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.

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.

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.

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.

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.

Tailoring the Third-Order Nonlinear Optical Property of a Hybrid Semiconductor Quantum Dot-Metal Nanoparticle: From Saturable to Fano-Enhanced Absorption.

Semiconductor-metal hybrid nanostructures present an exotic class of nonlinear optical materials due to their potential optoelectronic applications. However, most studies to date focus on their total optical responses instead of contributions from individual nonlinear orders. In this Letter, we present a theoretical study on the third-order nonlinear optical absorption of a hybrid colloidal semiconductor quantum dot (SQD)-metal nanoparticle (MNP) system. We develop a novel analytic treatment based on the nonlinear density matrix equation and derive a closed-form expression for the optical susceptibility. Our study identifies the parameter space that governs the system's optical transition from being a saturable absorber to a Fano-enhanced absorber. We attribute this transition to the plasmon-mediated self-interaction of the SQD. The findings provide a valuable guideline for optimized designs of functional nanophotonic devices based on SQD-MNP hybrid structures.