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Nanoporous metals are a class of nanostructured materials finding extensive applications in multiple fields thanks to their unique properties attributed to their high surface area and interconnected nanoscale ligaments. They can be prepared following different strategies, but the deposition of an arbitrary pure porous metal is still challenging. Recently, a dry synthesis of nanoporous films based on the plasma treatment of metal thin layers deposited by physical vapour deposition has been demonstrated, as a general route to form pure nanoporous films from a large set of metals. An interesting aspect related to this approach is the possibility to apply the same methodology to deposit the porous films as a multilayer. In this way, it is possible to explore the properties of different porous metals in close contact. As demonstrated in this paper, interesting plasmonic properties emerge in a nanoporous Au–Ag bi-layer. The versatility of the method coupled with the possibility to include many different metals, provides an opportunity to tailor their optical resonances and to exploit the chemical and mechanical properties of components, which is of great interest to applications ranging from sensing, to photochemistry and photocatalysis.

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.

The replacement of plastic with eco-friendly and biodegradable materials is one of the most stringent environmental challenges. In this respect, cellulose stands out as a biodegradable polymer. However, a significant challenge is to obtain biodegradable materials for high-end photonics that are robust in humid environments. Here, we demonstrate the fabrication of high-quality micro- and nanoscale photonic and plasmonic structures viareplica molding using pure cellulose and a blended version with nonedible agro-wastes. Both materials are biodegradable in soil and seawater according to the ISO 17556 standard. The pure cellulose films are transparent in the vis–NIR spectrum, having a refractive index similar to glass. The microstructured photonic crystals show high-quality diffractive properties that are maintained under extended exposure to water. Nanostructuring the cellulose transforms it to a biodegradable metasurface manifesting bright structural colors. A subsequent deposition of Ag endowed the metasurface with plasmonic properties used to produce plasmonic colors and for surface-enhanced Raman scattering.

Metal/Insulator/Metal nanocavities (MIMs) are highly versatile systems for nanometric light confinement and waveguiding, and their optical properties are mostly interpreted in terms of surface plasmon polaritons. Although classic electromagnetic theory accurately describes their behavior, it often lacks physical insight, leaving some fundamental aspects of light interaction with these structures unexplored. In this work, we elaborate a quantum mechanical description of the MIM cavity as a double barrier quantum well. We identify the square of the imaginary part κ of the refractive index ñof the metal as the optical potential and find that MIM cavity resonances are suppressed if the ratio n/κ exceeds a certain limit, which shows that low nand high κ values are desired for strong and sharp cavity resonances. Interestingly, the spectral regions of cavity mode suppression correspond to the interband transitions of the metals, where the optical processes are intrinsically non-Hermitian. The quantum treatment allows to describe the tunnel effect for photons and reveals that the MIM cavity resonances can be excited by resonant tunneling via illumination through the metal, without the need of momentum matching techniques such as prisms or grating couplers. By combining this analysis with spectroscopic ellipsometry on experimental MIM structures and by developing a simple harmonic oscillator model of the MIM for the calculation of its effective permittivity, we show that the cavity eigenmodes coincide with low-loss zeros of the effective permittivity. Therefore, the MIM resonances correspond to epsilon-near-zero(ENZ) eigenmodes that can be excited via resonant tunneling.Our approach provides a toolbox for the engineering of ENZ resonances throughout the entire visible range, which we demonstrate experimentally and theoretically. In particular, we apply our quantum mechanical approach to asymmetric MIM superabsorbers and use it for configuring broadly tunable refractive index sensors. Our work elucidates the role of MIM cavities as photonic analogues to tunnel diodes and opens new perspectives for metamaterials with designed ENZ response.

The coupling between multiple nanocavities in close vicinity leads to the hybridization of their modes. Stacked metal-insulator-metal (MIM) nanocavities constitute a highly versatile and very interesting model system to study and engineer such mode coupling, as they can be realized by lithography-free fabrication methods with fine control on the optical and geometrical parameters. The resonant modes of such MIM cavities are epsilon-near-zero (ENZ) resonances, which are appealing for nonlinear photophysics and a variety of applications. Here, we study the hybridization of ENZ resonances in MIMIM nanocavities, obtaining a very large mode splitting reaching 0.477 eV, Q-factors of the order of 40 in the visible spectral range, and fine control on the resonance wavelength and mode linewidth by tuning the thickness of the dielectric and metallic layers. A semiclassical approach that analyzes the MIMIM structure as a double quantum well system allows to derive the exact analytical dispersion relation of the ENZ resonances, achieving perfect agreement with numerical simulations and experiments. Interestingly, the asymmetry of the mode splitting in a symmetric MIMIM cavity is not reflected in the classical model of coupled oscillators, which can be directly related to quantum mechanical tunneling for the coupling of the two cavities. Interpreting the cavity resonances as resonant tunneling modes elucidates that they can be excited without momentum matching techniques. The broad tunability of high-quality ENZ resonances together with their strong coupling efficiency makes such MIMIM cavities an ideal platform for exploring light-matter interaction, for example, by the integration of quantum emitters in dielectric layers.

Surface plasmon resonance sensors are a well-established class of sensors that includes a very large variety of materials and detection schemes. However, the development of portable devices is still challenging due to the intrinsic complexity of the optical excitation/detection schemes. This work shows that nanoporous gold (NPG) films can overcome the said limitations by providing an excellent sensitivity without the need for sophisticated fabrication approaches and/or optical setups. The sensing mechanism is related to the co-localization of optical energy and analytes in the pores fostering an enhanced light–matter coupling. As a result, when molecules are adsorbed in the pores, the NPG film shows a significant spectral shift of the effective plasma frequency and an abrupt change of the reflectivity. By monitoring the reflectivity in the spectral region close to the plasma frequency (namely the plasma edge), it is possible to detect the analyte. Through a series of experiments, the authors demonstrated a sensitivity exceeding 15 000 nm per RIU in the near infrared range comparable with the state of the art of plasmonic metamaterials.

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.

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 viapropagating 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 CsPbBr3nanoplatelets (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/m2.

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-polemetamaterial, 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 compensatedmultishell, 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.

Innovative goods authentication strategies are of fundamental importance considering the increasing counterfeiting levels. Such a task has been effectively addressed with the so-called physical unclonable functions (PUFs), being physical properties of a system that characterize it univocally. PUFs are commonly implemented by exploiting naturally occurring non-idealities in clean-room fabrication processes. The broad availability of classic paradigm PUFs, however, makes them vulnerable. Here, we propose a hybrid plasmonic/photonic multilayered structure working as a three-level strong PUF. Our approach leverages on the combination of a functional nanostructured surface, a resonant response, and a unique chromatic signature all together in one single device. The structure consists of a resonant cavity, where the top mirror is replaced with a layer of plasmonic Ag nanoislands. The naturally random spatial distribution of clusters and nanoparticles formed by this deposition technique constitutes the manufacturer-resistant nanoscale morphological fingerprint of the proposed PUF. The presence of Ag nanoislands allows us to tailor the interplay between the photonic and plasmonic modes to achieve two additional security levels. The first one is constituted by the chromatic response and broad iridescence of our structures, while the second by their rich spectral response, accessible even through a common smartphone light-emitting diode. We demonstrate that the proposed architectures could also be used as an irreversible and quantitative temperature exposure label. The proposed PUFs are inexpensive, chip-to-wafer-size scalable, and can be deposited over a variety of substrates. They also hold a great promise as an encryption framework envisioning morpho-cryptography applications.