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Metal-halide perovskites deposited by wet-chemical deposition have demonstrated great potential for various electronic applications, including solar cells. A remaining question is how light-induced excess charges become distributed over such polycrystalline material. Here, we examine the local conductive properties of MAPbI3 and CsFAPbI3 by using scanning microwave microscopy (sMIM) in the dark and light. sMIM is an atomic force microscopy (AFM)-based technique measuring variations of the in-phase and out-of-phase signals due to changes in the tip-sample interaction, yielding MIM-Re and MIM-Im images, respectively. Combining this information leads to a picture for CsFAPbI3 in which excess charges are distributed evenly over the grains, but due to local defect-rich areas, possibly related to different crystal facets, local perturbations in carrier concentration exist. For solar cells, this distribution in carrier concentration under illumination leads to variation in the local Fermi level splitting, which should be suppressed to reduce the voltage deficit., ChemE/Opto-electronic Materials, ChemE/O&O groep

Despite intense research into the optoelectronic properties of metal halide perovskites (MHPs), sub-bandgap absorption in MHPs remains largely unexplored. Here we recorded two-photon absorption spectra of MHPs using the time-resolved microwave conductivity technique. A two-step upward trend is observed in the two-photon absorption spectrum for methylammonium lead iodide, and some analogues, which implies that the commonly used scaling law is not applicable to MHPs. This aspect is further confirmed by temperature-dependent conductivity measurements. Using an empirical multiband tight binding model, spectra for methylammonium lead iodide were calculated by integration over the entire Brillouin zone, showing compelling similarity with experimental results. We conclude that the second upward trend in the two-photon absorption spectrum originates from additional optical transitions to the heavy and light electron bands formed by the strong spin-orbit coupling. Hence, valuable insight can be obtained in the opto-electronic properties of MHPs by sub-bandgap spectroscopy, complemented by modelling., ChemE/Opto-electronic Materials, ChemE/O&O groep

Despite intense research into the optoelectronic properties of metal halide perovskites (MHPs), sub-bandgap absorption in MHPs remains largely unexplored. Here we recorded two-photon absorption spectra of MHPs using the time-resolved microwave conductivity technique. A two-step upward trend is observed in the two-photon absorption spectrum for methylammonium lead iodide, and some analogues, which implies that the commonly used scaling law is not applicable to MHPs. This aspect is further confirmed by temperature-dependent conductivity measurements. Using an empirical multiband tight binding model, spectra for methylammonium lead iodide were calculated by integration over the entire Brillouin zone, showing compelling similarity with experimental results. We conclude that the second upward trend in the two-photon absorption spectrum originates from additional optical transitions to the heavy and light electron bands formed by the strong spin-orbit coupling. Hence, valuable insight can be obtained in the opto-electronic properties of MHPs by sub-bandgap spectroscopy, complemented by modelling., ChemE/Opto-electronic Materials, ChemE/O&O groep

Contains fulltext : 192699.pdf (publisher's version ) (Open Access), Basic facial emotion recognition is suggested to be negatively affected by puberty onset reflected in a "pubertal dip" in performance compared to pre- or post-puberty. However, findings remain inconclusive. Further, research points to an own-age bias, i.e., a superior emotion recognition for peer faces. We explored adolescents' ability to recognize specific emotions. Ninety-five children and adolescents, aged 8-17 years, judged whether the emotions displayed by adolescent or adult faces were angry, sad, neutral, or happy. We assessed participants a priori by pubertal status while controlling for age. Results indicated no "pubertal dip", but decreasing reaction times across adolescence. No own-age bias was found. Taken together, basic facial emotion recognition does not seem to be disrupted during puberty as compared to pre- and post-puberty.

Contains fulltext : 192699.pdf (publisher's version ) (Open Access), Basic facial emotion recognition is suggested to be negatively affected by puberty onset reflected in a "pubertal dip" in performance compared to pre- or post-puberty. However, findings remain inconclusive. Further, research points to an own-age bias, i.e., a superior emotion recognition for peer faces. We explored adolescents' ability to recognize specific emotions. Ninety-five children and adolescents, aged 8-17 years, judged whether the emotions displayed by adolescent or adult faces were angry, sad, neutral, or happy. We assessed participants a priori by pubertal status while controlling for age. Results indicated no "pubertal dip", but decreasing reaction times across adolescence. No own-age bias was found. Taken together, basic facial emotion recognition does not seem to be disrupted during puberty as compared to pre- and post-puberty.

Contains fulltext : 192699.pdf (publisher's version ) (Open Access), Basic facial emotion recognition is suggested to be negatively affected by puberty onset reflected in a "pubertal dip" in performance compared to pre- or post-puberty. However, findings remain inconclusive. Further, research points to an own-age bias, i.e., a superior emotion recognition for peer faces. We explored adolescents' ability to recognize specific emotions. Ninety-five children and adolescents, aged 8-17 years, judged whether the emotions displayed by adolescent or adult faces were angry, sad, neutral, or happy. We assessed participants a priori by pubertal status while controlling for age. Results indicated no "pubertal dip", but decreasing reaction times across adolescence. No own-age bias was found. Taken together, basic facial emotion recognition does not seem to be disrupted during puberty as compared to pre- and post-puberty.

Contains fulltext : 181043.pdf (Publisher’s version ) (Closed access)

Contains fulltext : 181043.pdf (Publisher’s version ) (Closed access)

Contains fulltext : 181043.pdf (Publisher’s version ) (Closed access)

Transmission X-ray microscopy is a uniquely suited technique for studies of environmental colloids since it allows imaging in aqueous media with high spatial resolution, presently down to the 20 nm range. Such nanoscale morphological description of these high-specific-surface-area compounds show promise for improved understanding of soils, sediments or groundwater aquifers. However, present high-quality X-ray microscopes are located at synchrotron radiation facilities resulting in limited applicability and accessibility for colloid scientists. Here we investigate the applicability of a laboratory-scale transmission X-ray microscope for studies of colloids of the environment. The microscope is based on a laser-plasma source in combination with multilayer and zone plate optics. Samples are held at atmospheric pressure in their natural wet state. We show images revealing the nano-scale morphology of the clay nontronite, soils such as chernozem and luvisol, and the mineral hematite, an iron oxide. Comparative studies of dried substances clearly show the need for imaging in the wet state. The image quality approaches that of synchrotron-based microscopes, albeit at longer exposure times. Stereo imaging is investigated as a means for giving 3D information with shorter exposure times than tomography requires. Finally the future development of the laboratory X-ray microscope is discussed, especially with regard to the reduction of exposure times., QC 20121127

We summarize the recent progress in laboratory-scale soft and hard x-ray micro imaging in Stockholm. Our soft x-ray work is based on liquid-jet laser-plasma sources which are combined with diffractive and multilayer optics to form laboratory x-ray microscopes. In the hard x-ray regime the imaging is based on a liquid-metal-jet electron-impact source which provides the necessary coherence to allow phase-contrast imaging with high fidelity., QC 20110128

Most soft x-ray microscopes operating in the water window (lambda = 2.3 - 4.4 nm) rely on synchrotron radiation sources. In the future we believe scientists will use soft x-ray microscopes as one imaging tool among others in their own laboratory. For this purpose we have developed a full field soft x-ray microscope with a laser-plasma source compact enough to fit on an optical table. In this contribution we describe the current status of this microscope now featuring stable operation at lambda = 3.37 nm or lambda = 2.48 nm. In-house fabricated single element zone plates offering the possibility to perform phase contrast imaging have been implemented. We also report on the first application experiments for compact soft x-ray microscopy, including results from studies of clay minerals and colloids existing in nature and results from phase optics experiments. Planned upgrades of the microscope include increasing the source brightness, implementing more efficient condenser optics, and installing a cryo sample stage for tomography. These improvements will open up for further applications, especially in the field of biological imaging., QC 20110128

Colloids play an important role when describing parameters of and processes within soils, sediments or aquifers due to their abundance and their high specific surface area. It is of great importance to visualize the morphology of the structures formed by these particles as close as possible to environmental conditions. With X-ray microscopy colloids from the environment can be imaged directly in aqueous media with high spatial resolution. We demonstrate the first use of a compact laboratory x-ray microscope for studies of colloids from the environment, namely aqueous suspensions of clays and soils. The microscope is based on a high-brightness laser-produced-plasma X-ray source, a multilayer mirror and diffractive optics. The experiments show that such compact X-ray microscopes are reaching the image quality and operational maturity to make a significant impact in fields like environmental sciences., QC 20141014

The here presented combination of stereo imaging and elemental mapping with soft X-ray microscopy reveals the spatial arrangement of naturally aqueous colloidal systems, e.g. iron oxides in soil colloid clusters. Changes in the spatial arrangement can be induced by manipulating the sample in-situ and thus be investigated directly and as a function of time., QC 20141013

The analysis of pristine and functionalized carbon nanotubes by X-ray spectromicroscopy was demonstrated. It was shown that both the generation of COOH groups due to functionalization and the reaction of these groups with hexavalent uranium (surface complexation) influenses the NEXAFS spectra. The method may become a promising tool for "mapping" chemical properties such as the presence or absence of chemical elements or the type of binding between these elements on the surface of carbon nanotubes.

The analysis of pristine and functionalized carbon nanotubes by X-ray spectromicroscopy was demonstrated. It was shown that both the generation of COOH groups due to functionalization and the reaction of these groups with hexavalent uranium (surface complexation) influenses the NEXAFS spectra. The method may become a promising tool for "mapping" chemical properties such as the presence or absence of chemical elements or the type of binding between these elements on the surface of carbon nanotubes.

The analysis of pristine and functionalized carbon nanotubes by X-ray spectromicroscopy was demonstrated. It was shown that both the generation of COOH groups due to functionalization and the reaction of these groups with hexavalent uranium (surface complexation) influenses the NEXAFS spectra. The method may become a promising tool for "mapping" chemical properties such as the presence or absence of chemical elements or the type of binding between these elements on the surface of carbon nanotubes.

The analysis of pristine and functionalized carbon nanotubes by X-ray spectromicroscopy was demonstrated. It was shown that both the generation of COOH groups due to functionalization and the reaction of these groups with hexavalent uranium (surface complexation) influenses the NEXAFS spectra. The method may become a promising tool for "mapping" chemical properties such as the presence or absence of chemical elements or the type of binding between these elements on the surface of carbon nanotubes.

For more than two decades aquatic chemistry is constantly gaining knowledge about nanoscale processes in the environment. While in early years the co-transport of contaminants in the saturated zone of aquifers has been in the focus of aquatic nanosciences and nanogeosciences, nowadays the research activities have broadened and span across several disciplines. In the course of R & D activities on nanomaterials the question of the behavior, fate and useful or adverse effects of nanoparticles in the environment arose and has boosted the activities quite substantially. The working group Aquatic Nanosciences and Nanotechnology has responded to the current development by inviting European scientists from different fields to contribute their expertise into the group’s discussions and activities while still keeping the core expertise on characterization techniques inherited from the former working group “Colloids”. In 2007 the working group organized an international workshop which was held in Vienna during the 10th and 11th December. The aim of the event was to offer a platform for bridging the different disciplines and exchange the current knowledge in the fields. Scientists from aquatic and environmental chemistry, nanogeosciences, nano-engineering, eco-toxicology and risk assessment presented their contributions to the current state of the art. The overall conclusions drawn from 29 presentations are given.

For more than two decades aquatic chemistry is constantly gaining knowledge about nanoscale processes in the environment. While in early years the co-transport of contaminants in the saturated zone of aquifers has been in the focus of aquatic nanosciences and nanogeosciences, nowadays the research activities have broadened and span across several disciplines. In the course of R & D activities on nanomaterials the question of the behavior, fate and useful or adverse effects of nanoparticles in the environment arose and has boosted the activities quite substantially. The working group Aquatic Nanosciences and Nanotechnology has responded to the current development by inviting European scientists from different fields to contribute their expertise into the group’s discussions and activities while still keeping the core expertise on characterization techniques inherited from the former working group “Colloids”. In 2007 the working group organized an international workshop which was held in Vienna during the 10th and 11th December. The aim of the event was to offer a platform for bridging the different disciplines and exchange the current knowledge in the fields. Scientists from aquatic and environmental chemistry, nanogeosciences, nano-engineering, eco-toxicology and risk assessment presented their contributions to the current state of the art. The overall conclusions drawn from 29 presentations are given.

X-ray absorption near edge structure (XANES) spectra at the sulfur (S) K-edge (E=2472 eV) were compared for bulk soil material, humic and fulvic acid fractions, and different particle size separates from Ah horizons of two arable Luvisols, from an O and a Bs horizon of a Podzol under Norway spruce forest, and from an H horizon of a Histosol (peat bog). In the bulk soil samples, the contribution of reduced organic S (organic mono- and disulfides) to total sulfur increased from 27% to 52%, and the contribution of ester sulfate and SO42−-S decreased from 39% to 14% of total S in the following order: arable Luvisols Ah—forested Podzol O—Histosol H. This sequence reflects the increasing organic carbon content and the decreasing O2 availability in that order. Neither sulfonate nor inorganic sulfide was detected in any of the bulk soil samples. For all samples except the Podzol Bs, the XANES spectra of the bulk soils differed considerably from the spectra of the humic and acid fractions of the respective soils, with the latter containing less reduced S (16–44% of total S) and more oxidized S (sulfone S: 19–35%; ester sulfate S: 14–38% of total S). Also the S speciation of most particle size fractions extracted from the Ah horizon of the Viehhausen Luvisol and the Bs horizon of the Podzol was different from that of the bulk soil. For both soils, the contribution of oxidized S species to total S increased and the contribution of sulfoxides and organic mono- and disulfides decreased with decreasing particle size. Thus, sulfur K-edge XANES spectra of alkaline soil extracts, including humic and fulvic acids or of particle size separates are not representative for the S speciation of the original soil sample they are derived from. The differences can be attributed to (i) artificial changes of the sulfur speciation during alkaline extraction (conversion of reduced S into oxidized S, loss of SO42− during purification of the extracts by dialysis) or particle size separation (carry

QC 20120229

Synchrotron-based X-ray absorption near edge spectroscopy (XANES) at the S K-edge (2476 eV) is a powerful, non-invasive tool for the speciation of sulfur in soil. However, in many studies instead of bulk soil samples, which often yielded spectra which were too noisy to analyze, alkaline extracts or soil particle size fractions have been investigated, accepting that the S speciation of these fractions represents that of the bulk soil. To test that assumption we compared the S speciation as revealed by S K-edge XANES of bulk soil, humic acid, fulvic acid, and several particle size fractions from A horizons of two cropland Alfisols, from an O and a Bs horizon of a forested Spodosol, and from an H horizon of a peat bog. The XANES spectra at the K-edge of S (2476 eV) were acquired at beamline ID 21 of the European Synchrotron Radiation Facility (ESRF) in Grenoble/France. For all except one (Spodosol Bs) sample, the XANES spectra of the humic and the fulvic acid fractions differed considerably from those of the respective bulk soil, with the humic and fulvic acid fractions generally being depleted in reduced S (thiols, organic disulfide) and enriched in oxidized S (sulfone, sulfonate, ester sulfate). Also the spectra of most particle size fractions were clearly different from the spectrum of the respective bulk soil, with the clay fraction being enriched in oxidized S, and the sand fractions being enriched in reduced S. Our results show that neither the sulfur K edge XANES spectra of alkaline soil extracts, including humic and fulvic acids, nor those of the clay particle size fraction can be used as proxies for the S speciation of the original soil from which the fractions had been isolated.

NR 20140805

Kolloide sind Bestandteile aller aquatischen Systeme. Sie umfassen Feststoffe, deren Größe in zumindest einer Dimension zwischen 1 und 1.000 nm liegt. Sie können anorganischer (z. B. Tonteilchen, Karbonate oder Silikate) oder organischer (z. B. Ruß oder höhermolekulare organische Verbindungen wie Huminstoffe) Natur sein. Auch Bakterien, Viren, Sporen und Algen in diesem Größenbereich können zu den Kolloiden gerechnet werden (häufig als Bio-Kolloide bezeichnet). Kolloide können den Transport von (Schad-)stoffen im Untergrund und in Oberflächengewässern beeinflussen, insbesondere von Spurenelementen und hydrophoben organischen Verbindungen, oder zu unerwünschten Effekten wie Porenraumreduktion (Clogging) führen. Für die Hygiene des Trinkwassers ist das Verhalten von Bakterien, Viren und Sporen (den Bio-Kolloiden) von besonderer Bedeutung. Bisher ist das Verhalten von Kolloiden nur unzureichend verstanden. Dieser Artikel soll einen Beitrag zu dem Verständnis des physikalischen Verhaltens der Kolloide, deren Vorkommen in der aquatischen Umwelt sowie Relevanz in Form einer Übersichtsarbeit leisten.

Kolloide sind Bestandteile aller aquatischen Systeme. Das Verhalten der Kolloide in der Umwelt, deren Mobilisierung, Transport und Abscheidung und somit auch die Relevanz sind noch nicht vollständig verstanden. Dies liegt zum Teil an der Tatsache, dass die Kolloidanalytik extrem aufwändig ist. Sie gehört nicht zur Standardanalytik eines Wasserlabors. Keine Technik ist bisher zufriedenstellend in der Lage, Kolloide in ihrem gesamten Größenbereich auch bei geringsten Konzentrationen gleichzeitig zu quantifizieren und zu identifizieren. In der Regel ist eine Kombination von verschiedenen Techniken notwendig, um ausreichend Informationen über das Verhalten der Kolloide zu erhalten. Für die Bestimmung der Oberflächeneigenschaften stehen kaum Methoden zur Verfügung. Eine weitere, nicht zu unterschätzende Schwierigkeit ist die Probennahme und Probenaufbereitung. Für die Untersuchung von Kolloiden sind spezielle Probennahmetechniken und Protokolle notwendig, da ansonsten die ungestörten, natürlichen Bedingungen durch (Probennahme-)Artefakte maskiert werden. Dieser Artikel soll in Form einer Übersichtsarbeit Hinweise zur Probennahme geben und die verschiedenen Möglichkeiten der Kolloidanalytik aufzeigen.

In den vergangenen Jahren wurde grundsätzlich akzeptiert, dass Kolloide unter bestimmten Randbedingungen einen erheblichen Beitrag zum Transport von Stoffen in aquatischen Systemen leisten können. Nach wie vor ist jedoch umstritten, welche Relevanz der kolloidale Transport bei einer Vielzahl von Fragestellungen hat.

In den vergangenen Jahren wurde grundsätzlich akzeptiert, dass Kolloide unter bestimmten Randbedingungen einen erheblichen Beitrag zum Transport von Stoffen in aquatischen Systemen leisten können. Nach wie vor ist jedoch umstritten, welche Relevanz der kolloidale Transport bei einer Vielzahl von Fragestellungen hat.