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The authors regret to inform that in the caption of Fig. 2 it is mistakenly indicated DEA when instead the image shows the effect of dimethylamine borane complex on copper film morphology. Although the text makes clear that the error is in the caption, we believe it may be confusing. The authors would like to apologize for any inconvenience caused. Corrected caption (Fig. 2): “SEM [scale bar: 5 μm], EDS and AFM analysis of copper layer onto zinc (a, c) −2 mA/cm2, 70 °C, dimethylamine borane complex-free solution. (b, d) −2 mA/cm2, 70 °C, dimethylamine borane complex-containing solution. (e) Graphical representation of the Zn/Cu stack.”

We perform redundant x-ray diffraction versus temperature experiments in bulk transparent KTN. We find a violation of the standard perovskite cubic-to-tetragonal symmetry breaking at the Curie point in the form of an orthorhombic cell distortion. The lattice distortion spans coherently macroscopic volumes of the sample and is characterized by a negative-to-zero thermal volume expansion. Dielectric measurements and calorimetry indicate that the anomalous behavior is not associated to a distinct thermodynamic phase. The comparison of linear and nonlinear optical scattering experiments with structural data suggests that the lattice distortion is a consequence of strain relaxation to a 3D superlattice of polarization vortices.

We propose an innovative experimental approach to estimate the two-photon absorption (TPA) spectrum of a fluorescent material. Our method develops the standard indirect fluorescence-based method for the TPA measurement by employing a line-shaped excitation beam, generating a line-shaped fluorescence emission. Such a configuration, which requires a relatively high amount of optical power, permits to have a greatly increased fluorescence signal, thus avoiding the photon counterdetection devices usually used in these measurements, and allowing to employ detectors such as charge-coupled device (CCD) cameras. The method is finally tested on a fluorescent isothiocyanate sample, whose TPA spectrum, which is measured with the proposed technique, is compared with the TPA spectra reported in the literature, confirming the validity of our experimental approach.

Lithium niobate (LN) is an extremely interesting material for the realization of optical devices and circuits, thanks to its good optical and electro-optical properties. At the state of the art, the use of LN crystals for nonlinear optical functions is limited, despite the very large d33 nonlinear coefficient exhibited by this crystal, because LN is severely affected by the so called optical damage due to the photorefractive effect [1]. When a high intensity, spatially inhomogeneous, visible light beam impinges on the LN crystal, a significant and non uniform electric field is produced in the crystal, because of the low crystal photoconductivity, and this yields (through the electro-optic effect) a non-uniform modification of the crystal refractive indices. As a consequence, the efficiency of nonlinear interactions in LN can be greatly reduced, and it becomes necessary to operate the device at high temperature (in some cases even 200C), in order to get rid of photorefractivity. In order to operate the nonlinear device at room temperature (or close to it), it is possible to use LN crystals doped with a small quantity of appropriate elements able to significantly increase crystal photoconductivity, like Mg, In, or Sc [1], but it is difficult to obtain high-quality crystals when LN is doped with such ions. Recently it was shown that by using tetravalent ions, like Hf or Zr, the dopant concentration required to significantly reduce the crystal photorefractivity is considerably lower than that required for bivalent and trivalent dopants, even if some uncertainty about the exact required concentration is still present due to the discrepancies between the values reported in the literature. The low dopant-concentration, in combination with the fact that the segregation coefficient of the Zr ion is reported to be very close to 1, should allow growing more easily large homogeneous high-optical-quality Zr:LN crystals. © 2011 IEEE.

We investigate samples of compositionally disordered potassium-based perovskite single crystals with different composition and stoichiometry. The dielectric and Raman response is inspected over the nominal cubic-to-tetragonal long-range phase transition. The comparison between results shows that the occurrence of the phase transition is controlled by the temperature evolution of polar nanoregions (PNRs). We are able to correlate PNR order, formation, percolation, and freezing to the characteristic temperatures of each macroscopic crystal. The onset of the phase transition is found to occur when PNRs undergo a percolative ordering process, in correlation to the sudden arising of a specific high-frequency Raman mode.

In this work, Cu-Zn-Sn (CZT) is co-electrodeposited onto a flexible Mo substrate exploiting an alkaline bath (pH 10). The plating solution is studied by cyclic voltammetry, highlighting the effects of potassium pyrophosphate (K4P2O7) and EDTA-Na2 on the electrochemical behavior and stability of the metallic ionic species. The optimized synthesis results in a homogeneous precursor layer, with composition Cu 44 ± 2 at. %, Zn 28 ± 1 at. %, and Sn 28 ± 2 at. %. Soft and reactive annealing are employed respectively to promote intermetallic phase formation and sulfurization of the precursor to obtain CZTS. Microstructural (XRD, Raman), morphological (SEM), and compositional (EDX, XRF) characterization is carried out on CZT and CZTS films, showing a minor presence of secondary phases. Finally, photo-assisted water splitting tests are performed considering a CZTS/CdS/Pt photoelectrode, showing a photocurrent density of 1.01 mA cm−2 at 0 V vs. RHE under 1 sun illumination. Graphical abstract

Nonlinear response in a material increases with its index of refraction as $n^4$. Commonly, $n \sim$ 1 so that diffraction, dispersion, and chromatic walk-off limit nonlinear scattering. Ferroelectric crystals with a periodic 3D polarization structure overcome some of these constraints through versatile Cherenkov and quasi-phase-matching mechanisms. Three-dimensional self-structuring can also lead to a giant optical refraction. Here, we perform second-harmonic-generation experiments in KTN:Li in conditions of giant broadband refraction. Enhanced response causes wavelength conversion to occur in the form of bulk Cherenkov radiation without diffraction and chromatic walk-off, even in the presence of strong wave-vector mismatch and highly focused beams. The process occurs with a wide spectral acceptance of more than 100 nm in the near infrared spectrum, an ultra-wide angular acceptance of up to $\pm 40^{\circ}$, with no polarization selectivity, and can be tuned to allow bulk supercontinuum generation. Results pave the way to highly efficient and adaptable nonlinear optical devices with the promise of single-photon-to-single-photon nonlinear optics., 10 pages, 5 figures

Quantum dot solar cells are based on the concept of harvesting different parts of the solar light spectrum with a single, cheap semiconductor by simply changing the size of the nanoparticles. Of the many compositions explored, germanium is one of the most interesting as it has the major advantage of a large Bohr radius, which allows for the fabrication of larger particles. Moreover, germaniums possess very high optical absorption, and a small band gap give it free parameters to optimize the quantum dot solar cell. In a previous work, the germanium quantum dots were used in a Gratzel type solar cell containing an electrolyte, which is not desirable for applications. In this work instead, the n-doped germanium quantum dots were combined with a p-doped a-Si layer, making it the first all solid-state solar cell made from nanoparticles from a gas aggregation nanoparticle source. Remarkably, the effect of quantum confinement in both the germanium quantum dot assembled layer and a-Si was observed by peaks in the spectral response experiments. This work forms an important step toward realizing a germanium quantum dot based solar cell and studying quantum dot based solids.

Germanium quantum dots are very interesting for applications such as solar cells, photodetectors, and light emitters because their small bandgap can be tuned over a wide energy range by changing the particle size. One obstacle to applications is the presence of defects, both in the interior and at the surface of the nanoparticles. The defects function as nonradiative recombination centers or trap charge carriers, which will hinder further optical performance. Introducing hydrogen, as employed in a-Si:H solar cells, has proven to be a good method to counter such detrimental defect effects. In this work, germanium quantum dots were fabricated by an ultraclean, vacuum-based nanoparticle reactor in which hydrogen was supplied during growth. Optical spectroscopy of the a-Ge:H quantum dots, together with Raman and X-ray photoelectron spectroscopy, revealed a direct bandgap and that the presence of hydrogen resulted in amorphous Ge:H quantum dots. These a-Ge:H quantum dots are a step forward toward reducing charge carrier recombination in quantum dot solar cells.

In the present study, an ethylene glycol-based electrolyte is used to electrodeposit copper onto zinc for the synthesis of the Zn/Cu/Sn stack, precursor of Cu2ZnSnS4. The employed solution contains diethanolamine (DEA) which supports the formation of amine-complexes, whose features are studied by UV–vis absorption, ESI-MS, and FTIR measurements, providing insight on the optimal concentration of DEA for copper complexation. Cyclic voltammetries (CVs) are carried out at increasing [DEA]/[Cu2+] ratios, highlighting the amine effect on the reduction potential of the copper species. The displacement reaction between copper and zinc is investigated by immersion potential measurements, showing a direct correlation to the voltammetric data. The optimized copper solution resulted in a negligible displacement contribution, allowing the electrochemical synthesis of Mo(sub)/Zn/Cu/Sn stack on a relatively large area (4 cm2). The metallic precursor is analyzed by SEM/EDS, AFM, XRD, and GDOES techniques. Finally, the kesterite CZTS phase is obtained through reactive annealing with elemental sulfur and it is characterized by SEM/EDS, XRD, and Raman spectroscopy. Photoelectrochemical water splitting on CZTS/CdS/Pt heterostructure is carried out in an aqueous solution at pH 6.85, showing a photocurrent of -5.05 mA/cm2 at 0 V vs RHE. A maximum applied bias photon-to-current efficiency (ABPE) value of 2.15% was found at 0.84 V bias.

We experimentally investigate the two-photon absorption cross sections and spectra of eosin and hematoxylin for applications in nonlinear microscopy. The experiments are carried out on pure samples of the two dyes in DI-water solvent with different concentrations, in the typical range employed in standard staining procedures. Nonlinear fluorescence is excited by a line-shaped beam emitted by a Ti:Sapphire mode-locked laser in the wavelength range from 740 to 880 nm and is detected through a microscope setup. The two-photon absorption spectral response is systematically analyzed and discussed. Finally, the staining is applied on biological tissue samples, which are imaged by two-photon microscopy. Our results show that the employed dyes are fully suitable for applications in nonlinear imaging.

Double-loop electric-field vs polarization hysteresis is investigated in a depoled compositionally disordered lithium-enriched potassium tantalate niobate crystal. Comparing electro-optic response and dielectric spectroscopy indicates that the anomalous response occurs for those temperatures in which the sample also manifests a temperature hysteresis in the low-frequency dielectric function. An electric-field hysteresis at concurrent temperatures suggests an underlying role of reorienting mesoscopic polar regions that accompany the nonergodic phase.

The variation of total energy, entropy, Helmoltz free energy due to the application of a static electric field is calculated and discussed, under suitable conditions, in the case of a dielectric with either anisotropic or nonlinear response. The proposed approach starts from Frohlich's theory of dielectric thermodynamics and, by analyzing its assumptions, provides a method to generalize it. The obtained relationships can be employed for describing the thermodynamics of different classes of dielectric materials, also in experimental investigations. Specifically, the anisotropy and nonlinearity conditions are considered and relative examples are indicated and discussed.

During their employment in space applications, InGaP/InGaAs/Ge‐based multijunction solar cells undergo strong particle bombardments that decrease their performances. As InGaP is more resistant to radiation, the whole device is usually designed in “top‐limited” configuration. Then the development of high‐efficiency and reliable devices needs standard techniques for identifying the limiting subcell before and after irradiation. We here present a specific method to determine the limiting subcell and matching current in multijunction solar cell. This approach is based on using simultaneously a solar simulator and a suitable supplemental lamp for illuminating the cell in a restricted wavelength range where the top subcell only responds. The technique is tested on beginning‐of‐life and irradiated 3‐junction InGaP/InGaAs/Ge solar cells, and its reliability is discussed.

A chloride-free solution based on ethylene glycol was shown to be suitable for the electrodeposition of copper onto zinc, allowing the fabrication of a Mo/Zn/Cu/Sn metallic precursor stack. The addition of diethanolamine (DEA) played an essential role in minimizing displacement reactions by shifting copper reduction towards a more negative potential. The electrochemical behavior of copper species with and without DEA was studied by cyclic voltammetry, and subsequently confirmed by displacement reaction assessment (OCV and ICP-OES measurements). The metallic stack was characterized by SEM and AFM, showing the effectiveness of the copper plating solution. Reactive annealing was carried out in a tubular furnace to obtain the CZTS kesterite semiconductor, as confirmed by XRD and Raman spectroscopy. Keywords: Organic solution, Ethylene glycol, Diethanolamine, Chloride-free, CZTS

The most common multi-junction solar cell arrangement employs the InGaP/InGaAs/Ge configuration, which is usually exploited for high-efficiency space applications. We here test the reliability of a triple-junction device with an innovative low-thickness and flexible configuration: this is investigation is aimed at providing its main macroscopic features which must be taken into account for their applications. Notably, the specific optical and electrical features and the performance variation of these thin solar cells are systematically analyzed, both in begin-of-life (BOL) configuration and after irradiation (end-of-life, EOL) by either electrons or protons. Measurements of I – V curves, with correlated parameters, and of spectral responses (external quantum efficiency) are accomplished on several BOL and EOL samples: this allows to describe the inhomogeneous damage of the subjunctions and to follow the evolution of the solar cell physical quantities as a function of the kind and the amount of irradiation. Finally, photoluminescence emission spectra are measured, pointing out the effect of particle bombardment on luminescent features. Our results show that these innovative solar devices allow for the combination of high specific power, mechanical flexibility, high performance, and strong resistance to particle irradiation, making them an excellent option for space applications.

We present a comprehensive overview on a new hybrid sputtering-evaporation (HSE) system for the deposition of Cu(In,Ga) Se2 (CIGS) thin-films aimed at photovoltaic applications. Such a technique employs the sputtering process to deposit the metal precursors on suitable rotating transfer cylinders, from which they are subsequently evaporated, in Se atmosphere, on the substrate. This procedure allows to combine the features of both the sputtering and evaporation techniques, enabling a fine tuning of the stoichiometry and an easy transfer to industrial processes. The key elements of this growth method are here explained in detail. The HSE CIGS layers have been investigated through secondary ion mass spectrometry, Raman and photoluminescence spectroscopies, X-ray diffraction, scanning electron microscopy, energy dispersive X-ray spectroscopy. Moreover, the solar cell performance of the grown films has been investigated, through external quantum efficiency and J-V curves under 1 Sun illumination measurements. The obtained experimental results are exhaustively shown and discussed, indicating advantages and open issues of the presented deposition technique.

Photoluminescence spectra of pure CIGS thin films with different Ga in-depth gradients are systematically investigated. Pure Na-free films are prepared with an innovative hybrid deposition technique, whose optical luminescence emission is analyzed as a function of the depth and is correlated to the radiative intrinsic defects of the material. Finally, the highlighted features are correlated with the performances of test solar cells prepared with the same growths.

We demonstrate a steplike optical modulation based on the activation and deactivation of a bistable localized structure using a photoinduced and reconfigurable miniaturized 30 × 30 μm electroactivated funnel waveguide. Control of a single 10-μm-diameter spot in a 200-μm-diameter vertical-cavity surfaceemitting laser at 980 nm is achieved modulating the phase of an exciting beam in the specific position of the spot in the cavity. This localized on-off response can be scaled into arrays and offer a possible route to fast integrated optical logical functions and memory at low intensities at near-infrared wavelengths.