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1.
Phys Chem Chem Phys ; 24(43): 26458-26465, 2022 Nov 09.
Artículo en Inglés | MEDLINE | ID: mdl-36305893

RESUMEN

X-Ray as well as electron diffraction are powerful tools for structure determination of molecules. Studies on randomly oriented molecules in the gas phase address cases in which molecular crystals cannot be generated or the interaction-free molecular structure is to be addressed. Such studies usually yield partial geometrical information, such as interatomic distances. Here, we present a complementary approach, which allows obtaining insight into the structure, handedness, and even detailed geometrical features of molecules in the gas phase. Our approach combines Coulomb explosion imaging, the information that is encoded in the molecular-frame diffraction pattern of core-shell photoelectrons and ab initio computations. Using a loop-like analysis scheme, we are able to deduce specific molecular coordinates with sensitivity even to the handedness of chiral molecules and the positions of individual atoms, e.g., protons.


Asunto(s)
Electrones , Estructura Molecular , Estereoisomerismo , Rayos X
2.
Phys Chem Chem Phys ; 23(32): 17248-17258, 2021 Aug 28.
Artículo en Inglés | MEDLINE | ID: mdl-34346440

RESUMEN

The photoelectron circular dichroism (PECD) of the O 1s-photoelectrons of trifluoromethyloxirane (TFMOx) is studied experimentally and theoretically for different photoelectron kinetic energies. The experiments were performed employing circularly polarized synchrotron radiation and coincident electron and fragment ion detection using cold target recoil ion momentum spectroscopy. The corresponding calculations were performed by means of the single center method within the relaxed-core Hartree-Fock approximation. We concentrate on the energy dependence of the differential PECD of uniaxially oriented TFMOx molecules, which is accessible through the employed coincident detection. We also compare the results for the differential PECD of TFMOx to those obtained for the equivalent fragmentation channel and similar photoelectron kinetic energy of methyloxirane (MOx), studied in our previous work. Thereby, we investigate the influence of the substitution of the methyl group by the trifluoromethyl group at the chiral center on the molecular chiral response. Finally, the presently obtained angular distribution parameters are compared to those available in the literature.

3.
Phys Rev Lett ; 125(16): 163201, 2020 Oct 16.
Artículo en Inglés | MEDLINE | ID: mdl-33124863

RESUMEN

We report on a multiparticle coincidence experiment performed at the European X-ray Free-Electron Laser at the Small Quantum Systems instrument using a COLTRIMS reaction microscope. By measuring two ions and two electrons in coincidence, we investigate double core-hole generation in O_{2} molecules in the gas phase. Single-site and two-site double core holes have been identified and their molecular-frame electron angular distributions have been obtained for a breakup of the oxygen molecule into two doubly charged ions. The measured distributions are compared to results of calculations performed within the frozen- and relaxed-core Hartree-Fock approximations.

4.
Conserv Biol ; 29(4): 1017-1027, 2015 Aug.
Artículo en Inglés | MEDLINE | ID: mdl-25997361

RESUMEN

Farmland abandonment takes place across the world due to socio-economic and ecological drivers. In Europe agricultural and environmental policies aim to prevent abandonment and halt ecological succession. Ecological rewilding has been recently proposed as an alternative strategy. We developed a framework to assess opportunities for rewilding across different dimensions of wilderness in Europe. We mapped artificial light, human accessibility based on transport infrastructure, proportion of harvested primary productivity (i.e., ecosystem productivity appropriated by humans through agriculture or forestry), and deviation from potential natural vegetation in areas projected to be abandoned by 2040. At the continental level, the levels of artificial light were low and the deviation from potential natural vegetation was high in areas of abandonment. The relative importance of wilderness metrics differed regionally and was strongly connected to local environmental and socio-economic contexts. Large areas of projected abandonment were often located in or around Natura 2000 sites. Based on these results, we argue that management should be tailored to restore the aspects of wilderness that are lacking in each region. There are many remaining challenges regarding biodiversity in Europe, but megafauna species are already recovering. To further potentiate large-scale rewilding, Natura 2000 management would need to incorporate rewilding approaches. Our framework can be applied to assessing rewilding opportunities and challenges in other world regions, and our results could guide redirection of subsidies to manage social-ecological systems.


Mapeo de Oportunidades y Retos para el Retorno de la Vida Silvestre Resumen El abandono de tierras agrícolas ocurre en todo el mundo debido a factores socio-económicos y ecológicos. En Europa, las políticas ambientales y agrícolas tienen el objetivo de prevenir el abandono y frenar la sucesión ecológica. La reintroducción o el retorno de la vida silvestre ("rewilding") representa una estrategia alternativa a esto. Desarrollamos un marco de trabajo para evaluar las oportunidades de reintroducción en diferentes dimensiones de naturaleza a lo largo de Europa. Mapeamos la luz artificial, la accesibilidad para humanos con base en la infraestructura de transporte, la proporción de productividad primaria (es decir, la productividad del ecosistema incautado por los humanos por medio de la agricultura o la silvicultura) y la divergencia de vegetación natural potencial en áreas que se proyecta estarán abandonadas para el 2040. A nivel continental, los niveles de luz artificial fueron bajos y la divergencia de vegetación natural potencial fue alta en las áreas de abandono. La importancia relativa de las medidas de naturaleza difirió regionalmente y estuvieron conectadas fuertemente a los contextos ambientales y socio-económicos locales. Las grandes áreas de abandono proyectado estuvieron localizadas frecuentemente en o alrededor de sitios Natura 2000. Con base en estos resultados, argumentamos que el manejo debería ser fabricado para restaurar los aspectos de la naturaleza que son carentes en cada región. Todavía quedan muchos obstáculos con respecto a la biodiversidad en Europa, pero las especies de megafauna ya se están recuperando. Para potenciar aún más la reintroducción a gran escala, el manejo de Natura 2000 necesitaría incorporar estrategias de reintroducción. Nuestro marco de trabajo puede aplicarse a la evaluación de las oportunidades de reintroducción y a los obstáculos en otras regiones del mundo, y nuestros resultados pueden guiar la redirección de los subsidios para manejar los sistemas socio-ecológicos.


Asunto(s)
Biodiversidad , Conservación de los Recursos Naturales/métodos , Ecosistema , Agricultura , Conservación de los Recursos Naturales/legislación & jurisprudencia , Política Ambiental/legislación & jurisprudencia , Europa (Continente) , Vida Silvestre
5.
Sci Rep ; 12(1): 14387, 2022 08 23.
Artículo en Inglés | MEDLINE | ID: mdl-35999340

RESUMEN

The axonal cytoskeleton is organized in a highly periodic structure, the membrane-associated periodic skeleton (MPS), which is essential to maintain the structure and function of the axon. Here, we use stimulated emission depletion microscopy of primary rat cortical neurons in microfluidic chambers to analyze the temporal and spatial sequence of MPS formation at the distal end of growing axons and during regeneration after axotomy. We demonstrate that the MPS does not extend continuously into the growing axon but develops from patches of periodic ßII-spectrin arrangements that grow and coalesce into a continuous scaffold. We estimate that the underlying sequence of assembly, elongation, and subsequent coalescence of periodic ßII-spectrin patches takes around 15 h. Strikingly, we find that development of the MPS occurs faster in regenerating axons after axotomy and note marked differences in the morphology of the growth cone and adjacent axonal regions between regenerating and unlesioned axons. Moreover, we find that inhibition of the spectrin-cleaving enzyme calpain accelerates MPS formation in regenerating axons and increases the number of regenerating axons after axotomy. Taken together, we provide here a detailed nanoscale analysis of MPS development in growing axons.


Asunto(s)
Citoesqueleto , Espectrina , Animales , Axones/fisiología , Conos de Crecimiento , Regeneración Nerviosa/fisiología , Ratas , Regeneración
6.
Sci Rep ; 11(1): 19073, 2021 09 24.
Artículo en Inglés | MEDLINE | ID: mdl-34561517

RESUMEN

Citizen science platforms are quickly accumulating hundreds of millions of biodiversity observations around the world annually. Quantifying and correcting for the biases in citizen science datasets remains an important first step before these data are used to address ecological questions and monitor biodiversity. One source of potential bias among datasets is the difference between those citizen science programs that have unstructured protocols and those that have semi-structured or structured protocols for submitting observations. To quantify biases in an unstructured citizen science platform, we contrasted bird observations from the unstructured iNaturalist platform with that from a semi-structured citizen science platform-eBird-for the continental United States. We tested whether four traits of species (body size, commonness, flock size, and color) predicted if a species was under- or over-represented in the unstructured dataset compared with the semi-structured dataset. We found strong evidence that large-bodied birds were over-represented in the unstructured citizen science dataset; moderate evidence that common species were over-represented in the unstructured dataset; strong evidence that species in large groups were over-represented; and no evidence that colorful species were over-represented in unstructured citizen science data. Our results suggest that biases exist in unstructured citizen science data when compared with semi-structured data, likely as a result of the detectability of a species and the inherent recording process. Importantly, in programs like iNaturalist the detectability process is two-fold-first, an individual organism needs to be detected, and second, it needs to be photographed, which is likely easier for many large-bodied species. Our results indicate that caution is warranted when using unstructured citizen science data in ecological modelling, and highlight body size as a fundamental trait that can be used as a covariate for modelling opportunistic species occurrence records, representing the detectability or identifiability in unstructured citizen science datasets. Future research in this space should continue to focus on quantifying and documenting biases in citizen science data, and expand our research by including structured citizen science data to understand how biases differ among unstructured, semi-structured, and structured citizen science platforms.

7.
Environ Int ; 150: 106420, 2021 05.
Artículo en Inglés | MEDLINE | ID: mdl-33556912

RESUMEN

Biodiversity is a cornerstone of human health and well-being. However, while evidence of the contributions of nature to human health is rapidly building, research into how biodiversity relates to human health remains limited in important respects. In particular, a better mechanistic understanding of the range of pathways through which biodiversity can influence human health is needed. These pathways relate to both psychological and social processes as well as biophysical processes. Building on evidence from across the natural, social and health sciences, we present a conceptual framework organizing the pathways linking biodiversity to human health. Four domains of pathways-both beneficial as well as harmful-link biodiversity with human health: (i) reducing harm (e.g. provision of medicines, decreasing exposure to air and noise pollution); (ii) restoring capacities (e.g. attention restoration, stress reduction); (iii) building capacities (e.g. promoting physical activity, transcendent experiences); and (iv) causing harm (e.g. dangerous wildlife, zoonotic diseases, allergens). We discuss how to test components of the biodiversity-health framework with available analytical approaches and existing datasets. In a world with accelerating declines in biodiversity, profound land-use change, and an increase in non-communicable and zoonotic diseases globally, greater understanding of these pathways can reinforce biodiversity conservation as a strategy for the promotion of health for both people and nature. We conclude by identifying research avenues and recommendations for policy and practice to foster biodiversity-focused public health actions.


Asunto(s)
Biodiversidad , Zoonosis , Animales , Conservación de los Recursos Naturales , Ecosistema , Ejercicio Físico , Humanos , Salud Pública
8.
ChemistryOpen ; 9(3): 271, 2020 03.
Artículo en Inglés | MEDLINE | ID: mdl-32140380

RESUMEN

Invited this month's cover picture are the groups of Professor Michael Mehring and Professor Marc Armbrüster at Chemnitz University of Technology. The cover pictures shows a graffiti displaying a distinctive part of the city center of the town. The artwork is oversprayed with the letters "TUC" (Technische Universität Chemnitz) using an bismuth oxido cluster from solution to obtain a yellow semiconductor coating of bismuth oxide, used to degrade the medicinal drug ethinyl estradiol under visible light irradiation. Read the full text of their Full Paper at https://doi.org/10.1002/open.201900323.

9.
ChemistryOpen ; 9(3): 277-284, 2020 03.
Artículo en Inglés | MEDLINE | ID: mdl-32154048

RESUMEN

Thin coatings of Bi2O3 were deposited on glass substrates by ultrasonic spray coating of THF solutions of the molecular precursor [Bi38O45(OMc)24(DMSO)9] ⋅ 2DMSO ⋅ 7H2O (OMc=O2CC3H5) followed by hydrolysis and subsequent annealing. Depending on the synthetic protocol, the bismuth oxido cluster was transformed into either α- or ß-Bi2O3. The as-synthesized Bi2O3 coatings were characterized by powder X-ray diffraction (PXRD), thickness measurements, diffuse reflectance UV-Vis spectroscopy (DRS), photoluminescence (PL) spectroscopy, Raman spectroscopy and scanning electron microscopy (SEM). The thin coatings (thickness: 5-16 µm) were compared with regard to their performance in photocatalytic rhodamine B (RhB) decomposition under visible light irradiation. The ß-Bi2O3 coatings, that showed the highest photocatalytic activity, were used for the photocatalytic decomposition of other pollutants such as triclosan and ethinyl estradiol. In addition, the interplay between the photooxidation that is induced by the excitation of the catalyst using visible light and the photosensitized decomposition pathway was studied by degradation experiments of aqueous rhodamine B solutions using ß-Bi2O3 coatings.

10.
Appl Opt ; 42(12): 2052-62, 2003 Apr 20.
Artículo en Inglés | MEDLINE | ID: mdl-12716145

RESUMEN

The influence of pressure on laser-induced incandescence (LII) is investigated systematically in premixed, laminar sooting ethylene/air flames at 1-15 bar with wavelength-, laser fluence-, and time-resolved detection. In the investigated pressure range the LII signal decay rate is proportional to pressure. This observation is consistent with the prediction of heat-transfer models in the free-molecular regime. Pressure does not systematically affect the relationship between LII signal and laser fluence. With appropriate detection timing the pressure influence on LII signal's proportionality to soot volume faction obtained by extinction measurements is only minor compared with the variation observed in different flames at fixed pressures. The implications for particle sizing and soot volume fraction measurements using LII techniques at elevated pressures are discussed.

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