Conductance Growth of Single-Cluster Junctions with Increasing Sizes

Quantum-tunneling-based nanoelectronics has the potential for the miniaturization of electronics toward the sub-5 nm scale. However, the nature of phase-coherent quantum tunneling leads to the rapid decays of the electrical conductance with tunneling transport distance, especially in organic molecul...

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Published in:Journal of the American Chemical Society 2022-08, Vol.144 (34), p.15680-15688
Main Authors: Feng, Anni, Hou, Songjun, Yan, Juanzhu, Wu, Qingqing, Tang, Yongxiang, Yang, Yang, Shi, Jia, Xiao, Zong-Yuan, Lambert, Colin J., Zheng, Nanfeng, Hong, Wenjing
Format: Article
Language:English
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Summary:Quantum-tunneling-based nanoelectronics has the potential for the miniaturization of electronics toward the sub-5 nm scale. However, the nature of phase-coherent quantum tunneling leads to the rapid decays of the electrical conductance with tunneling transport distance, especially in organic molecule-based nanodevices. In this work, we investigated the conductance of the single-cluster junctions of a series of atomically well-defined silver nanoclusters, with varying sizes from 0.9 to 3.0 nm, using the mechanically controllable break junction (MCBJ) technique combined with quantum transport theory. Our charge transport investigations of these single-cluster junctions revealed that the conductance grows with increasing cluster size. The conductance decay constant was determined to be ∼−0.4 nm–1, which is of opposite sign to that of organic molecules. Comparison between experiment and theory reveals that although charge transport through the silver single-cluster junctions occurs via phase-coherent tunneling, this is compensated by a rapid decrease in the energy gap between the highest occupied molecular orbital and the lowest unoccupied molecular orbital (HOMO-LUMO gap) with size and the increase in the electrode–cluster coupling, which results in their conductance increase up to lengths of ∼3.0 nm. These results demonstrate that such families of nanoclusters provide unique bottom-up building blocks for the fabrication of nanodevices in the sub-5 nm size range.
ISSN:0002-7863
1520-5126
DOI:10.1021/jacs.2c05856