We introduce the concept of optical control of the fluorescence yield of CdSe quantum dots through plasmon-induced structural changes in random semicontinuous nanostructured gold films. We demonstrate that the wavelength- and polarization dependent coupling between quantum dots and the semicontinuous films, and thus the fluorescent emission spectrum, can be controlled and significantly increased through the optical extinction of a selective band of eigenmodes in the films. This optical method of effecting controlled changes in the metal nanostructure allows for versatile functionality in a single sample and opens a pathway to in situ control over the fluorescence spectrum.
We experimentally observe an effective PT-phase transition through the exceptional point in a hybrid plasmonic-dielectric waveguide system. Transmission experiments reveal fundamental changes in the underlying Eigenmode interactions as the environmental refractive index is tuned, which can be unambiguously attributed to a crossing through the plasmonic exceptional point. These results extend the design opportunities for tuneable non-Hermitian physics to plasmonic systems.
We consider periodic arrangements of metal nanostructures and study the effect of periodicity on the localised surface plasmon resonance of the structures within an electrostatic eigenmode approximation. We show that within this limit, the collective surface plasmon resonances of the periodic structures can be expressed in terms of superpositions of the eigenmodes of uncoupled nanostructures that exhibit a standing--wave character delocalised across the entire periodic structure. The formalism derived successfully enables the design and accounts for the observation of plasmonic edge-states in …
Strong light-matter interaction and high-efficiency optical collection of fluorescence from quantum emitters are crucial topics in quantum and nanophotonic fields. High-quality cavities, dispersive photonic crystal waveguides and even plasmonic structures have been used to enhance the interaction with quantum emitters, thus realize efficient collection of the fluorescence. In this work, a new method is proposed to collect the fluorescence of quantum dots (QDs) with a fiber-integrated multimode silver nanowire (AgNW) waveguide. Fluorescence lifetime measurement is performed to investigate the c…
Plasmonically enhanced fluorescence is a widely studied and applied phenomenon, however only a comparative theoretical and experimental analyses of coupled fluorophores and plasmonic nanoresonators makes it possible to uncover, how this phenomenon can be controlled. A numerical optimization method was applied to design configurations that are capable of resulting in an enhancement of excitation and emission, moreover of both phenomena simultaneously in coupled Cy5 dye molecule and gold nanorod systems. Parametric sensitivity studies revealed, how the fluorescence enhancement depends on the mol…
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 present measurements on plasmonic meta-molecules under local excitation using cathodoluminescence which show a spatial redistribution of the local density of optical states (LDOS) at the same frequency where a sharp spectral Fano-feature in the extinction cross section has been observed. Our analytical model shows that both near- and far-field effects arise due to interference of the same two eigenmodes of the system. We present quantitative insights both in a bare state, and in a dressed state picture that describe plasmonic Fano interference either as near-field amplitude transfer between…
We evaluate the sensing properties of plasmonic waveguide sensors by calculating their resonant transmission spectra in different regions of the non-Hermitian eigenmode space. We elucidate the pitfalls of using modal dispersion calculations in isolation to predict plasmonic sensor performance, which we address by using a simple model accounting for eigenmode excitation and propagation. Our transmission calculations show that resonant wavelength and spectral width crucially depend on the length of the sensing region, so that no single criterion obtained from modal dispersion calculations alone …
Single-molecule approaches to biology offer a powerful new vision to elucidate the mechanisms that underpin the functioning of living cells. However, conventional optical single molecule spectroscopy techniques such as Förster fluorescence resonance energy transfer (FRET) or fluorescence correlation spectroscopy (FCS) are limited by diffraction to the nanomolar concentration range, far below the physiological micromolar concentration range where most biological reaction occur. To breach the diffraction limit, zero mode waveguides and plasmonic antennas exploit the surface plasmon resonances to…
Single-molecule fluorescence techniques are essential for investigating the molecular mechanisms in biological processes. However, achieving sub-millisecond temporal resolution to monitor fast molecular dynamics remains a significant challenge. The fluorescence brightness is the key parameter that generally defines the temporal resolution for these techniques. Conventional microscopes and standard fluorescent emitters fall short in achieving the high brightness required for sub-millisecond monitoring. Plasmonic nanoantennas have been proposed as a solution, but despite huge fluorescence enhanc…
A novel numerical methodology has been developed, which makes possible to optimize arbitrary emitting dipole and plasmonic nano-resonator configuration with an arbitrary objective function. By selecting quantum efficiency as the objective function that has to be maximized at preselected Purcell factor criteria, optimization of plasmonic nanorod based configurations has been realized to enhance fluorescence of NV and SiV color centers in diamond. Gold and silver nanorod based configurations have been optimized to enhance excitation and emission separately, as well as both processes simultaneous…
We demonstrate effective background-free continuous wave nonlinear optical excitation of molecules that are sandwiched between asymmetrically constructed plasmonic gold nanoparticle clusters. We observe that near infrared photons are converted to visible photons through efficient plasmonic second harmonic generation. Our theoretical model and simulations demonstrate that Fano resonances may be responsible for being able to observe nonlinear conversion using a continuous wave light source. We show that nonlinearity enhancement of plasmonic nanostructures via coupled quantum mechanical oscillato…
We demonstrate an efficient eigen-decomposition method for analyzing the guided modes in metal nanoparticle chains. The proposed method has the advantage of showing the dispersion relation and mode quality simultaneously. It can also separate the material and geometrical properties, so its efficiency does not depend on the complexity of the material polarizability. The method is applied to analyze the guided modes of a single and a pair of metal chains. The more accurate dynamic dipole polarizability typically gives a red-shift compared with the results obtained with the broadly used quasistat…
Far-field radiation of bulk, edge and corner eigenmodes from a finite 2D Su-Schrieffer-Heeger plasmonic lattice
Instituto de Estructura de la Materia (IEM-CSIC)（物质结构研究所）；International Iberian Nanotechnology Laboratory (INL)（国际伊比利亚纳米技术实验室）；Universidad de Valladolid（巴利亚多利德大学）；Technology Innovation Institute（技术创新研究所）；Centre of Excellence ENSEMBLE3 sp. z o.o.（ENSEMB3卓越中心有限责任公司）
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…
A class of hybrid photonic-plasmonic structures (HPPS) with vertical cylindrical cavities is proposed and its performance in providing a coherent light from spontaneous emission is investigated. It is shown that the proposed easy-to-fabricate and robust anodic aluminum oxide structure dramatically enhances the temporal and spatial coherence compared to the previously examined HPPS. The physical mechanism of achieving the temporal and spatial coherence is explained based on the special optical properties of the proposed HPPS and it is discussed how this structure enables one adjusting hybrid ph…
Single molecule detection provides detailed information about molecular structures and functions, but it generally requires the presence of a fluorescent marker which can interfere with the activity of the target molecule or complicate the sample production. Detecting a single protein with its natural UV autofluorescence is an attractive approach to avoid all the issues related to fluorescence labelling. However, the UV autofluorescence signal from a single protein is generally extremely weak. Here, we use aluminum plasmonics to enhance the tryptophan autofluorescence emission of single protei…
We report on the experimental and theoretical study of the spatial fluctuations of the local density of states (EM-LDOS) and of the fluorescence intensity in the near-field of a gold nanoantenna. EM-LDOS, fluorescence intensity and topography maps are acquired simultaneously by scanning a fluorescent nanosource grafted on the tip of an atomic force microscope at the surface of the sample. The results are in good quantitative agreement with numerical simulations. This work paves the way for a full near-field characterization of an optical nanoantenna.
Plasmonic Fourier Surfaces Revisited: Relating Bandgaps with Bound States in the Continuum
Hamburg University of Technology（汉堡工业大学）；Ludwig-Maximilians-Universität München（慕尼黑大学）；ETH Zurich（苏黎世联邦理工学院）；National Research Nuclear University MEPhI（俄罗斯国立核研究医科大学）；National University of Science and Technology ‘MISIS’（莫斯科国立科技大学）
We theoretically and numerically investigate metal enhanced fluorescence of plasmonic core-shell nanoparticles doped with rare earth (RE) ions. Particle shape and size are engineered to maximize the average enhancement factor (AEF) of the overall doped shell. We show that the highest enhancement (11 in the visible and 7 in the near-infrared) are achieved by tuning either the dipolar or quadrupolar particle resonance to the rare earth ions excitation wavelength. Additionally, the calculated AEFs are compared to experimental data reported in the literature, obtained in similar conditions (plasmo…
Common intuition in physics is based on the concept of orthogonal eigenmodes. Those are well de- fined solutions of Hermitian equations used to describe many physical situations, from quantum mechanics to acoustics. A large variety of non-Hermitian problems, including gravitational waves close to black holes or leaky electromagnetic cavities require the use of bi-orthogonal eigenbasis. Physical consequences of non-Hermiticity challenge our physical understanding. However, the usual need to compensate for energy losses made the few successful attempts to probe non-Hermiticity extremely complica…
In this work, we use a site-selective functionalization strategy to decorate plasmonic nanopores with one or more fluorescent dyes. Using an easy and robust fabrication method, we manage to build single plasmonic rings on top of dielectric nanotubes with different inner diameters. The modulation of the dimension of the nanopores allows us to both tailor their field confinement and their Purcell Factor in the visible spectral range. In order to investigate how the changes in geometry influence the fluorescence emission efficiency, thiol-conjugated dyes are anchored on the plasmonic ring, thus f…
This document briefly introduces the key concepts to understand the phenomenon of fluorescence enhancement with optical nanostructures. The equations remain simple, with the major goal to illustrate the different physical effects at play. It also provides an overview of different recent approaches to enhance single molecule fluorescence with plasmonic and non-plasmonic nanoantennas, and describes three main biochemical applications.
Plasmonic coupling of metallic nanoparticles and adjacent pigments can dramatically increase the brightness of the pigments due to the enhanced local electric field. Here, we demonstrate that the fluorescence brightness of a single plant light-harvesting complex (LHCII) can be significantly enhanced when coupled to single gold nanorods (AuNRs). The AuNRs utilized in this study were prepared via chemical reactions, and the hybrid system was constructed using a simple and economical spin-assisted layer-by-layer technique. Enhancement of fluorescence brightness of up to 240-fold was observed, acc…
We propose the generalization of the Fourier modal method aimed at calculating localized eigenmodes of integrated optical resonators. The method is based on constructing the analytic continuation of the structure's scattering matrix and calculating its poles. The method allows one to calculate the complex frequency of the localized mode and the corresponding field distribution. We use the proposed method to calculate the eigenmodes of rectangular dielectric block located on metal surface. We show that excitation of these modes by surface plasmon-polariton (SPP) results in resonant features in …
A surrounding electromagnetic environment can engineer spontaneous emissions from quantum emitters through the Purcell effect. For instance, a plasmonic antenna can efficiently confine an electromagnetic field and enhance the fluorescent process. In this study, we demonstrate that a photonic microcavity can modulate plasmon-enhanced fluorescence by engineering the local electromagnetic environment. Consequently, we constructed a plasmon-enhanced emitter (PE-emitter), which comprised a nanorod and a nanodiamond, using the nanomanipulation technique. Furthermore, we controlled a polystyrene sphe…
Serving as a new two-dimensional plasmonic material, graphene has stimulated an intensive study of its optical properties which benefit from the unique electronic band structure of the underlying honeycomb lattice of carbon atoms. In classical electrodynamics, nanostructured graphene is commonly modeled by the computationally demanding problem of a three-dimensional conducting film of atomic-scale thickness. Here, we propose an efficient alternative two-dimensional electrostatic approach where all the calculation procedures are restricted to the plane of the graphene sheet. To explore possible…
Although fluorescence is the prevailing labeling technique in biosensing applications, sensitivity improvement is still a striving challenge. We show that coating standard microscope slides with nanoroughened silver films provides a high fluorescence signal enhancement due to plasmonic interactions. As a proof of concept, we applied these films with tailored plasmonic properties to DNA microarrays. Using common optical scanning devices, we achieved signal amplifications by more than 40-fold.
A nanodiamond (ND) hosting nitrogen-vacancy (NV) color centers is attached on the apex of an optical tip for near-field microscopy. Its fluorescence is used to launch surface plasmon-polaritons (SPPs) in a thin polycrystalline gold film. It is shown that the quantum nature of the initial source of light is preserved after conversion to SPPs. This opens the way to a deterministic quantum plasmonics, where single SPPs can be injected at well-defined positions in a plasmonic device produced by top-down approaches.
Investigating the cellular internalization pathways of single molecules or single nano-objects is important to understanding cell-matter interactions and to applications in drug delivery and discovery. Imaging and tracking the motion of single molecules on cell plasma membrane require high spatial resolution in three dimensions (3D). Fluorescence imaging along the axial dimension with nanometer resolution has been highly challenging but critical to revealing displacements in trans-membrane events. Here, utilizing a plasmonic ruler based on the sensitive distance dependence of near-infrared flu…
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 demonstrate that soliton-plasmon bound states appear naturally as propagating eigenmodes of nonlinear Maxwell's equations for a metal/dielectric/Kerr interface. By means of a variational method, we give an explicit and simplified expression for the full-vector nonlinear operator of the system. Soliplasmon states (propagating surface soliton-plasmon modes) can be then analytically calculated as eigenmodes of this non-selfadjoint operator. The theoretical treatment of the system predicts the key features of the stationary solutions and gives physical insight to understand the inherent stabili…
Plasmonic nano-optical tweezers enable the non-invasive manipulation of nano-objects under low illumination intensities, and have become a powerful tool for nanotechnology and biophysics. However, measuring the trap stiffness of nanotweezers remains a complicated task, which hinders the development of plasmonic trapping. Here, we describe an experimental method to measure the trap stiffness based on the temporal correlation of the fluorescence from the trapped object. The method is applied to characterize the trap stiffness in different double nanohole apertures and explore the influence of th…
In this article, we address fluorescence of single molecule inside a plasmonic picocavity by proposing a semi-classical theory via combining the macroscopic quantum electrodynamics theory and the open quantum system theory. To gain insights into the experimental results [Nat. Photonics, 14, 693 (2020)], we have further equipped this theory with the classical electromagnetic simulation of the pico-cavity, formed by single atom decorated silver STM tip and a silver substrate, and the time-dependent density functional theory calculation of zinc phthalocyanine molecule. Our simulations not only re…
Plasmonic waveguides offer the unique possibility to confine light far below the diffraction limit. Past room temperature experiments of single quantum emitters coupled to such waveguides have mainly focused on efficient channelling of the spontaneous emission into waveguide modes after a linear optical excitation. However, only the simultaneous interaction of the emitter with multiple plasmonic fields would lead to functionality in a plasmonic circuit. Here, we demonstrate the nonlinear optical interaction of a single molecule and propagating plasmons. An individual terrylene diimide (TDI) mo…
Optical Resonances: From Eigenmodes to Scattering Features
Qingdao Innovation and Development Center of Harbin Engineering University（哈尔滨工程大学青岛创新发展基地）；Department of Electronic Materials Engineering, Research School of Physics, Australian National University（澳大利亚国立大学物理研究学院电子材料工程系）
Nanophotonic devices take advantage of geometry-dependent optical properties to confine and enhance the interaction of light with matter on small scales. By carefully patterning nanoscale geometries, coupling of responses across distinct physical domains can be achieved, such as photon and phonon modes in optomechanical crystals. Extreme optical confinement of plasmonics can localize strong cross-domain interactions into nanometer-scale volumes, smaller than many nanosystem's thermal and mechanical eigenmodes, opening new regimes for engineering reconfigurable, dynamic nanosystems. Here, we pr…
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…
Plasmonic nanoapertures generate strong field gradients enabling efficient optical trapping of nano-objects. However, because the infrared laser used for trapping is also partly absorbed into the metal leading to Joule heating, plasmonic nano-optical tweezers face the issue of local temperature increase. Here, we develop three independent methods based on molecular fluorescence to quantify the temperature increase induced by a 1064 nm trapping beam focused on single and double nanoholes milled in gold films. We show that the temperature in the nanohole can be increased by 10°C even at the mode…
Using a realistic quantum master equation we show that the resonance fluorescence spectra of a two-level artificial atom (quantum dot) can be tuned by adjusting its photonic local density of states via biasing of one or more graphene monolayers. The structured photon reservoir is included using a photon Green function theory which fully accounts for the loss and dispersion. The field-driven Mollow triplet spectrum can be actively controlled by the graphene bias in the THz frequency regime. We also consider the effect of a dielectric support environment, and multiple graphene layers, on the emi…
We report a mathematically rigorous technique which facilitates the optimization of various optical properties of electromagnetic fields. The technique exploits the linearity of electromagnetic fields along with the quadratic nature of their interaction with matter. In this manner we may decompose the respective fields into optical quadratic measure eigenmodes (QME). Key applications include the optimization of the size of a focused spot, the transmission through photonic devices, and the structured illumination of photonic and plasmonic structures. We verify the validity of the QME approach t…
We use our vector Maxwell's nonlinear eigenmode solver to study the stationary solutions in 2D cross-section waveguides with Kerr nonlinear cores. This solver is based on the fixed power algorithm within the finite element method. First, studying nonlinear plasmonic slot waveguides, we demonstrate that, even in the low power regime, 1D studies may not provide accurate and meaningfull results compared to 2D ones. Second, we study at high powers the link between the nonlinear parameter $γ_{nl}$ and the change of the nonlinear propagation constant $Δβ$. Third, for a specific type of photonic crys…
We present a study of the highly nonlinear optical excitation of noble gases in tapered hollow waveguides using few-femtosecond laser pulses. The local plasmonic field enhancement induces the generation of a nanometric plasma, resulting in incoherent extreme-ultraviolet fluorescence from optical transitions of neutral and ionized xenon, argon, and neon. Despite sufficient intensity in the waveguide, high-order harmonic generation is not observed. The fluorescent emission exhibits a strong bistability manifest as an intensity hysteresis, giving strong indications for multistep collisional excit…
We present two applications of a single nitrogen vacancy center in a nanodiamond as quantum probe for plasmonic nanostructures. Coupling to the nanostructures is achieved in a highly controlled manner by picking up a pre-characterized nanocrystal with an atomic force microscope and placing it at the desired position. Local launching of single excitations into a nanowire with a spatial control of few nanometers is demonstrated. Further, a two dimensional map of the electromagnetic environment of a plasmonic bowtie antenna was derived, resembling an ultimate limit of fluorescence lifetime nanosc…
The nonclassical modification of plasmon-assisted fluorescence enhancement is theoretically explored by placing two-level dipole emitters at the narrow gaps encountered in canonical plasmonic architectures, namely dimers and trimers of different metallic nanoparticles. Through detailed simulations, in comparison with appropriate analytical modelling, it is shown that within classical electrodynamics, and for the reduced separations explored here, fluorescence enhancement factors of the order of $10^{5}$ can be achieved, with a divergent behaviour as the particle touching regime is approached. …
Benefitting from the excellent characteristics such as low cytotoxicity, functionalization versatility, and tunable fluorescence, nanodiamonds (NDs) have shown enormous application potentials in the biomedical field. Herein, we proposed, for the first time to our best knowledge, to integrate NDs on a plasmonic interface constructed on a side-polished fiber using drop-casting method. The added NDs engineers the plasmonic interface towards improving the sensing field, thus enhancing the sensitivity, which, moreover, is significantly dependent on the number of drop-casting cycles (DCs) and the us…
Self-assembled Plasmonic Nanoparticle Networks (PNN) composed of chains of 12-nm diameter crystalline gold nanoparticles exhibit a longitudinally coupled plasmon mode cen- tered at 700 nm. We have exploited this longitudinal absorption band to efficiently confine light fields and concentrate heat sources in the close vicinity of these plasmonic chain net- works. The mapping of the two phenomena on the same superstructures was performed by combining two-photon luminescence (TPL) and fluorescence polarization anisotropy (FPA) imaging techniques. Besides the light and heat concentration, we show …
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…
The study of nanostructured artificial media for optics has expanded rapidly over the last few decades, coupled with improvements of fabrication technology that have enabled investigation of previously unrealisable optical scattering systems. Such development is complemented by renewed impetus to understand the physics of optical scattering from complex subwavelength geometry and nanoparticle systems. Here I investigate specifically the optical properties of closely packed arrangements of nanoparticles, known as nanoparticle oligomers, which provide an intuitive platform for analytical and num…
Featured by prominent flexibility and fidelity in producing sophisticated stereoscopic structures transdimensionally, three-dimensional (3D) laser printing technique has vastly extended the toolkit for delivering diverse functional devices. Yet chiral nanoemitters heavily resorting to artificial structures that manifest efficient emission and tightly confined light-mater interactions simultaneously remains alluring but dauntingly challenging for this technique at this moment. In this work, we assert the chiral photoluminescence is implemented from silver nanostructures of optical duality in on…
On-chip optoelectronic and all-optical information processing paradigms require compact implementation of signal transfer for which nanoscale surface plasmons circuitry offers relevant solutions. This work demonstrates the directional signal transmittance mediated by 2D plasmonic eigenmodes supported by crystalline cavities. Channel devices comprising two mesoscopic triangular input and output ports and sustaining delocalized, higher-order plasmon resonances in the visible to infra-red range are shown to enable the controllable transmittance between two confined entry and exit ports coupled ov…
Linear Arrays of Metal-Coated Microspheres: a Polarization-Sensitive Hybrid Colloidal Plasmonic-Photonic Crystal
National Institute for Research and Development of Isotopic and Molecular Technologies INCDTIM（同位素和分子技术研究与发展国家研究所）；Institute for Interdisciplinary Research in Bio-Nano-Sciences, Babes-Bolyai University（巴比什-博尧伊大学生物纳米科学跨学科研究所）
