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Highly-efficient electrically-driven localized surface plasmon source enabled by resonant inelastic electron tunneling.

ABSTRACT: On-chip plasmonic circuitry offers a promising route to meet the ever-increasing requirement for device density and data bandwidth in information processing. As the key building block, electrically-driven nanoscale plasmonic sources such as nanoLEDs, nanolasers, and nanojunctions have attracted intense interest in recent years. Among them, surface plasmon (SP) sources based on inelastic electron tunneling (IET) have been demonstrated as an appealing candidate owing to the ultrafast quantum-mechanical tunneling response and great tunability. However, the major barrier to the demonstrated IET-based SP sources is their low SP excitation efficiency due to the fact that elastic tunneling of electrons is much more efficient than inelastic tunneling. Here, we remove this barrier by introducing resonant inelastic electron tunneling (RIET)-follow a recent theoretical proposal-at the visible/near-infrared (NIR) frequencies and demonstrate highly-efficient electrically-driven SP sources. In our system, RIET is supported by a TiN/Al₂O₃ metallic quantum well (MQW) heterostructure, while monocrystalline silver nanorods (AgNRs) were used for the SP generation (localized surface plasmons (LSPs)). In principle, this RIET approach can push the external quantum efficiency (EQE) close to unity, opening up a new era of SP sources for not only high-performance plasmonic circuitry, but also advanced optical sensing applications.

SUBMITTER: Qian H

PROVIDER: S-EPMC8149681 | biostudies-literature |

REPOSITORIES: biostudies-literature

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Project description:Cross-conjugated molecules are known to exhibit destructive quantum interference, a property that has recently received considerable attention in single-molecule electronics. Destructive quantum interference can be understood as an antiresonance in the elastic transmission near the Fermi energy and leading to suppressed levels of elastic current. In most theoretical studies, only the elastic contributions to the current are taken into account. In this paper, we study the inelastic contributions to the current in cross-conjugated molecules and find that while the inelastic contribution to the current is larger than for molecules without interference, the overall behavior of the molecule is still dominated by the quantum interference feature. Second, an ongoing challenge for single molecule electronics is understanding and controlling the local geometry at the molecule-surface interface. With this in mind, we investigate a spectroscopic method capable of providing insight into these junctions for cross-conjugated molecules: inelastic electron tunneling spectroscopy (IETS). IETS has the advantage that the molecule interface is probed directly by the tunneling current. Previously, it has been thought that overtones are not observable in IETS. Here, overtones are predicted to be strong and, in some cases, the dominant spectroscopic features. We study the origin of the overtones and find that the interference features in these molecules are the key ingredient. The interference feature is a property of the transmission channels of the π system only, and consequently, in the vicinity of the interference feature, the transmission channels of the σ system and the π system become equally transmissive. This allows for scattering between the different transmission channels, which serves as a pathway to bypass the interference feature. A simple model calculation is able to reproduce the results obtained from atomistic calculations, and we use this to interpret these findings.

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Highly-efficient electrically-driven localized surface plasmon source enabled by resonant inelastic electron tunneling.

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