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Register a new userStructural Order of the Molecular Adlayer Impacts the Stability of Nanoparticle-on-Mirror Plasmonic Cavities
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Immense field enhancement and nanoscale confinement of light are possible within nanoparticle-on-mirror (NPoM) plasmonic resonators, which enable novel optically-activated physical and chemical phenomena, and render these nanocavities greatly sensitive to minute structural changes, down to the atomic scale. Although a few of these structural parameters, primarily linked to the nanoparticle and the mirror morphology, have been identified, the impact of molecular assembly and organization of the spacer layer between them has often been left uncharacterized. Here, we experimentally investigate how the complex and reconfigurable nature of a thiol-based self-assembled monolayer (SAM) adsorbed on the mirror surface impacts the optical properties of the NPoMs. We fabricate NPoMs with distinct molecular organizations by controlling the incubation time of the mirror in the thiol solution. Afterwards, we investigate the structural changes that occur under laser irradiation by tracking the bonding dipole plasmon mode, while also monitoring Stokes and anti-Stokes Raman scattering from the molecules as a probe of their integrity. First, we find an effective decrease in the SAM height as the laser power increases, compatible with an irreversible change of molecule orientation caused by heating. Second, we observe that the nanocavities prepared with a densely packed and more ordered monolayer of molecules are more prone to changes in their resonance compared to samples with sparser and more disordered SAMs. Our measurements indicate that molecular orientation and packing on the mirror surface play a key role in determining the stability of NPoM structures and hence highlight the under-recognized significance of SAM characterization in the development of NPoM-based applications.
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Hybrid photonic-plasmonic cavities have emerged as a new platform to increase light-matter interaction capable to enhance the Purcell factor in a singular way not attainable with either photonic or plasmonic cavities separately. In the hybrid cavities proposed so far, mainly consisting of metallic bow-tie antennas, the plasmonic gap sizes defined by lithography in a repeatable way are limited to minimum values approx 10 nm. Nanoparticle-on-a-mirror (NPoM) cavities are far superior to achieve the smallest possible mode volumes, as gaps smaller than 1 nm can be created. Here, we design a hybrid cavity that combines a NPoM plasmonic cavity and a dielectric-nanobeam photonic crystal cavity operating at transverse-magnetic (TM) polarization. The metallic nanoparticle can be placed very close (< 1 nm) to the upper surface of the dielectric cavity, which acts as a low-reflectivity mirror. We demonstrate through numerical calculations that this kind of hybrid plasmonic-photonic cavity architecture exhibits quality factors, Q, above 10^{3} and normalized mode volumes, V , down to 10^{ um{-3}}, thus resulting in high Purcell factors (FP approx 10^5), whilst being experimentally feasible with current technology. Our results suggest that hybrid cavities with sub-nm gaps should open new avenues for boosting light-matter interaction in nanophotonic systems.
Orbital angular momentum of light is a core feature in photonics. Its confinement to surfaces using plasmonics has unlocked many phenomena and potential applications. Here we introduce the reflection from structural boundaries as a new degree of freedom to generate and control plasmonic orbital angular momentum. We experimentally demonstrate plasmonic vortex cavities, generating a succession of vortex pulses with increasing topological charge as a function of time. We track the spatio-temporal dynamics of these angularly decelerating plasmon pulse train within the cavities for over 300 femtoseconds using time-resolved Photoemission Electron Microscopy, showing that the angular momentum grows by multiples of the chiral order of the cavity. The introduction of this degree of freedom to tame orbital angular momentum delivered by plasmonic vortices, could miniaturize pump-probe-like quantum initialization schemes, increase the torque exerted by plasmonic tweezers and potentially achieve vortex lattice cavities with dynamically evolving topology.
Controlling absorption and emission of organic molecules is crucial for efficient light-emitting diodes, organic solar cells and single-molecule spectroscopy. Here, a new molecular absorption is activated inside a gold plasmonic nanocavity, and found to break selection rules via spin-orbit coupling. Photoluminescence excitation scans reveal absorption from a normally spin-forbidden singlet to triplet state transition, while drastically enhancing the emission rate by several thousand fold. The experimental results are supported by density functional theory, revealing the manipulation of molecular absorption by nearby metallic gold atoms.
Prospects of using metal hole arrays for the enhanced optical detection of molecular chirality in nanosize volumes are investigated. Light transmission through the holes filled with an optically active material is modeled and the activity enhancement by more than an order of magnitude is demonstrated. The spatial resolution of the chirality detection is shown to be of a few tens of nanometers. From comparing the effect in arrays of cylindrical holes and holes of complex chiral shape, it is concluded that the detection sensitivity is determined by the plasmonic near field enhancement. The intrinsic chirality of the arrays due to their shape appears to be less important.
Dark plasmonic modes have interesting properties, such as a longer lifetime and a narrower linewidth than their radiative counterpart, as well as little to no radiative losses. However, they have not been extensively studied yet due to their optical inaccessibility. Using electron-energy loss (EEL) and cathodoluminescence (CL) spectroscopy, the dark radial breathing modes (RBMs) in thin, monochrystalline gold nanodisks are systematically investigated in this work. It is found that the RBMs can be detected in a CL set-up despite only collecting the far-field. Their visibility in CL is attributed to the breaking of the mirror symmetry by the high-index substrate, creating an effective dipole moment. The outcoupling into the far-field is demonstrated to be enhanced by a factor of 4 by increasing the thickness of the supporting SiN membrane from 5 to 50 nm due to the increased net electric dipole moment in the substrate. Furthermore, it is shown that the resonance energy of RBMs can be easily tuned by varying the diameter of the nanodisk, making them promising candidates for nanophotonic applications.
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