论文标题
在非化学计时电解质中,氧化状态,无泵和非平凡离子转运
Oxidation states, Thouless' pumps, and non-trivial ionic transport in non-stoichiometric electrolytes
论文作者
论文摘要
无绝热粒子传输允许将整数拓扑电荷与电子间隙材料的每个原子相关联。如果这些电荷是加性的,并且独立于原子位置,则可以将原子氧化态和原子的严格定义鉴定为离子导体中的整数载体载体。每当满足这些条件时,电荷运输必然会是对流的,即,如果没有实质性离子流,即我们将其化为微不足道的运输状态。我们表明,如果系统受到适当定义的时间周期性的哈密顿量,则允许这些条件破坏的拓扑要求与您的泵机制相同。这些要求的出现决定了非平凡的运输方式,即使在电子绝缘体中,也可以在没有任何离子对流的情况下流动。这些结果首先是通过几个简单的分子模型证明的,这些模型在沿构型空间中的封闭环沿着封闭环的虚拟时间依赖性时显示了量子泵的机制。我们最终研究了我们的发现对非化学计量碱 - 甲基盐融化的运输特性的影响,在该熔体中,相同的拓扑条件将沿着配置空间中某些闭合环引起量子泵机制的相同拓扑条件也确定了非平凡的运输方式,因此,大多数总电荷电荷率最高的结果是不相关的,因此是从电源元素中不相关的。
Thouless' quantization of adiabatic particle transport permits to associate an integer topological charge with each atom of an electronically gapped material. If these charges are additive and independent of atomic positions, they provide a rigorous definition of atomic oxidation states and atoms can be identified as integer-charge carriers in ionic conductors. Whenever these conditions are met, charge transport is necessarily convective, i.e. it cannot occur without substantial ionic flow, a transport regime that we dub trivial. We show that the topological requirements that allow these conditions to be broken are the same that would determine a Thouless' pump mechanism if the system were subject to a suitably defined time-periodic Hamiltonian. The occurrence of these requirements determines a non-trivial transport regime whereby charge can flow without any ionic convection, even in electronic insulators. These results are first demonstrated with a couple of simple molecular models that display a quantum pump mechanism upon introduction of a fictitious time dependence of the atomic positions along a closed loop in configuration space. We finally examine the impact of our findings on the transport properties of non-stoichiometric alkali-halide melts, where the same topological conditions that would induce a quantum pump mechanism along certain closed loops in configuration space also determine a non-trivial transport regime such that most of the total charge current results to be uncorrelated from the ionic ones.