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In this study, we construct Fabry-Perot cavities in which nanostructured, thin resonant metasurfaces act as mirrors. We develop a temporal coupled-mode theory and provide an accurate description of the resonances supported by these cavities, deriving analytically their transmission characteristics. The presence of metasurface mirrors introduces a substantial group delay, causing the field concentration to shift from the bulk of the cavity towards the regions close to the two metasurfaces. This shift is accompanied by a significant increase in the quality factor of the resonances that is associated with the emergence of singular points in frequency space. These singular points exist even when the cavity separations are smaller than the cavity length of the fundamental mode in standard cavities, enabling meta-mirror Fabry-Perot cavities to outperform traditional cavities by achieving much higher quality factors despite displaying shorter cavity lengths.

The manipulation of low-energy matter properties such as superconductivity, ferromagnetism, and ferroelectricity via cavity quantum electrodynamics engineering has been suggested as a way to enhance these many-body collective phenomena. In this work, we investigate the effective interactions between low-energy matter excitations induced by the off-resonant coupling with cavity electromagnetic modes. We extend a previous work by going beyond the dipole approximation accounting for the full polarization and magnetization densities of matter. We further include the often neglected diamagnetic interaction and, for the cavity, we consider general linear absorbing media with possibly non-local and non-reciprocal response. We demonstrate that, even in this general scenario, the effective cavity-induced interactions between the matter degrees of freedom are of electrostatic and magnetostatic nature. This confirms the necessity of a multimode description for cavity engineering of matter systems where the low-energy assumption holds. Our findings provide a theoretical framework for studying the influence of general optical environments on extended low-energy matter excitations., (© 2024 Author(s). Published under an exclusive license by AIP Publishing.)

We demonstrate spontaneous symmetry breaking in the diffraction of a laser-driven grating with memory in its nonlinear response. We observe, experimentally and theoretically, asymmetric diffraction even when the grating and illumination are symmetric. Our analysis reveals how diffracted waves can spontaneously acquire momentum parallel to the lattice vector in quantities unconstrained by the grating period. Our findings point to numerous opportunities for imaging, sensing, and information processing with nonlinear periodic systems, which can leverage a much richer diffractive response than their linear counterparts.

Molecules are the building blocks of all of nature's functional components, serving as the machinery that captures, stores and releases energy or converts it into useful work. However, molecules interact with each other over extremely short distances, which hinders the spread of energy across molecular systems. Conversely, photons are inert, but they are fast and can traverse large distances very efficiently. Using optical resonators, these distinct entities can be mixed with each other, opening a path to new architectures that benefit from both the active nature of molecules and the long-range transport obtained by the coupling with light. In this Review, we present the physics underlying the enhancement of energy transfer and energy transport in molecular systems, and highlight the experimental and theoretical advances in this field over the past decade. Finally, we identify several key questions and theoretical challenges that remain to be resolved via future research., (© 2024. Springer Nature Limited.)

Magnetic order typically emerges due to the short-range exchange interaction between the constituent electronic spins. Recent discoveries have found a crucial role for spin-phonon coupling in various phenomena from optical ultrafast magnetization switching to dynamical control of the magnetic state. Here, we demonstrate theoretically the emergence of a biquadratic long-range interaction between spins mediated by their coupling to phonons hybridized with vacuum photons into polaritons. The resulting ordered state enabled by the exchange of virtual polaritons between spins is reminiscent of superconductivity mediated by the exchange of virtual phonons. The biquadratic nature of the spin-spin interaction promotes ordering without favoring ferro- or antiferromagnetism. It further makes the phase transition to magnetic order a first-order transition, unlike in conventional magnets. Consequently, a large magnetization develops abruptly on lowering the temperature which could enable magnetic memories admitting ultralow-power thermally-assisted writing while maintaining a high data stability. The role of photons in the phenomenon further enables an in-situ static control over the magnetism. These unique features make our predicted spin-spin interaction and magnetism highly unconventional paving the way for novel scientific and technological opportunities., (© 2024. The Author(s).)

Despite significant theoretical efforts devoted to studying the interaction between quantized light modes and matter, the so-called ultrastrong coupling regime still presents significant challenges for theoretical treatments and prevents the use of many common approximations. Here we demonstrate an approach that can describe the dynamics of hybrid quantum systems in any regime of interaction for an arbitrary electromagnetic (EM) environment. We extend a previous method developed for few-mode quantization of arbitrary systems to the case of ultrastrong light-matter coupling, and show that even such systems can be treated using a Lindblad master equation where decay operators act only on the photonic modes by ensuring that the effective spectral density of the EM environment is sufficiently suppressed at negative frequencies. We demonstrate the validity of our framework and show that it outperforms current state-of-the-art master equations for a simple model system, and then study a realistic nanoplasmonic setup where existing approaches cannot be applied.

Strong coupling between lead halide perovskite materials and optical resonators enables both polaritonic control of the photophysical properties of these emerging semiconductors and the observation of fundamental physical phenomena. However, the difficulty in achieving optical-quality perovskite quantum dot (PQD) films showing well-defined excitonic transitions has prevented the study of strong light-matter coupling in these materials, central to the field of optoelectronics. Herein we demonstrate the formation at room temperature of multiple cavity exciton-polaritons in metallic resonators embedding highly transparent Cesium Lead Bromide quantum dot (CsPbBr 3 -QD) solids, revealed by a significant reconfiguration of the absorption and emission properties of the system. Our results indicate that the effects of biexciton interaction or large polaron formation, frequently invoked to explain the properties of PQDs, are seemingly absent or compensated by other more conspicuous effects in the CsPbBr 3 -QD optical cavity. We observe that strong coupling enables a significant reduction of the photoemission line width, as well as the ultrafast modulation of the optical absorption, controllable by means of the excitation fluence. We find that the interplay of the polariton states with the large dark state reservoir plays a decisive role in determining the dynamics of the emission and transient absorption properties of the hybridized light-quantum dot solid system. Our results should serve as the basis for future investigations of PQD solids as polaritonic materials.

The full information about the interaction between a quantum emitter and an arbitrary electromagnetic environment is encoded in the so-called spectral density. We present an approach for describing such interaction in any coupling regime, providing a Lindblad-like master equation for the emitter dynamics when coupled to a general nanophotonic structure. Our framework is based on the splitting of the spectral density into two terms. On the one hand, a spectral density responsible for the non-Markovian and strong-coupling-based dynamics of the quantum emitter. On the other hand, a residual spectral density including the remaining weak-coupling terms. The former is treated nonperturbatively with a collection of lossy interacting discrete modes whose parameters are determined by a fit to the original spectral density in a frequency region encompassing the quantum emitter transition frequencies. The latter is treated perturbatively under a Markovian approximation. We illustrate the power and validity of our approach through numerical simulations in three different setups, thus offering a variety of scenarios for a full test, including the ultra-strong coupling regime., Competing Interests: Conflict of interest: Authors state no conflicts of interest., (© 2024 the author(s), published by De Gruyter, Berlin/Boston.)

Controlling quantum materials with light is of fundamental and technological importance. By utilizing the strong coupling of light and matter in optical cavities 1-3 , recent studies were able to modify some of their most defining features 4-6 . Here we study the magneto-optical properties of a van der Waals magnet that supports strong coupling of photons and excitons even in the absence of external cavity mirrors. In this material-the layered magnetic semiconductor CrSBr-emergent light-matter hybrids called polaritons are shown to substantially increase the spectral bandwidth of correlations between the magnetic, electronic and optical properties, enabling largely tunable optical responses to applied magnetic fields and magnons. Our results highlight the importance of exciton-photon self-hybridization in van der Waals magnets and motivate novel directions for the manipulation of quantum material properties by strong light-matter coupling., (© 2023. The Author(s), under exclusive licence to Springer Nature Limited.)

We investigate the generation of entanglement between two quantum emitters through the inverse-design engineering of their photonic environment. By means of a topology-optimization approach acting at the level of the electromagnetic Dyadic Green's function, we generate dielectric cloaks operating at different inter-emitter distances and incoherent pumping strengths. We show that the structures obtained maximize the dissipative coupling between the emitters under extremely different Purcell factor conditions, and yield steady-state concurrence values much larger than those attainable in free space. Finally, we benchmark our design strategy by proving that the entanglement enabled by our devices approaches the limit of maximum-entangled-mixed-states., (© 2022 the author(s), published by De Gruyter, Berlin/Boston.)

The control of the interaction between quantum emitters using nanophotonic structures holds great promise for quantum technology applications, while its theoretical description for complex nanostructures is a highly demanding task as the electromagnetic (EM) modes form a high-dimensional continuum. We here introduce an approach that permits a quantized description of the full EM field through a small number of discrete modes. This extends the previous work in ref. (I. Medina, F. J. García-Vidal, A. I. Fernández-Domínguez, and J. Feist, "Few-mode field quantization of arbitrary electromagnetic spectral densities," Phys. Rev. Lett. , vol. 126, p. 093601, 2021) to the case of an arbitrary number of emitters, without any restrictions on the emitter level structure or dipole operators. The low computational demand of this method makes it suitable for studying dynamics for a wide range of parameters. We illustrate the power of our approach for a system of three emitters placed within a hybrid metallodielectric photonic structure and show that excitation transfer is highly sensitive to the properties of the hybrid photonic-plasmonic modes., (© 2022 the author(s), published by De Gruyter, Berlin/Boston.)

In the past decade, much theoretical research has focused on studying the strong coupling between organic molecules (or quantum emitters, in general) and light modes. The description and prediction of polaritonic phenomena emerging in this light-matter interaction regime have proven to be difficult tasks. The challenge originates from the enormous number of degrees of freedom that need to be taken into account, both in the organic molecules and in their photonic environment. On one hand, the accurate treatment of the vibrational spectrum of the former is key, and simplified quantum models are not valid in many cases. On the other hand, most photonic setups have complex geometric and material characteristics, with the result that photon fields corresponding to more than just a single electromagnetic mode contribute to the light-matter interaction in these platforms. Moreover, loss and dissipation, in the form of absorption or radiation, must also be included in the theoretical description of polaritons. Here, we review and offer our own perspective on some of the work recently done in the modeling of interacting molecular and optical states with increasing complexity., Competing Interests: The authors declare no competing financial interest., (© 2022 The Authors. Published by American Chemical Society.)

We investigate the quantum-optical properties of the light emitted by a nanoparticle-on-mirror cavity filled with a single quantum emitter. Inspired by recent experiments, we model a dark-field setup and explore the photon statistics of the scattered light under grazing laser illumination. Exploiting analytical solutions to Maxwell's equations, we quantize the nanophotonic cavity fields and describe the formation of plasmon-exciton polaritons (or plexcitons) in the system. This way, we reveal that the rich plasmonic spectrum of the nanocavity offers unexplored mechanisms for nonclassical light generation that are more efficient than the resonant interaction between the emitter natural transition and the brightest optical mode. Specifically, we find three different sample configurations in which strongly antibunched light is produced. Finally, we illustrate the power of our approach by showing that the introduction of a second emitter in the platform can enhance photon correlations further.

The recent development of organic polaritonic solar cells, in which sunlight absorbers and photon modes of a resonator are hybridized as a result of their strong coupling, has revealed the potential this interaction offers to control and enhance the performance of these devices. In this approach, the photovoltaic cell is built in such a way that it also behaves as an optical cavity supporting spectrally well-defined resonances, which match the broad absorption bands of the dyes employed. Herein we focus on the experimental and theoretical analysis of the specific spectral and angular optical absorption characteristics of a broadband light harvester, namely a subphthalocyanine, when operating in the ultrastrong coupling regime. We discuss the implications of having a broad distribution of oscillator strengths and demonstrate that rational design of the layered structure is needed to optimize both the spectral and the angular response of the sunlight harvester dye.

We develop a framework that provides a few-mode master equation description of the interaction between a single quantum emitter and an arbitrary electromagnetic environment. The field quantization requires only the fitting of the spectral density, obtained through classical electromagnetic simulations, to a model system involving a small number of lossy and interacting modes. We illustrate the power and validity of our approach by describing the population and electric field spatial dynamics in the spontaneous decay of an emitter placed in a complex hybrid plasmonic-photonic structure.

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 ultrafast exciton dynamics in the large Purcell enhancement regime and the corresponding emission spectrum, showing that these magnitudes are not accurately represented by the simplified models used up to date. Specifically, both the two-level system model and the single vibrational mode model can only reproduce the dynamics over short time scales, whereas the Fermi's golden rule approach accounts only for the behavior at very long times. We demonstrate that including the whole set of vibrational modes is necessary to capture most of the dynamics and the corresponding spectrum. Moreover, by disentangling the coupling of the molecule to radiative and nonradiative plasmonic modes, we also shed light into the quenching phenomenology taking place in the system., Competing Interests: The authors declare no competing financial interest., (© 2020 American Chemical Society.)

Luminescence arising from β -decay of radiotracers has garnered much interest recently as a viable in-vivo imaging technique. The emitted Cerenkov radiation can be directly detected by high sensitivity cameras or used to excite highly efficient fluorescent dyes. Here, we investigate the enhancement of visible and infrared emission driven by β -decay of radioisotopes in the presence of a hyperbolic nanocavity. By means of a transfer matrix approach, we obtain quasi-analytic expressions for the fluorescence enhancement factor at the dielectric core of the metalodielectric cavity, reporting a hundred-fold amplification in periodic structures. A particle swarm optimization of the layered shell geometry reveals that up to a ten-thousand-fold enhancement is possible thanks to the hybridization and spectral overlapping of whispering-gallery and localized-plasmon modes. Our findings may find application in nuclear-optical medical imaging, as they provide a strategy for the exploitation of highly energetic gamma rays, Cerenkov luminescence, and visible and near-infrared fluorescence through the same nanotracer.

Conventional approaches to probing ultrafast molecular dynamics rely on the use of synchronized laser pulses with a well-defined time delay. Typically, a pump pulse excites a molecular wavepacket. A subsequent probe pulse can then dissociate or ionize the molecule, and measurement of the molecular fragments provides information about where the wavepacket was for each time delay. Here, we propose to exploit the ultrafast nuclear-position-dependent emission obtained due to large light-matter coupling in plasmonic nanocavities to image wavepacket dynamics using only a single pump pulse. We show that the time-resolved emission from the cavity provides information about when the wavepacket passes a given region in nuclear configuration space. This approach can image both cavity-modified dynamics on polaritonic (hybrid light-matter) potentials in the strong light-matter coupling regime and bare-molecule dynamics in the intermediate coupling regime of large Purcell enhancements, and provides a route towards ultrafast molecular spectroscopy with plasmonic nanocavities.

Atomically-sharp tips in close proximity of metal surfaces create plasmonic nanocavities supporting both radiative (bright) and non-radiative (dark) localized surface plasmon modes. Disentangling their respective contributions to the total density of optical states remains a challenge. Electroluminescence due to tunnelling through the tip-substrate gap could allow the identification of the radiative component, but this information is inherently convoluted 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 microscope luminescence spectra by confronting them with spectroscopic information extracted from elastic current measurements. Comparison against electromagnetic calculations demonstrates that this procedure allows the characterization of the meV shifts experienced by the nanocavity plasmonic modes under atomic-scale gap size changes. Therefore, the method gives access to the frequency-dependent radiative Purcell enhancement that a microscopic light emitter would undergo when placed at such nanocavity.

Recently, exciton-photon strong coupling has been proposed as a means to control and enhance energy transfer in ensembles of organic molecules. Here, we demonstrate that the exciton dynamics in an archetypal purple bacterial photosynthetic unit, composed of six LH2 antennas surrounding a single LH1 complex, is greatly modified by its interaction with an optical cavity. We develop a Bloch-Redfield master equation approach that accounts for the interplay between the B800 and B850 bacteriochlorophyll molecules within each LH2 antenna, as well as their interactions with the central LH1 complex. Using a realistic parametrization of both the photosynthetic unit and optical cavity, we investigate the formation of polaritons in the system, revealing that these can be tuned to accelerate its exciton dynamics by 3 orders of magnitude. This yields a significant occupation of the LH1 complex, the stage immediately prior to the reaction center, with only a few-femtosecond delay after the initial excitation of the LH2 B800 pigments. Our theoretical findings unveil polaritonic phenomena as a promising route for the characterization, tailoring, and optimization of light-harvesting mechanisms in natural and artificial photosynthetic processes.

We analyze the properties of strongly coupled excitons and photons in systems made of semiconducting two-dimensional transition-metal dichalcogenides embedded in optical cavities. Through a detailed microscopic analysis of the coupling, we unveil novel, highly tunable features of the spectrum that result in polariton splitting and a breaking of light-matter selection rules. The dynamics of the composite polaritons is influenced by the Berry phase arising both from their constituents and from the confinement-enhanced coupling. We find that light-matter coupling emerges as a mechanism that enhances the Berry phase of polaritons well beyond that of its elementary constituents, paving the way to achieve a polariton anomalous Hall effect.

This corrects the article DOI: 10.1038/ncomms14479.

As the size of a molecular emitter becomes comparable to the dimensions of a nearby optical resonator, the standard approach that considers the emitter to be a point-like dipole breaks down. By adoption of a quantum description of the electronic transitions of organic molecular emitters, coupled to a plasmonic electromagnetic field, we are able to accurately calculate the position-dependent coupling strength between a plasmon and an emitter. The spatial distribution of excitonic and photonic quantum states is found to be a key aspect in determining the dynamics of molecular emission in ultrasmall cavities both in the weak and strong coupling regimes. Moreover, we show that the extreme localization of plasmonic fields leads to the selection rule breaking of molecular excitations.

We demonstrate in this work that the use of metasurfaces provides a viable strategy to largely tune and enhance near-field radiative heat transfer between extended structures. In particular, using a rigorous coupled wave analysis, we predict that Si-based metasurfaces featuring two-dimensional periodic arrays of holes can exhibit a room-temperature near-field radiative heat conductance much larger than any unstructured material to date. We show that this enhancement, which takes place in a broad range of separations, relies on the possibility to largely tune the properties of the surface plasmon polaritons that dominate the radiative heat transfer in the near-field regime.

Radiative heat transfer in Ångström- and nanometre-sized gaps is of great interest because of both its technological importance and open questions regarding the physics of energy transfer in this regime. Here we report studies of radiative heat transfer in few Å to 5 nm gap sizes, performed under ultrahigh vacuum conditions between a Au-coated probe featuring embedded nanoscale thermocouples and a heated planar Au substrate that were both subjected to various surface-cleaning procedures. By drawing on the apparent tunnelling barrier height as a signature of cleanliness, we found that upon systematically cleaning via a plasma or locally pushing the tip into the substrate by a few nanometres, the observed radiative conductances decreased from unexpectedly large values to extremely small ones-below the detection limit of our probe-as expected from our computational results. Our results show that it is possible to avoid the confounding effects of surface contamination and systematically study thermal radiation in Ångström- and nanometre-sized gaps.

Nanoscale laser sources based on single metallic nanoparticles (spasers) have attracted significant interest for their fundamental implications and technological potential. Here we theoretically investigate the spatio-temporal dynamics of lasing action in core-shell metallic nanoparticles that include optically pumped four-level gain media. By using detailed semiclassical simulations based on a time-domain generalization of the finite-element method, we study the evolution of the lasing dynamics when going from a spherical case to an elongated nanorod configuration. Our calculations show that there exists an optimal nanoparticle elongation that exhibits significantly improved lasing threshold and slope efficiency over those obtained for its spherical counterpart. These results are accounted for in terms of a coupled-mode theory analysis of the variation with elongation of the light confinement properties of localized surface plasmons. This work could be of importance for further development of nanoscale light sources based on localized surface plasmon resonances.

We investigate the conditions yielding plasmon-exciton strong coupling at the single emitter level in the gap between two metal nanoparticles. Inspired by transformation optics ideas, a quasianalytical approach is developed that makes possible a thorough exploration of this hybrid system incorporating the full richness of its plasmonic spectrum. This allows us to reveal that by placing the emitter away from the cavity center, its coupling to multipolar dark modes of both even and odd parity increases remarkably. This way, reversible dynamics in the population of the quantum emitter takes place in feasible implementations of this archetypal nanocavity.

Radiative transfer of energy at the nanometre length scale is of great importance to a variety of technologies including heat-assisted magnetic recording, near-field thermophotovoltaics and lithography. Although experimental advances have enabled elucidation of near-field radiative heat transfer in gaps as small as 20-30 nanometres (refs 4-6), quantitative analysis in the extreme near field (less than 10 nanometres) has been greatly limited by experimental challenges. Moreover, the results of pioneering measurements differed from theoretical predictions by orders of magnitude. Here we use custom-fabricated scanning probes with embedded thermocouples, in conjunction with new microdevices capable of periodic temperature modulation, to measure radiative heat transfer down to gaps as small as two nanometres. For our experiments we deposited suitably chosen metal or dielectric layers on the scanning probes and microdevices, enabling direct study of extreme near-field radiation between silica-silica, silicon nitride-silicon nitride and gold-gold surfaces to reveal marked, gap-size-dependent enhancements of radiative heat transfer. Furthermore, our state-of-the-art calculations of radiative heat transfer, performed within the theoretical framework of fluctuational electrodynamics, are in excellent agreement with our experimental results, providing unambiguous evidence that confirms the validity of this theory for modelling radiative heat transfer in gaps as small as a few nanometres. This work lays the foundations required for the rational design of novel technologies that leverage nanoscale radiative heat transfer.

Transition metal dichalcogenides (TMDs) are layered semiconductors with indirect band gaps comparable to Si. These compounds can be grown in large area, while their gap(s) can be tuned by changing their chemical composition or by applying a gate voltage. The experimental evidence collected so far points toward a strong interaction with light, which contrasts with the small photovoltaic efficiencies η ≤ 1% extracted from bulk crystals or exfoliated monolayers. Here, we evaluate the potential of these compounds by studying the photovoltaic response of electrostatically generated PN-junctions composed of approximately 10 atomic layers of MoSe2 stacked onto the dielectric h-BN. In addition to ideal diode-like response, we find that these junctions can yield, under AM-1.5 illumination, photovoltaic efficiencies η exceeding 14%, with fill factors of ~70%. Given the available strategies for increasing η such as gap tuning, improving the quality of the electrical contacts, or the fabrication of tandem cells, our study suggests a remarkable potential for photovoltaic applications based on TMDs.

We show that a single quantum emitter can efficiently couple to the tunable plasmons of a highly doped single-wall carbon nanotube (SWCNT). Plasmons in these quasi-one-dimensional carbon structures exhibit deep subwavelength confinement that pushes the coupling efficiency close to 100% over a very broad spectral range. This phenomenon takes place for distances and tube diameters comprising the nanometer and micrometer scales. In particular, we find a β factor ≈1 for QEs placed 1-100 nm away from SWCNTs that are just a few nanometers in diameter, while the corresponding Purcell factor exceeds 10(6).

Efficient light-matter interaction lies at the heart of many emerging technologies that seek on-chip integration of solid-state photonic systems. Plasmonic waveguides, which guide the radiation in the form of strongly confined surface plasmon-polariton modes, represent a promising solution to manipulate single photons in coplanar architectures with unprecedented small footprints. Here we demonstrate coupling of the emission from a single quantum emitter to the channel plasmon polaritons supported by a V-groove plasmonic waveguide. Extensive theoretical simulations enable us to determine the position and orientation of the quantum emitter for optimum coupling. Concomitantly with these predictions, we demonstrate experimentally that 42% of a single nitrogen-vacancy centre emission efficiently couples into the supported modes of the V-groove. This work paves the way towards practical realization of efficient and long distance transfer of energy for integrated solid-state quantum systems.

The stacking orders in few-layer graphene (FLG) strongly influences the electronic properties of the material. To explore the stacking-specific properties of FLG in detail, one needs powerful microscopy techniques that visualize stacking domains with sufficient spatial resolution. We demonstrate that infrared (IR) scattering scanning near-field optical microscopy (sSNOM) directly maps out the stacking domains of FLG with a nanometric resolution, based on the stacking-specific IR conductivities of FLG. The intensity and phase contrasts of sSNOM are compared with the sSNOM contrast model, which is based on the dipolar tip-sample coupling and the theoretical conductivity spectra of FLG, allowing a clear assignment of each FLG domain as Bernal, rhombohedral, or intermediate stacks for tri-, tetra-, and pentalayer graphene. The method offers 10-100 times better spatial resolution than the far-field Raman and infrared spectroscopic methods, yet it allows far more experimental flexibility than the scanning tunneling microscopy and electron microscopy.

We present an ab initio study of the anisotropy and atomic relaxation effects on the optical properties of nanoparticle dimers. Special emphasis is placed on the hybridization process of localized surface plasmons, plasmon-mediated photoinduced currents, and electric-field enhancement in the dimer junction. We show that there is a critical range of separations between the clusters (0.1-0.5 nm) in which the detailed atomic structure in the junction and the relative orientation of the nanoparticles have to be considered to obtain quantitative predictions for realistic nanoplasmonic devices. It is worth noting that this regime is characterized by the emergence of electron tunneling as a response to the driven electromagnetic field. The orientation of the particles not only modifies the attainable electric field enhancement but can lead to qualitative changes in the optical absorption spectrum of the system.

The optical response of plasmonic nanogaps is challenging to address when the separation between the two nanoparticles forming the gap is reduced to a few nanometers or even subnanometer distances. We have compared results of the plasmon response within different levels of approximation, and identified a classical local regime, a nonlocal regime and a quantum regime of interaction. For separations of a few Ångstroms, in the quantum regime, optical tunneling can occur, strongly modifying the optics of the nanogap. We have considered a classical effective model, so called Quantum Corrected Model (QCM), that has been introduced to correctly describe the main features of optical transport in plasmonic nanogaps. The basics of this model are explained in detail, and its implementation is extended to include nonlocal effects and address practical situations involving different materials and temperatures of operation.

In this Letter we introduce a novel route for achieving negative-group-velocity waveguiding at deep-subwavelength scales. Our scheme is based on the strong electromagnetic coupling between two conformal surface plasmon structures. Using symmetry arguments and detailed numerical simulations, we show that the coupled system can be geometrically tailored to yield negative-index dispersion. A high degree of subwavelength modal confinement, of λ/10 in the transversal dimensions, is also demonstrated. These results can assist in the development of ultrathin surface circuitry for the low-frequency region (microwave and terahertz regimes) of the electromagnetic spectrum.

Here we present the theoretical foundation of the strong coupling phenomenon between quantum emitters and propagating surface plasmons observed in two-dimensional metal surfaces. For that purpose, we develop a quantum framework that accounts for the coherent coupling between emitters and surface plasmons and incorporates the presence of dissipation and dephasing. Our formalism is able to reveal the key physical mechanisms that explain the reported phenomenology and also determine the physical parameters that optimize the strong coupling. A discussion regarding the classical or quantum nature of this phenomenon is also presented.

One-dimensional light harvesting structures with a realistic geometry nano-patterned on an opaque metallic film are optimized to render high transmission efficiencies at optical and infrared frequencies. Simple design rules are developed for the particular case of a slit-groove array with a given number of grooves that are symmetrically distributed with respect to a central slit. These rules take advantage of the hybridization of Fabry-Perot modes in the slit and surface modes of the corrugated metal surface. Same design rules apply for optical and infrared frequencies. The parameter space of the groove array is also examined with a conjugate gradient optimization algorithm that used as a seed the geometries optimized following physical intuition. Both uniform and nonuniform groove arrays are considered. The largest transmission enhancement, with respect to a uniform array, is obtained for a chirped groove profile. Such relative enhancement is a function of the wavelength. It decreases from 39 % in the optical part of the spectrum to 15 % at the long wavelength infrared.

Here we investigate theoretically and numerically the coupling between surface plasmon polaritons (SPPs) in monolayer graphene sheet arrays that have a period much smaller than the wavelength. We show that when the collective SPP is excited with an out-of-phase illumination, the beam tends to propagate toward the opposite direction of the Bloch momentum, reflecting a negative coupling between the constituent SPPs. In contrast, for in-phase illumination, the incident beam is split into two collective SPPs that are highly collimated and display low propagation loss. Moreover, the coupling between the individual SPPs results in a reduction of the modal wavelength of the SPP in comparison with that of a single graphene sheet.

We develop an insightful transformation-optics approach to investigate the impact that nonlocality has on the optical properties of plasmonic nanostructures. The light-harvesting performance of a dimer of touching nanowires is studied by using the hydrodynamical Drude model, which reveals nonlocal resonances not predicted by previous local calculations. Our method clarifies the interplay between radiative and nonlocal effects in this nanoparticle configuration, which enables us to elucidate the optimum size that maximizes its absorption and field enhancement capabilities.

The propagation of surface plasmon polaritons in dielectric loaded waveguides with randomly placed scatterers is studied using both numerical simulations and a simplified transfer matrix framework. Despite the importance of losses in this system, we find fingerprints of the localized behavior of one-dimensional disordered systems. Furthermore, losses amplify the impact of the necklace states on the transport properties for systems not much larger than the localization length. The system presented here also offers the possibility to use localization effects for engineering purposes by means of deliberately introduced disorder.

Nanoscale metallic barriers embedded in terahertz (THz) slot antennas are shown to provide unprecedented control of the transition state arising at the crossover between the full- and half-wavelength resonant modes of such antennas. We demonstrate strong near-field coupling between two paired THz slot antennas separated by a 5 nm wide nanobarrier, almost fully inducing the shift to the resonance of the double-length slot antenna. This increases by a factor of 50 the length-scale needed to observe similar coupling strengths in conventional air-gap antennas (around 0.1 nm), making the transition state readily accessible to experiment. Our measurements are in good agreement with a quantitative theoretical modeling, which also provides a simple physical picture of our observations.

It is shown that submicrometer holes with very acute angles present extraordinary optical transmission peaks associated to strongly localized modes. The positions of these peaks are: (i) strongly redshifted with respect to the peak position that could be expected if the considered hole were in a film made of perfect electric conductor, (ii) independent on the angle of incidence for a large range of angles and (iii) strongly dependent on the direction of the incident electric field. In addition, it is demonstrated that these properties are linked to the mechanisms leading to the existence of channel-plasmon-polaritons.

We present an analytical expression for the electromagnetic field at the surface radiated by a hole in a metal film. This expression is valid for any metal, from the optical range to longer wavelengths, and for distances to the hole larger than a few tens of nanometers. The field pattern presents a rich behavior, showing three regions (a complex short distance, an intermediate range dominated by surface plasmon polaritons, and a long-distance one dominated by Norton waves). The crossover distances between these regimes depend strongly on both the wavelength and the angle with respect to the incident field.

We show how both the subwavelength confinement associated with surface plasmons and the one-dimensional character of plasmonic waveguides can be exploited to enhance the coupling between quantum emitters. Resonance energy transfer and the phenomenon of superradiance are investigated in three different waveguiding schemes (wires, wedges, and channels) by means of the Finite Element Method. We also develop a simplified model that is able to capture the main features of the numerical results.

A new strategy to control the flow of surface plasmon polaritons at metallic surfaces is presented. It is based on the application of the concept of transformation optics to devise the optical parameters of the dielectric medium placed on top of the metal surface. We describe the general methodology for the design of transformation optical devices for surface plasmons and analyze, for proof-of-principle purposes, three representative examples with different functionalities: a beam shifter, a cylindrical cloak, and a ground-plane cloak.

Enhanced optical transmission (EOT) through a single aperture is usually achieved by exciting surface plasmon polaritons with periodic grooves. Surface plasmon polaritons are only excited by p-polarized incident light, i.e. with the electric field perpendicular to the direction of the grooves. The present study experimentally investigates EOT for s-polarized light. A subwavelength slit surrounded on each side by periodic grooves has been fabricated in a gold film and covered by a thin dielectric layer. The excitation of s-polarized dielectric waveguide modes inside the dielectric film strongly increases the s-polarized transmission. A 25 fold increase is measured as compared to the case without the dielectric film. Transmission measurements are compared with a coupled mode method and show good qualitative agreement. Adding a waveguide can improve light transmission through subwavelength apertures, as both s and p-polarization can be efficiently transmitted.

Enhanced polarization conversion in reflection for the Otto and Kretschmann configurations is introduced as a new method for hybrid-mode spectroscopy. Polarization conversion in reflection occurs when hybrid modes are excited in a guiding structure composed of at least one anisotropic medium. In contrast to a dark dip, in this case modes are associated with a peak in the converted reflectance spectrum, increasing the detection sensitivity and avoiding confusion with reflection dips associated with other processes, such as transmission.