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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.

Plasmonic nanoantennas offer intense confinement of light, to volumes even below the diffraction limit. Routine scattering analysis offers limited information on near-field intricacies. Therefore, we adopt a quasinormal mode approach to reveal the strong facet morphology dependence of rhombicuboctahedron-on-mirror near-field charge distributions, as well as far-field out-coupling. Thus allows for structural identification from far-field measurements.

In the past decade, advances in nanotechnology have led to the development of plasmonic nanocavities that facilitate light–matter strong coupling in ambient conditions. The most robust example is t...

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 bio-sensing for single molecules but also opens up new pathways towards room-temperature quantum sensing enabled by biomolecular inspired protocols linked with quantum nanoplasmonics., Just Accepted Manuscript, Nano Letters 2019

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 (

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 SiO 2 nanospheres fused to plasmonic nanojunctions. Drastic improvements in Raman efficiencies are consistently achieved, with (single-wavelength) emissions reaching 10 7 counts⋅mW −1 ⋅s −1 and 5 × 10 5 counts∙mW −1 ∙s −1 ∙molecule −1 , for enhancement factors >10 11 . 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.

Plasmonic nanoantennas are able to produce extreme enhancements by concentrating electromagnetic fields into sub-wavelength volumes. Recently, one of the most commonly used nanoantennas is the nanoparticle-on-mirror geometry, which allowed for the room temperature strong coupling of a single molecule. Very few studies offer analysis of near-field mode decompositions, and they mainly focus on spherical and/or cylindrically-faceted nanoparticle-on-mirror geometries. Perfectly spherical nanoparticles are not easy to fabricate, with recent publications revealing that a rhombicuboctahedron is a commonly occurring nanoparticle shape – due to the crystalline nature of metallic nanoparticles. In this paper, we perform a quasi-normal mode analysis for the rhombicuboctahedron-on-mirror nanoantenna and map the field distributions of each mode. We examine how the geometry of the cavity defines the near-field distribution and energies of the modes, and we show that in some cases the mode degeneracies break. This has a significant impact on the radiative emission and far-field profile of each mode, which are measured experimentally. Understanding how realistic nanoantenna geometries behave in the near-field and far-field helps us design antennas with specific properties for controlling and sensing quantum emitters in plasmonic systems.

Significance Imaging of single to a few molecules has received much recent interest. While superresolution microscopies access subdiffraction resolution, they do not work for plasmonic hot spots due to the loss of positional information that results from plasmonic coupling. Here, we show how to reconstruct the spatial locations of molecules within a plasmonic hot spot with 1-nm precision. We use a plasmonic nanoball lens to demonstrate that plasmonic nanocavities can be used simultaneously as a nanoscopic and spectroscopic tool. This work opens up possibilities for studying the behavior of a few to single molecules in plasmonic nanoresonators, while simultaneously tracking their movements and spectral features. Our plasmonic nanolens is useful for nanosensing, nanochemistry, and biofunctional imaging., 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.

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.

Strong light–matter interaction is at the heart of modern quantum technological applications and is the basis for a wide range of rich optical phenomena. Coupling a single quantum emitter strongly with electromagnetic fields provides an unprecedented control over its quantum states and enables high-fidelity quantum operations. However, single-emitter strong coupling is exceptionally fragile and has been realized mostly at cryogenic temperatures. Recent experiments have, however, demonstrated that single-emitter strong coupling can be realized at room temperature by using plasmonic nanocavities that confine optical fields via surface plasmons strongly on metal surfaces and facilitate sub-picosecond light–matter interaction. Here, we outline recent theoretical developments and experimental demonstrations of room-temperature strong coupling in the plasmonic platform, from emitter ensembles down to the single emitter limit, before placing a focus on selective studies that explore and provide insight into applications of plexcitonic strong coupling including sensing of single biological molecules, qubit entanglement generation, and reconfigurable single-photon sources and provide an outline of research directions in quantum sensing, quantum information processing, and ultrafast spectroscopy.

Emission properties of a quantum emitter can be significantly modified inside nanometre-sized gaps between two plasmonic nanostructures. This forms a nanoscopic optical cavity which allows single-molecule detection and single-molecule strong-coupling at room temperature. However, plasmonic resonances of a plasmonic nanocavity are highly sensitive to the exact gap morphology. In this article, we shed light on the effect of gap morphology on the plasmonic resonances of a faceted nanoparticle-on-mirror (NPoM) nanocavity and their interaction with quantum emitters. We find that with increasing facet width the NPoM nanocavity provides weaker field enhancement and thus less coupling strength to a single quantum emitter since the effective mode volume increases with the facet width. However, if multiple emitters are present, a faceted NPoM nanocavity is capable of accommodating a larger number of emitters, and hence the overall coupling strength is larger due to the collective and coherent energy exchange from all the emitters. Our findings pave the way to more efficient designs of nanocavities for room-temperature light-matter strong-coupling, thus providing a big step forward to a non-cryogenic platform for quantum technologies.

An emitter in the vicinity of a metal nanostructure is quenched by its decay through nonradiative channels, leading to the belief in a zone of inactivity for emitters placed within

Fluorescence emission of a quantum emitter is dominated by its optical environment, and it was proven that an emitter is quenched when it is placed too closed to metal nanoparticles. Here, we present the spatio-temporal dynamics of the emitter and demonstrate that quenching can in fact be suppressed in plasmonic nanocavities. By varying the lateral position of an emitter through DNA-origami technique, our results are confirmed with experimental measurements.

We propose a smooth pseudopotential for the contact interaction acting between ultracold atoms confined to two dimensions. The pseudopotential reproduces the scattering properties of the repulsive contact interaction up to 200 times more accurately than a hard disk potential, and in the attractive branch gives a 10-fold improvement in accuracy over the square well potential. Furthermore, the new potential enables diffusion Monte Carlo simulations of the ultracold gas to be run 15 times quicker than was previously possible.

Recent experiments and kinetic Monte Carlo (KMC) simulations [H. Greve et al., Appl. Phys. Lett. 88, 123103 (2006), L. Rosenthal et al., J. Appl. Phys. 114, 044305 (2013)] demonstrated that physical vapor co-deposition of a metal alloy (Fe-Ni-Co) and a polymer (Teflon AF) is a suitable method to grow magnetic nanocolumns in a self-organized one-step process. While only thermal sources have been used so far, in this work, we analyze the feasibility of this process for the case of a sputtering source. For that purpose, we extend our previous simulation model by including a process that takes into account the influence of ions impinging on the substrate. The simulation results predict that metal nanocolumn formation should be possible. Furthermore, we show that the effect of ions that create trapping sites for the metal particles is to increase the number of nanocolumns.

We numerically demonstrate strongly-driven, dynamic entanglement of quantum emitters using time-varying, sub-diffracted light from a near-field transducer. Using cavity-free environments, a controlled-NOT quantum logic operation is performed and ultrafast, single-photon emission is demonstrated.