Tailoring the optical properties of dilute nitride semiconductors at the nanometer scale.

We report on the innovative approaches we developed for the fabrication of site-controlled semiconductor nanostructures [e.g. quantum dots (QDs), nanowires], based on the spatially selective incorporation and/or removal of hydrogen in dilute nitride semiconductor alloys [e.g. Ga(AsN) and (InGa)(AsN)]. In such systems, the formation of stable nitrogen-hydrogen complexes removes the effects nitrogen has on the alloy properties, which in turn paves the way to the direct engineering of the material's electronic-and, thus, optical-properties: not only the bandgap energy, but also the refractive index and the polarization properties of the system can indeed be tailored with high precision and in a reversible manner. Here, lithographic approaches and/or plasmon-assisted optical irradiation-coupled to the ultra-sharp diffusion profile of hydrogen in dilute nitrides-are employed to control the hydrogen implantation and/or removal process at a nanometer scale. This results in a highly deterministic control of the spatial and spectral properties of the fabricated nanostructures, eventually obtaining semiconductor nanowires with controlled polarization properties, as well as site-controlled QDs with an extremely high control on their spatial and spectral properties. The nanostructures fabricated with these techniques, whose optical properties have also been simulated by finite-element-method calculations, are naturally suited for a deterministic coupling in optical nanocavities (i.e. photonic crystal cavities and circular Bragg resonators) and are therefore of potential interest for emerging quantum technologies.

Narrow-linewidth carbon nanotube emission in silicon hollow-core photonic crystal cavity.

Polymer-sorted semiconducting single-walled carbon nanotubes (SWNTs) provide room-temperature emission at near-infrared wavelengths, with potential for large volume production of high-quality solutions and wafer-scale deposition. These features make SWNTs a very attractive material for the realization of on-chip light sources. Coupling SWNT into optical microcavities could enhance and guide their emission, while enabling spectral selection by cavity resonance engineering. This could allow the realization of bright, narrowband sources. Here, we report the first demonstration of coupling SWNTs into the resonant modes of Si hollow-core photonic crystal cavities. We exploit the strong evanescent field in these resonators to interact with SWNT emission, coupling it into an integrated access waveguide. Based on this concept, we demonstrate narrowband SWNT emission resonantly coupled into a Si bus waveguide with a full width at half-maximum of 0.34 nm and an off-resonance rejection exceeding 5 dB.

Direct Determination of Carrier Parameters in Indium Tin Oxide Nanocrystals.

We develop here a comprehensive experimental approach to independently determine charge carrier parameters, namely, carrier density and mass, in plasmonic indium tin oxide nanocrystals. Typically, in plasmonic nanocrystals, only the ratio between these two parameters is accessible through optical absorption experiments. The multitechnique methodology proposed here combines single particle and ensemble optical and magneto-optical spectroscopies, also using 119Sn solid-state nuclear magnetic resonance spectroscopy to probe the surface depletion layer. Our methodology overcomes the limitations of standard fitting approaches based on absorption spectroscopy and ultimately gives access to carrier effective mass directly on the NCs, discarding the use of literature value based on bulk or thin film materials. We found that mass values depart appreciably from those measured on thin films; consequently, we found carrier density values that are different from reported literature values for similar systems. The effective mass was found to deviate from the parabolic approximation at a high carrier density. Finally, the dopant activation and defect diagram for ITO NCs for tin doping between 2.5 and 15% are determined. This approach can be generalized to other plasmonic heavily doped semiconductor nanostructures and represents, to the best of our knowledge, the only method to date to characterize the full Drude parameter space of 0-D nanosystems.

Temperature-Dependent Amplified Spontaneous Emission in CsPbBr3 Thin Films Deposited by Single-Step RF-Magnetron Sputtering.

Due to their high optical efficiency, low-cost fabrication and wide variety in composition and bandgap, halide perovskites are recognized nowadays as real contenders for the development of the next generation of optoelectronic devices, which, among others, often require high quality over large areas which is readily attainable by vacuum deposition. Here, we report the amplified spontaneous emission (ASE) properties of two CsPbBr3 films obtained by single-step RF-magnetron sputtering from a target containing precursors with variable compositions. Both the samples show ASE over a broad range of temperatures from 10 K up to 270 K. The ASE threshold results strongly temperature dependent, with the best performance occurring at about 50 K (down to 100 µJ/cm2), whereas at higher temperatures, there is evidence of thermally induced optical quenching. The observed temperature dependence is consistent with exciton detrapping up to about 50 K. At higher temperatures, progressive free exciton dissociation favors higher carrier mobility and increases trapping at defect states with consequent emission reduction and increased thresholds. The reported results open the way for effective large-area, high quality, organic solution-free deposited perovskite thin films for optoelectronic applications, with a remarkable capability to finely tune their physical properties.

Large-Area Nanocrystalline Caesium Lead Chloride Thin Films: A Focus on the Exciton Recombination Dynamics.

Caesium lead halide perovskites were recently demonstrated to be a relevant class of semiconductors for photonics and optoelectronics. Unlike CsPbBr3 and CsPbI3, the realization of high-quality thin films of CsPbCl3, particularly interesting for highly efficient white LEDs when coupled to converting phosphors, is still a very demanding task. In this work we report the first successful deposition of nanocrystalline CsPbCl3 thin films (70-150 nm) by radio frequency magnetron sputtering on large-area substrates. We present a detailed investigation of the optical properties by high resolution photoluminescence (PL) spectroscopy, resolved in time and space in the range 10-300 K, providing quantitative information concerning carriers and excitons recombination dynamics. The PL is characterized by a limited inhomogeneous broadening (~15 meV at 10 K) and its origin is discussed from detailed analysis with investigations at the micro-scale. The samples, obtained without any post-growth treatment, show a homogeneous PL emission in spectrum and intensity on large sample areas (several cm2). Temperature dependent and time-resolved PL spectra elucidate the role of carrier trapping in determining the PL quenching up to room temperature. Our results open the route for the realization of large-area inorganic halide perovskite films for photonic and optoelectronic devices.

First Proof-of-Principle of Inorganic Lead Halide Perovskites Deposition by Magnetron-Sputtering.

The present work reports the application of RF-magnetron sputtering technique to realize CsPbBr 3 70 nm thick films on glass substrate by means of a one-step procedure. The obtained films show highly uniform surface morphology and homogeneous thickness as evidenced by AFM and SEM investigations. XRD measurements demonstrate the presence of two phases: a dominant orthorhombic CsPbBr 3 and a subordinate CsPb 2 Br 5 . Finally, XPS data reveals surface bromine depletion respect to the stoichiometrical CsPbBr 3 composition, nevertheless photoluminescence spectroscopy results confirm the formation of a highly luminescent film. These preliminary results demonstrate that our approach could be of great relevance for easy fabrication of large area perovskite thin films. Future developments, based on this approach, may include the realization of multijunction solar cells and multicolor light emitting devices.

GaAs epilayers grown on patterned (001) silicon substrates via suspended Ge layers.

We demonstrate the growth of low density anti-phase boundaries, crack-free GaAs epilayers, by Molecular Beam Epitaxy on silicon (001) substrates. The method relies on the deposition of thick GaAs on a suspended Ge buffer realized on top of deeply patterned Si substrates by means of a three-temperature procedure for the growth. This approach allows to suppress, at the same time, both threading dislocations and thermal strain in the epilayer and to remove anti-phase boundaries even in absence of substrate tilt. Photoluminescence measurements show the good uniformity and the high optical quality of AlGaAs/GaAs quantum well structures realized on top of such GaAs layer.

Tailoring carbon nanotubes optical properties through chirality-wise silicon ring resonators.

Semiconducting single walled carbon nanotubes (s-SWNT) have an immense potential for the development of active optoelectronic functionalities in ultra-compact hybrid photonic circuits. Specifically, s-SWNT have been identified as a very promising solution to implement light sources in the silicon photonics platform. Still, two major challenges remain to fully exploit the potential of this hybrid technology: the limited interaction between s-SWNTs and Si waveguides and the low quantum efficiency of s-SWNTs emission. Silicon micro-ring resonators have the potential capability to overcome these limitations, by providing enhanced light s-SWNT interaction through resonant light recirculation. Here, we demonstrate that Si ring resonators provide SWNT chirality-wise photoluminescence resonance enhancement, releasing a new degree of freedom to tailor s-SWNT optical properties. Specifically, we show that judicious design of the micro-ring geometry allows selectively promoting the emission enhancement of either (8,6) or (8,7) SWNT chiralities present in a high-purity polymer-sorted s-SWNT solution. In addition, we present an analysis of nanometric-sized silicon-on-insulator waveguides that predicts stronger light s-SWNT interaction for transverse-magnetic (TM) modes than for conventionally used transverse-electric (TE) modes.

Generalized Fano lineshapes reveal exceptional points in photonic molecules.

The optical behavior of coupled systems, in which the breaking of parity and time-reversal symmetry occurs, is drawing increasing attention to address the physics of the exceptional point singularity, i.e., when the real and imaginary parts of the normal-mode eigenfrequencies coincide. At this stage, fascinating phenomena are predicted, including electromagnetic-induced transparency and phase transitions. To experimentally observe the exceptional points, the near-field coupling to waveguide proposed so far was proved to work only in peculiar cases. Here, we extend the interference detection scheme, which lies at the heart of the Fano lineshape, by introducing generalized Fano lineshapes as a signature of the exceptional point occurrence in resonant-scattering experiments. We investigate photonic molecules and necklace states in disordered media by means of a near-field hyperspectral mapping. Generalized Fano profiles in material science could extend the characterization of composite nanoresonators, semiconductor nanostructures, and plasmonic and metamaterial devices.

Site-Controlled Single-Photon Emitters Fabricated by Near-Field Illumination.

Many of the most advanced applications of semiconductor quantum dots (QDs) in quantum information technology require a fine control of the QDs' position and confinement potential, which cannot be achieved with conventional growth techniques. Here, a novel and versatile approach for the fabrication of site-controlled QDs is presented. Hydrogen incorporation in GaAsN results in the formation of N-2H and N-2H-H complexes, which neutralize all the effects of N on GaAs, including the N-induced large reduction of the bandgap energy. Starting from a fully hydrogenated GaAs/GaAsN:H/GaAs quantum well, the NH bonds located within the light spot generated by a scanning near-field optical microscope tip are broken, thus obtaining site-controlled GaAsN QDs surrounded by a barrier of GaAsN:H (laterally) and GaAs (above and below). By adjusting the laser power density and exposure time, the optical properties of the QDs can be finely controlled and optimized, tuning the quantum confinement energy over more than 100 meV and resulting in the observation of single-photon emission from both the exciton and biexciton recombinations. This novel fabrication technique reaches a position accuracy <100 nm and it can easily be applied to the realization of more complex nanostructures.