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Due to their narrow band gap and compatibility with silicon processing, germanium-tin (Ge$_{1-x}$Sn$_x$) alloys are a versatile platform for scalable integrated mid-infrared photonics. These semiconductors are typically grown on silicon wafers using Ge as an interlayer. However, the large lattice mismatch in this heteroepitaxy protocol leads to the build-up of compressive strain in the grown layers. This compressive strain limits the material quality and its thermal stability besides expanding the band gap, thereby increasing the Sn content needed to cover a broader range in the mid-infrared. Released Ge$_{1-x}$Sn$_x$ membranes provide an effective way to mitigate these harmful effects of the epitaxial strain and control the band gap energy while enabling the hybrid integration onto different substrates. With this perspective, herein strain-relaxed Ge$_{0.89}$Sn$_{0.11}$ membranes are fabricated and subsequently transfer-printed with metal contacts to create multiple photodetectors in a single transfer step. The resulting photodetectors exhibit an extended photodetection cutoff reaching a wavelength of $3.1 \,\mu$m, coupled with a significant reduction in the dark current of two orders of magnitude as compared to as-grown photoconductive devices. The latter yields a reduced cutoff of $2.8 \,\mu$m due to the inherent compressive strain. Furthermore, the impact of chemical treatment and annealing on the device performance was also investigated showing a further reduction in the dark current. The demonstrated transfer printing, along with the use of an adhesive layer, would allow the transfer of multiple GeSn membranes onto virtually any substrate. This approach paves the way for scalable fabrication of hybrid optoelectronic devices leveraging the tunable band gap of Ge$_{1-x}$Sn$_x$ in the mid-wave infrared range.

Quantum dot light-emitting diodes (QLEDs) are promising building blocks for prospective lighting and display applications. Despite the significant advancements achieved towards increasing the efficiency and brightness levels of QLEDs, the unavoidable demand for an inert atmosphere during the fabrication process restrains their potential for large-scale manufacturing. Here, we demonstrate ZnCdSe/ZnSe/ZnSeS/ZnS core/multi-shell QDs with ultra-thick shell (14 monolayers), significantly suppressing the diffusion of moisture and oxidative species to realize efficient all solution-processed QLED devices fully fabricated under ambient air conditions. The lattice-mismatch-engineered shell growth in the synthesized QDs leads to the strong confinement of charge carriers inside the core and near-unity photoluminescence quantum yield (PLQY) in the amber-to-red wavelength region (595-625 nm). The best amber-emitting QLED devices exhibit an external quantum efficiency (EQE) of 14.8%, a current efficiency (CE) of 41.1 cd/A, and a luminance of 5.6 x 105 cd/m2 at 12 V. To the best of our knowledge, these are the highest efficiency levels achieved in air-fabricated QLEDs. Importantly, the demonstrated devices show significant suppression of non-radiative Auger recombination and optimal charge balance, leading to negligible EQE roll-off (i.e., droop-free behavior) at the maximum luminance level. Furthermore, employing a refractive-index-matched optical compound to enhance light out-coupling increases the EQE to 26.6%, which is comparable to the best devices fabricated in an inert atmosphere. Collectively, these advances will greatly facilitate the large-scale industrial fabrication of air-stable QLEDs., Comment: 22 pages, 5 figures

In recent years, the large electric field enhancement and tight spatial confinement supported by the so-called epsilon-near-zero (ENZ) mode have attracted significant attention for the realization of efficient nonlinear optical devices. Here, we experimentally demonstrate a new type of antenna, termed an ENZ photonic gap antenna (PGA), which consists of a dielectric pillar within which a thin slab of indium tin oxide (ITO) material is embedded. In ENZ PGAs, hybrid dielectric-ENZ modes emerge from strong coupling between the dielectric antenna modes and the ENZ bulk plasmon resonance. These hybrid modes efficiently couple to free space and allow for large enhancements of the incident electric field over nearly an octave bandwidth, without the stringent lateral nanofabrication requirements required by conventional plasmonic or dielectric nanoantennas. The linear response of single ENZ PGAs is probed using dark field scattering and interpreted using a simple coupled oscillator framework. Third harmonic generation is used to probe the field enhancement and large enhancements are observed in the THG efficiency over a broad spectral range. This proof of concept demonstrates the potential of ENZ PGAs, which we have previously shown can support electric field enhancements of up to 100--200X, which is comparable with those of the best plasmonic antennas.

We demonstrate that in photonic gap antennas composed of an epsilon-near-zero (ENZ) layer embedded within a high-index dielectric, hybrid modes emerge from the strong coupling between the ENZ thin film and the photonic modes of the dielectric antenna. These hybrid modes show giant electric field enhancements, large enhancements of the far-field spontaneous emission rate and a unidirectional radiation response. We analyze both parent and hybrid modes using quasinormal mode theory and find that the hybridization can be well understood using a coupled oscillator model. Under plane wave illumination, hybrid ENZ antennas can concentrate light with an electric field amplitude $\sim$100 times higher than that of the incident wave, which places them on par with the best plasmonic antennas. In addition, the far-field spontaneous emission rate of a dipole embedded at the antenna hotspot reaches up to $\sim$2300 that in free space, with nearly perfect unidirectional emission., Comment: 5 figures, 6 pages

Optical antennas made of low-loss dielectrics have several advantages over plasmonic antennas, including high radiative quantum efficiency, negligible heating and excellent photostability. However, due to weak spatial confinement, conventional dielectric antennas fail to offer light-matter interaction strengths on par with those of plasmonic antennas. We propose here an all-dielectric antenna configuration that can support strongly confined modes ($V\sim10^{-4}\lambda_{0}^3$) while maintaining unity antenna quantum efficiency. This configuration consists of a high-index pillar structure with a transverse gap that is filled with a low-index material, where the contrast of indices induces a strong enhancement of the electric field perpendicular to the gap. We provide a detailed explanation of the operation principle of such Photonic Gap Antennas (PGAs) based on the dispersion relation of symmetric and asymmetric horizontal slot-waveguides. To discuss the properties of PGAs, we consider silicon pillars with air or CYTOP as the gap-material. We show by full-wave simulations that PGAs with an emitter embedded in the gap can enhance the spontaneous emission rate by a factor of $\sim$1000 for air gaps and $\sim$400 for CYTOP gaps over a spectral bandwidth of $\Delta\lambda\approx300$ nm at $\lambda=1.25$ \textmu m. Furthermore, the PGAs can be designed to provide unidirectional out-of-plane radiation across a substantial portion of their spectral bandwidth. This is achieved by setting the position of the gap at an optimized off-centered position of the pillar so as to properly break the vertical symmetry of the structure. We also demonstrate that, when acting as receivers, PGAs can lead to a near-field intensity enhancement by a factor of $\sim$3000 for air gaps and $\sim$1200 for CYTOP gaps.

Strong optical nonlinearities play a central role in realizing quantum photonic technologies. In solid state systems, exciton-polaritons, which result from the hybridization of material excitations and cavity photons, are an attractive candidate to realize such nonlinearities. Here, the interaction between excitons forms the basis of the polaritonic nonlinearity. While the interaction between ground state excitons generates a notable optical nonlinearity, the strength of such ground state interactions is generally not sufficient to reach the regime of quantum nonlinear optics and strong single-polariton interactions. Excited states, however, feature enhanced interactions and therefore hold promise for accessing the quantum domain of single-photon nonlinearities, as demonstrated with high-lying Rydberg states of cold atomic systems. Excitons in excited states have recently been observed in monolayer transition metal dichalcogenides. Here we demonstrate the formation of exciton-polaritons using the first excited excitonic state in monolayer tungsten diselenide (WSe2) embedded in a microcavity. Owing to the larger exciton size compared to their ground state counterpart, the realized polaritons exhibit an enhanced nonlinear response by more than an order of magnitude, as evidenced through a modification of the cavity Rabi splitting. The demonstration of excited exciton-polaritons in two-dimensional semiconductors and their enhanced nonlinear response presents the first step towards the generation of strong photon interactions in solid state systems, a necessary building block for quantum photonic technologies.

The mid-infrared (MIR) spectral range is of immense use for civilian and military applications. The large number of vibrational absorption bands in this range can be used for gas sensing, process control and spectroscopy. In addition, there exists transparency windows in the atmosphere such as that between 3.6-3.8 $\mu$m, which are ideal for free-space optical communication, range finding and thermal imaging. A number of different semiconductor platforms have been used for MIR light-emission. This includes InAsSb/InAs quantum wells, InSb/AlInSb, GaInAsSbP pentanary alloys, and intersubband transitions in group III-V compounds. These approaches, however, are costly and lack the potential for integration on silicon and silicon-on-insulator platforms. In this respect, two-dimensional (2D) materials are particularly attractive due to the ease with which they can be heterointegrated. Weak interactions between neighbouring atomic layers in these materials allows for deposition on arbitrary substrates and van der Waals heterostructures enable the design of devices with targeted optoelectronic properties. In this Letter, we demonstrate a light-emitting diode (LED) based on the 2D semiconductor black phosphorus (BP). The device, which is composed of a BP/molybdenum disulfide (MoS$_2$) heterojunction emits polarized light at $\lambda$ = 3.68 $\mu$m with room-temperature internal and external quantum efficiencies (IQE and EQE) of ~1$\%$ and $\sim3\times10^{-2}\%$, respectively. The ability to tune the bandgap, and consequently emission wavelength of BP, with layer number, strain and electric field make it a particularly attractive platform for MIR emission.

Conventional surface-relief gratings are inefficient at deflecting normally-incident light by large angles. This constrains their use in many applications and limits the overall efficiency of any optical instrument integrating gratings. Here, we demonstrate a simple approach for the design of diffraction gratings that can be highly efficient for large deflection angles, while also offering additional functionality. The gratings are composed of a unit cell comprising a vertically-oriented asymmetric slot-waveguide. The unit cell shows oscillating unidirectional scattering behavior that can be precisely tuned as a function of the waveguide length. This occurs due to interference between multiple modes excited by the incident light. In contrast to metasurface-based gratings with multiple resonant sub-elements, a periodic arrangement of such non-resonant diffracting elements allows for broadband operation and a strong tolerance for variations in angle of incidence. Full-wave simulations show that our grating designs can exhibit diffraction efficiencies ranging from 94% for a deflection angle of 47$^\circ$ to 80% for deflection angle of 80$^\circ$. To demonstrate the multifunctionality of our grating design technique, we have also proposed a flat polarization beamsplitter, which allows for the separation of the two orthogonal polarizations by 80$^\circ$, with an efficiency of 80%.

We have fabricated black phosphorus photodetectors and characterized their full spectral responsivity. These devices, which are effectively in the bulk thin film limit, show broadband responsivity ranging from <400 nm to the ~3.8 $\mu$m bandgap. In the visible, an intrinsic responsivity >7 A/W can be obtained due to internal gain mechanisms. By examining the full spectral response, we identify a sharp contrast between the visible and infrared behavior. In particular, the visible responsivity shows a large photoconductive gain and gate-voltge dependence, while the infrared responsivity is nearly independent of gate voltage and incident light intensity under most conditions. This is attributed to a contribution from the surface oxide. In addition, we find that the polarization anisotropy in responsivity along armchair and zigzag directions can be as large as 103 and extends from the band edge to 500 nm. The devices were fabricated in an inert atmosphere and encapsulated by Al$_2$O$_3$ providing stable operation for more than 6 months.

Owing to their exceptional semiconducting properties, hybrid inorganic-organic perovskites show great promise as photovoltaic absorbers. In these materials, long-range diffusion of charge carriers allows for most of the photogenerated carriers to contribute to the photovoltaic efficiency. Here, time-resolved photoluminescence (PL) microscopy is used to directly probe ambipolar carrier diffusion and recombination kinetics in hybrid perovskites. This technique is applied to thin films of methylammonium lead tri-iodide MAPbI$_3$ obtained with two different fabrication routes, methylammonium lead tribromide (MAPbBr$_3$), and an alloy of formamidinium lead tri-iodide (FAPbI$_3$) and methylammonium lead bromide FA$_{0.85}$MA$_{0.15}$Pb(I$_{0.85}$Br_${0.15}$)$_3$. Average diffusion coefficients in the films leading to the highest device efficiencies and longest lifetimes, i.e., in FA$_{0.85}$MA$_{0.15}$Pb(I$_{0.85}$Br$_{0.15}$)$_3$ and acetonitrile-processed MAPbI$_3$, are found to be several orders of magnitude lower than in the other films. Further examination of the time-dependence shows strong evidence for non-diffusive transport. In particular, acetonitrile-processed MAPbI$_3$ shows distinct diffusion regimes on short and long timescales with an effective diffusion constant varying over 2 orders of magnitude. Our results also highlight the fact that increases in carrier lifetime in this class of materials are not necessarily concomitant with increased diffusion lengths and that the PL quantum efficiency under solar cell operating conditions is a greater indication of material, and ultimately device, quality.

We explore the electroluminescence efficiency for a quantum mechanical model of a large number of molecular emitters embedded in an optical microcavity. We characterize the circumstances under which a microcavity enhances harvesting of triplet excitons via reverse intersystem-crossing (R-ISC) into singlet populations that can emit light. For that end, we develop a time-local master equation in a variationally optimized frame which allows for the exploration of the population dynamics of chemically relevant species in different regimes of emitter coupling to the condensed phase vibrational bath and to the microcavity photonic mode. For a vibrational bath that equilibrates faster than R-ISC (in emitters with weak singlet-triplet mixing), our results reveal that significant improvements in efficiencies with respect to the cavity-free counterpart can be obtained for strong coupling of the singlet exciton to a photonic mode, as long as the singlet to triplet exciton transition is within the inverted Marcus regime; under these circumstances, we show the possibility to overcome the detrimental delocalization of the polariton states across a macroscopic number of molecules. On the other hand, for a vibrational bath that equilibrates slower than R-ISC (i.e., emitters with strong singlet-triplet mixing), we find that while enhancemnents in photoluminiscence can be obtained via vibrational relaxation into polaritons, this only occurs for small number of emitters coupled to the photon mode, with delocalization of the polaritons across many emitters eventually being detrimental to electroluminescence efficiency. These findings provide insight on the tunability of optoelectronic processes in molecular materials due to weak and strong light-matter coupling.

In organic microcavities, hybrid light-matter states can form with energies that differ from the bare molecular excitation energies by nearly 1 eV. A timely question, given recent advances in the development of thermally activated delayed fluorescence materials, is whether strong light-matter coupling can be used to invert the ordering of singlet and triplet states and, in addition, enhance reverse intersystem crossing (RISC) rates. Here, we demonstrate a complete inversion of the singlet lower polariton and triplet excited states. We also unambiguously measure the RISC rate in strongly-coupled organic microcavities and find that, regardless of the large energy level shifts, it is unchanged compared to films of the bare molecules. This observation is a consequence of slow RISC to the lower polariton due to the delocalized nature of the state across many molecules and an inability to compete with RISC to the dark exciton reservoir, which occurs at a rate comparable to that in bare molecules.

We demonstrate a novel grating coupler design based on double asymmetric and vertically oriented waveguide scatterers to efficiently couple normally incident light to a fundamental mode silicon waveguide laying on a buried oxide layer., Comment: 4 pages, 1 figure

Atomically thin transition metal dichalcogenides (TMDs) possess a number of properties that make them attractive for realizing room-temperature polariton devices. An ideal platform for manipulating polariton fluids within monolayer TMDs is that of Bloch surface waves, which confine the electric field to a small volume near the surface of a dielectric mirror. Here we demonstrate that monolayer tungsten disulfide ($\text{WS}_2$) can sustain Bloch surface wave polaritons (BSWPs) with a Rabi splitting of 43 meV and propagation constants reaching 33 $\mu$m. In addition, we evidence strong polariton-polariton nonlinearities within BSWPs, which manifest themselves as a reversible blueshift of the lower polariton resonance by up to 12.9$\pm$0.5 meV. Such nonlinearities are at the heart of polariton devices and have not yet been demonstrated in TMD polaritons. As a proof of concept, we use the nonlinearity to implement a nonlinear polariton source. Our results demonstrate that BSWPs using TMDs can support long-range propagation combined with strong nonlinearities, enabling potential applications in integrated optical processing and polaritonic circuits., Comment: 7 pages, 4 figures

In organic photodiodes (OPDs) light is absorbed by excitons, which dissociate to generate photocurrent. Here, we demonstrate a novel type of OPD in which light is absorbed by polaritons, hybrid light-matter states. We demonstrate polariton OPDs operating in the ultra-strong coupling regime at visible and infrared wavelengths. These devices can be engineered to show narrow responsivity with a very weak angle-dependence. More importantly, they can be tuned to operate in a spectral range outside that of the bare exciton absorption. Remarkably, we show that the responsivity of a polariton OPD can be pushed to near infrared wavelengths, where few organic absorbers are available, with external quantum efficiencies exceeding those of a control OPD.

Singlet fission is an important candidate to increase energy conversion efficiency in organic photovoltaics by providing a pathway to increase the quantum yield of excitons per photon absorbed in select materials. We investigate the dependence of exciton quantum yield for acenes in the strong light-matter interaction (polariton) regime, where the materials are embedded in optical microcavities. Starting from an open-quantum-systems approach, we build a kinetic model for time-evolution of species of interest in the presence of quenchers and show that polaritons can decrease or increase exciton quantum yields compared to the cavity-free case. In particular, we find that hexacene, a typically poor singlet-fission candidate, can feature a higher yield than cavity-free pentacene when assisted by polaritonic effects. Similarly, we show that pentacene yield can be increased when assisted by polariton states. Finally, we address how various relaxation processes between bright and dark states in lossy microcavities affect polariton photochemistry. Our results also provide insights on how to choose microcavities to enhance similarly related chemical processes., Comment: 12 pages, 4 figures

Strong inter-particle interactions between polaritons have traditionally stemmed from their exciton component. In this work, we impart a strong photonic nonlinearity to a polaritonic mode by embedding a nonlinear polymethine dye within a high-Q all-metal microcavity. We demonstrate nonlinear microcavities operating in the ultrastrong coupling regime with a normalized coupling ratio of 62\%, the highest reported to date. When pumping the lower polariton branch, we observe tunable third-harmonic generation spanning the entire visible spectrum, with internal conversion enhancements more than three orders of magnitude larger than in bare films. Transfer matrix calculations indicate that the observed enhancements are consistent with the enhanced pump electric field., Comment: 7 pages, 5 figures

Superfluidity---the suppression of scattering in a quantum fluid at velocities below a critical value---is one of the most striking manifestations of the collective behaviour typical of Bose-Einstein condensates. This phenomenon, akin to superconductivity in metals, has until now only been observed at prohibitively low cryogenic temperatures. For atoms, this limit is imposed by the small thermal de Broglie wavelength, which is inversely related to the particle mass. Even in the case of ultralight quasiparticles such as exciton-polaritons, superfluidity has only been demonstrated at liquid helium temperatures. In this case, the limit is not imposed by the mass, but instead by the small exciton binding energy of Wannier-Mott excitons, which places the upper temperature limit. Here we demonstrate a transition from normal to superfluid flow in an organic microcavity supporting stable Frenkel exciton-polaritons at room temperature. This result paves the way not only to table-top studies of quantum hydrodynamics, but also to room-temperature polariton devices that can be robustly protected from scattering., Comment: 14 pages, 5 figures, supporting information 7 pages, 9 figures

By imaging single-shot realizations of an organic polariton quantum fluid, we observe the long-sought dynamical instability of non-equilibrium condensates. Without any free parameters, we find an excellent agreement between the experimental data and a numerical simulation of the open-dissipative Gross-Pitaevskii equation, which allows us to draw several important conclusions about the physics of the system. We find that the reservoir dynamics are in the strongly nonadiabatic regime, which renders the complex Ginzburg-Landau description invalid. The observed transition from stable to unstable fluid can only be explained by taking into account the specific form of reservoir-mediated instability as well as particle currents induced by the finite extent of the pump spot., Comment: 9 pages, 8 figures

We study the use of exciton-polaritons in semiconductor microcavities to generate radiation spanning the infrared to terahertz regions of the spectrum by exploiting transitions between upper and lower polariton branches. The process, which is analogous to difference-frequency generation (DFG), relies on the use of semiconductors with a nonvanishing second-order susceptibility. For an organic microcavity composed of a nonlinear optical polymer, we predict a DFG irradiance enhancement of $2.8\cdot10^2$, as compared to a bare nonlinear polymer film, when triple resonance with the fundamental cavity mode is satisfied. In the case of an inorganic microcavity composed of (111) GaAs, an enhancement of $8.8\cdot10^3$ is found, as compared to a bare GaAs slab. Both structures show high wavelength tunability and relaxed design constraints due to the high modal overlap of polariton modes., Comment: 8 pages, 7 figures

Although only a handful of organic materials have shown polariton condensation, their study is rapidly becoming more accessible. The spontaneous appearance of long-range spatial coherence is often recognized as a defining feature of such condensates. In this work, we study the emergence of spatial coherence in an organic microcavity and demonstrate a number of unique features stemming from the peculiarities of this material set. Despite its disordered nature, we find that correlations extend over the entire spot size and we measure $g^{(1)}(r,r')$ values of nearly unity at short distances and of 50% for points separated by nearly 10 $\mu$m. We show that for large spots, strong shot to shot fluctuations emerge as varying phase gradients and defects, including the spontaneous formation of vortices. These are consistent with the presence of modulation instabilities. Furthermore, we find that measurements with flat-top spots are significantly influenced by disorder and can, in some cases, lead to the formation of mutually incoherent localized condensates., Comment: Revised version

Realizing laterally continuous ultra-thin gold films on transparent substrates is a challenge of significant technological importance. In the present work, formation of ultra-thin gold films on fused silica is studied, demonstrating how suppression of island formation and reduction of plasmonic absorption can be achieved by treating substrates with (3-mercaptopropyl) trimethoxysilane prior to deposition. Void-free fi lms with deposition thickness as low as 5.4 nm are realized and remain structurally stable at room temperature. Based on detailed structural analysis of the fi lms by specular and diffuse X-ray reflectivity measurements, it is shown that optical transmission properties of continuous ultra-thin films can be accounted for using the bulk dielectric function of gold. However, it is important to take into account the non-abrupt transition zone between the metal and the surrounding dielectrics, which extends through several lattice constants for the laterally continuous ultra-thin films (film thickness below 10 nm). This results in a significant reduction of optical transmission, as compared to the case of abrupt interfaces. These findings imply that the atomic-scale interface structure plays an important role when continuous ultra-thin films are considered, e.g., as semi-transparent electrical contacts, since optical transmission deviates significantly from the theoretical predictions for ideal films., Comment: appears in Advanced Optical Materials 2014

Two dimensional (2D) atomic crystals of graphene, and transition metal dichalcogenides have emerged as a class of materials that show strong light-matter interaction. This interaction can be further controlled by embedding such materials into optical microcavities. When the interaction is engineered to be stronger than the dissipation of light and matter entities, one approaches the strong coupling regime resulting in the formation of half-light half-matter bosonic quasiparticles called microcavity polaritons. Here we report the evidence of strong light-matter coupling and formation of microcavity polaritons in a two dimensional atomic crystal of molybdenum disulphide (MoS2) embedded inside a dielectric microcavity at room temperature. A Rabi splitting of 46 meV and highly directional emission is observed from the MoS2 microcavity owing to the coupling between the 2D excitons and the cavity photons. Realizing strong coupling effects at room temperature in a disorder free potential landscape is central to the development of practical polaritonic circuits and switches., Comment: 25 pages, 7 figures

Polariton lasing has recently been observed in strongly coupled crystalline anthracene microcavities. A simple model is developed describing the onset of the non-linear threshold based on a master equation including the relevant relaxation processes and employing realistic material parameters. The mechanism governing the build-up of the polariton population - namely bosonic stimulated scattering from the exciton reservoir via a vibronically assisted process - is characterized and its efficiency calculated on the basis of a microscopic theory. The role of polariton-polariton bimolecular quenching is identified and temperature dependent effects are discussed., Comment: 7 pages main text plus 3 appendices. 10 figures

Single surface plasmon polaritons are excited using photons generated via spontaneous parametric down-conversion. The mean excitation rates, intensity correlations and Fock state populations are studied. The observed dependence of the second order coherence in our experiment is consistent with a linear uncorrelated Markovian environment in the quantum regime. Our results provide important information about the effect of loss for assessing the potential of plasmonic waveguides for future nanophotonic circuitry in the quantum regime., Comment: 21 pages, 6 figures, published in Nano Letters, publication date (web): March 27 (2012)