The Purcell factor is the standard figure of merit for spontaneous emission enhancement in microcavities, that has also been proposed to describe emission enhancements for plasmonic resonances. A comparison is made of quality factor, mode volume and Purcell factor for single and coupled plasmon spheres to exact calculations of emission rates. The paper explains why the Purcell factor is not appropriate for plasmon antennas.
The Purcell factor $F_p$ is a key quantity in cavity quantum electrodynamics (cQED) that quantifies the coupling rate between a dipolar emitter and a cavity mode. Its simple form $F_p\propto Q/V$ unravels the possible strategies to enhance and control light-matter interaction. Practically, efficient light-matter interaction is achieved thanks to either i) high quality factor $Q$ at the basis of cQED or ii) low modal volume $V$ at the basis of nanophotonics and plasmonics. In the last decade, strong efforts have been done to derive a plasmonic Purcell factor in order to transpose cQED concepts …
The use of metamaterial as a way to mitigate the negative effects of absorption in metals on the Purcell effect in metal-dielectric structures is investigated. A layered metal-dielectric structure is considered as an anisotropic medium in the long-wavelength limit. The dispersion of the surface plasmon appearing at the boundary between such a structure and a different dielectric material, as well as the position of the peak in the local density of states are studied for various combinations of materials and filling factors of the periodic structure. The calculated frequency dependence of the P…
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, …
Purcell effect of nitrogen-vacancy centers in nanodiamond coupled to propagating and localized surface plasmons revealed by photon-correlation cathodoluminescence
Integrated photonic circuits are an integral part of all-optical and on-chip quantum information processing and quantum computer. Deterministically integrated single-photon sources in nanoplasmonic circuits lead to densely packed scalable quantum logic circuits operating beyond the diffraction limit. Here, we report the coupling efficiency of single-photon sources to the plasmonic waveguide, characteristic transmission spectrum, propagation length, decay length, and plasmonic Purcell factor. We simulated the transmission spectrum to find the appropriate wavelength for various width of the diel…
Hybrid photonic-plasmonic cavities can be tailored to display high Q-factors and extremely small mode volumes simultaneously, which results in large values of the Purcell factor, FP. Amongst the different hybrid configurations, those based on a nanoparticle-on-a-mirror (NPoM) plasmonic cavity provide one of the lowest mode volumes, though so far their operation has been constrained to wavelengths below 1 μm. Here, we propose a hybrid configuration consisting of a silicon photonic crystal cavity with a slot at its center in which a gold nanoparticle is introduced. This hybrid system operates at…
The Purcell effect - the modification of the spontaneous emission rate in presence of resonant cavities or other resonant objects - is a fundamental effect of quantum electrodynamics. However, a change of the emission rate caused by environment different from free space has a classical counterpart. Not only quantum emitters, but any small antenna tuned to the resonance is an oscillator with radiative losses, and the influence of the environment on its radiation can be understood and measured in terms of the antenna radiation resistance. We present a general approach which is applicable to meas…
For integrated optical devices, realistic utilization of the superior wave-matter interaction offered by plasmonics is typically impeded by optical losses, which increase rapidly with mode volume reduction. Although coupled-mode plasmonic structures has demonstrated effective alleviation of the loss-confinement trade-off, stringent symmetry requirements must be enforced for such reduction to prevail. In this work, we report an asymmetric plasmonic waveguide that is not only capable of guiding subwavelength optical mode with long-range propagation, but is also unrestricted by structural, materi…
The local density of optical states governs an emitters lifetime and quantum yield through the Purcell effect. It can be modified by a surface plasmon electromagnetic field, but such a field has a spatial extension limited to a few hundreds of nanometers, which complicates the use of optical methods to spatially probe the emitter-plasmon coupling. Here we show that a combination of electron-based imaging, spectroscopies and photon-based correlation spectroscopy enables measurement of the Purcell effect with nanometer and nanosecond spatio-temporal resolutions. Due to the large variability of r…
Using either quasi-static approximation or exact Mie expansion, we characterize the localized surface plasmons supported by a metallic spherical nanoparticle. We estimate the quality factor $Q_n$ and define the effective volume $V_n$ of the $n^{th}$ mode in a such a way that coupling strength with a neighbouring dipolar emitter is proportional to the ratio $Q_n/V_n$ (Purcell factor). The role of Joule losses, far-field scattering and mode confinement in the coupling mechanism are introduced and discussed with simple physical understanding, with particular attention paid to energy conservation.
The vast majority of proteins are intrinsically fluorescent in the ultraviolet, thanks to the emission from their tryptophan and tyrosine amino-acid constituents. However, the protein autofluorescence quantum yields are generally very low due to the prevailing quenching mechanisms by other amino acids inside the protein. This motivates the interest to enhance the radiative emission rate of proteins using nanophotonic structures. Although there have been numerous reports of Purcell effect and local density of optical states (LDOS) control in the visible range using single dipole quantum emitter…
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）
The Purcell effect is defined as the modification of spontaneous decay in the presence of a resonator, and in plasmonics it is usually associated with the large local-field enhancement in "hot spots" due to surface plasmon polaritons. Here we propose a novel strategy for enhancing the Purcell effect through engineering the radiation directivity without a strict requirement of the local field enhancement. Employing this approach, we demonstrate how to enhance the Purcell effect by two orders of magnitude in all-dielectric nanostructures recently suggested as building blocks of low-loss nanophot…
The radiation dynamics of optical emitters can be manipulated by properly designed material structures providing high local density of photonic states, a phenomenon often referred to as the Purcell effect. Plasmonic nanorod metamaterials with hyperbolic dispersion of electromagnetic modes are believed to deliver a significant Purcell enhancement with both broadband and non-resonant nature. Here, we have investigated finite-size cavities formed by nanorod metamaterials and shown that the main mechanism of the Purcell effect in these hyperbolic resonators originates from the cavity hyperbolic mo…
Strong interaction between light and a single quantum emitter is essential to a great number of applications, including single photon sources. Microcavities and plasmonic antennas have been used frequently to enhance these interactions through the Purcell effect. Both can provide large emission enhancements: the cavity typically through long photon lifetimes (high $Q$), and the antenna mostly through strong field enhancement (low mode volume $V$). In this work, we demonstrate that a hybrid system, which combines a cavity and a dipolar antenna, can achieve stronger emission enhancements than th…
We develop a theory for spontaneous decay of a quantum emitter (QE) situated near metal-dielectric structure supporting localized surface plasmons. If plasmon resonance is tuned close to the QE emission frequency, the emission is enhanced due to energy transfer from the QE to a localized plasmon mode followed by photon emission by plasmonic antenna. The emission rate is determined by intimate interplay between the plasmon coupling to radiation field and the Ohmic losses in metal. Here we develop plasmon Green's function approach that includes plasmon's interaction with radiation to obtain expl…
Plasmonic antennas are key elements to control the luminescence of quantum emitters. However, the antenna's influence is often hidden by quenching losses. Here, the luminescence of a quantum dot coupled to a gold dimer antenna is investigated. Detailed analysis of the multiply excited states quantifies the antenna's influence on the excitation intensity and the luminescence quantum yield separately.
We develop a theory of cooperative emission mediated by cooperative energy transfer (CET) from an ensemble of quantum emitters (QE) to plasmonic antenna at a rate equal to the sum of individual QE-plasmon energy transfer rates. If the antenna radiation efficiency is sufficiently high, the transferred energy is radiated away at approximately the same cooperative rate that scales with the ensemble size. We derive explicit expressions, in terms of local fields, for cooperative Purcell factor and enhancement factor for power spectrum valid for plasmonic structures of any shape with characteristic …
Micro/nanoscale single photon source is a building block of on-chip quantum information devices. Owing to possessing ultrasmall optical mode volume, plasmon structures can provide large Purcell enhancement, however scattering and absorption are two barriers to prevent them from being used in practice. To overcome these barriers, we propose the topological photonic structure containing resonant plasmon nanoantenna, where nanoantenna provides large Purcell enhancement while topological photonic crystal guides all scattering light into its edge state. Through the optical mode design, the rate of …
The Purcell effect is usually described as a modification of the spontaneous decay rate in the presence of a resonator. In plasmonics, this effect is commonly associated with a large local-field enhancement in "hot spots" due to the excitation of surface plasmons. However, high-index dielectric nanostructures, which become the basis of all-dielectric nanophotonics, can not provide high values of the local-field enhancement due to larger radiation losses. Here, we demonstrate how to achieve a strong Purcell effect in all-dielectric nanostructures, and show theoretically that the Purcell factor …
In this paper we report on numerical study of plasmonic nanoparticle chains with long-range dipole-dipole interaction. We have shown that introduction of positional disorder gives a peak in the density of resonant states (DOS) at the frequency of individual nanoparticle resonance. This peak is referred to Dyson singularity in one-dimensional disordered structures [Dyson F., 1953] and, according to our calculations, governs the spectral properties of local DOS. This provides disorder-induced Purcell enhancement that can found its applications in random lasers and for SERS spectroscopy. We stres…
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…
We report on the structural and optical properties of individual bowtie nanoantennas both on glass and semiconducting GaAs substrates. The antennas on glass (GaAs) are shown to be of excellent quality and high uniformity reflected by narrow size distributions with standard deviations for the triangle and gap size of $σ_s^{glass}=4.5nm$ ($σ_s^{GaAs}=2.6nm$) and $σ_g^{glass}=5.4nm$ ($σ_g^{GaAs}=3.8nm$), respectively. The corresponding optical properties of individual nanoantennas studied by differential reflection spectroscopy show a strong reduction of the localised surface plasmon polariton re…
Molecule-by-molecule nanoresolved picosecond Purcell-enhanced emission at room-temperature in hollow plasmonic nanocone metamaterials
Institut Langevin, ESPCI Paris, Université PSL, CNRS（朗之万研究所，巴黎高等物理化工学院，巴黎文理研究大学，法国国家科学研究中心）；Department of Physics, University of Ottawa（渥太华大学物理系）；Department of Chemical Engineering, MESA+ Institute, University of Twente（特温特大学应用科学学院，MESA+纳米技术研究所）；Mesoscale Chemical Systems, MESA+ Institute, University of Twente（特温特大学MESA+纳米技术研究所介观化学系统组）；Donostia International Physics Center (DIPC)（圣塞巴斯蒂安国际物理中心）；University of Rochester, Institute of Optics（罗切斯特大学光学研究所）
Localized surface plasmon polaritons in conducting structures give rise to enhancements of electromagnetic local fields and extinction efficiencies. Resonant conducting structures are conventionally fabricated with a fixed geometry that determines their plasmonic response. Here, we challenge this conventional approach by demonstrating the photo-generation of plasmonic materials (THz plasmonic antennas) on a flat semiconductor layer by the structured optical illumination through a spatial light modulator. Free charge carriers are photo-excited only on selected areas, which enables the definitio…
Plasmonic antennas offer promising opportunities to control the emission of quantum objects. As a consequence, the fluorescence enhancement factor is widely used as a figure of merit for a practical antenna realization. However, the fluorescence enhancement factor is not an intrinsic property of the antenna. It critically depends on several parameters, some of which are often disregarded. In this contribution, I explore the influence of the setup collection efficiency, emitter's quantum yield and excitation intensity. Improperly setting these parameters may significantly alter the enhancement …
We propose a plasmon-based reconfigurable antenna to controllably distribute emission from single quantum emitters in spatially separated channels. Our calculations show that crossed particle arrays can split the stream of photons from a single emitter into multiple narrow beams. We predict that beams can be switched on and off by switching host refractive index. The design method is based on engineering the dispersion relations of plasmon chains and is generally applicable to traveling wave antennas. Controllable photon delivery has potential applications in classical and quantum communicatio…
Plasmonic gratings of different periodicities are fabricated on top of Silicon nanocrystals embedded in Silicon Dioxide. Purcell enhancements of up to 2 were observed, which matches the value from simulations. Plasmonic enhancements are observed for the first three orders of the plasmonic modes, with the peak enhancement wavelength varying with the periodicity. Biharmonic gratings are also fabricated to extract the enhanced emission from the first order plasmonic mode, resulting in enhancements with quality factors of up to 16.
In a recent paper by Menzel et al. (Opt. Exp. 22, 9971 (2014)), its authors analyze the spectral red-shift effect of plasmonic resonances of metallic nano-antennas between the far-field and near-field regimes. Here, we demonstrate that their interpretation of this effect is done under the same perspective as one recently reported in Langmuir 29, 6715 (2013); however, the former is incomplete and needs some remarks and clarifications which require additional relevant concepts and arguments of physical significance.
We introduce a design of Yagi-Uda plasmonic nanoantennas for enhancing the antenna gain and achieving control over the angular emission of light. We demonstrate that tapering of antenna elements allows to decrease spacing between the antenna elements tenfold also enhancing its emission directivity. We find the optimal tapering angle that provides the maximum directivity enhancement and the minimum end-fire beamwidth.
Plasmonic nanoantennas, the properties of which are essentially determined by their resonance modes, are of interest both fundamentally and for various applications. Antennas with various shapes, geometries and compositions have been demonstrated, each possessing unique properties and potential applications. Here, we propose the use of a sidewall coating as an additional degree of freedom to manipulate plasmonic gap cavity modes in strongly coupled metallic nanodisks. It is demonstrated that for a dielectric middle layer with a thickness of a few tens of nanometers and a sidewall plasmonic coa…
Single-emitter plasmonic patch antennas are room-temperature deterministic single photon sources, which exhibit highly accelerated and directed single photon emission. However, for efficient operation these structures require three-dimensional nanoscale deterministic control of emitter positioning within the device, which is a demanding task, esp. when emitter damage during fabrication is a major concern. To overcome this limitation, our deterministic room-temperature in situ optical lithography protocol uses spatially modulated light to position a plasmonic structure non-destructively on any …
Plasmon resonant arrays or meta-surfaces shape both the incoming optical field and the local density of states for emission processes. They provide large regions of enhanced emission from emitters and greater design flexibility than single nanoantennas. This makes them of great interest for engineering optical absorption and emission. Here we study the coupling of a single quantum emitter, a self-assembled semiconductor quantum dot, to a plasmonic meta-surface. We investigate the influence of the spectral properties of the nanoantennas and the position of the emitter in the unit cell of the st…
We propose highly efficient hybrid plasmonic bullseye antennas for collecting photon emission from nm-sized quantum emitters. In our approach, the emitter radiation is coupled to surface plasmon polaritons that are consequently converted into highly directional out-of-plane emission. The proposed configuration consists of a high-index titania bullseye grating separated from a planar silver film by a thin low-index silica spacer layer. Such hybrid systems are theoretically capable of directing 85 % of the dipole emission into a 0.9 NA objective, while featuring a spectrally narrow-band tunable …
The present work deals with a theoretical research on the emission and radiation properties of a dipole emitter source close to a dimer graphene plasmonic antenna. Modification of the radiation and the quantum efficiencies resulting from varying the position of the emitter and the orientation of its dipole moment are calculated by using a rigorous electromagnetic method based on Green's second identity. Large enhancements in the emission and the radiation of the emitter occur due to the coupling with the antenna surface plasmons in the spectral region from 4THz to 15THz. Our results show that …
Hybrid mesoscale-structures that can combine dielectric optical resonances with plasmon-polaritons are of interest in chip-scale nano-optical communication and sensing. This experimental study shows how a fluorescent microsphere coupled to a silver nanowire can act as a remotely-excited optical antenna. To realize this architecture, self-assembly methodology is used to couple a fluorescent silica microsphere to a single silver nanowire. By exciting propagating surface plasmon polaritons at one end of the nanowire, remote excitation of the Stokes-shifted whispering gallery modes (WGMs) of the m…
Controlling the launching efficiencies and the directionality of surface plasmon polaritons (SPPs) and their decoupling to freely propagating light is a major goal for the development of plasmonic devices and systems. Here, we report on the design and experimental observation of a highly efficient unidirectional surface plasmon launcher composed of eleven subwavelength grooves, each with a distinct depth and width. Our observations show that, under normal illumination by a focused Gaussian beam, unidirectional SPP launching with an efficiency of at least 52% is achieved experimentally with a c…
V-shaped nanoantennas are among the popular choices for the unit element of a metasurface, a nanostructured surface used for its ability to mold and control the wavefront of light. In general, the motivation for choosing the V-antenna as the unit element comes from its bimodal nature, where the introduction of the second mode offers extra control over the scattered wavefronts. Here, through near-field scanning optical microscopy, we study a 1D metastructure comprised of V-antennas in the context of generating asymmetric surface plasmon polariton (SPP) wavefronts. The key point is that the use …
We experimentally demonstrate the control of the spontaneous emission rate and the radiation pattern of colloidal quantum dots deterministically positioned in a plasmonic patch antenna. The antenna consists of a thin gold microdisk 30 nm above a thick gold layer. The emitters are shown to radiate through the entire patch antenna in a highly directional and vertical radiation pattern. Strong acceleration of spontaneous emission is observed, depending of the antenna size. Considering the double dipole structure of the emitters, this corresponds to a Purcell factor up to 80 for dipoles perpendicu…
Research on photonic cavities with low mode volume and high quality factor garners much attention because of applications ranging from optoelectronics to cavity quantum electrodynamics (QED). We propose a cavity based on surface plasmon modes confined by metallic distributed Bragg reflectors. We analyze the structure with Finite Difference Time Domain simulations and obtain modes with quality factor 1000 (including losses from metals), reduced mode volume relative to photonic crystal cavities, Purcell enhancements of hundreds, and even the capability of enabling cavity QED strong coupling.
Plasmonic nanoantenna is of promising applications in optical sensing, single-molecular detection, and enhancement of optical nonlinear effect, surface optical spectroscopy, photochemistry, photoemission, photovoltaics, etc. Here we show that in a carefully-designed dimer gap-antenna made by two metallic nanorods, the longitudinal plasmon antenna mode (AM) of bonding dipoles can compete with the transverse plasmonic cavity modes (CMs), yielding dramatically enhanced or suppressed scattering efficiency, depending on the CMs symmetry characteristics (e.g., the radial order n and the azimuthal qu…
We use spatially and angle-resolved cathodoluminescence imaging spectroscopy to study, with deep subwavelength resolution, the radiation mechanism of single plasmonic ridge antennas with lengths ranging from 100 to 2000 nm. We measure the antenna's standing wave resonances up to the fifth order and measure the dispersion of the strongly confined guided plasmon mode. By directly detecting the emitted antenna radiation with a 2D CCD camera we are able to measure the angular emission patterns associated with each individual antenna resonance. We demonstrate that the shortest ridges can be modeled…
We present a combined experimental and simulation study of a single self-assembled InGaAs quantum dot coupled to a nearby ($\sim 25nm$) plasmonic antenna. Micro-photoluminescence spectroscopy shows a $\sim 2.4\times$ increase of intensity, which is attributed to spatial far-field redistribution of the emission from the quantum dot-antenna system. Power-dependent studies show similar saturation powers of $2.5μW$ for both coupled and uncoupled quantum dot emission in polarization-resolved measurements. Moreover, time-resolved spectroscopy reveals the absence of Purcell-enhancement of the quantum…
