By means of quantum tensor network calculations, we investigate the large Purcell effect experienced by an organic molecule placed in the vicinity of a plasmonic nanostructure. In particular, we consider a donor-π bridge-acceptor dye at the gap of two Ag nanospheres. Our theoretical approach allows for a realistic description of the continua of both molecular vibrations and optical nanocavity modes. We analyze both the exciton dynamics and the corresponding emission spectrum, showing that these magnitudes are not accurately represented by the simplified models used up to date. By disentangling the molecule coupling to radiative and non-radiative plasmonic modes, we also shed light into the quenching phenomenology taking place in the system.
We theoretically investigate the spontaneous emission of a point--like dipolar emitter located near a two--dimensional (2D) plasmonic waveguide of arbitrary form. We invoke an explicite link with the density of modes of the waveguide describing the electromagnetic channels into which the emitter can couple. We obtain a closed form expression for the coupling to propagative plasmon, extending thus the Purcell factor to plasmonic configurations. Radiative and non-radiative contributions to the spontaneous emission are also discussed in details.
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 …
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…
The rate of spontaneous emission is known to depend on the environment of a light source, and the enhancement of one-photon emission in a resonant cavity is known as the Purcell effect. Here we develop a theory of spontaneous two-photon emission for a general electromagnetic environment including inhomogeneous dispersive and absorptive media. This theory is used to evaluate the two-photon Purcell enhancement in the vicinity of metallic nanoparticles and it is demonstrated that the surface plasmon resonances supported by these particles can enhance the emission rate by more than two orders of m…
Plasmonic nanopatch antennas that incorporate dielectric gaps hundreds of picometers to several nanometers thick have drawn increasing attention over the past decade because they confine electromagnetic fields to grossly sub-diffraction limited volumes. Substantial control over the optical properties of excitons and color centers confined within these plasmonic cavities has already been demonstrated with far-field optical spectroscopies, but near-field optical spectroscopies are essential to an improved understanding of the plasmon-emitter interaction at the nanoscale. Here, we characterize th…
Purely organic materials with negative and near-zero dielectric permittivity can be easily fabricated. Here we develop a theory of nonlinear non-steady-state organic plasmonics with strong laser pulses. The bistability response of the electron-vibrational model of organic materials in the condensed phase has been demonstrated. Non-steady-state organic plasmonics enable us to obtain near-zero dielectric permittivity during a short time. We have proposed to use non-steady-state organic plasmonics for the enhancement of intersite dipolar energy-transfer interaction in the quantum dot wire that in…
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 interactions between the excited states of a single chromophore with static and dynamic electric fields confined to a plasmonic cavity of picometer dimensions are investigated in a joint experimental and theoretical effort. In this configuration, the spatial extensions of the confined fields are smaller than the one of the molecular exciton, a property that is used to generate fluorescence maps of the chromophores with intra-molecular resolution. Theoretical simulations of the electrostatic and electrodynamic interactions occurring at the chromophore-picocavity junction are able to reprodu…
Vertical nanowires facilitate an innovative mechanism to channel the optical field in the orthogonal direction and act as a nanoscale light source. Subwavelength, vertically oriented nanowire platforms, both of plasmonic and semiconducting variety can facilitate interesting far field emission profiles and potentially carry orbital angular momentum states. Motivated by these prospects, in this letter, we show how a hybrid plasmonic - organic platform can be harnessed to engineer far field radiation. The system that we have employed is an organic nanowire made of diaminoanthroquinone grown on a …
Graphene plasmons provide a suitable alternative to noble-metal plasmons because they exhibit much larger confinement and relatively long propagation distances, with the advantage of being highly tunable via electrostatic gating. We report strong light- matter interaction assisted by graphene plasmons, and in particular, we predict unprecedented high decay rates of quantum emitters in the proximity of a carbon sheet, large vacuum Rabi splitting and Purcell factors, and extinction cross sections exceeding the geometrical area in graphene ribbons and nanometer-sized disks. Our results provide th…
We derive effective Hamiltonians for a single dipolar emitter coupled to a metal nanoparticle (MNP) with particular attention devoted to the role of losses. For small particles sizes, absorption dominates and a non hermitian effective Hamiltonian describes the dynamics of the hybrid emitter-MNP nanosource. We discuss the coupled system dynamics in the weak and strong coupling regimes offering a simple understanding of the energy exchange, including radiative and non radiative processes. We define the plasmon Purcell factors for each mode. For large particle sizes, radiative leakages can signif…
Metal nanostructures are key elements in nanooptics owing to their strong resonant interaction with light through local plasmonic charge oscillations. Their ability to shape light at the nanoscale have made them important across a multitude of areas, including biosensing, energy conversion and ultrathin flat metaoptics. Yet another dimension of avenues is foreseen for dynamic nanoantennas, ranging from tuneable metalenses for miniaturized medical devices to adaptable windows that control radiation flows in and out of buildings. However, enabling nano-optical antennas to be dynamically controll…
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…
We describe the possibility of drastically boosting the spontaneous emission of a collection of two-level quantum emitters by embedding them in an epsilon-near-zero (ENZ) environment, consisting of a plasmonic waveguide operated at cut-off. This phenomenon relies on the combination of Purcell enhancement and Dicke superradiance effects, exploiting the large and uniform local density of states in ENZ channels, which is shown to significantly extend the spatial extent of these quantum effects. We envision exciting applications in optical sensing, molecular detection and low-threshold lasing.
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…
Intermixed light-matter quasiparticles - polaritons - possess unique optical properties owned to their compositional nature. These intriguing hybrid states have been extensively studied over the past decades in a wide range of realizations aiming at both basic science and emerging applications. However, recently it has been demonstrated that not only optical, but also material-related properties, such as chemical reactivity and charge transport, may be significantly altered in the strong coupling regime of light-matter interactions. Here, we show that a nanoscale system, comprised of a plasmon…
Cavity mode theory and analysis of open cavities and plasmonic particles is an essential component of optical resonator physics, offering considerable insight and efficiency for connecting to classical and quantum optical properties such as the Purcell effect. However, obtaining the dissipative modes in normalized form for arbitrarily shaped open cavity systems is notoriously difficult, often involving complex spatial integrations, even after performing the necessary full space solutions to Maxwell's equations. The formal solutions are termed quasinormal modes which are known to diverge in spa…
Single-walled carbon nanotubes (SWCNTs) are promising absorbers and emitters to enable novel photonic and optoelectronic applications but are also known to severely suffer from low optical quantum yields. Here we demonstrate SWCNTs excitons coupled to plasmonic nanocavities reaching deeply into the Purcell regime with FP=234 (average FP=76), near unity quantum yields of 70% (average 41%), and a photon emission rate of 1.7 MHz into the first lens. The measured ultra-narrow exciton linewidth (18 micro eV) implies furthermore generation of indistinguishable single photons from a SWCNT. To demonst…
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…
We provide a self-consistent electromagnetic theory of the coupling between dipole emitters and dissipative nanoresonators. The theory that relies on the concept of quasi-normal modes with complex frequencies provides an accurate closed-form expression for the electromagnetic local density of states (LDOS) of any photonic or plasmonic resonator with strong radiation leakage, absorption and material dispersion. It represents a powerful tool to calculate and conceptualize the electromagnetic response of systems that are governed by a small number of resonance modes. We use the formalism to revis…
Films of close-packed Au nanoparticles are coupled electrodynamically through their collective plasmon resonances. This collective optical response results in enhanced light-matter interactions, which can be exploited in various applications. Here, we demonstrate their application in sensing volatile organic compounds, using methanol as a test-case. Ordered films over several cm2 were obtained by interfacial self-assembly of colloidal Au nanoparticles (~10 nm diameter) through controlled evaporation of the solvent. Even though isolated nanoparticles of this size are inherently non-scattering, …
Disentangling the contributions of radiative and non-radiative localized plasmonic modes from the photonic density of states of metallic nanocavities between atomically-sharp tips and flat substrates remains an experimental challenge nowadays. Electroluminescence due to tunnelling through the tip-substrate gap allows discerning solely the excitation of radiative modes, but this information is inherently convolved with that of the electronic structure of the system. In this work we present a fully experimental procedure to eliminate the electronic-structure factors from the scanning tunnelling …
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…
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…
We report the observation of the generation and routing of single plasmons generated by localized excitons in a WSe$_2$ monolayer flake exfoliated onto lithographically defined Au-plasmonic waveguides. Statistical analysis of the position of different quantum emitters shows that they are $(3.3 \pm 0.7)\times$ more likely to form close to the edges of the plasmonic waveguides. By characterizing individual emitters we confirm their single-photon character via the observation of antibunching of the signal ($g^{(2)}(0) = 0.42$) and demonstrate that specific emitters couple to the modes of the prox…
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…
Nonlocal effects have been shown to be responsible for a variety of non-trivial optical effects in small-size plasmonic nanoparticles, beyond classical electrodynamics. However, it is not clear whether optical mode descriptions can be applied to such extreme confinement regimes. Here, we present a powerful and intuitive quasinormal mode description of the nonlocal optical response for three-dimensional plasmonic nanoresonators. The nonlocal hydrodynamical model and a generalized nonlocal optical response model for plasmonic nanoresonators are used to construct an intuitive modal theory and to …
Understanding light-matter interactions using localized surface plasmons (LSPs) is of fundamental interest in classical and quantum plasmonics and has a wide range of applications. In order to understand the spatial properties of LSPs, electron energy loss spectroscopy (EELS) is a common and powerful method of spatially resolving the extreme localized fields that can be obtained with metal resonators. However, modelling EELS for general shaped resonators presents a major challenge in computational electrodynamics, requiring the full photon Green function as a function of two space points and f…
Dynamic dipolar toroidal response is demonstrated by an optical plasmonic metamaterial composed of double disks. This response with a hotspot of localized E-field concentration is a well-behaved toroidal cavity mode that exhibits a large Purcell factor due to its deep-subwavelength mode volume. All-optical Hall effect (photovoltaic) due to this optical toroidal moment is demonstrated numerically, in mimicking the magnetoelectric effect in multiferroic systems. The result shows a promising avenue to explore various optical phenomena associated with this intriguing dynamic toroidal moment.
Deterministically integrating semiconductor quantum emitters with plasmonic nano-devices paves the way towards chip-scale integrable, true nanoscale quantum photonics technologies. For this purpose, stable and bright semiconductor emitters are needed, which moreover allow for CMOS-compatibility and optical activity in the telecommunication band. Here, we demonstrate strongly enhanced light-matter coupling of single near-surface ($<10\,nm$) InAs quantum dots monolithically integrated into electromagnetic hot-spots of sub-wavelength sized metal nanoantennas. The antenna strongly enhances the emi…
The fluorescence of organic fluorophore molecules is enhanced when they are placed in contact with certain metals (Al, Ag, Cu, Au, etc.) whose surface plasmon waves couple into the radiative modes of the molecules and increase the radiative efficiency. Here, we report a hitherto unknown size dependence of this metal enhanced fluorescence (MEF) effect in the nanoscale. When the molecules are deposited in nanoporous anodic alumina films with exposed aluminum at the bottom of the pores, they form organic nanowires standing on aluminum nanoparticles whose plasmon waves have much larger amplitudes.…
