.当与表面的键为(\ sqrt {2})乘以分子键时,这会发生这种情况。对于较少的对称情况,此值略有弱。多么简单,该结论涉及分子催化剂系统的高阶扰动溶液。 This model is further simplified to discuss how an environment-induced critical phenomenon can be evaluated through an idealized perturbative tunneling microscopy set-up.在这种情况下,一个或两个原子中的能量不确定性是洛伦兹或高斯。前者是由费米黄金法则的结果,即马尔可夫近似。高斯的不确定性与非马克维亚的破坏性过程有关,需要引入自旋浴的特定模型。部分相干的隧穿电流是从广义的Landauer-Büttiker方程中获得的。 The resonances observed in these transport parameters reflect, in many cases, the critical properties of the resonances in the molecular spectrum.

Through an appropriate election of the molecular orbital basis, we show analytically that the molecular dissociation occurring in a Heyrovsky reaction can be interpreted as a Quantum Dynamical Phase Transition, i.e., an analytical discontinuity in the molecular energy spectrum induced by the catalyst. The metallic substrate plays the role of an environment that produces an energy uncertainty on the adatom. This broadening induces a critical behavior not possible in a quantum closed system. We use suitable approximations on symmetry, together with both Lanczos and canonical transformations, to give analytical estimates for the critical parameters of molecular dissociation. This occurs when the bonding to the surface is (\sqrt{2}) times the molecular bonding. This value is slightly weakened for less symmetric situations. However simple, this conclusion involves a high order perturbative solution of the molecule-catalyst system. This model is further simplified to discuss how an environment-induced critical phenomenon can be evaluated through an idealized perturbative tunneling microscopy set-up. In this case, the energy uncertainties in one or both atoms are either Lorentzian or Gaussian. The former results from the Fermi Golden Rule, i.e., a Markovian approximation. The Gaussian uncertainty, associated with non-Markovian decoherent processes, requires the introduction of a particular model of a spin bath. The partially coherent tunneling current is obtained from the Generalized Landauer-Büttiker Equations. The resonances observed in these transport parameters reflect, in many cases, the critical properties of the resonances in the molecular spectrum.

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