We extend Lamb's reduced density matrix laser theory to analyze the inhomogeneous molecular couplings and the mode-correlation in a plasmonic nano-laser consisting of a gold sphere and many dye molecules interacting with a driving optical field and with the quantized plasmon modes. The molecular inhomogeneity is accounted for by simulating their random distribution around the sphere. Our analysis shows that in order to obtain lasing we must employ a large number of strongly driven molecules to compensate strong damping of the plasmon modes. The compact molecular arrangement, however, can lead to molecular energy-shifts and thus reduce the excitation of the plasmon modes and ultimately suggests a maximum limit for the plasmon excitation for any specific system.
Strong coupling between a single quantum emitter and an electromagnetic mode is one of the key effects in quantum optics. In the cavity QED approach to plasmonics, strongly coupled systems are usually understood as single-transition emitters resonantly coupled to a single radiative plasmonic mode. However, plasmonic cavities also support non-radiative (or "dark") modes, which offer much higher coupling strengths. On the other hand, realistic quantum emitters often support multiple electronic transitions of various symmetry, which could overlap with higher order plasmonic transitions -- in the …
Metal nanostructures can be used to harvest and guide the emission of single photon emitters on-chip via surface plasmon polaritons. In order to develop and characterize photonic devices based on emitter-plasmon hybrid structures a deterministic and scalable fabrication method for such structures is desirable. Here we demonstrate deterministic and scalable top-down fabrication of metal wires onto preselected nitrogen vacancy centers in nanodiamonds using clean room nano-fabrication methods. We observe a life-time reduction of the emitter emission that is consistent with earlier proof-of-princi…
We theoretically demonstrate the generation and radiation of coherent nanoplasmons powered by a single three-level quantum emitter on a plasmonic nanoresonator. By pumping the three-level emitter in a Raman configuration, we show a pathway to achieve macroscopic accumulation of nanoplasmons due to stimulated emission in the nanoresonator despite their fast relaxation. Thanks to the antenna effect of the nanoresonator, the system acts as an efficient and bright nanoscopic coherent light source with a photon emission rate of hundreds of Terahertz and could be realized with solid-state emitters a…
Herein we report on our studies of radiative and non-radiative interaction between an individual quantum emitter and an anisotropic plasmonic nanostructure: a gold nanotriangle. Our theoretical and three-dimensional electromagnetic simulation studies highlight an interesting connection between: dipole-orientation of the quantum emitter, anisotropy of the plasmonic nanostructure and, radiative and non-radiative energy transfer processes between the emitter and the plasmonic geometry. For the out of plane orientation of quantum emitter, the total decay rate and non-radiative decay rate was found…
Two-dimensional transition metal di-chalcogenide semiconductors provide unique possibilities to investigate strongly confined excitonic physics and a plasmonic platform integrable to such materials constitutes a hybrid system that can be of interest to enable manipulation of their cumulative optical properties. Here we report tuning of excitonic emission from monolayer WSe2, mechanically exfoliated on top of a periodic two dimensional plasmonic array of elliptical gold (Au) nanodiscs. By exploiting the polarization-dependent nature of plasmonic resonance of the nano plasmonic array (NPA), the …
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 …
Localized-surface plasmon resonance is of importance in both fundamental and applied physics for the subwavelength confinement of optical field, but realization of quantum coherent processes is confronted with challenges due to strong dissipation. Here we propose to engineer the electromagnetic environment of metallic nanoparticles (MNPs) using optical microcavities. An analytical quantum model is built to describe the MNP-microcavity interaction, revealing the significantly enhanced dipolar radiation and consequentially reduced Ohmic dissipation of the plasmonic modes. As a result, when inter…
We present an optical investigation of surface plasmon polaritons propagating along nanoscale Au-wires, lithographically defined on GaAs substrates. A two-axis confocal microscope was used to perform spatially and polarization resolved measurements in order to confirm the guiding of surface plasmon polaritons over lengths ranging from $5-20 μm$ along nanowires with a lateral dimension of only $\approx 100 nm$. Finite difference time domain simulations are used to corroborate our experimental observations and highlight the potential to couple proximal quantum dot emitters to propagating plasmon…
We discuss the possibility of realizing utlrabroadband omnidirectional absorbers and angularly selective coherent thermal emitters based on properly patterned plasmonic metastructures. Instead of relying on resonant concentration effects that inherently limit the bandwidth, we base our design on the combination of two inherently nonresonant effects: plasmonic Brewster funneling and adiabatic plasmonic focusing. With this approach, we demonstrate compact, broadband absorption and emission spanning terahertz, infrared and optical frequencies, ideal for various energy and defense applications.
In recent years the controlled coupling of single photon emitters to propagating surface plasmons has been intensely studied, which is fueled by the prospect of a giant photonic non-linearity on a nano-scaled platform. In this article we will review the recent progress on coupling single emitters to nano-wires towards the construction of a new platform for strong light-matter interaction. The control over such a platform might open new doors for quantum information processing and quantum sensing at the nanoscale, and for the study of fundamental physics in the ultra-strong coupling regime.
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…
Plasmonic antennas are attractive optical structures for many applications in nano and quantum technologies. By providing enhanced interaction between a nanoemitter and light, they efficiently accelerate and direct spontaneous emission. One challenge, however, is the precise nanoscale positioning of the emitter in the structure. Here we present a laser etching protocol that deterministically positions a single colloidal CdSe/CdS core/shell quantum dot emitter inside a subwavelength plasmonic patch antenna with three-dimensional nanoscale control. By exploiting the properties of metal-insulator…
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…
The spontaneous emission rate of dipole emitters close to plasmonic dimers are theoretically studied within a nonlocal hydrodynamic model. A nonlocal model has to be used since quantum emitters in the immediate environment of a metallic nanoparticle probe its electronic structure. Compared to local calculations, the emission rate is significantly reduced. The influence is mostly pronounced if the emitter is located close to sharp edges. We suggest to use quantum emitters to test nonlocal effects in experimentally feasible configurations.
Hybrid plasmonic nanoemitters based on the combination of quantum dot emitters (QD) and plasmonic nanoantennas open up new perspectives in the control of light. However, precise positioning of any active medium at the nanoscale constitutes a challenge. Here, we report on the optimal overlap of antenna's near-field and active medium whose spatial distribution is controlled via a plasmon-triggered 2-photon polymerization of a photosensitive formulation containing QDs. Au nanoparticles of various geometries are considered. The response of these hybrid nano-emitters is shown to be highly sensitive…
Plasmonic waveguides are key elements in nanophotonic devices serving as optical interconnects between nanoscale light sources and detectors. Multimode operation in plasmonic two-wire transmission lines promises important degrees of freedom for near-field manipulation and information encoding. However, highly confined plasmon propagation in gold nanostructures is typically limited to the near-infrared region due to ohmic losses, excluding all visible quantum emitters from plasmonic circuitry. Here, we report on top-down fabrication of complex plasmonic nanostructures in single-crystalline silv…
We demonstrate that the fluorescent emitters can increase light emission from the plasmonic nanostructures in turn. With the help of atomic force microscopy, a hybrid system consisting of a fluorescent nanodiamond and a gold nanoparticle was assembled step-by-step for in situ optical measurements. We found that the emission from the nanoparticle increased compared with that before coupling. The interaction between plasmonic nanostructures and fluorescent emitter was understood as an entity based on the concept of a quantized optical cavity by considering the nanodiamond and the nanoparticle as…
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…
Monolithic integration of quantum emitters in nanoscale plasmonic circuitry requires low-loss plasmonic configurations capable of confining light well below the diffraction limit. We demonstrate on-chip remote excitation of nanodiamond-embedded single quantum emitters by plasmonic modes of dielectric ridges atop colloidal silver crystals. The nanodiamonds are produced to incorporate single germanium-vacancy (GeV) centers, providing bright, spectrally narrow and stable single-photon sources suitable for highly integrated circuits. Using electron-beam lithography with hydrogen silsesquioxane (HS…
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…
We introduce a numerical framework for calculating decay rate contributions when excited two-level quantum emitters are located near layered plasmonic nanostructures, particularly emphasizing the case of plasmonic nanostructures atop metal substrates where three decay channels exist: free space radiation, Ohmic losses, and excitation of surface plasmon polaritons (SPPs). The calculation of decay rate contributions is based on Huygen's equivalence principle together with a near-field to far-field transformation of the local electric field, thereby allowing us to discern the part of the electrom…
Realizing strong coupling between a single quantum emitter (QE) and an optical cavity is of crucial importance in the context of various quantum optical applications. While Rabi splitting of single quantum emitters coupled to high-Q diffraction limited cavities have been reported in numerous configurations, attaining single emitter Rabi splitting with a plasmonic nanostructure is still elusive. Here, we establish the analytical condition for strong coupling between a single QE and a plasmonic nanocavity and apply it to study various plasmonic arrangements that were shown to enable Rabi splitti…
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…
Exciton harvesting is demonstrated in an ensemble of quantum emitters coupled to localized surface plasmons. When the interaction between emitters and the dipole mode of a metallic nanosphere reaches the strong coupling regime, the exciton conductance is greatly increased. The spatial map of the conductance matches the plasmon field intensity profile, which indicates that transport properties can be tuned by adequately tailoring the field of the plasmonic resonance. Under strong coupling, we find that pure dephasing can have detrimental or beneficial effects on the conductance, depending on th…
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 analytically study the spontaneous emission of a single optical dipole emitter in the vicinity of a plasmonic nanoshell, based on the Lorenz-Mie theory. We show that the fluorescence enhancement due to the coupling between optical emitter and sphere can be tuned by the aspect ratio of the core-shell nanosphere and by the distance between the quantum emitter and its surface. In particular, we demonstrate that both the enhancement and quenching of the fluorescence intensity are associated with plasmonic Fano resonances induced by near- and far-field interactions. These Fano resonances have as…
We develop a self-consistent finite element method to study spontaneous emission at nanoscale proximity of plasmonic waveguides. In the model, it is assumed that only one guided mode is dominatingly excited by the quantum emitter. With such one dominating mode assumption, the cross section of the plasmonic waveguide can be arbitrary. We apply our numerical method to calculate the coupling of a quantum emitter to a cylindrical nanowire and a rectangular waveguide, and compare the cylindrical nanowire to previous work valid in quasistatic approximation. The fraction of the energy coupled to the …
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, …
We address the issue of the second-order coherence of single surface plasmons launched by a quantum source of light into extended gold films. The quantum source of light is made of a scanning fluorescent nanodiamond hosting five nitrogen-vacancy (NV) color centers. By using a specially designed microscopy that combines near-field optics with far-field leakage-radiation microscopy in the Fourier space and adapted spatial filtering, we find that the quantum statistics of the initial source of light is preserved after conversion to surface plasmons and propagation along the polycrystalline gold f…
We report here fabrication of interdigitated photoconductive antenna (iPCA) terahertz (THz) emitters based on plasmonic electrode design. Novel design of this iPCA enables it to work without microlens array focusing, which is otherwise required for photo excitation of selective photoconductive regions to avoid the destructive interference of emitted THz radiation from oppositely biased regions. Benefit of iPCA over single active region PCA is that photo excitation can be done at larger area, hence avoiding the saturation effected at higher optical excitation density. The emitted THz radiation …
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…
Semiconductor quantum dots (QDs) provide an essential link between light and matter in emerging fields such as light-harvesting, all-solid-state quantum communication, and quantum computing. QDs are excellent single-photon sources and can store quantum bits for extended periods making them promising interconnects between light and matter in integrated quantum information networks. To this end the light-matter interaction strength must be strongly enhanced using nanophotonic structures such as photonic crystal cavities and waveguides or plasmonic nanowires. So far it has been assumed that QDs c…
We demonstrate a plasmonic route to control the collective spontaneous emission of two-level quantum emitters. Superradiance and subradiance effects are observed over distances comparable to the operating wavelength inside plasmonic nanochannels. These plasmonic waveguides can provide an effective epsilon-near-zero operation in their cut-off frequency and Fabry-Perot resonances at higher frequencies. The related plasmonic resonant modes are found to efficiently enhance the constructive (superradiance) or destructive (subradiance) interference between different quantum emitters located inside t…
Nanoscale pulsed light is highly desirable in nano-integrated optics. In this letter, we obtained femtosecond pulses with THz repetition frequency via the strong coupling between quantum emitters (QEs) and plasmonic resonators. Our structure consists of a V-groove (VG) plasmonic resonator and a nanowire embedded with two-level QEs. The influences of the incident light intensity and QE number density on the transmission response for this hybrid system are investigated through semi-classical theory and simulation. It is found that the transmission response can be modulated to the pulse form. The…
Recent years have seen a growing interest in strong coupling between plasmons and excitons, as a way to generate new quantum optical testbeds and influence chemical dynamics and reactivity. Strong coupling to bright plasmonic modes has been achieved even with single quantum emitters. Dark plasmonic modes fare better in some applications due to longer lifetimes, but are difficult to probe as they are subradiant. Here, we apply electron energy loss (EEL) spectroscopy to demonstrate that a dark mode of an individual plasmonic bowtie can interact with a small number of quantum emitters, as evidenc…
Quantum plasmonic systems suffer from significant decoherence due to the intrinsically large dissipative and radiative dampings. Based on our quantum simulations via a quantum tensor network algorithm, we numerically demonstrate the mitigation of this restrictive drawback by hybridizing a plasmonic nanocavity with an emitter ensemble with inhomogeneously-broadened transition frequencies. By burning two narrow spectral holes in the spectral density of the emitter ensemble, the coherent time of Rabi oscillation for the hybrid system is increased tenfold. With the suppressed decoherence, we move …
Plasmonic nano-objects have shown great potential in enhancing biological and chemical sensing, light harvesting and energy transfer, and optical and quantum computing to name a few. Therefore, an extensive effort has been vested in optimizing plasmonic systems and exploiting their field enhancement properties. Super-resolution imaging with quantum dots (QDs) is a promising method to probe plasmonic near-fields, but is hindered by the distortion of the emission intensity and radiation pattern. Here we investigate the interaction between QDs and 'L-shaped' gold nanoantennas, and demonstrate bot…
We provide a general theoretical platform based on quantized radiation in absorptive and inhomogeneous media for investigating the coherent interaction of light with metallic structures in the immediate vicinity of quantum emitters. In the case of a very small metallic cluster, we demonstrate extreme regimes where a single emitter can either counteract or enhance particle absorption by three orders of magnitude. For larger structures, we show that an emitter can eliminate both scattering and absorption and cloak a plasmonic antenna. We provide physical interpretations of our results and discus…
The thermal emission of refractory plasmonic metamaterial - a titanium nitride 1D grating - is studied at high operating temperature (540 °C). By choosing a refractory material, we fabricate thermal gratings with high brightness that are emitting mid-infrared radiation centered around 3 $μ$m. We demonstrate experimentally that the thermal excitation of plasmon-polariton on the surface of the grating produces a well-collimated beam with a spatial coherence length of 32λ (angular divergence of 1.8°) which is quasi-monochromatic with a full width at half maximum of 70 nm. These experimental resul…
Control of nonlinear response of nanostructures via path interference effects, i.e. Fano resonances, has been studied extensively. In such materials, a frequency conversion process which takes place near a hot spot has been considered. Here, we study a different case. The frequency conversion process takes place along the body of a nonlinear crystal. Metal nanoparticle-quantum emitter dimers control the down-conversion process, taking place throughout the crystal body, via introducing interfering conversion paths. Dimers behave as interaction centers. We show that a 2 order of magnitude enhanc…
The absorption process of an emitter close to a plasmonic antenna is enhanced due to strong local electromagnetic (EM) fields. The emission process, if resonant with the plasmonic system, re-radiates to the far-field by coupling with the antenna due to the availability of plasmonic states. This increases the local density of states (LDOS), effectively providing more, or alternate, pathways for emission. Through the mapping of localized emission events from single molecules close to plasmonic antennas, performed using far-field data, one gains combined information on both the local EM field str…
Simultaneous spatio-temporal confinement of energetic electron pulses to femtosecond and nanometer scales is a topic of great interest in the scientific community, given the potential impact of such development on a wide spectrum of scientific and industrial applications. For example, in ultrafast electron scattering, nanoscale probes would enable accurate maps of structural dynamics in materials with nanoscale heterogeneity, thereby understanding the role of boundaries and defects on macroscopic properties. On the other hand, advances in this field are mostly limited by the electron source br…
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…
Control of nonlinear response of nanostructures via path interference effects, i.e., Fano resonances, has been studied extensively. In such studies, a frequency conversion process takes place near a hot spot. Here, we study the case where the frequency conversion process takes place \textit{along the body of a nonlinear crystal}. Metal nanoparticle-quantum emitter dimers control the down-conversion process, taking place throughout the crystal body, via introducing interfering conversion paths. Dimers behave as interaction centers. We show that a 2 orders of magnitude enhancement is possible, o…
We present a quantum theory for the interaction of a two level emitter with surface plasmon polaritons confined in single-mode waveguide resonators. Based on the Green's function approach, we develop the conditions for the weak and strong coupling regimes by taking into account the sources of dissipation and decoherence: radiative and non-radiative decays, internal loss processes in the emitter, as well as propagation and leakage losses of the plasmons in the resonator. The theory is supported by numerical calculations for several quantum emitters, GaAs and CdSe quantum dots and NV centers tog…
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 …
On-chip realization of complex photonic functionalities is essential for further progress in planar integrated nanophotonics, especially when involving nonclassical light sources such as quantum emitters (QEs). Hybrid plasmonic nanocircuits integrated with QEs have been attracting considerable attention due to the prospects of significantly enhancing QE emission rates and miniaturizing quantum nanophotonic components. Spin-orbit interactions on subwavelength scales have been increasingly explored in both conventional and quantum nanophotonics for realization and utilization of the spin-depende…
We investigate the impact of the dipole-active modes formed via the mode-mixing of the dipole mode with higher-order surface plasmon modes of a nanoegg on the radiative decay rate and quantum yield of an excited molecule near the nanoegg. The Purcell factor, rate of power dissipation by the emitter, antenna efficiency of the nanoegg, as well as quantum yield enhancement of the emitter, were studied using the quasistatic approximation and the semiclassical theory of radiation, following the Gersten-Nitzan and Ford-Weber approaches. Compared to the concentric nanoshell, we show that the dielectr…
Assembly of quantum nanophotonic systems with plasmonic resonators are important for fundamental studies of single photon sources as well as for on-chip information processing. In this work, we demonstrate controllable nanoassembly of gold nanospheres with ultra-bright quantum emitters in 2D layered hexagonal boron nitride (hBN). We utilize an atomic force microscope (AFM) tip to precisely position gold nanospheres to close proximity of the quantum emitters and observe the resulting emission enhancement and fluorescence lifetime reduction. A fluorescence enhancement of over 300% is achieved ex…
We present a microscopic model describing the transition to strong coupling regime for an emitter resonantly coupled to a surface plasmon in a metal-dielectric structure. We demonstrate that the shape of scattering spectra is determined by an interplay of two distinct mechanisms. First is the near-field coupling between the emitter and the plasmon mode which underpins energy exchange between the system components and gives rise to exciton-induced transparency minimum in scattering spectra prior the transition to strong coupling regime. The second mechanism is Fano interference between the plas…
