分子投影态密度（PDOS）能系统地用于电导分析吗？
Can molecular projected density-of-states (PDOS) be systematically used in electronic conductance analysis?
摘要：
以苯-二胺和苯-二硫醇分子结为基准，我们研究了量子输运电导$\mathcal{G}(ε)$在分子轨道上的投影态密度（PDOS）的广泛分析。我们首先考虑两种不同的方法来确定相关的MO：1）对角化的孤立分子的哈密顿量，和2）对角化的子矩阵的结的哈密顿量构造只考虑本地化的基础元素的分子。我们发现，这两种方法可以导致实质上不同的MO，因此PDOS。此外，在方法1中，PDOS可以根据选择用于表示分子结的分离分子（例如苯-二硫醇或-二硫醇盐）而不同;并且在方法2中，PDOS取决于选择的基组。我们表明，这些差异可能是至关重要的，当PDOS是用来提供一个物理解释的电导（特别是，当它有小的值，因为它通常发生在零偏置）。在这项工作中，我们提出了一种新的方法，试图调和这两种传统的方法。虽然取得了一些进展，但主要问题仍未得到解决。我们的研究结果提出了更普遍的问题和怀疑的PDOS为基础的分析电导。
英文摘要：
Using benzene-diamine and benzene-dithiol molecular junctions as benchmarks, we investigate the widespread analysis of the quantum transport conductance $\mathcal{G}(ε)$ in terms of the projected density of states (PDOS) onto molecular orbitals (MOs). We first consider two different methods for identifying the relevant MOs: 1) diagonalization of the Hamiltonian of the isolated molecule, and 2) diagonalization of a submatrix of the junction Hamiltonian constructed by considering only basis elements localized on the molecule. We find that these two methods can lead to substantially different MOs and hence PDOS. Furthermore, within Method 1, the PDOS can differ depending on the isolated molecule chosen to represent the molecular junction (e.g. benzene-dithiol or -dithiolate); and, within Method 2, the PDOS depends on the chosen basis set. We show that these differences can be critical when the PDOS is used to provide a physical interpretation of the conductance (especially, when it has small values as it happens typically at zero bias). In this work, we propose a new approach trying to reconcile the two traditional methods. Though some improvements are achieved, the main problems are still unsolved. Our results raise more general questions and doubts on a PDOS-based analysis of the conductance.
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