Plasmonic Response of Metallic Nanojunctions Driven by Single Atom Motion: Quantum Transport Revealed in Optics

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• 作者：Federico Marchesin ; Peter Koval ; Marc Barbry ; Javier Aizpurua ; Daniel Sánchez-Portal
• 刊名：ACS Photonics
• 出版年：2016
• 出版时间：February 17, 2016
• 年：2016
• 卷：3
• 期：2
• 页码：269-277
• 全文大小：613K
• ISSN：2330-4022

文摘

The correlation between transport properties across subnanometric metallic gaps and the optical response of the system is a complex effect that is determined by the fine atomic-scale details of the junction structure. As experimental advances are progressively accessing transport and optical characterization of smaller nanojunctions, a clear connection between the structural, electronic, and optical properties in these nanocavities is needed. Using ab initio calculations, we present here a study of the simultaneous evolution of the structure and the optical response of a plasmonic junction as the particles forming the cavity, two Na₃₈₀ clusters, approach and retract. Atomic reorganizations are responsible for a large hysteresis of the plasmonic response of the system, which shows a jump-to-contact instability during the approach process and the formation of an atom-sized neck across the junction during retraction. Our calculations demonstrate that, due to the quantization of the conductance in metal nanocontacts, atomic-scale reconfigurations play a crucial role in determining the optical response of the whole system. We observe abrupt changes in the intensities and spectral positions of the dominating plasmon resonances and find a one-to-one correspondence between these jumps and those of the quantized transport as the neck cross-section diminishes. These results reveal an important connection between transport and optics at the atomic scale, which is at the frontier of current optoelectronics and can drive new options in optical engineering of signals driven by the motion and manipulation of single atoms.