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.
We refute all claims of the "Comment on "Normalization of quasinormal modes in leaky optical cavities and plasmonic resonators" " by E. A. Muljarov and W. Langbein (arXiv:1602.07278v1). Based entirely on information already contained in our original article (P. T. Kristensen, R.-C. Ge and S. Hughes, Physical Review A 92, 053810 (2015)), we dismiss every point of criticism as being completely unjustified and point out how important parts of our argumentation appear to have been overlooked by the Comment Authors. In addition, we provide additional calculations showing directly the link between t…
Recently, Kristensen, Ge and Hughes have compared [Phys. Rev. A 92, 053810 (2015)] three different methods for normalization of quasinormal modes in open optical systems, and concluded that they all provide the same result. We show here that this conclusion is incorrect and illustrate that the normalization of [Opt. Lett. 37, 1649 (2012)] is divergent for any optical mode having a finite quality factor, and that the Silver-Mueller radiation condition is not fulfilled for quasinormal modes.
Plasmon polaritons in van der Waals (vdW) materials hold promise for next-generation photonics. The ability to deterministically imprint spatial patterns of high carrier density in cavities and circuitry with nanoscale features underlies future progress in nonlinear nanophotonics and strong light-matter interactions. Here, we demonstrate a general strategy to atomically imprint low-loss graphene plasmonic structures using oxidation-activated charge transfer (OCT). We cover graphene with a monolayer of WSe$_2$, which is subsequently oxidized into high work-function WOx to activate charge transf…
We measured a change in the current transport of an antenna-coupled, multi-gate, GaAs/AlGaAs field-effect transistor when terahertz electromagnetic waves irradiated the transistor and attribute the change to bolometric heating of the electrons in the two-dimensional electron channel. The observed terahertz absorption spectrum indicates coherence between plasmons excited under adjacent biased device gates. The experimental results agree quantitatively with a theoretical model we developed that is based on a generalized plasmonic transmission line formalism and describes an evolution of the plas…
We discuss three formally different formulas for normalization of quasinormal modes currently in use for modeling optical cavities and plasmonic resonators and show that they are complementary and provide the same result. Regardless of the formula used for normalization, one can use the norm to define an effective mode volume for use in Purcell factor calculations.
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…
We found that very strong negative optical pressure can be induced in plasmonic cavities by LC resonance. This interesting effect could be described qualitatively by a Lagrangian model which shows that the negative optical pressure is driven by the internal inductance and the kinetic energy of the conduction electrons. If the metal is replaced by perfect conductors, the optical pressure becomes much smaller and positive.
We introduce a second quantization scheme based on quasinormal modes, which are the dissipative modes of leaky optical cavities and plasmonic resonators with complex eigenfrequencies. The theory enables the construction of multi-plasmon/photon Fock states for arbitrary three-dimensional dissipative resonators and gives a solid understanding to the limits of phenomenological dissipative Jaynes-Cummings models. In the general case, we show how different quasinormal modes interfere through an off-diagonal mode coupling and demonstrate how these results affect cavity-modified spontaneous emission.…
We design a polarization-sensitive resonator for use in midinfrared photodetectors, utilizing a photonic crystal cavity and a single or double-metal plasmonic waveguide to achieve enhanced detector efficiency due to superior optical confinement within the active region. As the cavity is highly frequency and polarization-sensitive, this resonator structure could be used in chip-based infrared spectrometers and cameras that can distinguish among different materials and temperatures to a high degree of precision.
Electromagnetic cavity modes in photonic and plasmonic resonators offer rich and attractive regimes for tailoring the properties of light-matter interactions. Yet there is a disturbing lack of a precise definition for what constitutes a cavity mode, and as a result their mathematical properties remain largely unspecified. The lack of a definition is evidenced in part by the diverse nomenclature at use - "resonance", "leaky mode", "quasimode", to name but a few - suggesting that the dissipative nature of cavity modes somehow makes them different from other modes, but an explicit distinction is …
Spin defects in hexagonal boron nitride, and specifically the negatively charged boron vacancy (VB) centres, are emerging candidates for quantum sensing. However, the VB defects suffer from low quantum efficiency and as a result exhibit weak photoluminescence. In this work, we demonstrate a scalable approach to dramatically enhance the VB- emission by coupling to a plasmonic gap cavity. The plasmonic cavity is composed of a flat gold surface and a silver cube, with few-layer hBN flakes positioned in between. Employing these plasmonic cavities, we extracted two orders of magnitude in photolumin…
In this article, we present a numerical study of the optical properties of a metal nanowire interacting with a localized cavity in a two dimensional photonic crystal. The nature of the modes, their wavelength and width are investigated as a function of the particle radius. It is shown in particular that a particle with diameter about the lattice constant presents very narrow resonances corresponding to hybrid photonic-plasmonic modes, where increased lifetime is attributed to the decrease of the radiative losses by interaction with the photonic crystal. These results open interesting applicati…
Molecular vibrations and their dynamics are of outstanding importance for electronic and thermal transport in nanoscale devices as well as for molecular catalysis. The vibrational dynamics of <100 molecules are studied through three-colour time-resolved coherent anti-Stokes Raman spectroscopy (trCARS) using plasmonic nanoantennas. This isolates molecular signals from four-wave mixing (FWM), while using exceptionally low nanowatt powers to avoid molecular damage via single-photon lock-in detection. FWM is found to be strongly suppressed in nm-wide plasmonic gaps compared to plasmonic nanopartic…
We demonstrate that the surface second-harmonic generation can lead to the formation of nonlinear plasmonic whispering-gallery modes (WGMs) in microcavities made of metallic nanowires. Since these WGMs are excited by induced surface nonlinear dipoles, they can be generated even when they are not coupled to the radiation continuum. Consequently, the quality factor of these nonlinear modes can be as large as the theoretical limit imposed by the optical losses in the metal. Remarkably, our theoretical analysis shows that nonlinear plasmonic WGMs are characterized by fractional azimuthal modal num…
We demonstrate an approach, based on plasmonic apertures and gratings, to enhance the radiative decay rate of single NV centers in diamond, while simultaneously improving their collection efficiency. Our structures are based on metallic resonators formed by surrounding sub-wavelength diamond nanoposts with a silver film, which can enhance the spontaneous emission rate of an embedded NV center. However, the collection efficiency of emitted photons remains low due to losses to surface plasmons and reflections at the diamond-air interface. In this work, we mitigate photon losses into these channe…
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 ho…
Plasmon-enhanced Raman scattering can push single-molecule vibrational spectroscopy beyond a regime addressable by classical electrodynamics. We employ a quantum electrodynamics (QED) description of the coherent interaction of plasmons and molecular vibrations that reveal the emergence of nonlinearities in the inelastic response of the system. For realistic situations, we predict the onset of \textit{phonon-stimulated Raman scattering} and an counter-intuitive dependence of the anti-Stokes emission on the frequency of excitation. We further show that this novel QED framework opens a venue to a…
By means of ab-initio time dependent density functional theory calculations carried out on an prototypical hybrid plasmonic device (two metallic nanoparticles bridged by a one-atom junction), we demonstrate the strong interplay between photoinduced excitation of localized surface plasmons and electron transport through the single atom. Such an interplay is remarkably sensitive to the atomic orbitals of the junction. Therefore, we show the possibility of a twofold tuning (plasmonic response and photoinduced current across the juntion) just by changing a single atom in the device.
Purcell enhancement of photogalvanic currents in a van der Waals plasmonic self-cavity
Max Planck Institute for the Structure and Dynamics of Matter（马克斯·普朗克物质结构与动力学研究所）；Center for Free-Electron Laser Science（自由电子激光科学中心）；Department of Physics, Columbia University（哥伦比亚大学物理系）
Over the last few years, optical nanoantennas are continuously attracting interest owing to their ability to efficiently confine, localize resonance, and significantly enhanced electromagnetic fields at subwavelength scale. However, such strong confinement can be further enhanced by using an appropriate combination of optical nanoantenna and Slanted Bound states in the continuum cavities. Here, we propose to synergistically bridge the plasmonic nanoantenna and high optical quality-factor cavities to numerically demonstrate three orders of magnitude local intensity enhancement. The proposed hyb…
The strong interaction of individual quantum emitters with resonant cavities is of fundamental interest for understanding light matter interactions. Plasmonic cavities hold the promise of attaining the strong coupling regime even under ambient conditions and within subdiffraction volumes. Recent experiments revealed strong coupling between individual plasmonic structures and multiple organic molecules, but so far strong coupling at the limit of a single quantum emitter has not been reported. Here we demonstrate vacuum Rabi splitting, a manifestation of strong coupling, using silver bowtie plas…
By modifying the density of optical states at the location of an emitter, weak cavity-emitter coupling can enable a host of potential applications in quantum optics, from the development of low- threshold lasers to brighter single-photon sources for quantum cryptography. Although some of the first demonstrations of spontaneous emission modification occurred in metallic structures, it was only after the recent demonstration of cavity quantum electrodynamics effects in dielectric optical cavities that metal-based optical cavities were considered for quantum optics applications. Advantages of met…
We have combined atomic layer lithography and template stripping to produce a new class of substrates for surface-enhanced infrared absorption (SEIRA) spectroscopy. Our structure consists of a buried and U-shaped metal-insulator-metal waveguide whose folded vertical arms efficiently couple normally incident light. The insulator is formed by atomic layer deposition (ALD) of Al2O3 and precisely defines the gap size. The buried nanocavities are protected from contamination by a silicon template until ready for use and exposed by template stripping on demand. The exposed nanocavity generates stron…
Plasmonic cavities can confine electromagnetic radiation to deep sub-wavelength regimes. This facilitates strong coupling phenomena to be observed at the limit of individual quantum emitters. Here we report an extensive set of measurements of plasmonic cavities hosting one to a few semiconductor quantum dots. Scattering spectra show Rabi splitting, demonstrating that these devices are close to the strong coupling regime. Using Hanbury Brown and Twiss interferometry, we observe non-classical emission, allowing us to directly determine the number of emitters in each device. Surprising features i…
Disorder-Engineered Hybrid Plasmonic Cavities for Emission Control of Defects in hBN
Middle East Technical University（中东技术大学）；Izmir Institute of Technology（伊兹密尔理工大学）；Tampere University（坦佩雷大学）；Eindhoven University of Technology（埃因霍温理工大学）；Sabancı University（萨班哲大学）
We describe an efficient near-field to far-field transformation for optical quasinormal modes, which are the dissipative modes of open cavities and plasmonic resonators with complex eigenfrequencies. As an application of the theory, we show how one can compute the reservoir modes (or regularized quasinormal modes) outside the resonator, which are essential to use in both classical and quantum optics. We subsequently demonstrate how to efficiently compute the quantum optical parameters necessary in the theory of quantized quasinormal modes [Franke et al., Phys. Rev. Lett. 122, 213901 (2019)]. T…
Half-wave plasmonic nanolasers near the localization limit
Harvard Medical School（哈佛医学院）；Massachusetts General Hospital（麻省总医院）；Rice University（莱斯大学）；Harvard-MIT Health Sciences and Technology（哈佛-麻省理工学院健康科学与技术）；Massachusetts Institute of Technology（麻省理工学院）
We present an analytical study to the structure-modulated plasmonic angular momentum trapped on periodic metal-dielectric nano-wedges in the core region of a sectorial indefinite metamaterial. Employing a transfer-matrix calculation and a conformal-mapping technique, our theory is capable of dealing with realistic configurations of arbitrary sector numbers and rounded wedge tips. We demonstrate that in the deep-subwavelength regime strong electric field carrying high azimuthal variation can exist within only ten-nanometer length scale close to the structural center, and is naturally bounded by…
Material-Specific Mapping of Plasmonic Modal Dispersion via Discrete Momentum-Space Probes
Moulay Ismail University（穆莱·伊斯梅尔大学）；Laboratory of Optics, Information Processing, Mechanics, Energetics and Electronics, Department of Physics, Moulay Ismail University（光学、信息处理、力学、能源与电子实验室，物理系，穆莱·伊斯梅尔大学）；Institut d’Electronique, de Microélectonique et de Nanotechnologie, UMR CNRS 8520, Département de Physique, Université de Lille（电子、微电子和纳米技术研究所，CNRS联合研究单位8520，物理系，里尔大学）
