ABSTRACT:The optical response of a plasmonic gapantenna is mainly determined by the Coulomb interaction of the two constituent arms of the antenna. Using rigorous calculations supported by simple analytical models, we observe how the morphology of a nanometric gap separating two metallic rods dramatically modifies the plasmonic response. In the case of rounded terminations at the gap, a conventional set of bonding modes is found that red-shifts strongly with decreasing separation. However, in the case of flat surfaces, a distinctly different situation is found with the appearance of two sets of modes: (i) strongly radiating longitudinal antenna plasmons (LAPs), which exhibit a red-shift that saturates for very narrow gaps, and (ii) transverse cavity plasmons (TCPs) confined to the gap, which are weakly radiative and strongly dependent on the separation distance between the two arms. The two sets of modes can be independently tuned, providing detailed control of both the near-and far-field response of the antenna. We illustrate these properties also with an application to larger infrared gap-antennas made of polar materials such as SiC. Finally we use the quantum corrected model (QCM) to show that the morphology of the gap has a dramatic influence on the plasmonic response also for subnanometer gaps. This effect can be crucial for the correct interpretation of charge transfer processes in metallic cavities where quantum effects such as electron tunneling are important. KEYWORDS: optical antennas, plasmonic gaps, cavity modes, antenna modes, quantum effects, quantum corrected model, plasmonic resonances, phononic resonances M etallic particles can show a strong optical response due to the excitation of resonant plasmonic modes, making light manipulation possible in structures of dimensions comparable to or smaller than the wavelength. Typical effects are the efficient emission of radiation and the concentration of the incoming light energy in small volumes, thus justifying the characterization of these metallic structures as optical antennas. 1,2 Modifications of the geometry, size, or materials 3−6 affect the optical response. In particular, the resonant modes of optical antennas consisting of two metallic particles separated by a narrow gap show significant sensitivity to the properties of the gap. 7−19 In an optical antenna, a change in geometry can simultaneously affect both the strength and wavelength of its resonances and modify both the far-and near-field response. It is usually a challenge, for example, to control the near field without affecting the far-field properties. In this theoretical work, we discuss how the coexistence 20,21 of two different and mostly spectrally decoupled types of modes in flat-gap antennas, namely, transverse cavity modes 22 and longitudinal antenna modes, 15 allows for a more flexible tuning of far-and near-field properties compared to that of the conventional spherical-gap terminations 13,17,23 The importance of the gap morphology 24 is particularly pronounced for nanometer-...

We employ near-infrared single-cycle pulse pairs to drive interferometric autocorrelations of the ultrafast current produced by optical field emission at the nanogap of a single plasmonic nanocircuit. This highly nonlinear process depends fully on the precise temporal field profile of the optical driving pulse. Current autocorrelations are acquired with sub-femtosecond temporal resolution as a function of both pulse delay and absolute carrierenvelope phase. In this way, we study the ultrafast dynamics of electronic nanotransport. Quantitative Additional information

Plasmonic multinanoparticle systems exhibit collective electric and magnetic resonances that are fundamental for the development of state-of-the-art optical nanoantennas, metamaterials, and surface-enhanced spectroscopy substrates. While electric dipolar modes have been investigated in both the classical and quantum realm, little attention has been given to magnetic and other "dark" modes at the smallest dimensions. Here, we study the collective electric, magnetic, and dark modes of colloidally synthesized silver nanosphere trimers with varying interparticle separation using scanning transmission electron microscopy (STEM) and electron energy-loss spectroscopy (EELS). This technique enables direct visualization and spatially selective excitation of individual trimers, as well as manipulation of the interparticle distance into the subnanometer regime with the electron beam. Our experiments reveal that bonding electric and magnetic modes are significantly impacted by quantum effects, exhibiting a relative blueshift and reduced EELS amplitude compared to classical predictions. In contrast, the trimer's electric dark mode is not affected by quantum tunneling for even Ångström-scale interparticle separations. We employ a quantum-corrected model to simulate the effect of electron tunneling in the trimer which shows excellent agreement with experimental results. This understanding of classical and quantum-influenced hybridized modes may impact the development of future quantum plasmonic materials and devices, including Fano-like molecular sensors and quantum metamaterials.