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 metal-optical cavities include their compatibility with a large variety of emitters and their broadband cavity spectra, which enable enhancement of spectrally-broad emitters. Here, we demonstrate a metal- based nanocavity structure that achieves radiative emission rate enhancements of 1000, opening up the possibility of pursuing cavity electrodynamics investigations with intrinsically broad optical emitters, including organic dyes and colloidal quantum dots.
An emitter in the vicinity of a metal nanostructure is quenched by its decay through non-radiative channels, leading to the belief in a zone of inactivity for emitters placed within $<$10nm of a plasmonic nanostructure. Here we demonstrate that in tightly-coupled plasmonic resonators forming nanocavities "quenching is quenched" due to plasmon mixing. Unlike isolated nanoparticles, plasmonic nanocavities show mode hybridization which massively enhances emitter excitation and decay via radiative channels. This creates ideal conditions for realizing single-molecule strong-coupling with plasmons, …
Nanoparticle-on-mirror plasmonic nanocavities, capable of extreme optical confinement and enhancement, have triggered state-of-the-art progress in nanophotonics and development of applications in enhanced spectroscopies and molecular detection. However, the optical quality factor and thus performance of these nanoconstructs are undermined by the granular polycrystalline metal films used as a mirror. Here, we report an atomically smooth single-crystalline platform for low-loss nanocavities using chemically-synthesized gold microflakes as a mirror. Nanocavities constructed using gold nanorods on…
We study the physics of a new type of subwavelength nanocavities. They are based on U-shaped metal-insulator-metal waveguides supporting the excitation of surface plasmon polaritons. The waveguides are simultaneously excited from both sides of the U by incident plane waves. Due to their finite length discrete modes emerge within the nanocavity. We show that the excitation symmetry with respect to the cavity ends permits the observation of even and odd modes. Our investigations include near and far field simulations and predict a strong spectral far field response of the comparable small nanore…
Fabricating nanocavities in which optically-active single quantum emitters are precisely positioned, is crucial for building nanophotonic devices. Here we show that self-assembly based on robust DNA-origami constructs can precisely position single molecules laterally within sub-5nm gaps between plasmonic substrates that support intense optical confinement. By placing single-molecules at the center of a nanocavity, we show modification of the plasmon cavity resonance before and after bleaching the chromophore, and obtain enhancements of $\geq4\times10^3$ with high quantum yield ($\geq50$%). By …
Metallic optical systems can confine light to deep sub-wavelength dimensions, but verifying the level of confinement at these length scales typically requires specialized techniques and equipment for probing the near-field of the structure. We experimentally measured the confinement of a metal-based optical cavity by using the cavity modes themselves as a sensitive probe of the cavity characteristics. By perturbing the cavity modes with conformal dielectric layers of sub-nm thickness using atomic layer deposition, we find the exponential decay length of the modes to be less than 5% of the free…
Strong-coupling of monolayer metal dichalcogenide semiconductors with light offers encouraging prospects for realistic exciton devices at room temperature. However, the nature of this coupling depends extremely sensitively on the optical confinement and the orientation of electronic dipoles and fields. Here, we show how plasmon strong coupling can be achieved in compact robust easily-assembled gold nano-gap resonators at room temperature. We prove that strong coupling is impossible with monolayers due to the large exciton coherence size, but resolve clear anti-crossings for 8 layer devices wit…
Localized plasmonic modes of metallic nanoparticles may hybridize like those of atoms forming a molecule. However, the rapid decay of the plasmonic fields outside the metal severely limits the range of these interactions to tens of nanometers. Herein, we demonstrate very strong coupling of nanocavities in metal films, sparked by propagating surface plasmons and evident even at much larger distances of hundreds of nanometers for the properly selected metal/wavelength combination. Such strong coupling drastically changes the symmetry of the charge distribution around the nanocavities making it a…
In the past decade, advances in nanotechnology have led to the development of plasmonic nanocavities which facilitate light-matter strong coupling in ambient conditions. The most robust example is the nanoparticle-on-mirror (NPoM) structure whose geometry is controlled with subnanometer precision. The excited plasmons in such nanocavities are extremely sensitive to the exact morphology of the nanocavity, giving rise to unexpected optical behaviors. So far, most theoretical and experimental studies on such nanocavities have been based solely on their scattering and absorption properties. Howeve…
There is an active demand to develop efficient nanoscale nonlinear sources for applications in photonic circuitry, quantum optics and biosensing. To this end, plasmonic systems have been utilized to boost the nonlinear signal generation, however high efficiencies of frequency conversion for realistic applications remain a challenge. Metal-insulator-metal (MIM) nanocavities are good candidates for strongly concentrating the fields at the nanoscale to enhance the optical nonlinearities, however they typically suffer from the requirement to have a quadrupolar resonance at the emission wavelength.…
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 molecul…
Strong interactions between surface plasmons in ultra-compact nanocavities and excitons in two dimensional materials have attracted wide interests for its prospective realization of polariton devices at room temperature. Here, we propose a continuous transition from weak coupling to strong coupling between excitons in MoS2 monolayer and highly localized plasmons in ultra-compact nanoantenna. The nanoantenna is assembled by a silver nanocube positioned over a gold film and separated by a dielectric spacer layer. We observed a 1570-fold enhancement in the photoluminescence at weak coupling regim…
When two or more metallic nanoparticles are in close proximity, their plasmonic modes may interact through the near field, leading to additional resonances of the coupled system or to shifts of their resonant frequencies. This process is analogous to atom-hybridization, as had been proposed by Gersten and Nitzan and modeled by Nordlander et al. The coupling between plasmonic modes can be in-phase (symmetric) or out-of-phase (anti-symmetric), reflecting correspondingly, the "bonding" and "anti-bonding" nature of such configurations. Since the incoming light redistributes the charge distribution…
Metal nanoantennas enable the manipulation of light emission and detection at the single photon level by confining light into very small volumes. Emitters coupled to these plasmonic structures are thus ideal candidates for usage in quantum information technology. However, controllably and reproducibly placing quantum emitters into nanocavities has been challenging due to the sizes of the systems involved. Here, we investigate the trapping dynamics of single emitters into nanocavities via optical gradient forces by using single-molecule super-resolution imaging and tracking. We show that molecu…
Recent developments in surface-enhanced Raman scattering (SERS) enable observation of single-bond vibrations in real-time at room temperature. By contrast, mid-infrared (MIR) vibrational spectroscopy is limited to inefficient slow detection. Here we develop a new method for MIR sensing using SERS. This method utilizes nanoparticle-on-foil (NPoF) nanocavities supporting both visible and MIR plasmonic hotspots in the same nano-gap formed by a monolayer of molecules. Molecular SERS signals from individual NPoF nanocavities are modulated in the presence of MIR photons. The strength of this modulat…
Solid-state single-quantum emitters are a crucial resource for on-chip photonic quantum technologies and require efficient cavity-emitter coupling to realize quantum networks beyond the single-node level. Previous approaches to enhance light-matter interactions rely on forming nanocavities around randomly located quantum dots or color centers but lack spatial control of the quantum emitter itself that is required for scaling. Here we demonstrate a deterministic approach to achieve Purcell-enhancement at lithographically defined locations using the sharp corner of a metal nanocube for both elec…
Strong coupling between light and matter is the foundation of promising quantum photonic devices such as deterministic single photon sources, single atom lasers and photonic quantum gates, which consist of an atom and a photonic cavity. Unlike atom-based systems, a strong coupling unit based on an emitter-plasmonic nanocavity system has the potential to bring these devices to the microchip scale at ambient conditions. However, efficiently and precisely positioning a single or a few emitters into a plasmonic nanocavity is challenging. In addition, placing a strong coupling unit on a designated …
Optimizing the shape of nanostructures and nano antennas for specific optical properties has evolved to be a very fruitful activity. With modern fabrication tools a large variety of possibilities is available for shaping both nanoparticles and nanocavities; in particular nanocavities in thin metal films have emerged as attractive candidates for new metamaterials and strong linear and nonlinear optical systems. Here we rationally design metallic nanocavities to boost their Four Wave Mixing response by resonating the optical plasmonic resonances with the incoming and generated beams. The linear …
Lasers are ubiquitous for information storage, processing, communications, sensing, biological research, and medical applications [1]. To decrease their energy and materials usage, a key quest is to miniaturize lasers down to nanocavities [2]. Obtaining the smallest mode volumes demands plasmonic nanocavities, but for these, gain comes from only single or few emitters. Until now, lasing in such devices was unobtainable due to low gain and high cavity losses [3]. Here, we demonstrate a plasmonic nanolaser approaching the single-molecule emitter regime. The lasing transition significantly broade…
We provide a numerical study showing that a bottom reflector is indispensable to achieve unidirectional emission from a photonic-crystal (PhC) nanolaser. First, we study a PhC slab nanocavity suspended over a flat mirror formed by a dielectric or metal substrate. We find that the laser's vertical emission can be enhanced by more than a factor of six compared with the device in the absence of the mirror. Then, we study the situation where the PhC nanocavity is in contact with a flat metal surface. The underlying metal substrate may serve as both an electrical current pathway and a heat sink, wh…
Continuous-wave, high-resolution, ultra-broadband mid-infrared nonlinear spectroscopy with tunable plasmonic nanocavities
Institute of Physics, Ecole Polytechnique Fédérale de Lausanne (EPFL)（洛桑联邦理工学院物理研究所）；State Key Laboratory of Precision Spectroscopy, East China Normal University（华东师范大学精密光谱科学国家重点实验室）
Enhancing magneto-optical effects is crucial for size reduction of key photonic devices based on non-reciprocal propagation of light and to enable active nanophotonics. We disclose a so far unexplored approach that exploits dark plasmons to produce an unprecedented amplification of magneto-optical activity. We designed and fabricated non-concentric magnetoplasmonic-disk/plasmonic-ring-resonator nanocavities supporting multipolar dark modes. The broken geometrical symmetry of the design enables coupling with free-space light and hybridization of dark modes of the ring nanoresonator with the dip…
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 review the latest theoretical advances in the application of the framework of Transformation Optics for the analytical description of deeply sub-wavelength electromagnetic phenomena. First, we present a general description of the technique, together with its usual exploitation for metamaterial conception and optimization in different areas of wave physics. Next, we discuss in detail the design of plasmonic metasurfaces, including the description of singular geometries which allow for broadband absorption in ultrathin platforms. Finally, we discuss the quasi-analytical treatment of plasmon-e…
Monolayer transition metal dichalcogenides, coupled to metal plasmonic nanocavities, have recently emerged as new platforms for strong light-matter interactions. These systems are expected to have nonlinear optical properties that will enable them to be used as entangled photon sources, compact wave-mixing devices, and other elements for classical and quantum photonic technologies. Here we report the first experimental investigation of the nonlinear properties of these strongly coupled systems, by observing second harmonic generation from a WSe2 monolayer strongly coupled to a single gold nano…
We have conducted a theoretical study of harmonic generation from a silver grating having slits filled with GaAs. By working in the enhanced transmission regime, and by exploiting phase-locking between the pump and its harmonics, we guarantee strong field localization and enhanced harmonic generation under conditions of high absorption at visible and UV wavelengths. Silver is treated using the hydrodynamic model, which includes Coulomb and Lorentz forces, convection, electron gas pressure, plus bulk X(3) contributions. For GaAs we use nonlinear Lorentz oscillators, with characteristic X(2) and…
Plasmon-mediated superradiance for molecules around metallic nanospheres was proposed ten years ago. However, its demonstration has not been achieved yet due to the experimental difficulty of positioning molecules, and the theoretical limitation to the enhanced collective rate of low excited molecules. In this Letter, we propose that the ultrafast plasmon-mediated superradiant pulses can be observed with strongly excited methylene blue molecules standing vertically inside gold nanoparticle-on-mirror nanocavities. Our simulations indicate that in this system the molecules could interact with ea…
Harmonic generation mechanisms are of great interest in nanoscience and nanotechnology, since they allow generating visible light by using near-infrared radiation, which is particularly suitable for its endless applications in bio-nanophotonics and opto-electronics. In this context, multilayer metal-dielectric nanocavities are widely used for light confinement and waveguiding at the nanoscale. They exhibit intense and localized resonances that can be conveniently tuned in the near-infrared and are therefore ideal for enhancing nonlinear effects in this spectral range. In this work, we experime…
Room-temperature strong coupling between plasmonic nanocavities and monolayer semiconductors is a prominent path towards efficient, integrated light-matter interactions. However, designing such systems is challenging due to the nontrivial dependence of the strong coupling on various properties of the cavity and emitter, as well as the subwavelength scale of the interaction. In this work, we develop a methodology for obtaining hybrid nanostructures consisting of plasmonic metasurfaces coupled to atomically thin WS2 layers, exhibiting extreme values of Rabi splitting, by inverse design of the ne…
Optical isolator remains one of the main missing elements for photonic integrated circuits despite several decades of research. The best solutions up to now are based on transverse magneto-optical effect using either narrow-band resonators or high-gyrotropy magneto-optical materials with difficult integration on usual photonic platforms. We propose in this paper a radically new concept which enables performing broad-band non-reciprocal transmission even in the case of low-gyrotropy material. The principle explores the separation of back and forth light paths, due to the magneto-biplasmonic eff…
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…
Plasmonic nanocavities enable the confinement of molecules and electromagnetic fields within nano-metric volumes. As a consequence, the molecules experience a remarkably strong interaction with the electromagnetic field, to such an extent that the quantum states of the system become hybrids between light and matter: polaritons. Here we present a non-perturbative method to simulate the emerging properties of such polaritons: it combines a high-level quantum chemical description of the molecule with a quantized description of the localized surface plasmons in the nanocavity. We apply the method …
Plasmonic nanoparticles provide an ideal environment for the enhancement of fluorescent emission. On the one hand, they locally amplify the electromagnetic fields, increasing the emitter excitation rate, and on the other hand, they provide a high local density of states that accelerates spontaneous emission. However, when the emitter is placed in close proximity to a single metal nanoparticle, the number of nonradiative states increases dramatically, causing the fluorescence to quench. It has been predicted theoretically that, through a judicious placing of the emitter, fluorescence in plasmon…
Plasmonic nanocavities have proven to be a powerful optical platform for confining light at a length scale much smaller than the diffraction limit. Enhanced electromagnetic fields within the cavity mode volume enable multiple significant effects that lead to applications in both the linear and nonlinear optical regimes. In this work, we demonstrate enhanced second harmonic generation from individual plasmonic nanopatch antennas which are formed by separating silver nanocubes from a smooth gold film using a sub-10 nm zinc oxide spacer layer. When the nanopatch antennas are excited at their fund…
We analyze how the photorelaxation dynamics of a molecule can be controlled by modifying its electromagnetic environment using a nanocavity mode. In particular, we consider the photorelaxation of the RNA nucleobase uracil, which is the natural mechanism to prevent photodamage. In our theoretical work, we identify the operative conditions in which strong coupling with the cavity mode can open an efficient photoprotective channel, resulting in a relaxation dynamics twice as fast than the natural one. We rely on a state-of-the-art chemically-detailed molecular model and a non-Hermitian Hamiltonia…
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…
Ultrafast emission rates obtained from quantum emitters coupled to plasmonic nanoantennas have recently opened fundamentally new possibilities in quantum information and sensing applications. Plasmonic nanoantennas greatly improve the brightness of quantum emitters by dramatically shortening their fluorescence lifetimes. Gap plasmonic nanocavities that support strongly confined modes are of particular interest for such applications. We demonstrate single-photon emission from nitrogen-vacancy (NV) centers in nanodiamonds coupled to nanosized gap plasmonic cavities with internal mode volumes abo…
Influence of metal nanoparticles on whispering gallery modes of a microcavity
Indian Institute of Technology Madras（印度马德拉斯理工学院）；Indian Institute of Technology Patna（印度巴特那理工学院）；Applied Materials Inc.（应用材料公司）；Optoelectronics Research Centre, University of Southampton（南安普顿大学光电研究中心）；New York University Tandon School of Engineering（纽约大学坦登工程学院）
