Range‐separated hybrid (RSH) functionals have been recently used to overcome the tendency of traditional density functional theory (DFT) calculations to overestimate the conductance of molecular junctions. Non‐equilibrium conditions are addressed following non‐equilibrium Green's function (NEGF) formulation with RSH functionals to study negative differential resistance (NDR) in molecular junctions of oligo phenylene ethylene derivatives linking gold electrodes. It is shown that the RSH‐NEGF calculations indicate NDR onset bias that agrees well with measured trends, associate NDR to orbital localization at the drain contact, and analyze the role of junction asymmetry in NDR. The RSH‐NEGF results are also compared with alternative DFT‐NEGF combinations to highlight the importance of basing the computational study on a functional that achieves physically significant frontier orbitals. Finally, the effects of thermally accessible molecular fluctuations to enhance the NDR conductance drop are also discussed.

中文翻译：

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使用距离分隔的混合函数实现分子连接中负微分电阻的预测描述

范围分隔混合（RSH）功能最近已被用来克服传统密度泛函理论（DFT）计算过高估计分子连接的电导率的趋势。根据具有RSH功能的非平衡格林函数（NEGF）公式解决了非平衡条件，以研究连接金电极的低聚亚苯基乙烯衍生物的分子连接处的负微分电阻（NDR）。结果表明，RSH-NEGF计算表明NDR的起始偏差与测得的趋势非常吻合，将NDR与漏极接触处的轨道定位相关联，并分析了结不对称在NDR中的作用。还将RSH-NEGF结果与其他DFT-NEGF组合进行了比较，以强调将计算研究基于实现具有物理意义的前沿轨道的功能的重要性。最后，还讨论了热可及分子波动对增强NDR电导下降的影响。