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Promising applications in photonics are driven by the ability to fabricate crystal-quality metal thin films of controlled thickness down to a few nanometers. In particular, these materials exhibit a highly nonlinear response to optical fields owing to the induced ultrafast electron dynamics, which is however poorly understood on such mesoscopic length scales. Here, we reveal a new mechanism that controls the nonlinear optical response of thin metallic films, dominated by ultrafast electronic heat transport when the thickness is sufficiently small. By experimentally and theoretically studying electronic transport in such materials, we explain the observed temporal evolution of photoluminescence in pump-probe measurements that we report for crystalline gold flakes. Incorporating a first-principles description of the electronic band structures, we model electronic transport and find that ultrafast thermal dynamics plays a pivotal role in determining the strength and time-dependent characteristics of the nonlinear photoluminescence signal, which is largely influenced by the distribution of hot electrons and holes, subject to diffusion across the film as well as relaxation to lattice modes. Our findings introduce conceptually novel elements triggering the nonlinear optical response of nanoscale materials while suggesting additional ways to control and leverage hot carrier distributions in metallic films., Comment: 20 pages, 6 figures, 64 references

Immense field enhancement and nanoscale confinement of light are possible within nanoparticle-on-mirror (NPoM) plasmonic resonators, which enable novel optically-activated physical and chemical phenomena, and render these nanocavities greatly sensitive to minute structural changes, down to the atomic scale. Although a few of these structural parameters, primarily linked to the nanoparticle and the mirror morphology, have been identified, the impact of molecular assembly and organization of the spacer layer between them has often been left uncharacterized. Here, we experimentally investigate how the complex and reconfigurable nature of a thiol-based self-assembled monolayer (SAM) adsorbed on the mirror surface impacts the optical properties of the NPoMs. We fabricate NPoMs with distinct molecular organizations by controlling the incubation time of the mirror in the thiol solution. Afterwards, we investigate the structural changes that occur under laser irradiation by tracking the bonding dipole plasmon mode, while also monitoring Stokes and anti-Stokes Raman scattering from the molecules as a probe of their integrity. First, we find an effective decrease in the SAM height as the laser power increases, compatible with an irreversible change of molecule orientation caused by heating. Second, we observe that the nanocavities prepared with a densely packed and more ordered monolayer of molecules are more prone to changes in their resonance compared to samples with sparser and more disordered SAMs. Our measurements indicate that molecular orientation and packing on the mirror surface play a key role in determining the stability of NPoM structures and hence highlight the under-recognized significance of SAM characterization in the development of NPoM-based applications.

The accurate determination of electronic temperatures in metallic nanostructures is essential for many technological applications, like plasmon-enhanced catalysis or lithographic nanofabrication procedures. In this Letter, we demonstrate that the electronic temperature can be accurately measured by the shape of the tunnel electroluminescence emission edge in tunnel plasmonic nanocavities, which follows a universal thermal distribution with the bias voltage as the chemical potential of the photon population. A significant deviation between electronic and lattice temperatures is found below 30 K for tunnel currents larger than 15 nA. This deviation is rationalized as the result of a two-electron process in which the second electron excites plasmon modes with an energy distribution that reflects the higher temperature following the first tunneling event. These results dispel a long-standing controversy on the nature of overbias emission in tunnel junctions and adds a new method for the determination of electronic temperatures and quasiparticle dynamics., R.M. and R.O. acknowledge financial support from the Spanish Ministry for Economy and Competitiveness (Grants PGC2018-098613-B-C21, PGC2018-096047-B-I00), the regional government of Comunidad de Madrid (Grant S2018/NMT-4321), Universidad Autónoma de Madrid (UAM/48) and IMDEA Nanoscience. Both IMDEA Nanoscience and IFIMAC acknowledge support from the Severo Ochoa and Maria de Maeztu Programmes for Centres and Units of Excellence in R&D (MINECO, Grants SEV-2016-0686 and CEX2018-000805-M). R.O. acknowledges support from the excellence programme Echegaray, funded by the regional government of Madrid. A.A. and V.M.S. acknowledge support from the Spanish Ministry of Science and Innovation (Grants Nos. PID2019-103910GB-I00 and PID2019-105488GB-I00, respectively) and from the Projects of the Basque Government for consolidated groups of the Basque University, through the Department of Universities (Grant Nos. IT-1246-19 and IT-1164-19, respectively).

An effective approach to improve the detection efficiency of nanoscale light sources relies on a planar antenna configuration, which beams the emitted light into a narrow cone. Planar antennas operate like optical Yagi-Uda antennas, where reflector and director elements are made of metal films. Here we introduce and investigate, both theoretically and experimentally, a scanning implementation of a planar antenna. Using a small ensemble of molecules contained in fluorescent nanobeads placed in the antenna, we independently address the intensity, radiation pattern, and decay rate as a function of distance between a flat-tip scanning gold wire (reflector) and a thin gold film coated on a glass coverslip (director). The scanning planar antenna changes the radiation pattern of a single fluorescent bead, and it beams light into a narrow cone down to angles of 45 ∘ (full width at half maximum). Moreover, the collected signal compared to the case of a glass coverslip is larger than a factor of three, which is mainly due to the excitation enhancement. These results offer a better understanding of the modification of light–matter interaction by planar antennas, and they hold promise for applications such as sensing, imaging, and diagnostics.

Fluoride-based compounds doped with rare-earth cations are the preferred choice of materials to achieve efficient upconversion, of interest for a plethora of applications ranging from bioimaging to energy harvesting. Herein, we demonstrate a simple route to fabricate bright upconverting films that are transparent, self-standing, flexible, and emit different colors. Starting from the solvothermal synthesis of uniform and colloidally stable yttrium fluoride nanoparticles doped with Yb3+ and Er3+, Ho3+, or Tm3+, we find the experimental conditions to process the nanophosphors as optical quality films of controlled thickness between few hundreds of nanometers and several micrometers. A thorough analysis of both structural and photophysical properties of films annealed at different temperatures reveals a tradeoff between the oxidation of the matrix, which transitions through an oxyfluoride crystal phase, and the efficiency of the upconversion photoluminescence process. It represents a significant step forward in the understanding of the fundamental properties of upconverting materials and can be leveraged for the optimization of upconversion systems in general. We prove bright multicolor upconversion photoluminescence in oxyfluoride-based phosphor transparent films upon excitation with a 980 nm laser for both rigid and flexible versions of the layers, being possible to use the latter to coat surfaces of arbitrary shape. Our results pave the way toward the development of upconverting coatings that can be conveniently integrated in applications that demand a large degree of versatility.

GeSn alloys have been regarded as a potential lasing material for a complementary metal-oxide-semiconductor (CMOS)-compatible light source. Despite their remarkable progress, all GeSn lasers reported to date have large device footprints and active areas, which prevent the realization of densely integrated on-chip lasers operating at low power consumption. Here, we present a 1D photonic crystal (PC) nanobeam with a very small device footprint of 7 ${\mu}m^2$ and a compact active area of ~1.2 ${\mu}m^2$ on a high-quality GeSn-on-insulator (GeSnOI) substrate. We also report that the improved directness in our strain-free nanobeam lasers leads to a lower threshold density and a higher operating temperature compared to the compressive strained counterparts. The threshold density of the strain-free nanobeam laser is ~18.2 kW cm$^{ -2}$ at 4 K, which is significantly lower than that of the unreleased nanobeam laser (~38.4 kW cm$^{ -2}$ at 4 K). Lasing in the strain-free nanobeam device persists up to 90 K, whereas the unreleased nanobeam shows a quenching of the lasing at a temperature of 70 K. Our demonstration offers a new avenue towards developing practical group-IV light sources with high-density integration and low power consumption., Comment: 14 pages, 6 figures

The ever-stronger attention paid to enhancing safety in the workplace has led to novel sensor development and improvement. Despite the technological progress, nanostructured sensors are not being commercially transferred due to expensive and non-microelectronic compatible materials and processing approaches. In this paper, the realization of a cost-effective sensor based on ultrathin silicon nanowires (Si NWs) for the detection of nitrogen dioxide (NO2) is reported. A modification of the metal-assisted chemical etching method allows light-emitting silicon nanowires to be obtained through a fast, low-cost, and industrially compatible approach. NO2 is a well-known dangerous gas that, even with a small concentration of 3 ppm, represents a serious hazard for human health. We exploit the particular optical and electrical properties of these Si NWs to reveal low NO2 concentrations through their photoluminescence (PL) and resistance variations reaching 2 ppm of NO2. Indeed, these Si NWs offer a fast response and reversibility with both electrical and optical transductions. Despite the macro contacts affecting the electrical transduction, the sensing performances are of high interest for further developments. These promising performances coupled with the scalable Si NW synthesis could unfold opportunities for smaller sized and better performing sensors reaching the market for environmental monitoring.

International audience; 2-Dimensional metal Halide Perovskites (2D-HP) are at the limelight for their potential exploitation in light-emission related applications. In particular, the most-investigated

Luminescent multifunctional nanomaterials are important because of their potential impact on the development of key technologies such as smart luminescent sensors and solid-state lightings. To be technologically viable, the luminescent material needs to fulfil a number of requirements such as facile and cost-effective fabrication, a high quantum yield, structural robustness, and long-term material stability. To achieve these requirements, an eco-friendly and scalable synthesis of a highly photoluminescent, multistimuli responsive and electroluminescent silver-based metal-organic framework (Ag-MOF), termed "OX-2" was developed. Its exceptional photophysical and mechanically resilient properties that can be reversibly switched by temperature and pressure make this material stood out over other competing luminescent materials. The potential use of OX-2 MOF as a good electroluminescent material was tested by constructing a proof-of-concept MOF-LED (light emitting diode) device, further contributing to the rare examples of electroluminescent MOFs. The results reveal the huge potential for exploiting the Ag MOF as a multitasking platform to engineer innovative photonic technologies., 33 pages, 7 figures, Supplementary Information

Theoretical simulations are necessary to scientifically progress, envisage and gain the first hand knowledge of the properties of semiconductor quantum dot (QD) structure. The impact of dual ternary-quaternary/quaternary-ternary capping layers on the square based truncated pyramidal InAs QD and their influence on the energy band structure as well as the strain profile has been investigated in this study. A comparative analysis has been demonstrated with binary, ternary and quaternary capping layer counterparts. The capping layers are: GaAs (binary), InGaAs/GaAs (ternary), InAlGaAs/GaAs (quaternary), InGaAs/InAlGaAs/GaAs (dual ternary-quaternary) and InAlGaAs/InGaAs/GaAs (dual quaternary-ternary). The hydrostatic and biaxial strain for all the heterostructures have also been computed and compared. The biaxial strain was highest for the QD capped with InAlGaAs/GaAs and InAlGaAs/InGaAs/GaAs, leading to the red shift of the ground state emission in the photoluminescence (PL) spectrum. The possible absorption peaks were also calculated for all QDs from the electron (EL) and hole (HL) eigenstates. The lowest energy transition (EL1-HL1) at 300 K is near to the communication wavelength for the optimum (InAlGaAs/InGaAs/GaAs capped) QD, which is at 1.35 µm. The optimized QD heterostructure claimed the highest electrostatic potential of 0.4986 V. This study will be helpful in predicting few optical and electrical characteristics based on the strain distribution inside the structure. The optimized QD structure having a consistent strain profile inside it would render superior luminescence characteristics. Finally, to verify the accuracy of the simulation, the simulated transition peaks at 19 K and 300 K were validated with the experimental PL data, and the percentage error was within 5%.

Metal halide perovskites are generating enormous excitement for use in solar cells and light-emission applications, but devices still show substantial non-radiative losses. Here, we show that by combining light and atmospheric treatments, we can increase the internal luminescence quantum efficiencies of polycrystalline perovskite films from 1% to 89%, with carrier lifetimes of 32 μs and diffusion lengths of 77 μm, comparable with perovskite single crystals. Remarkably, the surface recombination velocity of holes in the treated films is 0.4 cm/s, approaching the values for fully passivated crystalline silicon, which has the lowest values for any semiconductor to date. The enhancements translate to solar cell power-conversion efficiencies of 19.2%, with a near-instant rise to stabilized power output, consistent with suppression of ion migration. We propose a mechanism in which light creates superoxide species from oxygen that remove shallow surface states. The work reveals an industrially scalable post-treatment capable of producing state-of-the-art semiconducting films. Metal halide perovskites are exciting materials for low-cost optoelectronic devices such as solar cells and LEDs. In order to reach the theoretical efficiency limits for both applications, any parasitic non-radiative charge-carrier recombination losses, such as those mediated by carrier trapping, must be eliminated. At present, perovskite materials still suffer from substantial non-radiative decay, particularly under solar illumination conditions, and are therefore yet to reach their full potential. Perovskite single crystals have very low trap concentrations but their controlled growth into devices does not lend themselves to the advantages offered by solution-processing thin films such as roll-to-roll depositions. Here, we demonstrate the use of light and atmospheric treatments on polycrystalline perovskite films, resulting in minimal non-radiative losses and properties approaching those of perovskite single crystals and even the best crystalline semiconductors reported to date. The authors demonstrate the use of light and atmospheric treatments on polycrystalline perovskite thin films, resulting in properties approaching those of the best crystalline semiconductors reported to date. The results translate to exceptional photovoltaic device performances with rapid rises to stabilized power output consistent with an inhibition of ionic migration.

The effect of the capping layer and the number of strain-coupled stacks on the optoelectrical properties of In0.5Ga0.5As quantum dot infrared photodetectors (QDIPs) are reported in this paper. GaAs-capped and InGaAs-capped bilayer, trilayer, pentalayer, and heptalayer QDIPs were grown for the first time and analyzed. The ground-state photoluminescence emission of all coupled QDIPs redshifted relative to that of the uncoupled QDIPs. All coupled InGaAs-capped QDIPs exhibited monomodal spectral response, whereas among GaAs-capped QDIPs, only the bilayer QDIP exhibited monomodal response. The optimal activation energy (339.87 meV) and full width at half maximum (FWHM; 16 meV) as well as the lowest dark current density (6.5E−8 A/cm2) at 100 K, and −1 V bias were observed for the InGaAs-capped trilayer QDIP among all due to better dot confinement, homogeneity, and also better strain coupling between the vertically stacks QD layers. The peak spectral response at 7.08 µm obtained from this QDIP had an ultranarrow FWHM of 8.67 meV, making it useful for hyperspectral applications in the infrared region.

The identification of a complete three-dimensional (3D) photonic band gap in real crystals always employs theoretical or numerical models that invoke idealized crystal structures. Thus, this approach is prone to false positives (gap wrongly assigned) or false negatives (gap missed). Therefore, we propose a purely experimental probe of the 3D photonic band gap that pertains to many different classes of photonic materials. We study position and polarization-resolved reflectivity spectra of 3D inverse woodpile structures that consist of two perpendicular nanopore arrays etched in silicon. We observe intense reflectivity peaks $(R > 90\%)$ typical of high-quality crystals with broad stopbands. We track the stopband width versus pore radius, which agrees much better with the predicted 3D photonic band gap than with a directional stop gap on account of the large numerical aperture used. A parametric plot of s-polarized versus p-polarized stopband width agrees very well with the 3D band gap and is model-free. This practical probe provides fast feedback on the advanced nanofabrication needed for 3D photonic crystals and stimulates practical applications of band gaps in 3D silicon nanophotonics and photonic integrated circuits, photovoltaics, cavity QED, and quantum information processing., 11 pages, 12 figures

From Marge Simpson’s family quilt to my Northern Irish paternal grandmother’s patchworks; from 19th century US homesteaders to rural Ulster farmers; from traditional salvage frugality to the new eco-sustainability; from poly-cotton duvets washable at 40° to ‘smart’ and intelligent textile technology...my paper examines the emotionally-rich content captured in the fabrication, materiality and design of textile quilts, and indicate how their combinations of cerebral and ‘felt’ substance and affect provides a template for emotionally meaningful textile design within a ‘craft futures’ scenario. Functional, utilitarian and decorative, quilts mark the commonplace rituals and universal emotions of bed, and the momentous and miniscule events and significations of life. Those quilts are embedded with human experience, an interface where a human subject performatively meets and merges with a designed object. Conventionally, the future for textile design is described as hi-tech / ‘smart’ (wearable computers, bio-mimetic fibres, electronic and digital fabrics, geo-textiles, engineering textile composites...) and ‘eco’ (sustainable, biodegradable, recyclable processes and products). Where does emotional design fit in? My paper advocates a fresh examination of the very particular traditions, characteristics, processes and outcomes of hand-crafted, fabric-salvaged, highly-functional, labour-intensive, emotionally-invested, collectively-stitched, pre-industrial, domestic quilts both in the US and in my family. I will indicate how those aesthetics and materialities might allow a redefinition of ‘textile design futures’. I will disclose one practical aspect of my vision of how technological textile innovations and advances might allow emotionally-rich, quality-measurable, poetically-valuable designed future living.

Despite being widely used in reporter technologies, bioluminescent systems are largely understudied. Of at least forty different bioluminescent systems thought to exist in nature, molecular components of only seven light-emitting reactions are known, and the full biochemical pathway leading to light emission is only understood for two of them. Here, we provide a succinct overview of currently known bioluminescent systems highlighting available tools for research and discussing future applications.

Four new 1,8-naphthalimide based compounds, 4-(1,3-dioxo-1H,3H-benzo[de]isoquinolin-2-ylmethyl)-benzoic acid (LH), 4(1,3-dioxo-1H,3H-benzo [de]isoquinolin-2-ylmethyp-benzoic acid methyl ester (LMe), 4-(1,3-dioxo-1H,3H-benzo[de]isoquinolin-2-ylmethyl)-benzoyl chloride (LCl), and 4-(1,3-dioxo-1H,3H-benzo [de]isoquinolin-2-ylmethyl)benzoic acid hydrazide (LN) are synthesized and characterized using spectral data and X-ray crystallography. They form nanoaggregates in aqueous-DMF solution and exhibited aggregation enhanced emission. The nano aggregates are characterized using their scanning electron and atomic force microscopy images. The emission intensity follows the order as LH > LMe > LCl > LN. Their photophysical properties are recorded both in solution and in the solid-state and are correlated with the nature of benzoic acid derivatives owing to the combinatorial effect of pi-pi stacking and intermolecular and intramolecular interactions. The density functional theory calculations empower the understanding of their molecular and cumulative electronic behaviors. Antiparallel dimeric interactions in the solid-state extend a herringbone arrangement to LH and 2D channel and stair-like arrangement for LCl and LN, respectively.

Precise knowledge of the local density of optical states (LDOS) is fundamental to understanding nanophotonic systems and devices. Complete LDOS mapping requires resolution in energy, momentum, and space, and hence a versatile measurement approach capable of providing simultaneous access to the LDOS components is highly desirable. Here, we explore a modality of cathodoluminescence spectroscopy able to resolve, in single acquisitions, the dispersion in energy and momentum of the radiative LDOS. We perform measurements on a titanium nitride diffraction grating, bulk molybdenum disulfide, and silicon to demonstrate that the technique can probe and disentangle the dispersion of coherent and incoherent cathodoluminescence signals. The approach presented raises cathodoluminescence spectroscopy to a versatile tool for subwavelength design and optimization of nanophotonic devices in the reciprocal space.

In this work a novel process allowing for the production of nanoporous Ge thin films is presented. This process uses the combination of two techniques: Ge sputtering on SiO2 and dopant ion implantation. The process entails four successive steps: (i) Ge sputtering on SiO2, (ii) implantation preannealing, (iii) high-dose dopant implantation, and (iv) implantation postannealing. Scanning electron microscopy and transmission electron microscopy were used to characterize the morphology of the Ge film at different process steps under different postannealing conditions. For the same postannealing conditions, the Ge film topology was shown to be similar for different implantation doses and different dopants. However, the film topology can be controlled by adjusting the postannealing conditions.

Electromechanical coupling through piezoelectric polymer chains allows the emission of organic molecules in active nanowires to be tuned. This effect is evidenced by highly bendable arrays of counter-ion dye-doped nanowires made of a poly(vinylidenefluoride) copolymer. A reversible redshift of the dye emission is found upon the application of dynamic stress during highly accurate bending experiments. By density functional theory calculations it is found that these photophysical properties are associated with mechanical stresses applied to electrostatically interacting molecular systems, namely to counterion-mediated states that involve light-emitting molecules as well as charged regions of piezoelectric polymer chains. These systems are an electrostatic class of supramolecular functional stress-sensitive units, which might impart new functionalities in hybrid molecular nanosystems and anisotropic nanostructures for sensing devices and soft robotics., Comment: 32 pages, 18 figures

Silicon-nanocrystals (Si-NCs) realized by SiOx8 MV/cm; independent of temperature), while for lower electric fields (5-8 MV/cm) at higher temperatures, the trap-related Generalized Poole-Frenkel (GPF) is dominant. This signified the role of traps in modifying the conduction in bulk ICPCVD SiO2 films. We then present the conduction in ML samples. For multilayer samples with SiO2 sublayer thickness of 1.5 nm and 2.5 nm, Direct Tunneling (DT) is observed to be dominant, while for SiO2 sublayer thickness of 3.5 nm, Space Charge Limited Conduction (SCLC) with exponential trap distribution is found to be the dominant conduction mechanism. This signifies the role of traps in modifying the conduction in Si-NC multilayer samples and SiO2 sublayer thickness dependence. (C) 2016 Elsevier B.V. All rights reserved.

Strong and directionally specific forward scattering from optical nanoantennas is of utmost importance for various applications in the broader context of photovoltaics and integrated light sources. Here, we outline a simple yet powerful design principle to perceive a nanoantenna that provides directional scattering into a higher index substrate based on the interference of multiple electric dipoles. A structural implementation of the electric dipole distribution is possible using plasmonic nanoparticles with a fairly simple geometry, i.e. two coupled rectangular nanoparticles, forming a dimer, on top of a substrate. The key to achieve directionality is to choose a sufficiently large size for the nanoparticles. This promotes the excitation of vertical electric dipole moments due to the bi-anisotropy of the nanoantenna. In turn, asymmetric scattering is obtained by ensuring the appropriate phase relation between the vertical electric dipole moments. The scattering strength and angular spread for an optimized nanoantenna can be shown to be broadband and robust against changes in the incidence angle. The scattering directionality is maintained even for an array configuration of the dimer. It only requires the preferred scattering direction of the isolated nanoantenna not to be prohibited by interference. (C) 2016 Optical Society of America

Many proteins require a non-covalently bound ligand to be functional. How ligand binding affects protein conformation is often unknown. Here we address thermal unfolding of the free and ligand-bound forms of photoprotein obelin. Fluorescence and far-UV circular dichroism (CD) data show that the various ligand-dependent conformational states of obelin differ significantly in stability against thermal unfolding. Binding of coelenterazine and calcium considerably stabilizes obelin. In solution, all obelin structures are similar, except for apo-obelin without calcium. This latter protein is an ensemble of conformational states, the populations of which alter upon increasing temperature.

We report on an experimental study with UV and visible ultrafast time-gated emission and transient absorption of the early photodynamics of horse heart Cytochrome c in both ferric and ferrous redox states. A clear separation in time and energy of tryptophan and haem emission is observed. Excitation of the haem via resonant energy transfer from the tryptophan residue is observed in the subsequent haem electronic relaxation. Different Trp-haem energy transfer time constants of the ferrous and ferric forms are obtained. An almost instantaneous relaxation to the lowest singlet excited state (corresponding to the so-called Q band) characterizes the earliest electronic dynamics of the haem, independent of excitation energy, while dark intermediate states govern the ground-state recovery. The information gathered in these two experiments and in the literature allows us to propose a simple scheme for the electronic relaxation leading to ligand dissociation.

Herein, we report the synthesis, separation and characterisation of the E- and Z-isomers of dipyrrolyldiphenylethene to study their emission behaviour in the aggregation state and solid state. The E-isomer showed pronounced aggregation induced emission (AIE) whereas the Z-isomer showed crystallization induced emission (CIE). The present study explains that the emission behaviour (AIE/CIE) is dependent on the inter/intra molecular interactions between the molecules. The study also confirms that restriction of intramolecular rotation (RIR) is the main cause of AIE/CIE in olefinic luminogens Tetraphenylethylene (TPE) type systems rather than E/Z isomerisation.

Transparent monoliths and films of urea cross-linked tripodal siloxane-based hybrids (named tri-ureasils) were prepared by the sol-gel process, under controlled atmosphere (inside a glove box) and ambient conditions and their structure and optical features were compared. X-ray diffraction data point out that all the materials are essentially amorphous and Si-29 NMR reveal an increase in the condensation degree (0.97) for the hybrids prepared under controlled atmosphere relatively to that found for those prepared under ambient conditions (0.84-0.91). The tri-ureasils are white light emitters under UV/Visible excitation (from 250 to 453 nm) being observed for the composites prepared inside the glove box a significant enhancement (60-80 %) of the absorption coefficient and higher emission quantum yield values (similar to 0.27 and similar to 0.20 for monoliths and films, respectively) relatively to those synthesized under ambient condition.

This work reports the synthesis of novel sol-gel derived urea cross-linked tripodal siloxane-based hybrids (classed as tri-ureasils) modified by the addition of phenyltriethoxysilane (PTES) and diphenyldimethoxysilane (DPDMS). The materials were produced as transparent monoliths and thin films (thickness = 3.3-17.5 +/- A 0.1 mu m) and characterized by X-ray diffraction, mid-infrared spectroscopy, Si-29 and C-13 nuclear magnetic resonance, thermogravimetric analysis, ultraviolet/visible (UV/Vis) absorption and photoluminescence spectroscopies. The role played by PTES and DPDMS as light harvesting chromophores has been discussed and quantified through emission quantum yield and UV/Vis absorption measurements. All the hybrids show efficient emission at room temperature in the blue spectral region with maximum emission quantum yield values ranging from 0.01 +/- A 0.001 to 0.10 +/- A 0.01. The highest values were found for the tri-ureasils incorporating PTES and DPDMS essentially due to an increase in the absorption coefficient (from 1.4 x 10(3) cm(-1), for the pristine tri-ureasil, to 8.6 x 10(3) cm(-1), for the hybrids modified by the chromophores). The existence of energy transfer between the DPDMS and PTES excited states and the hybrid host intrinsic emitting levels (NH/C=O- and siliceous-related levels) has been discussed.

The observation of stimulated Raman scattering in amorphous silicon nanoparticles embedded in Si-rich nitride/silicon superlattice structures (SRN/Si-SLs) is reported. Using a 1427 nm continuous-wavelength pump laser, an amplification of Stokes signal up to 0.9 dB/cm at 1540.6 nm and a significant reduction in threshold power of about 40% with respect to silicon are experimentally demonstrated. Our results indicate that amorphous silicon nanoparticles are a great promise for Si-based Raman lasers.

The optical properties of InAs/GaAs quantum dots capped with a GaAsSb quantum well are investigated by means of power-dependent and time-resolved photoluminescence. The structure exhibits the coexistence of a type-I ground state and few type-II excited states, the latter characterized by a simultaneous carrier density shift of the peak position and wavelength-dependent carrier lifetimes. Complex emission dynamics are observed under a high-power excitation regime, with the different states undergoing shifts during specific phases of the measurement. These features are satisfactorily explained in terms of band structure and energy level modifications induced by two competitive carrier interactions inside the structure. (C) 2012 American Institute of Physics. (http://dx.doi.org/10.1063/1.4769431)

Germanium nanocrystals embedded in a siliconoxide matrix has been fabricated by single femtosecond laser pulse irradiation of germanium doped SiO2 thin films deposited with plasma enhanced chemical vapor deposition. SEM and AFM are used to analyze surface modification induced by laser irradiation. Crystallization of Ge in the oxide matrix is monitored with the optic phonon at 300 cm(-1) as a function of laser fluence. Both the position the linewidth of the phonon provides clear signature for crystallization of Ge. In PL experiments, strong luminescence around 600 nm has been observed. (C) 2012 American Vacuum Society. [DOI: 10.1116/1.3677829]

We devise new optical antennas that reduce the excited-state radiative lifetimes of emitters to the order of 100 femtoseconds while maintaining quantum efficiencies of about 80% at a broadband operation. Here, we combine metallic nanoparticles with planar dielectric structures and exploit design strategies from plasmonic nanoantennas and concepts from Cavity Quantum Electrodynamics to maximize the local density of states and minimize the nonradiative losses incurred by the metallic constituents. The proposed metallo-dielectric hybrid antennas promise important impact on various fundamental and applied research fields, including photophysics, ultrafast plasmonics, bright single photon sources and Raman spectroscopy.

Optical transitions in silicon nanocrystals with different surface passivations were probed at low temperatures on a single-particle level. A type of quasidirect recombination process, different from the quantum-confined exciton transition, is identified. The luminescence spectra have different emission energies, but the contribution of a no-phonon transition is significantly higher than expected from the quantum-confinement model. Its relative strength was found to be temperature dependent, suggesting spatial localization of excitons as a possible origin. QC 20111103

We report on some surprising optical properties of diluted nitride InGaAs(1-epsilon)N(epsilon)/GaAs (epsilon << 1) pyramidal site-controlled quantum dots, grown by metalorganic vapor phase epitaxy on patterned GaAs (111)B substrates. Microphotoluminescence characterizations showed antibinding exciton/biexciton behavior, a spread of exciton lifetimes in an otherwise very uniform sample, with unexpected long neutral exciton lifetimes (up to 7 ns) and a nearly zero fine structure splitting on a majority of dots. (C) 2010 American Institute of Physics. (doi:10.1063/1.3481675)

The air fluorescence detector of the Pierre Auger Observatory is designed to perforin calorimetric measurements of extensive air showers created by Cosmic rays of above 10(18) eV. To correct these measurements for the effects introduced by atmospheric fluctuations, the Observatory contains a group Of monitoring instruments to record atmospheric conditions across the detector site, ail area exceeding 3000 km(2). The atmospheric data are used extensively in the reconstruction of air showers, and are particularly important for the correct determination of shower energies and the depths of shower maxima. This paper contains a summary of the molecular and aerosol conditions measured at the Pierre Auger Observatory since the start of regular operations in 2004, and includes a discussion of the impact of these measurements oil air shower reconstructions. Between 10(18) and 10(20) eV, the systematic Uncertainties due to all atmospheric effects increase from 4% to 8% in measurements of shower energy, and 4 g cm(-2) to 8 g cm(-2) in measurements of the shower maximum., The successful installation and commissioning of the Pierre Auger Observatory would not have been possible without the strong commitment and effort from the technical and administrative staff in Malargüe. We are very grateful to the following agencies and organizations for financial support: Comisión Nacional de Energía Atómica, Fundación Antorchas, Gobierno De La Provincia de Mendoza, Municipalidad de Malargüe, NDM Holdings and Valle Las Leñas, in gratitude for their continuing cooperation over land access, Argentina; the Australian Research Council; Conselho Nacional de Desenvolvimento Científico e Tecnológico (CNPq), Financiadora de Estudos e Projetos (FINEP), Fundaçao de Amparo à Pesquisa do Estado de Rio de Janeiro (FAPERJ), Fundaçao de Amparo à Pesquisa do Estado de Sao Paulo (FAPESP), Ministério de Ciência e Tecnologia (MCT), Brazil; AVCR AV0Z10100502 and AV0Z10100522, GAAV KJB300100801 and KJB100100904, MSMT-CR LA08016, LC527, 1M06002, and MSM0021620859, Czech Republic; Centre de Calcul IN2P3/CNRS, Centre National de la Recherche Scientifique (CNRS), Conseil Régional Ile-de-France, Département Physique Nucléaire et Corpusculaire (PNC-IN2P3/CNRS), Département Sciences de l’Univers (SDU-INSU/CNRS), France; Bundesministerium für Bildung und Forschung (BMBF), Deutsche Forschungsgemeinschaft (DFG), Finanzministerium Baden- Württemberg, Helmholtz-Gemeinschaft Deutscher Forschungszentren (HGF), Ministerium für Wissenschaft und Forschung, Nordrhein-Westfalen, Ministerium für Wissenschaft, Forschung und Kunst, Baden-W¨urttemberg, Germany; Istituto Nazionale di Fisica Nucleare (INFN), Ministero dell’Istruzione,dell’Università e della Ricerca (MIUR), Italy; Consejo Nacional de Ciencia y Tecnología (CONACYT), Mexico; Ministerie van Onderwijs, Cultuur en Wetenschap, Nederlandse Organisatie voor Wetenschappelijk Onderzoek (NWO), Stichting voor Fundamenteel Onderzoek der Materie (FOM), Netherlands; Ministry of Science and Higher Education, Grant Nos. 1 P03 D 014 30, N202 090 31/0623, and PAP/218/2006, Poland; Fundaçao para a Ciência e a Tecnologia, Portugal; Ministry for Higher Education, Science, and Technology, Slovenian Research Agency, Slovenia; Comunidad de Madrid, Consejería de Educación de la Comunidad de Castilla La Mancha, FEDER funds, Ministerio de Ciencia e Innovación, Xunta de Galicia, Spain; Science and Technology Facilities Council, United Kingdom; Department of Energy, Contract No. DE-AC02-07CH11359, National Science Foundation, Grant No. 0450696, The Grainger Foundation USA; ALFA-EC / HELEN, European Union 6th Framework Program, Grant No. MEIF-CT-2005-025057, European Union 7th Framework Program, Grant No. PIEF-GA-2008-220240, and UNESCO.

We report on the realisation of a few pairs dielectric Distributed Bragg Reflectors fabricated by reactive electron-beam deposition, with state-of-the-art performances, such as very high reflectance (up to about 99.4%), wide stop band (up to 160 nm) in the visible range, and smooth interfaces (roughness as low as 1.5 nm). As a demonstrator of the very high quality of the mirrors we realized a polymer-based vertical microcavity laser by an imprinting-like approach. The device exhibits laser action at 519 nm, indicating low-loss dielectric reflectors grown by electron-beam techniques as promising tools for organic solid-state lasers. (c) 2006 Optical Society of America.

Much research has suggested that night-time light (NTL) can be used as a proxy for a number of variables, including urbanization, density, and economic growth. As governments around the world either collect census data infrequently or are scaling back the amount of detail collected, alternate sources of population and economic information like NTL are being considered. But, just how close is the statistical relationship between NTL and economic activity at a fine-grained geographical level? This paper uses a combination of correlation analysis and geographically weighted regressions in order to examine if light can function as a proxy for economic activities at a finer level. We use a fine-grained geo-coded residential and industrial full sample micro-data set for Sweden, and match it with both radiance and saturated light emissions. We find that the correlation between NTL and economic activity is strong enough to make it a relatively good proxy for population and establishment density, but the correlation is weaker in relation to wages. In general, we find a stronger relation between light and density values, than with light and total values. We also find a closer connection between radiance light and economic activity, than with saturated light. Further, we find the link between light and economic activity, especially estimated by wages, to be slightly overestimated in large urban areas and underestimated in rural areas.