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  • Huotari, S.; Sahle, Ch J.; Henriquet, Ch; Al-Zein, A.; Martel, K.; Simonelli, L.; Verbeni, R.; Gonzalez, H.; Lagier, M. -C.; Ponchut, C.; Sala, M. Moretti; Krisch, M.; Monaco, G. (2017)
    An end-station for X-ray Raman scattering spectroscopy at beamline ID20 of the European Synchrotron Radiation Facility is described. This end-station is dedicated to the study of shallow core electronic excitations using non-resonant inelastic X-ray scattering. The spectrometer has 72 spherically bent analyzer crystals arranged in six modular groups of 12 analyzer crystals each for a combined maximum flexibility and large solid angle of detection. Each of the six analyzer modules houses one pixelated area detector allowing for X-ray Raman scattering based imaging and efficient separation of the desired signal from the sample and spurious scattering from the often used complicated sample environments. This new end-station provides an unprecedented instrument for X-ray Raman scattering, which is a spectroscopic tool of great interest for the study of low-energy X-ray absorption spectra in materials under insitu conditions, such as inoperando batteries and fuel cells, insitu catalytic reactions, and extreme pressure and temperature conditions.
  • Xavier, Carlton; Rusanen, Anton; Zhou, Putian; Chen, Dean; Pichelstorfer, Lukas; Pontus, Roldin; Boy, Michael (2019)
    In this study we modeled secondary organic aerosol (SOA) mass loadings from the oxidation (by O-3, OH and NO3) of five representative biogenic volatile organic compounds (BVOCs): isoprene, endocyclic bond-containing monoterpenes (alpha-pinene and limonene), exocyclic double-bond compound (beta-pinene) and a sesquiterpene (beta-caryophyllene). The simulations were designed to replicate an idealized smog chamber and oxidative flow reactors (OFRs). The Master Chemical Mechanism (MCM) together with the peroxy radical autoxidation mechanism (PRAM) were used to simulate the gas-phase chemistry. The aim of this study was to compare the potency of MCM and MCM + PRAM in predicting SOA formation. SOA yields were in good agreement with experimental values for chamber simulations when MCM + PRAM was applied, while a stand-alone MCM underpredicted the SOA yields. Compared to experimental yields, the OFR simulations using MCM + PRAM yields were in good agreement for BVOCs oxidized by both O-3 and OH. On the other hand, a stand-alone MCM underpredicted the SOA mass yields. SOA yields increased with decreasing temperatures and NO concentrations and vice versa. This highlights the limitations posed when using fixed SOA yields in a majority of global and regional models. Few compounds that play a crucial role (> 95% of mass load) in contributing to SOA mass increase (using MCM + PRAM) are identified. The results further emphasized that incorporating PRAM in conjunction with MCM does improve SOA mass yield estimation.
  • Tossavainen, Helena; Kukkurainen, Sampo; Määttä, Juha A. E.; Kähkönen, Niklas; Pihlajamaa, Tero; Hytönen, Vesa P.; Kulomaa, Markku S.; Permi, Perttu (2014)
  • Zona, Donatella; Gioli, Beniamino; Commane, Roisin; Lindaas, Jakob; Wofsy, Steven C.; Miller, Charles E.; Dinardo, Steven J.; Dengel, Sigrid; Sweeney, Colm; Karion, Anna; Chang, Rachel Y. -W.; Henderson, John M.; Murphy, Patrick C.; Goodrich, Jordan P.; Moreaux, Virginie; Liljedahl, Anna; Watts, Jennifer D.; Kimball, John S.; Lipson, David A.; Oechel, Walter C. (2016)
    Arctic terrestrial ecosystems are major global sources of methane (CH4); hence, it is important to understand the seasonal and climatic controls on CH4 emissions from these systems. Here, we report year-round CH4 emissions from Alaskan Arctic tundra eddy flux sites and regional fluxes derived from aircraft data. We find that emissions during the cold season (September to May) account for >= 50% of the annual CH4 flux, with the highest emissions from noninundated upland tundra. A major fraction of cold season emissions occur during the "zero curtain" period, when subsurface soil temperatures are poised near 0 degrees C. The zero curtain may persist longer than the growing season, and CH4 emissions are enhanced when the duration is extended by a deep thawed layer as can occur with thick snow cover. Regional scale fluxes of CH4 derived from aircraft data demonstrate the large spatial extent of late season CH4 emissions. Scaled to the circumpolar Arctic, cold season fluxes from tundra total 12 +/- 5 (95% confidence interval) Tg CH4 y(-1), similar to 25% of global emissions from extratropical wetlands, or similar to 6% of total global wetland methane emissions. The dominance of late-season emissions, sensitivity to soil environmental conditions, and importance of dry tundra are not currently simulated in most global climate models. Because Arctic warming disproportionally impacts the cold season, our results suggest that higher cold-season CH4 emissions will result from observed and predicted increases in snow thickness, active layer depth, and soil temperature, representing important positive feedbacks on climate warming.
  • Rovelli, L.; Attard, K. M.; Heppell, C. M.; Binley, A.; Trimmer, M.; Glud, R. N. (2018)
    Headwater streams are important in the carbon cycle and there is a need to better parametrize and quantify exchange of carbon-relevant gases. Thus, we characterized variability in the gas exchange coefficient (k(2)) and dissolved oxygen (O-2) gas transfer velocity (k) in two lowland headwaters of the River Avon (UK). The traditional one-station open-water method was complemented by in situ quantification of riverine sources and sinks of O-2 (i.e., groundwater inflow, photosynthesis, and respiration in both the water column and benthic compartment) enabling direct hourly estimates of k(2) at the reach-scale (similar to 150 m) without relying on the nighttime regression method. Obtained k(2) values ranged from 0.001 h(-1) to 0.600 h(-1). Average daytime k(2) were a factor two higher than values at night, likely due to diel changes in water temperature and wind. Temperature contributed up to 46% of the variability in k on an hourly scale, but clustering temperature incrementally strengthened the statistical relationship. Our analysis suggested that k variability is aligned with dominant temperature trends rather than with short-term changes. Similarly, wind correlation with k increased when clustering wind speeds in increments correspondent with dominant variations (1 m s(-1)). Time scale is thus an important consideration when resolving physical drivers of gas exchange. Mean estimates of k(600) from recent parametrizations proposed for upscaling, when applied to the settings of this study, were found to be in agreement with our independent O-2 budget assessment (within <10%), adding further support to the validity of upscaling efforts aiming at quantifying large-scale riverine gas emissions.
  • Juvela, Mika; He, Jinhua; Pattle, Katherine; Liu, Tie; Bendo, George; Eden, David J.; Feher, Orsolya; Fich, Michel; Fuller, Gary; Hirano, Naomi; Kim, Kee-Tae; Li, Di; Liu, Sheng-Yuan; Malinen, Johanna; Marshall, Douglas J.; Paradis, Deborah; Parsons, Harriet; Pelkonen, Veli-Matti; Rawlings, Mark G.; Ristorcelli, Isabelle; Samal, Manash R.; Tatematsu, Ken'ichi; Thompson, Mark; Traficante, Alessio; Wang, Ke; Ward-Thompson, Derek; Wu, Yuefang; Yi, Hee-Weon; Yoo, Hyunju (2018)
    Context. Analysis of all-sky Planck submillimetre observations and the IRAS 100 mu m data has led to the detection of a population of Galactic cold clumps. The clumps can be used to study star formation and dust properties in a wide range of Galactic environments. Aims. Our aim is to measure dust spectral energy distribution ( SED) variations as a function of the spatial scale and the wavelength. Methods. We examined the SEDs at large scales using IRAS, Planck, and Herschel data. At smaller scales, we compared JCMT/SCUBA-2 850 mu m maps with Herschel data that were filtered using the SCUBA-2 pipeline. Clumps were extracted using the Fellwalker method, and their spectra were modelled as modified blackbody functions. Results. According to IRAS and Planck data, most fields have dust colour temperatures T-C similar to 14-18K and opacity spectral index values of beta = 1.5-1.9. The clumps and cores identified in SCUBA-2 maps have T similar to 13K and similar beta values. There are some indications of the dust emission spectrum becoming flatter at wavelengths longer than 500 mu m. In fits involving Planck data, the significance is limited by the uncertainty of the corrections for CO line contamination. The fits to the SPIRE data give a median beta value that is slightly above 1.8. In the joint SPIRE and SCUBA-2 850 mu m fits, the value decreases to beta similar to 1.6. Most of the observed T-beta anticorrelation can be explained by noise. Conclusions. The typical submillimetre opacity spectral index fi of cold clumps is found to be similar to 1.7. This is above the values of diffuse clouds, but lower than in some previous studies of dense clumps. There is only tentative evidence of a T-beta anticorrelation and beta decreasing at millimetre wavelengths.
  • Kittler, Fanny; Burjack, Ina; Corradi, Chiara A. R.; Heimann, Martin; Kolle, Olaf; Merbold, Lutz; Zimov, Nikita; Zimov, Sergey; Gockede, Mathias (2016)
    Hydrologic conditions are a major controlling factor for carbon exchange processes in high-latitude ecosystems. The presence or absence of water-logged conditions can lead to significant shifts in ecosystem structure and carbon cycle processes. In this study, we compared growing season CO2 fluxes of a wet tussock tundra ecosystem from an area affected by decadal drainage to an undisturbed area on the Kolyma floodplain in northeastern Siberia. For this comparison we found the sink strength for CO2 in recent years (2013-2015) to be systematically reduced within the drained area, with a minor increase in photosynthetic uptake due to a higher abundance of shrubs outweighed by a more pronounced increase in respiration due to warmer near-surface soil layers. Still, in comparison to the strong reduction of fluxes immediately following the drainage disturbance in 2005, recent CO2 exchange with the atmosphere over this disturbed part of the tundra indicate a higher carbon turnover, and a seasonal amplitude that is comparable again to that within the control section. This indicates that the local permafrost ecosystem is capable of adapting to significantly different hydrologic conditions without losing its capacity to act as a net sink for CO2 over the growing season. The comparison of undisturbed CO2 flux rates from 2013-2015 to the period of 2002-2004 indicates that CO2 exchange with the atmosphere was intensified, with increased component fluxes (ecosystem respiration and gross primary production) over the past decade. Net changes in CO2 fluxes are dominated by a major increase in photosynthetic uptake, resulting in a stronger CO2 sink in 2013-2015. Application of a MODIS-based classification scheme to separate the growing season into four sub-seasons improved the interpretation of interannual variability by illustrating the systematic shifts in CO2 uptake patterns that have occurred in this ecosystem over the past 10 years and highlighting the important role of the late growing season for net CO2 flux budgets.
  • Lehmkuehler, Felix; Forov, Yury; Buening, Thomas; Sahle, Christoph J.; Steinke, Ingo; Julius, Karin; Buslaps, Thomas; Tolan, Metin; Hakala, Mikko; Sternemann, Christian (2016)
    We studied the structure and energetics of supercooled water by means of X-ray Raman and Compton scattering. Under supercooled conditions down to 255 K, the oxygen K-edge measured by X-ray Raman scattering suggests an increase of tetrahedral order similar to the conventional temperature effect observed in non-supercooled water. Compton profile differences indicate contributions beyond the theoretically predicted temperature effect and provide a deeper insight into local structural changes. These contributions suggest a decrease of the electron mean kinetic energy by 3.3 +/- 0.7 kJ (mol K)(-1) that cannot be modeled within established water models. Our surprising results emphasize the need for water models that capture in detail the intramolecular structural changes and quantum effects to explain this complex liquid.
  • Kittler, Fanny; Heimann, Martin; Kolle, Olaf; Zimov, Nikita; Zimov, Sergei; Gockede, Mathias (2017)
    Permafrost landscapes in northern high latitudes with their massive organic carbon stocks are an important, poorly known, component of the global carbon cycle. However, in light of future Arctic warming, the sustainability of these carbon pools is uncertain. To a large part, this is due to a limited understanding of the carbon cycle processes because of sparse observations in Arctic permafrost ecosystems. Here we present an eddy covariance data set covering more than 3 years of continuous CO2 and CH4 flux observations within a moist tussock tundra ecosystem near Chersky in north-eastern Siberia. Through parallel observations of a disturbed (drained) area and a control area nearby, we aim to evaluate the long-term effects of a persistently lowered water table on the net vertical carbon exchange budgets and the dominating biogeochemical mechanisms. Persistently drier soils trigger systematic shifts in the tundra ecosystem carbon cycle patterns. Both, uptake rates of CO2 and emissions of CH4 decreased. Year-round measurements emphasize the importance of the non-growing seasonin particular the zero-curtain period in the fallto the annual budget. Approximately 60% of the CO2 uptake in the growing season is lost during the cold seasons, while CH4 emissions during the non-growing season account for 30% of the annual budget. Year-to-year variability in temperature conditions during the late growing season was identified as the primary control of the interannual variability observed in the CO2 and CH4 fluxes.
  • Liu, Yi-Nan; Ahlgren, T.; Bukonte, L.; Nordlund, K.; Shu, Xiaolin; Yu, Yi; Li, Xiao-Chun; Lu, Guang-Hong (2013)
  • Ade, P. A. R.; Juvela, M.; Keihanen, E.; Kurki-Suonio, H.; Suur-Uski, A. -S.; Planck Collaboration (2014)
  • Nordlund, Kai; Zinkle, Steven J.; Sand, Andrea E.; Granberg, Fredric; Averback, Robert S.; Stoller, Roger E.; Suzudo, Tomoaki; Malerba, Lorenzo; Banhart, Florian; Weber, William J.; Willaime, Francois; Dudarev, Sergei L.; Simeone, David (2018)
    Scientific understanding of any kind of radiation effects starts from the primary damage, i.e. the defects that are produced right after an initial atomic displacement event initiated by a high-energy particle. In this Review, we consider the extensive experimental and computer simulation studies that have been performed over the past several decades on what the nature of the primary damage is. We review both the production of crystallographic or topological defects in materials as well as radiation mixing, i.e. the process where atoms in perfect crystallographic positions exchange positions with other ones in non-defective positions. All classes of materials except biological materials are considered. We also consider the recent effort to provide alternatives to the current international standard for quantifying this energetic particle damage, the Norgett-Robinson-Torrens displacements per atom (NRT-dpa) model for metals. We present in detail new complementary displacement production estimators ("athermal recombination corrected dpa", arc-dpa) and atomic mixing ("replacements per atom", rpa) functions that extend the NRT-dpa, and discuss their advantages and limitations. (C) 2018 The Authors. Published by Elsevier B.V.
  • Bingen, Christine; Robert, Charles E.; Stebel, Kerstin; Bruehl, Christoph; Schallock, Jennifer; Vanhellemont, Filip; Mateshvili, Nina; Hoepfner, Michael; Trickl, Thomas; Barnes, John E.; Jumelet, Julien; Vernier, Jean-Paul; Popp, Thomas; de Leeuw, Gerrit; Pinnock, Simon (2017)
    This paper presents stratospheric aerosol climate records developed in the framework of the Aerosol_cci project, one of the 14 parallel projects from the ESA Climate Change Initiative. These data records were processed from a stratospheric aerosol dataset derived from the GOMOS experiment, using an inversion algorithm optimized for aerosol retrieval, called AerGOM. They provide a suite of aerosol parameters, such as the aerosol extinction coefficient at different wavelengths in the UV-visible range.The extinction record includes the total extinction as well as separate fields for liquid sulfate aerosols and polar stratospheric clouds (PSCs). Several additional fields (PSC flag, etc.) are also provided. The resulting stratospheric aerosol dataset, which spans the whole duration of the GOMOS mission (2002-2012), was validated using different reference datasets (lidar and balloon profiles). In the present paper, the emphasis is put on the extinction records. After a thorough analysis of the original AerGOM dataset, we describe the methodology used to construct the gridded CCI-GOMOS dataset and the resulting improvements on both the AerGOM algorithm and the binning procedure, in terms of spatio-temporal resolution, coverage and data quality. The extinction datasets were validated using lidar profiles from three ground-based stations (Mauna Loa, Garmisch-Partenkirchen, Dumont d'Urville). The median difference of the CCI-GOMOS (Level 3) extinction and ground-based lidar profiles is between similar to 15% and similar to 45% in the 16-21 km altitude range, depending on the considered site and aerosol type. The CCI-GOMOS dataset was subsequently used, together with a MIPAS SO2 time series, to update a volcanic eruption inventory published previously, thus providing a more comprehensive list of eruptions for the ENVISAT period (2002-2012). The number of quantified eruptions increases from 102 to 230 in the updated inventory. This new inventory was used to simulate the evolution of the global radiative forcing by application of the EMAC chemistry-climate model. Results of this simulation improve the agreement between modelled global radiative forcing of stratospheric aerosols at about 100 hPa compared to values estimated from observations. Medium eruptions like the ones of Soufriere Hills/Rabaul (2006), Sarychev (2009) and Nabro (2011) cause a forcing change from about -0.1 W/m(2) to -0.2 W/m(2). (C) 2017 The Authors. Published by Elsevier Inc.
  • Donner, Kristian (2021)
    Time is largely a hidden variable in vision. It is the condition for seeing interesting things such as spatial forms and patterns, colours and movements in the external world, and yet is not meant to be noticed in itself. Temporal aspects of visual processing have received comparatively little attention in research. Temporal properties have been made explicit mainly in measurements of resolution and integration in simple tasks such as detection of spatially homogeneous flicker or light pulses of varying duration. Only through a mechanistic understanding of their basis in retinal photoreceptors and circuits can such measures guide modelling of natural vision in different species and illuminate functional and evolutionary trade-offs. Temporal vision research would benefit from bridging traditions that speak different languages. Towards that goal, I here review studies from the fields of human psychophysics, retinal physiology and neuroethology, with a focus on fundamental constraints set by early vision.