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Confining near-infrared (NIR) and mid-infrared (MIR) radiation (1–10 μm) at the nanoscale is one of the main challenges in photonics. Thanks to the transparency of silicon in the NIR-MIR range, optoelectronic systems like electro-optical modulators have been broadly designed in this range. However, the trade-off between energy-per-bit consumption and speed still constitutes a significant bottleneck, preventing such a technology to express its full potentialities. Moreover, the harmless nature of NIR radiation makes it ideal for bio-photonic applications. In this work, we theoretically showcase a new kind of electro-optical modulators in the NIR-MIR range that optimize the trade-off between power consumption, switching speed, and light confinement, leveraging on the interplay between graphene and metamaterials. We investigate several configurations among which the one consisting in a SiO2/graphene hyperbolic metamaterial (HMM) outstands. The peculiar multilayered configuration of the HMM allowed one also to minimize the equivalent electrical capacitance to achieve attoJoule electro/optical modulation at about 500 MHz switching speed. This system manifests the so-called dielectric singularity, in correspondence to which an HMM lens with resolving power of λ/1660 has been designed, allowing to resolve 3 nm-wide objects placed at an interdistance of 3 nm and to overcome the diffraction limit by 3 orders of magnitude. The imaging possibilities opened by such technologies are evident especially in bio-photonic applications, where the investigation of biological entities with tailored/broadband-wavelength radiation and nanometer precision is necessary. Moreover, the modulation performances demonstrated by the graphene-based HMM configure it as a promise for ultrafast and low-power opto-electronics applications. [ABSTRACT FROM AUTHOR]

We propose here a new colloidal approach for the synthesis of both all-inorganic and hybrid organic-inorganic lead halide perovskite nanocrystals (NCs). The main limitation of the protocols that are currently in use, such as the hot injection and the ligand-assisted reprecipitation routes, is that they employ PbX2 (X = Cl, Br, or I) salts as both lead and halide precursors. This imposes restrictions on being able to precisely tune the amount of reaction species and, consequently, on being able to regulate the composition of the final NCs. In order to overcome this issue, we show here that benzoyl halides can be efficiently used as halide sources to be injected in a solution of metal cations (mainly in the form of metal carboxylates) for the synthesis of APbX[sub 3] NCs (in which A = Cs+, CH3NH3+, or CH(NH[sub 2])[sub 2]+). In this way, it is possible to independently tune the amount of both cations and halide precursors in the synthesis. The APbX3 NCs that were prepared with our protocol show excellent optical properties, such as high photoluminescence quantum yields, low amplified spontaneous emission thresholds, and enhanced stability in air. It is noteworthy that CsPbI3 NCs, which crystallize in the cubic α phase, are stable in air for weeks without any postsynthesis treatment. The improved properties of our CsPbX3 perovskite NCs can be ascribed to the formation of lead halide terminated surfaces, in which Cs cations are replaced by alkylammonium ions. [ABSTRACT FROM AUTHOR]

Polaritons can be generated by tuning the optical transitions of a light emitter to the resonances of a photonic cavity. We show that a dye-doped cavity generates resonant tunneling polaritons with Epsilon-Near-Zero (ENZ) effective permittivity. We studied the polariton spectral dispersion in dye-doped metal-dielectric-metal (MDM) cavities as a function of the in-plane ( k || ) and out-of-plane ( k ⊥ ) components of the incident wavevector. The dependence on k || was investigated through ellipsometry, revealing the ENZ modes. The k ⊥ dependence was measured by varying the cavity thickness under normal incidence using a Surface Force Apparatus (SFA). Both methods revealed a large Rabi splitting well exceeding 100 meV. The SFA-based investigation highlighted the collective nature of strong coupling by producing a splitting proportional to the square root of the involved photons. This study demonstrates the possibility of generating ENZ polaritons and introduces the SFA as a powerful tool for the characterization of strong light-matter interactions.

Colloidal nanocrystals are a promising fluorescent class of materials whose spontaneous emission features can be tuned over a broad spectral range via their composition, geometry, and size. However, toward embedding nanocrystal films in elaborated device geometries, one significant drawback is the sensitivity of their emission properties on further fabrication processes like lithography, metal or oxide deposition, etc. In this work, we demonstrate how bright-emitting and robust thin films can be obtained by combining nanocrystal deposition from solutions via spin coating with subsequent atomic layer deposition of alumina. For the resulting composite films, the layer thickness can be controlled on the nanoscale and their refractive index can be finely tuned by the amount of deposited alumina. Ellipsometry is used to measure the real and imaginary part of the dielectric permittivity, which gives direct access to the wavelength dependent refractive index and absorbance of the film. Detailed analysis of the photophysics of thin films of core-shell nanocrystals with different shapes and different shell thicknesses allows to correlate the behavior of the photoluminescence and of the decay lifetime to the changes in the nonradiative rate that are induced by the alumina deposition. We show that the photoemission properties of such composite films are stable in wavelength and intensity over several months and that the photoluminescence completely recovers from heating processes up to 240 °C. The latter is particularly interesting since it demonstrates robustness to the typical heat treatment that is needed in several process steps like resist-based lithography and deposition by thermal or electron beam evaporation of metals or oxides.

The enhancement of the photophysical response of fluorophores is a crucial factor for photonic and optoelectronic technologies that involve fluorophores as gain media. Recent advances in the development of an extreme light propagation regime, called epsilon-near-zero (ENZ), provide a promising approach in this respect. In this work, we design metal/dielectric nanocavities to be resonant with the absorption and emission bands of the employed fluorophores. Using CsPbBr 3 perovskite nanocrystal films as light emitters, we study the spontaneous emission and decay rate enhancement induced by a specifically tailored double-epsilon-near-zero (double ENZ) structure. We experimentally demonstrate the existence of two ENZ wavelengths, by directly measuring their dielectric permittivity via ellipsometric analysis. The double ENZ nature of this plasmonic nanocavity has been exploited to achieve both surface plasmon enhanced absorption (SPEA) and surface plasmon coupled emission (SPCE), inducing a significant enhancement of both the spontaneous emission and the decay rate of the perovskite nanocrystal film that is placed on top of the nanocavity. Finally, we discuss the possibility of tailoring the two ENZ wavelengths of this structure within the visible spectrum simply by finely designing the thickness of the two dielectric layers, which enables resonance matching with a broad variety of dyes. Our device design is appealing for many practical applications, ranging from sensing to low threshold amplified spontaneous emission, since we achieve a strong PL enhancement with structures that allow for straightforward fluorophore deposition on a planar surface that keeps the fluorophores exposed and accessible., Competing Interests: The authors declare no competing financial interest., (Copyright © 2018 American Chemical Society.)

We propose here a new colloidal approach for the synthesis of both all-inorganic and hybrid organic-inorganic lead halide perovskite nanocrystals (NCs). The main limitation of the protocols that are currently in use, such as the hot injection and the ligand-assisted reprecipitation routes, is that they employ PbX 2 (X = Cl, Br, or I) salts as both lead and halide precursors. This imposes restrictions on being able to precisely tune the amount of reaction species and, consequently, on being able to regulate the composition of the final NCs. In order to overcome this issue, we show here that benzoyl halides can be efficiently used as halide sources to be injected in a solution of metal cations (mainly in the form of metal carboxylates) for the synthesis of APbX 3 NCs (in which A = Cs + , CH 3 NH 3 + , or CH(NH 2 ) 2 + ). In this way, it is possible to independently tune the amount of both cations and halide precursors in the synthesis. The APbX 3 NCs that were prepared with our protocol show excellent optical properties, such as high photoluminescence quantum yields, low amplified spontaneous emission thresholds, and enhanced stability in air. It is noteworthy that CsPbI 3 NCs, which crystallize in the cubic α phase, are stable in air for weeks without any postsynthesis treatment. The improved properties of our CsPbX 3 perovskite NCs can be ascribed to the formation of lead halide terminated surfaces, in which Cs cations are replaced by alkylammonium ions.

Plasmonic quasi-periodic structures are well-known to exhibit several surprising phenomena with respect to their periodic counterparts, due to their long-range order and higher rotational symmetry. Thanks to their specific geometrical arrangement, plasmonic quasi-crystals offer unique possibilities in tailoring the coupling and propagation of surface plasmons through their lattice, a scenario in which a plethora of fascinating phenomena can take place. In this paper we investigate the extraordinary transmission phenomenon occurring in specifically patterned Thue-Morse nanocavities, demonstrating noticeable enhanced transmission, directly revealed by near-field optical experiments, performed by means of a scanning near-field optical microscope (SNOM). SNOM further provides an intuitive picture of confined plasmon modes inside the nanocavities and confirms that localization of plasmon modes is based on size and depth of nanocavities, while cross talk between close cavities via propagating plasmons holds the polarization response of patterned quasi-crystals. Our performed numerical simulations are in good agreement with the experimental results. Thus, the control on cavity size and incident polarization can be used to alter the intensity and spatial properties of confined cavity modes in such structures, which can be exploited in order to design a plasmonic device with customized optical properties and desired functionalities, to be used for several applications in quantum plasmonics.

Lead halide perovskite nanocrystals are an emerging class of materials that have gained wide interest due to their facile color tuning and high photoluminescence quantum yield. However, the lack of techniques to translate the high performance of nanocrystals into solid films restricts the successful exploitation of such materials in optoelectronics applications. Here, we report a heat-up and large-scale synthesis of quantum-confined, blue-emitting CsPbBr 3 nanoplatelets (NPLs) that self-assemble into stacked lamellar structures. Spin-coated films fabricated from these NPLs show a stable blue emission with a photoluminescence quantum yield (PLQY) of 25%. The morphology and the optoelectronic properties of such films can be dramatically modified by UV-light irradiation under ambient conditions at a high power, which transforms the self-assembled stacks of NPLs into much larger structures, such as square-shaped disks and nanobelts. The emission from the transformed thin films falls within the green spectral region with a record PLQY of 65%, and they manifest an amplified spontaneous emission with a sharp line width of 4 nm at full-width at half-maximum under femtosecond-pulsed excitation. The transformed films show stable photocurrents with a responsivity of up to 15 mA/W and response times of tens of milliseconds and are robust under treatment with different solvents. We exploit their insolubility in ethanol to fabricate green-emitting, all-solution-processed light-emitting diodes with an external quantum efficiency of 1.1% and a luminance of 590 Cd/m 2 .

We present a detailed study on the resonant gain (RG) phenomena occurring in two nanostructures, in which the presence of dielectric singularities is used to reach a huge amplification of the emitted photons resonantly interacting with the system. The presence of gain molecules in the considered nanoresonator systems makes it possible to obtain optical features that are able to unlock several applications. Two noticeable cases have been investigated: a 1D nanoresonator based on hyperbolic metamaterials and a 3D metal/dielectric spherical multishell. The former has been designed in the framework of the effective medium theory, in order to behave as an epsilon-near-zero-and-pole metamaterial, showing extraordinary light confinement and collimation. Such a peculiarity represents the key to lead to a RG behavior, a condition in which the system is demonstrated to behave as a self-amplifying perfect lens. Very high enhancement and spectral sharpness of 1 nm of the emitted light are demonstrated by means of a transfer matrix method simulation. The latter system consists of a metal/doped-dielectric multishell. A dedicated theoretical approach has been set up to finely engineer its doubly tunable resonant nature. The RG condition has been demonstrated also in this case. Finite element method-based simulations, together with an analytical model, clarify the electric field distribution inside the multishell and suggest the opportunity to use this device as a self-enhanced loss compensated multishell, being a favorable scenario for low-threshold SPASER action. Counterintuitively, exceeding the resonant gain amount of molecules in both systems causes a significant drop in the amplitude of the resonance.