O 1s excitation and ionization processes in the CO2 molecule studied via detection of low-energy fluorescence emission

Oxygen 1s excitation and ionization processes in the CO2 molecule have been studied with dispersed and non-dispersed fluorescence spectroscopy as well as with the vacuum ultraviolet (VUV) photon?photoion coincidence technique. The intensity of the neutral O emission line at 845 nm shows particular sensitivity to core-to-Rydberg excitations and core?valence double excitations, while shape resonances are suppressed. In contrast, the partial fluorescence yield in the wavelength window 300?650 nm and the excitation functions of selected O+ and C+ emission lines in the wavelength range 400?500 nm display all of the absorption features. The relative intensity of ionic emission in the visible range increases towards higher photon energies, which is attributed to O 1s shake-off photoionization. VUV photon?photoion coincidence spectra reveal major contributions from the C+ and O+ ions and a minor contribution from C2+. No conclusive changes in the intensity ratios among the different ions are observed above the O 1s threshold. The line shape of the VUV?O+ coincidence peak in the mass spectrum carries some information on the initial core excitation

Emission control of InGaN nanocolumns grown by molecular-beam epitaxy on Si(111) substrates

This work studies the effect of the growth temperature on the morphology and emission characteristics of self-assembled InGaN nanocolumns grown by plasma assisted molecular beam epitaxy. Morphology changes are assessed by scanning electron microscopy, while emission is measured by photoluminescence. Within the growth temperature range of 750 to 650 °C, an increase in In incorporation for decreasing temperature is observed. This effect allows tailoring the InGaN nanocolumns emission line shape by using temperature gradients during growth. Depending on the gradient rate, span, and sign, broad emission line shapes are obtained, covering the yellow to green range, even yielding white emission

One dimensional exciton luminescence induced by extended defects in nonpolar (Al,Ga)N/GaN quantum wells

In this study, we present the optical properties of nonpolar GaN/(Al,Ga)N single quantum wells (QWs) grown on either a- or m-plane GaN templates for Al contents set below 15%. In order to reduce the density of extended defects, the templates have been processed using the epitaxial lateral overgrowth technique. As expected for polarization-free heterostructures, the larger the QW width for a given Al content, the narrower the QW emission line. In structures with an Al content set to 5 or 10%, we also observe emission from excitons bound to the intersection of I1-type basal plane stacking faults (BSFs) with the QW. Similarly to what is seen in bulk material, the temperature dependence of BSF-bound QW exciton luminescence reveals intra-BSF localization. A qualitative model evidences the large spatial extension of the wavefunction of these BSF-bound QW excitons, making them extremely sensitive to potential fluctuations located in and away from BSF. Finally, polarization-dependent measurements show a strong emission anisotropy for BSF-bound QW excitons, which is related to their one-dimensional character and that confirms that the intersection between a BSF and a GaN/(Al,Ga)N QW can be described as a quantum wire.

Technical developments for computed tomography on the CENBG nanobeam line

The use of ion microbeams as probes for computedtomography has proven to be a powerful tool for the three-dimensional characterization of specimens a few tens of micrometers in size. Compared to other types of probes, the main advantage is that quantitative information about mass density and composition can be obtained directly, using specific reconstruction codes. At the Centre d’Etudes Nucléaires de Bordeaux Gradignan (CENBG), this technique was initially developed for applications in cellular biology. However, the observation of the cell ultrastructure requires a sub-micron resolution. The construction of the nanobeamline at the Applications Interdisciplinaires des Faisceaux d’Ions en Region Aquitaine (AIFIRA) irradiation facility has opened new perspectives for such applications. The implementation of computedtomography on the nanobeamline of CENBG has required a careful design of the analysis chamber, especially microscopes for precise sample visualization, and detectors for scanning transmission ion microscopy (STIM) and for particle induced X-ray emission (PIXE). The sample can be precisely positioned in the three directions X, Y, Z and a stepper motor coupled to a goniometer ensures the rotational motion. First images of 3D tomography were obtained on a reference sample containing microspheres of certified diameter, showing the good stability of the beam and the sample stage, and the precision of the motion.

On-line measurement of soil properties without direct spectral response in near infrared spectral range

So far, the majority of reports on on-line measurement considered soil properties with direct spectral responses in near infrared spectroscopy (NIRS). This work reports on the results of on-line measurement of soil properties with indirect spectral responses, e.g. pH, cation exchange capacity (CEC), exchangeable calcium (Caex) and exchangeable magnesium (Mgex) in one field in Bedfordshire in the UK. The on-line sensor consisted of a subsoiler coupled with an AgroSpec mobile, fibre type, visible and near infrared (vis–NIR) spectrophotometer (tec5 Technology for Spectroscopy, Germany), with a measurement range 305–2200 nm to acquire soil spectra in diffuse reflectance mode. General calibration models for the studied soil properties were developed with a partial least squares regression (PLSR) with one-leave-out cross validation, using spectra measured under non-mobile laboratory conditions of 160 soil samples collected from different fields in four farms in Europe, namely, Czech Republic, Denmark, Netherland and UK. A group of 25 samples independent from the calibration set was used as independent validation set. Higher accuracy was obtained for laboratory scanning as compared to on-line scanning of the 25 independent samples. The prediction accuracy for the laboratory and on-line measurements was classified as excellent/very good for pH (RPD = 2.69 and 2.14 and r2 = 0.86 and 0.78, respectively), and moderately good for CEC (RPD = 1.77 and 1.61 and r2 = 0.68 and 0.62, respectively) and Mgex (RPD = 1.72 and 1.49 and r2 = 0.66 and 0.67, respectively). For Caex, very good accuracy was calculated for laboratory method (RPD = 2.19 and r2 = 0.86), as compared to the poor accuracy reported for the on-line method (RPD = 1.30 and r2 = 0.61). The ability of collecting large number of data points per field area (about 12,800 point per 21 ha) and the simultaneous analysis of several soil properties without direct spectral response in the NIR range at relatively high operational speed and appreciable accuracy, encourage the recommendation of the on-line measurement system for site specific fertilisation.

Beyond filtered backprojection: a reconstruction software package for ion beam microtomography data

A new version of the TomoRebuild data reduction software package is presented, for the reconstruction of scanning transmission ion microscopy tomography (STIMT) and particle induced X-ray emission tomography (PIXET) images. First, we present a state of the art of the reconstruction codes available for ion beam microtomography. The algorithm proposed here brings several advantages. It is a portable, multi-platform code, designed in C++ with well-separated classes for easier use and evolution. Data reduction is separated in different steps and the intermediate results may be checked if necessary. Although no additional graphic library or numerical tool is required to run the program as a command line, a user friendly interface was designed in Java, as an ImageJ plugin. All experimental and reconstruction parameters may be entered either through this plugin or directly in text format files. A simple standard format is proposed for the input of experimental data. Optional graphic applications using the ROOT interface may be used separately to display and fit energy spectra. Regarding the reconstruction process, the filtered backprojection (FBP) algorithm, already present in the previous version of the code, was optimized so that it is about 10 times as fast. In addition, Maximum Likelihood Expectation Maximization (MLEM) and its accelerated version Ordered Subsets Expectation Maximization (OSEM) algorithms were implemented. A detailed user guide in English is available. A reconstruction example of experimental data from a biological sample is given. It shows the capability of the code to reduce noise in the sinograms and to deal with incomplete data, which puts a new perspective on tomography using low number of projections or limited angle.

Testing JEFF-3.1.1 and ENDF/B-VII.1 Decay and Fission Yield Nuclear Data Libraries with Fission Pulse Neutron Emission and Decay Heat Experiments

The aim of this work is to test the present status of Evaluated Nuclear Decay and Fission Yield Data Libraries to predict decay heat and delayed neutron emission rate, average neutron energy and neutron delayed spectra after a neutron fission pulse. Calculations are performed with JEFF-3.1.1 and ENDF/B-VII.1, and these are compared with experimental values. An uncertainty propagation assessment of the current nuclear data uncertainties is performed.

Self assembled and ordered group III nitride nanocolumnar structures for light emitting applications

El objetivo de este trabajo es un estudio profundo del crecimiento selectivo de nanoestructuras de InGaN por epitaxia de haces moleculares asistido por plasma, concentrandose en el potencial de estas estructuras como bloques constituyentes en LEDs de nueva generación. Varias aproximaciones al problema son discutidas; desde estructuras axiales InGaN/GaN, a estructuras core-shell, o nanoestructuras crecidas en sustratos con orientaciones menos convencionales (semi polar y no polar). La primera sección revisa los aspectos básicos del crecimiento auto-ensamblado de nanocolumnas de GaN en sustratos de Si(111). Su morfología y propiedades ópticas son comparadas con las de capas compactas de GaN sobre Si(111). En el caso de las columnas auto-ensambladas de InGaN sobre Si(111), se presentan resultados sobre el efecto de la temperatura de crecimiento en la incorporación de In. Por último, se discute la inclusión de nanodiscos de InGaN en las nanocolumnas de GaN. La segunda sección revisa los mecanismos básicos del crecimiento ordenado de nanoestructuras basadas en GaN, sobre templates de GaN/zafiro. Aumentando la relación III/V localmente, se observan cambios morfológicos; desde islas piramidales, a nanocolumnas de GaN terminadas en planos semipolares, y finalmente, a nanocolumnas finalizadas en planos c polares. Al crecer nanodiscos de InGaN insertados en las nanocolumnas de GaN, las diferentes morfologias mencionadas dan lugar a diferentes propiedades ópticas de los nanodiscos, debido al diferente carácter (semi polar o polar) de los planos cristalinos involucrados. La tercera sección recoge experimentos acerca de los efectos que la temperatura de crecimiento y la razón In/Ga tienen en la morfología y emisión de nanocolumnas ordenadas de InGaN crecidas sobre templates GaN/zafiro. En el rango de temperaturas entre 650 y 750 C, la incorporacion de In puede modificarse bien por la temperatura de crecimiento, o por la razón In/Ga. Controlar estos factores permite la optimización de la longitud de onda de emisión de las nanocolumnas de InGaN. En el caso particular de la generación de luz blanca, se han seguidos dos aproximaciones. En la primera, se obtiene emisión amarilla-blanca a temperatura ambiente de nanoestructuras donde la región de InGaN consiste en un gradiente de composiciones de In, que se ha obtenido a partir de un gradiente de temperatura durante el crecimiento. En la segunda, el apilamiento de segmentos emitiendo en azul, verde y rojo, consiguiendo la integración monolítica de estas estructuras en cada una de las nanocolumnas individuales, da lugar a emisores ordenados con un amplio espectro de emisión. En esta última aproximación, la forma espectral puede controlarse con la longitud (duración del crecimiento) de cada uno de los segmentos de InGaN. Más adelante, se presenta el crecimiento ordenado, por epitaxia de haces moleculares, de arrays de nanocolumnas que son diodos InGaN/GaN cada una de ellas, emitiendo en azul (441 nm), verde (502 nm) y amarillo (568 nm). La zona activa del dispositivo consiste en una sección de InGaN, de composición constante nominalmente y longitud entre 250 y 500 nm, y libre de defectos extendidos en contraste con capas compactas de InGaN de similares composiciones y espesores. Los espectros de electroluminiscencia muestran un muy pequeño desplazamiento al azul al aumentar la corriente inyectada (desplazamiento casi inexistente en el caso del dispositivo amarillo), y emisiones ligeramente más anchas que en el caso del estado del arte en pozos cuánticos de InGaN. A continuación, se presenta y discute el crecimiento ordenado de nanocolumnas de In(Ga)N/GaN en sustratos de Si(111). Nanocolumnas ordenadas emitiendo desde el ultravioleta (3.2 eV) al infrarrojo (0.78 eV) se crecieron sobre sustratos de Si(111) utilizando una capa compacta (“buffer”) de GaN. La morfología y eficiencia de emisión de las nanocolumnas emitiendo en el rango espectral verde pueden ser mejoradas ajustando las relaciones In/Ga y III/N, y una eficiencia cuántica interna del 30% se deriva de las medidas de fotoluminiscencia en nanocolumnas optimizadas. En la siguiente sección de este trabajo se presenta en detalle el mecanismo tras el crecimiento ordenado de nanocolumnas de InGaN/GaN emitiendo en el verde, y sus propiedades ópticas. Nanocolumnas de InGaN/GaN con secciones largas de InGaN (330-830 nm) se crecieron tanto en sustratos GaN/zafiro como GaN/Si(111). Se encuentra que la morfología y la distribución espacial del In dentro de las nanocolumnas dependen de las relaciones III/N e In/Ga locales en el frente de crecimiento de las nanocolumnas. La dispersión en el contenido de In entre diferentes nanocolumnas dentro de la misma muestra es despreciable, como indica las casi identicas formas espectrales de la catodoluminiscencia de una sola nanocolumna y del conjunto de ellas. Para las nanocolumnas de InGaN/GaN crecidas sobre GaN/Si(111) y emitiendo en el rango espectral verde, la eficiencia cuántica interna aumenta hasta el 30% al disminuir la temperatura de crecimiento y aumentar el nitrógeno activo. Este comportamiento se debe probablemente a la formación de estados altamente localizados, como indica la particular evolución de la energía de fotoluminiscencia con la temperatura (ausencia de “s-shape”) en muestras con una alta eficiencia cuántica interna. Por otro lado, no se ha encontrado la misma dependencia entre condiciones de crecimiento y efiencia cuántica interna en las nanoestructuras InGaN/GaN crecidas en GaN/zafiro, donde la máxima eficiencia encontrada ha sido de 3.7%. Como alternativa a las nanoestructuras axiales de InGaN/GaN, la sección 4 presenta resultados sobre el crecimiento y caracterización de estructuras core-shell de InGaN/GaN, re-crecidas sobre arrays de micropilares de GaN fabricados por ataque de un template GaN/zafiro (aproximación top-down). El crecimiento de InGaN/GaN es conformal, con componentes axiales y radiales en el crecimiento, que dan lugar a la estructuras core-shell con claras facetas hexagonales. El crecimiento radial (shell) se ve confirmado por medidas de catodoluminiscencia con resolución espacial efectuadas en un microscopio electrónico de barrido, asi como por medidas de microscopía de transmisión de electrones. Más adelante, el crecimiento de micro-pilares core-shell de InGaN se realizó en pilares GaN (cores) crecidos selectivamente por epitaxia de metal-orgánicos en fase vapor. Con el crecimiento de InGaN se forman estructuras core-shell con emisión alrededor de 3 eV. Medidas de catodoluminiscencia resuelta espacialmente indican un aumento en el contenido de indio del shell en dirección a la parte superior del pilar, que se manifiesta en un desplazamiento de la emisión de 3.2 eV en la parte inferior, a 3.0 eV en la parte superior del shell. Este desplazamiento está relacionado con variaciones locales de la razón III/V en las facetas laterales. Finalmente, se demuestra la fabricación de una estructura pin basada en estos pilares core-shell. Medidas de electroluminiscencia resuelta espacialmente, realizadas en pilares individuales, confirman que la electroluminiscencia proveniente del shell de InGaN (diodo lateral) está alrededor de 3.0 eV, mientras que la emisión desde la parte superior del pilar (diodo axial) está alrededor de 2.3 eV. Para finalizar, se presentan resultados sobre el crecimiento ordenado de GaN, con y sin inserciones de InGaN, en templates semi polares (GaN(11-22)/zafiro) y no polares (GaN(11-20)/zafiro). Tras el crecimiento ordenado, gran parte de los defectos presentes en los templates originales se ven reducidos, manifestándose en una gran mejora de las propiedades ópticas. En el caso de crecimiento selectivo sobre templates con orientación GaN(11-22), no polar, la formación de nanoestructuras con una particular morfología (baja relación entre crecimiento perpedicular frente a paralelo al plano) permite, a partir de la coalescencia de estas nanoestructuras, la fabricación de pseudo-templates no polares de GaN de alta calidad. ABSTRACT The aim of this work is to gain insight into the selective area growth of InGaN nanostructures by plasma assisted molecular beam epitaxy, focusing on their potential as building blocks for next generation LEDs. Several nanocolumn-based approaches such as standard axial InGaN/GaN structures, InGaN/GaN core-shell structures, or InGaN/GaN nanostructures grown on semi- and non-polar substrates are discussed. The first section reviews the basics of the self-assembled growth of GaN nanocolumns on Si(111). Morphology differences and optical properties are compared to those of GaN layer grown directly on Si(111). The effects of the growth temperature on the In incorporation in self-assembled InGaN nanocolumns grown on Si(111) is described. The second section reviews the basic growth mechanisms of selectively grown GaNbased nanostructures on c-plane GaN/sapphire templates. By increasing the local III/V ratio morphological changes from pyramidal islands, to GaN nanocolumns with top semi-polar planes, and further to GaN nanocolumns with top polar c-planes are observed. When growing InGaN nano-disks embedded into the GaN nanocolumns, the different morphologies mentioned lead to different optical properties, due to the semipolar and polar nature of the crystal planes involved. The third section reports on the effect of the growth temperature and In/Ga ratio on the morphology and light emission characteristics of ordered InGaN nanocolumns grown on c-plane GaN/sapphire templates. Within the growth temperature range of 650 to 750oC the In incorporation can be modified either by the growth temperature, or the In/Ga ratio. Control of these factors allows the optimization of the InGaN nanocolumns light emission wavelength. In order to achieve white light emission two approaches are used. First yellow-white light emission can be obtained at room temperature from nanostructures where the InGaN region is composition-graded by using temperature gradients during growth. In a second approach the stacking of red, green and blue emitting segments was used to achieve the monolithic integration of these structures in one single InGaN nanocolumn leading to ordered broad spectrum emitters. With this approach, the spectral shape can be controlled by changing the thickness of the respective InGaN segments. Furthermore the growth of ordered arrays of InGaN/GaN nanocolumnar light emitting diodes by molecular beam epitaxy, emitting in the blue (441 nm), green (502 nm), and yellow (568 nm) spectral range is reported. The device active region, consisting of a nanocolumnar InGaN section of nominally constant composition and 250 to 500 nm length, is free of extended defects, which is in strong contrast to InGaN layers (planar) of similar composition and thickness. Electroluminescence spectra show a very small blue shift with increasing current, (almost negligible in the yellow device) and line widths slightly broader than those of state-of-the-art InGaN quantum wells. Next the selective area growth of In(Ga)N/GaN nanocolumns on Si(111) substrates is discussed. Ordered In(Ga)N/GaN nanocolumns emitting from ultraviolet (3.2 eV) to infrared (0.78 eV) were then grown on top of GaN-buffered Si substrates. The morphology and the emission efficiency of the In(Ga)N/GaN nanocolumns emitting in the green could be substantially improved by tuning the In/Ga and total III/N ratios, where an estimated internal quantum efficiency of 30 % was derived from photoluminescence data. In the next section, this work presents a study on the selective area growth mechanisms of green-emitting InGaN/GaN nanocolumns and their optical properties. InGaN/GaN nanocolumns with long InGaN sections (330-830nm) were grown on GaN/sapphire and GaN-buffered Si(111). The nanocolumn’s morphology and spatial indium distribution is found to depend on the local group (III)/N and In/Ga ratios at the nanocolumn’s top. A negligible spread of the average indium incorporation among different nanostructures is found as indicated by similar shapes of the cathodoluminescence spectra taken from single nanocolumns and ensembles of nanocolumns. For InGaN/GaN nanocolumns grown on GaN-buffered Si(111), all emitting in the green spectral range, the internal quantum efficiency increases up to 30% when decreasing growth temperature and increasing active nitrogen. This behavior is likely due to the formation of highly localized states, as indicated by the absence of a complete s-shape behavior of the PL peak position with temperature (up to room temperature) in samples with high internal quantum efficiency. On the other hand, no dependence of the internal quantum efficiency on the growth conditions is found for InGaN/GaN nanostructures grown on GaN/sapphire, where the maximum achieved efficiency is 3.7%. As alternative to axial InGaN/GaN nanostructures, section 4 reports on the growth and characterization of InGaN/GaN core-shell structures on an ordered array of top-down patterned GaN microrods etched from a GaN/sapphire template. Growth of InGaN/GaN is conformal, with axial and radial growth components leading to core-shell structures with clear hexagonal facets. The radial InGaN growth (shell) is confirmed by spatially resolved cathodoluminescence performed in a scanning electron microscopy as well as in scanning transmission electron microscopy. Furthermore the growth of InGaN core-shell micro pillars using an ordered array of GaN cores grown by metal organic vapor phase epitaxy as a template is demonstrated. Upon InGaN overgrowth core-shell structures with emission at around 3.0 eV are formed. With spatially resolved cathodoluminescence, an increasing In content towards the pillar top is found to be present in the InGaN shell, as indicated by a shift of CL peak position from 3.2 eV at the shell bottom to 3.0 eV at the shell top. This shift is related to variations of the local III/V ratio at the side facets. Further, the successful fabrication of a core-shell pin diode structure is demonstrated. Spatially resolved electroluminescence measurements performed on individual micro LEDs, confirm emission from the InGaN shell (lateral diode) at around 3.0 eV, as well as from the pillar top facet (axial diode) at around 2.3 eV. Finally, this work reports on the selective area growth of GaN, with and without InGaN insertion, on semi-polar (11-22) and non-polar (11-20) templates. Upon SAG the high defect density present in the GaN templates is strongly reduced as indicated by TEM and a dramatic improvement of the optical properties. In case of SAG on non-polar (11-22) templates the formation of nanostructures with a low aspect ratio took place allowing for the fabrication of high-quality, non-polar GaN pseudo-templates by coalescence of the nanostructures.

Emission regimes in a distributed feedback tapered master-oscillator power-amplifier at 1.5 µm

Integrated master-oscillator power amplifiers driven under steady-state injection conditions are known to show a complex dynamics resulting in a variety of emission regimes. We present experimental results on the emission characteristics of a 1.5 µm distributed feedback tapered master-oscillator power-amplifier in a wide range of steady-state injection conditions, showing different dynamic behaviors. The study combines the optical and radio-frequency spectra recorded under different levels of injected current into the master oscillator and the power amplifier sections. Under low injection current of the master oscillator the correlation between the optical and radio-frequency spectral maps allows to identify operation regimes in which the device emission arises from either the master oscillator mode or from the compound cavity modes allowed by the residual reflectance of the amplifier front facet. The quasi-periodic occurrence of these emission regimes as a function of the amplifier current is interpreted in terms of a thermally tuned competition between the modes of the master oscillator and the compound cavity modes. Under high injection current of the masteroscillator, two different regimes alternate quasi-periodically as a function of the injected current in the power amplifier: a stable regime with a single mode emission at the master oscillator frequency, and an unstable and complex self-pulsating regime showing strong peaks in the radio-frequency spectra as well as multiple frequencies in the optical spectra.

Measurement of plasma electron density generated in an experiment of laser shock processing, utilizing the H­α­-line

In this work we have realized plasma diagnosis produced by Laser (LPP), by means of emission spectroscopy in a Laser Shock Processing (LSP). The LSP has been proposed as an alternative technology, competitive with classical surface treatments. The ionic species present in the plasma together with electron density and its temperature provide significant indicators of the degree of surface effect of the treated material. In order to analyze these indicators, we have realized spectroscopic studies of optical emission in the laser-generated plasmas in different situations. We have worked focusing on an aluminum sample (Al2024) in air and/or in LSP conditions (water flow) a Q-switched laser of Nd:YAG (λ = 1.06 μm, 10 ns of pulse duration, running at 10 Hz repetition rate). The pulse energy was set at 2,5 J per pulse. The electron density has been measured using, in every case, the Stark broadening of H Balmer α line (656.27 nm). In the case of the air, this measure has been contrasted with the value obtained with the line of 281.62 nm of Al II. Special attention has been paid to the self-absorption of the spectral lines used. The measures were realized with different delay times after the pulse of the laser (1–8 μs) and with a time window of 1 μs. In LSP the electron density obtained was between 1017 cm−3 for the shortest delays (4–6 μs), and 1016 cm−3 for the greatest delays (7,8 μs).