Electrochemically Switchable Multimode Strong Coupling in Plasmonic Nanocavities.

The strong-coupling interaction between quantum emitters and cavities provides the archetypical platform for fundamental quantum electrodynamics. Here we show that methylene blue (MB) molecules interact coherently with subwavelength plasmonic nanocavity modes at room temperature. Experimental results show that the strong coupling can be switched on and off reversibly when MB molecules undergo redox reactions which transform them to leuco-methylene blue molecules. In simulations we demonstrate the strong coupling between the second excited plasmonic cavity mode and resonant emitters. However, we also show that other detuned modes simultaneously couple efficiently to the molecular transitions, creating unusual cascades of mode spectral shifts and polariton formation. This is possible due to the relatively large plasmonic particle size resulting in reduced mode splittings. The results open significant potential for device applications utilizing active control of strong coupling.

Nanoscale Gap-Plasmon-Enhanced Superconducting Photon Detectors at Single-Photon Level.

With a growing demand for detecting light at the single-photon level in various fields, researchers are focused on optimizing the performance of superconducting single-photon detectors (SSPDs) by using multiple approaches. However, input light coupling for visible light has remained a challenge in the development of efficient SSPDs. To overcome these limitations, we developed a novel system that integrates NbN superconducting microwire photon detectors (SMPDs) with gap-plasmon resonators to improve the photon detection efficiency to 98% while preserving all detector performance features, such as polarization insensitivity. The plasmonic SMPDs exhibit a hot-belt effect that generates a nonlinear photoresponse in the visible range operated at 9 K (∼0.64Tc), resulting in a 233-fold increase in phonon-electron interaction factor (γ) compared to pristine SMPDs at resonance under CW illumination. These findings open up new opportunities for ultrasensitive single-photon detection in areas like quantum information processing, quantum optics, imaging, and sensing at visible wavelengths.

Substrate engineering of plasmonic nanocavity antenna modes.

Plasmonic nanocavities have emerged as a promising platform for next-generation spectroscopy, sensing and photonic quantum information processing technologies, benefiting from a unique confluence of nanoscale compactness and integrability, ultrafast functionality and room-temperature viability. Harnessing their unprecedented optical field confinement and enhancement properties for such diverse application domains, however, demands continued innovation in cavity design and robust strategies for engineering their plasmonic mode characteristics, with the aim of optimizing spatial and spectral matching conditions for strong light-matter interaction involving embedded quantum emitters. Adopting the canonical gold bowtie nanoantenna, we show that the complex refractive index, n + ik, of the substrate material provides additional design flexibility in tailoring the properties of plasmonic nanocavity modes, including their resonance wavelengths, hotspot locations, intracavity field polarization and radiative decay rates. In particular, we predict that highly refractive (n ≥ 4) or highly absorptive (k ≥ 4) substrates provide two complementary approaches to engineering nanocavity modes that are especially desirable for coupling two-dimensional quantum materials, featuring namely an elevated hotspot with a dominantly in-plane polarized near-field, as well as a strongly radiative character. Our study elucidates the benefits and intricacies of a largely unexplored facet of nanocavity mode manipulation, beyond the widely practiced synthetic control over the cavity topology or physical dimensions, and paves the way for plasmonic cavity quantum electrodynamics with two-dimensional excitonic matter.

Nanoscopy through a plasmonic nanolens.

Plasmonics now delivers sensors capable of detecting single molecules. The emission enhancements and nanometer-scale optical confinement achieved by these metallic nanostructures vastly increase spectroscopic sensitivity, enabling real-time tracking. However, the interaction of light with such nanostructures typically loses all information about the spatial location of molecules within a plasmonic hot spot. Here, we show that ultrathin plasmonic nanogaps support complete mode sets which strongly influence the far-field emission patterns of embedded emitters and allow the reconstruction of dipole positions with 1-nm precision. Emitters in different locations radiate spots, rings, and askew halo images, arising from interference of 2 radiating antenna modes differently coupling light out of the nanogap, highlighting the imaging potential of these plasmonic "crystal balls." Emitters at the center are now found to live indefinitely, because they radiate so rapidly.

Cascaded nanooptics to probe microsecond atomic-scale phenomena.

Plasmonic nanostructures can focus light far below the diffraction limit, and the nearly thousandfold field enhancements obtained routinely enable few- and single-molecule detection. However, for processes happening on the molecular scale to be tracked with any relevant time resolution, the emission strengths need to be well beyond what current plasmonic devices provide. Here, we develop hybrid nanostructures incorporating both refractive and plasmonic optics, by creating SiO2 nanospheres fused to plasmonic nanojunctions. Drastic improvements in Raman efficiencies are consistently achieved, with (single-wavelength) emissions reaching 107 counts⋅mW-1⋅s-1 and 5 × 105 counts∙mW-1∙s-1∙molecule-1, for enhancement factors >1011 We demonstrate that such high efficiencies indeed enable tracking of single gold atoms and molecules with 17-µs time resolution, more than a thousandfold improvement over conventional high-performance plasmonic devices. Moreover, the obtained (integrated) megahertz count rates rival (even exceed) those of luminescent sources such as single-dye molecules and quantum dots, without bleaching or blinking.

Near-Field Generation and Control of Ultrafast, Multipartite Entanglement for Quantum Nanoplasmonic Networks.

For a quantum Internet, one needs reliable sources of entangled particles that are compatible with measurement techniques enabling time-dependent, quantum error correction. Ideally, they will be operable at room temperature with a manageable decoherence versus generation time. To accomplish this, we theoretically establish a scalable, plasmonically based archetype that uses quantum dots (QD) as quantum emitters, known for relatively low decoherence rates near room temperature, that are excited using subdiffracted light from a near-field transducer (NFT). NFTs are a developing technology that allow rasterization across arrays of qubits and remarkably generate enough power to strongly drive energy transitions on the nanoscale. This eases the fabrication of QD media, while efficiently controlling picosecond-scale dynamic entanglement of a multiqubit system that approaches maximum fidelity, along with fluctuation between tripartite and bipartite entanglement. Our strategy radically increases the scalability and accessibility of quantum information devices while permitting fault-tolerant quantum computing using time-repetition algorithms.

Single-molecule strong coupling at room temperature in plasmonic nanocavities.

Photon emitters placed in an optical cavity experience an environment that changes how they are coupled to the surrounding light field. In the weak-coupling regime, the extraction of light from the emitter is enhanced. But more profound effects emerge when single-emitter strong coupling occurs: mixed states are produced that are part light, part matter1, 2, forming building blocks for quantum information systems and for ultralow-power switches and lasers. Such cavity quantum electrodynamics has until now been the preserve of low temperatures and complicated fabrication methods, compromising its use. Here, by scaling the cavity volume to less than 40 cubic nanometres and using host­guest chemistry to align one to ten protectively isolated methylene-blue molecules, we reach the strong-coupling regime at room temperature and in ambient conditions. Dispersion curves from more than 50 such plasmonic nanocavities display characteristic light­matter mixing, with Rabi frequencies of 300 millielectronvolts for ten methylene-blue molecules, decreasing to 90 millielectronvolts for single molecules­matching quantitative models. Statistical analysis of vibrational spectroscopy time series and dark-field scattering spectra provides evidence of single-molecule strong coupling. This dressing of molecules with light can modify photochemistry, opening up the exploration of complex natural processes such as photosynthesis and the possibility of manipulating chemical bonds.

Gate-Tunable Plasmon-Enhanced Photodetection in a Monolayer MoS2 Phototransistor with Ultrahigh Photoresponsivity.

Monolayer transition metal dichalcogenides (TMDs), direct bandgap materials with an atomically thin nature, are promising materials for electronics and photonics, especially at highly scaled lateral dimensions. However, the characteristically low total absorption of photons in the monolayer TMD has become a challenge in the access to and realization of monolayer TMD-based high-performance optoelectronic functionalities and devices. Here, we demonstrate gate-tunable plasmonic phototransistors (photoFETs) that consist of monolayer molybdenum disulfide (MoS2) photoFETs integrated with the two-dimensional plasmonic crystals. The plasmonic photoFET has an ultrahigh photoresponsivity of 2.7 × 104 AW-1, achieving a 7.2-fold enhancement in the photocurrent compared to pristine photoFETs. This benefits predominately from the combination of the enhancement of the photon-absorption-rate via the strongly localized-electromagnetic-field and the gate-tunable plasmon-induced photocarrier-generation-rate in the monolayer MoS2. These results demonstrate a systematic methodology for designing ultrathin plasmon-enhanced photodetectors based on monolayer TMDs for next-generation ultracompact optoelectronic devices in the trans-Moore era.

Controlled Cavity-Free, Single-Photon Emission and Bipartite Entanglement of Near-Field-Excited Quantum Emitters.

We report theoretical statistics of 1- and 2-qubit (bipartite) systems, namely, photon antibunching and entanglement, of near-field excited quantum emitters. The sub-diffraction focusing of a plasmonic waveguide is shown to generate enough power over a sufficiently small region (<50 × 50 nm2) to strongly drive quantum emitters. This enables ultrafast (10-14 s) single-photon emission as well as creates entangled states between two emitters when performing a controlled-NOT operation. A comparative analysis of silicon and near-zero index materials demonstrates advantages and uncovers challenges of embedding quantum emitters for single-photon emission and for bipartite entanglement. The use of a movable plasmonic waveguide, in lieu of stationary nanostructures, allows high-speed rasterization between sets of qubits and enables spatially flexible data storage and quantum information processing. Furthermore, the sub-diffraction focusing of the waveguide is shown to achieve cavity-free dynamic entanglement. This greatly reduces fabrication constraints and increases the speed and scalability of nanophotonic quantum devices.

Generation of plasmonic hot carriers from d-bands in metallic nanoparticles.

We present an approach to master the well-known challenge of calculating the contribution of d-bands to plasmon-induced hot carrier rates in metallic nanoparticles. We generalize the widely used spherical well model for the nanoparticle wavefunctions to flat d-bands using the envelope function technique. Using Fermi's golden rule, we calculate the generation rates of hot carriers after the decay of the plasmon due to transitions either from a d-band state to an sp-band state or from an sp-band state to another sp-band state. We apply this formalism to spherical silver nanoparticles with radii up to 20 nm and also study the dependence of hot carrier rates on the energy of the d-bands. We find that for nanoparticles with a radius less than 2.5 nm, sp-band state to sp-band state transitions dominate hot carrier production, while d-band state to sp-band state transitions give the largest contribution for larger nanoparticles.

Quantum Plasmonic Immunoassay Sensing.

Plasmon-polaritons are among the most promising candidates for next-generation optical sensors due to their ability to support extremely confined electromagnetic fields and empower strong coupling of light and matter. Here we propose quantum plasmonic immunoassay sensing as an innovative scheme, which embeds immunoassay sensing with recently demonstrated room-temperature strong coupling in nanoplasmonic cavities. In our protocol, the antibody-antigen-antibody complex is chemically linked with a quantum emitter label. Placing the quantum-emitter-enhanced antibody-antigen-antibody complexes inside or close to a nanoplasmonic (hemisphere dimer) cavity facilitates strong coupling between the plasmon-polaritons and the emitter label resulting in signature Rabi splitting. Through rigorous statistical analysis of multiple analytes randomly distributed on the substrate in extensive realistic computational experiments, we demonstrate a drastic enhancement of the sensitivity up to nearly 1500% compared to conventional shifting-type plasmonic sensors. Most importantly and in stark contrast to classical sensing, we achieve in the strong-coupling (quantum) sensing regime an enhanced sensitivity that is no longer dependent on the concentration of antibody-antigen-antibody complexes down to the single-analyte limit. The quantum plasmonic immunoassay scheme thus not only leads to the development of plasmonic biosensing for single molecules but also opens up new pathways toward room-temperature quantum sensing enabled by biomolecular inspired protocols linked with quantum nanoplasmonics.

Asymmetric transmission of light in hybrid waveguide-integrated plasmonic crystals on a silicon-on-insulator platform.

We demonstrate asymmetric transmission of light in hybrid waveguide-integrated plasmonic crystals where triangular silver islands create a regular array of nanogaps which couple to an underlying silicon-on-insulator optical waveguide. Up to 60% difference is observed between light transmission in the forward and backward directions. This asymmetric transmission of light is not caused by an external magnetic field or nonlinearity, but solely a consequence of the structure geometry.

Mapping Nanoscale Hotspots with Single-Molecule Emitters Assembled into Plasmonic Nanocavities Using DNA Origami.

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-5 nm 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 ≥4 × 103 with high quantum yield (≥50%). By varying the lateral position of the molecule in the gap, we directly map the spatial profile of the local density of optical states with a resolution of ±1.5 nm. Our approach introduces a straightforward noninvasive way to measure and quantify confined optical modes on the nanoscale.

Tunable surface waves at the interface separating different graphene-dielectric composite hyperbolic metamaterials.

Despite the fact that metal is the most common conducting constituent element in the fabrication of metamaterials, one of the advantages of graphene over metal is that its conductivity can be controlled by the Fermi energy. Here, we theoretically investigate multilayer structures comprising alternating graphene and dielectric layers as a class of hyperbolic metamaterials for THz frequencies based on a general simple model of the graphene and the dielectric layers. By employing a method of matching the tangential components of the electrical and magnetic fields, we derive the relevant dispersion relations and demonstrate that tuning can be achieved by modifying the Fermi energy. Moreover, tunability of the graphene-dielectric heterostructures can be enhanced further by changing either the thickness of the dielectric layers or the number of graphene sheets employed. Calculated dispersion relations, propagation lengths of plasmon modes in the system are presented. This allows us to characterize and categorize the modes into two groups: Ferrel-Berreman modes and surface plasmon polaritons.

Group Theoretical Route to Deterministic Weyl Points in Chiral Photonic Lattices.

Topological phases derived from point degeneracies in photonic band structures show intriguing and unique behavior. Previously identified band degeneracies are based on accidental degeneracies and subject to engineering on a case-by-case basis. Here we show that deterministic pseudo Weyl points with nontrivial topology and hyperconic dispersion exist at the Brillouin zone center of chiral cubic symmetries. This conceivably allows realization of topologically protected frequency isolated surface bands in 3D and n=0 properties as demonstrated for a nanoplasmonic system and a photonic crystal.

Completely stopped and dispersionless light in plasmonic waveguides.

We introduce a scheme where a time-dependent source excites "complex-frequency" modes in uniform plasmonic heterostructures, enabling complete and dispersionless stopping of light pulses, resilient to realistic levels of dissipative, radiative, and surface-roughness losses. Using transparent conducting oxides at telecommunication wavelengths we show how, without increasing optical losses, multiple light pulses can decay with time precisely at their injection points, unable to propagate despite the complete absence of barriers in front or behind them. Our results theoretically demonstrate extraordinary large light-deceleration factors (of the order of 1.5×107) in integrated nanophotonic media, comparable only to those attainable with ultracold atomic vapors or with quantum coherence effects, such as coherent population oscillations, in ruby crystals.

Ultrafast photoluminescence and multiscale light amplification in nanoplasmonic cavity glass.

Interactions between plasmons and exciton nanoemitters in plexcitonic systems lead to fast and intense luminescence, desirable in optoelectonic devices, ultrafast optical switches and quantum information science. While luminescence enhancement through exciton-plasmon coupling has thus far been mostly demonstrated in micro- and nanoscale structures, analogous demonstrations in bulk materials have been largely neglected. Here we present a bulk nanocomposite glass doped with cadmium telluride quantum dots (CdTe QDs) and silver nanoparticles, nAg, which act as exciton and plasmon sources, respectively. This glass exhibits ultranarrow, FWHM = 13 nm, and ultrafast, 90 ps, amplified photoluminescence (PL), λem≅503 nm, at room temperature under continuous-wave excitation, λexc = 405 nm. Numerical simulations confirm that the observed improvement in emission is a result of a multiscale light enhancement owing to the ensemble of QD-populated plasmonic nanocavities in the material. Power-dependent measurements indicate that >100 mW coherent light amplification occurs. These types of bulk plasmon-exciton composites could be designed comprising a plethora of components/functionalities, including emitters (QDs, rare earth and transition metal ions) and nanoplasmonic elements (Ag/Au/TCO, spherical/anisotropic/miscellaneous), to achieve targeted applications.

Self-focusing of femtosecond surface plasmon polaritons.

We study the propagation of femtosecond pulses in nonlinear metal-dielectric plasmonic waveguiding structures by employing the finite-difference time-domain numerical method. Self-focusing of plasmon pulses is observed for defocusing Kerr-like nonlinearity of the dielectric medium due to normal dispersion. We compare the nonlinear propagation of plasmon pulses along a single metal-dielectric interface with the propagation within a metal-dielectric-metal slot waveguide and observe that nonlinear effects are more pronounced for the single surface where longer propagation length may compensate for lower field confinement.

Scattering of core-shell nanowires with the interference of electric and magnetic resonances.

We study the scattering of normally incident waves by core-shell nanowires, which support both electric and magnetic resonances. Within such nanowires, for p-polarized incident waves, each electric resonance corresponds to two degenerate scattering channels while the magnetic resonance corresponds to only one channel. Consequently, when the electric dipole (ED) and magnetic dipole (MD) are tuned to overlap spectrally, the magnitude of the ED is twice that of the magnetic one, leading to a pair of angles of vanishing scattering. We further demonstrate that the scattering features of nanowires are polarization dependent, and vanishing scattering angles also can be induced by Fano resonances due to the interference of higher-order electric modes with the broad MD mode.

Dirac-like plasmons in honeycomb lattices of metallic nanoparticles.

We consider a two-dimensional honeycomb lattice of metallic nanoparticles, each supporting a localized surface plasmon, and study the quantum properties of the collective plasmons resulting from the near-field dipolar interaction between the nanoparticles. We analytically investigate the dispersion, the effective Hamiltonian, and the eigenstates of the collective plasmons for an arbitrary orientation of the individual dipole moments. When the polarization points close to the normal to the plane, the spectrum presents Dirac cones, similar to those present in the electronic band structure of graphene. We derive the effective Dirac Hamiltonian for the collective plasmons and show that the corresponding spinor eigenstates represent Dirac-like massless bosonic excitations that present similar effects to electrons in graphene, such as a nontrivial Berry phase and the absence of backscattering off smooth inhomogeneities. We further discuss how one can manipulate the Dirac points in the Brillouin zone and open a gap in the collective plasmon dispersion by modifying the polarization of the localized surface plasmons, paving the way for a fully tunable plasmonic analogue of graphene.