Hyllested Louise O H, Prestholm Idunn, Solomon Gemma C
Department of Chemistry and Nano-Science Center, University of Copenhagen, Copenhagen 2100, Denmark.
NNF Quantum Computing Programme, Niels Bohr Institute, University of Copenhagen, Copenhagen 2100, Denmark.
ACS Nanosci Au. 2024 Oct 4;4(6):426-434. doi: 10.1021/acsnanoscienceau.4c00041. eCollection 2024 Dec 18.
Destructive quantum interference (DQI) leads to a decrease in the conductance of certain well-documented molecules. Experimental observations have revealed both direct and indirect manifestations of DQI, although a comprehensive understanding of the underlying causes of these distinct outcomes remains elusive. In both cases, DQI lowers the conductance, but only the direct case exhibits a characteristic V-shaped dip in differential conductance. Currently, the direct signature has exclusively been observed in monolayers and gated single-molecule systems. In this study, we employ density functional theory to elucidate a plausible explanation for the absence of a direct DQI signature in single molecules. Specifically, we attribute the direct DQI signature to a resonance shift induced by intermolecular interactions, which are absent in the individual molecules. By illustrating the impact of these intermolecular interactions, we emphasize the need for explicit treatment of intermolecular interactions when simulating monolayers.
破坏性量子干涉（DQI）会导致某些有充分记录的分子的电导降低。实验观察揭示了DQI的直接和间接表现，尽管对这些不同结果的根本原因的全面理解仍然难以捉摸。在这两种情况下，DQI都会降低电导，但只有直接情况在微分电导中呈现出特征性的V形凹陷。目前，直接特征仅在单层和门控单分子系统中被观察到。在本研究中，我们采用密度泛函理论来阐明单分子中不存在直接DQI特征的一个合理原因。具体而言，我们将直接DQI特征归因于分子间相互作用引起的共振位移，而在单个分子中不存在这种相互作用。通过说明这些分子间相互作用的影响，我们强调在模拟单层时需要明确处理分子间相互作用。
