Effects of deposit-feeding bivalve (Macomona liliana) density on intertidal sediment stability

Effects of macrofaunal feeding and bioturbation on intertidal sediment stability (u*crit) were investigated by manipulating density (0-3 x ambient) of the facultative deposit-feeding wedge shell (Macomona liliana) on the Tuapiro sandflat in Tauranga Harbour, New Zealand. Sediment stability increased up to 200% with decreasing M. liliana density and this was correlated with greater sediment microalgal biomass and mucilage content. The change in stability occurred despite homogeneity of grain size amongst experimental treatments, highlighting the importance of macrofaunal-microbial relationships in determining estuarine sediment erodibility

Modeled global effects of airborne desert dust on air quality and premature mortality

Fine particulate matter is one of the most important factors contributing to air pollution. Epidemiological studies have related increased levels of atmospheric particulate matter to premature human mortality caused by cardiopulmonary disease and lung cancer. However, a limited number of investigations have focused on the contribution of airborne desert dust particles. Here we assess the effects of dust particles with an aerodynamic diameter smaller than 2.5 μm (DU_2.5) on human mortality for the year 2005. We used the EMAC atmospheric–chemistry general circulation model at high resolution to simulate global atmospheric dust concentrations. We applied a health impact function to estimate premature mortality for the global population of 30 yr and older, using parameters from epidemiological studies. We estimate a global cardiopulmonary mortality of about 402 000 in 2005. The associated years of life lost are about 3.47 million per year. We estimate the global fraction of the cardiopulmonary deaths caused by atmospheric desert dust to be about 1.8%, though in the 20 countries most affected by dust this is much higher, about 15–50%. These countries are primarily found in the so-called "dust belt" from North Africa across the Middle East and South Asia to East Asi

Model simulations and aircraft measurements of vertical, seasonal and latitudinal O3 and CO distributions over Europe

During a series of 8 measurement campaigns within the SPURT project (2001-2003), vertical profiles of CO and O3 have been obtained at subtropical, middle and high latitudes over western Europe, covering the troposphere and lowermost stratosphere up to ~14 km altitude during all seasons. The seasonal and latitudinal variation of the measured trace gas profiles are compared to simulations with the chemical transport model MATCH. In the troposphere reasonable agreement between observations and model predictions is achieved for CO and O3, in particular at subtropical and mid-latitudes, while the model overestimates (underestimates) CO (O3 in the lowermost stratosphere particularly at high latitudes, indicating too strong simulated bi-directional exchange across the tropopause. By the use of tagged tracers in the model, long-range transport of Asian air masses is identified as the dominant source of CO pollution over Europe in the free troposphere

A hierarchical time-splitting approach for solving finite-time optimal control problems

The self-cleaning or oxidation capacity of the atmosphere is principally controlled by hydroxyl (OH) radicals in the troposphere. Hydroxyl has primary (P) and secondary (S) sources, the former mainly through the photodissociation of ozone, the latter through OH recycling in radical reaction chains. We used the recent Mainz Organics Mechanism (MOM) to advance volatile organic carbon (VOC) chemistry in the general circulation model EMAC (ECHAM/MESSy Atmospheric Chemistry) and show that S is larger than previously assumed. By including emissions of a large number of primary VOC, and accounting for their complete breakdown and intermediate products, MOM is mass-conserving and calculates substantially higher OH reactivity from VOC oxidation compared to predecessor models. Whereas previously P and S were found to be of similar magnitude, the present work indicates that S may be twice as large, mostly due to OH recycling in the free troposphere. Further, we find that nighttime OH formation may be significant in the polluted subtropical boundary layer in summer. With a mean OH recycling probability of about 67 %, global OH is buffered and not sensitive to perturbations by natural or anthropogenic emission changes. Complementary primary and secondary OH formation mechanisms in pristine and polluted environments in the continental and marine troposphere, connected through long-range transport of O3, can maintain stable global OH levels

A two-channel, Thermal Dissociation Cavity-Ringdown Spectrometer for the detection of ambient NO2, RO2NO2 and RONO2

Creative Commons Attribution License 3.0We describe a thermal dissociation cavity ring-down spectrometer (TD-CRDS) for measurement of ambient NO2, total peroxy nitrates (ΣPNs) and total alkyl nitrates (ΣANs). The spectrometer has two separate cavities operating at  ∼  405.2 and 408.5 nm. One cavity (reference) samples NO2 continuously from an inlet at ambient temperature, the other samples sequentially from an inlet at 473 K in which PNs are converted to NO2 or from an inlet at 723 K in which both PNs and ANs are converted to NO2, difference signals being used to derive mixing ratios of ΣPNs and ΣANs. We describe an extensive set of laboratory experiments and numerical simulations to characterise the fate of organic radicals in the hot inlets and cavity and derive correction factors to account for the bias resulting from the interaction of peroxy radicals with ambient NO and NO2. Finally, we present the first measurements and comparison with other instruments during a field campaign, outline the limitations of the present instrument and provide an outlook for future improvements.Publication funded by the Max Planck Societ

Improved simulation of isoprene oxidation chemistry with the ECHAM5/MESSy chemistry-climate model: lessons from the GABRIEL airborne field campaign

The GABRIEL airborne field measurement campaign, conducted over the Guyanas in October 2005, produced measurements of hydroxyl radical (OH) concentration which are significantly higher than can be simulated using current generation models of atmospheric chemistry. Based on the hypothesis that this "missing OH" is due to an as-yet undiscovered mechanism for recycling OH during the oxidation chain of isoprene, we determine that an OH recycling of about 40–50% (compared with 5–10% in current generation isoprene oxidation mechanisms) is necessary in order for our modelled OH to approach the lower error bounds of the OH observed during GABRIEL. Such a large amount of OH in our model leads to unrealistically low mixing ratios of isoprene. In order for our modelled isoprene mixing ratios to match those observed during the campaign, we also require that the effective rate constant for the reaction of isoprene with OH be reduced by about 50% compared with the lower bound of the range recommended by IUPAC. We show that a reasonable explanation for this lower effective rate constant could be the segregation of isoprene and OH in the mixed layer. Our modelling results are consistent with a global, annual isoprene source of about 500 Tg(C) yr<sup>−1</sup>, allowing experimentally derived and established isoprene flux rates to be reconciled with global models

Description and evaluation of GMXe: a new aerosol submodel for global simulations (v1)

We present a new aerosol microphysics and gas aerosol partitioning submodel (Global Modal-aerosol eXtension, GMXe) implemented within the ECHAM/MESSy Atmospheric Chemistry model (EMAC, version 1.8). The submodel is computationally efficient and is suitable for medium to long term simulations with global and regional models. The aerosol size distribution is treated using 7 log-normal modes and has the same microphysical core as the M7 submodel (Vignati et al., 2004). <br><br> The main developments in this work are: (i) the extension of the aerosol emission routines and the M7 microphysics, so that an increased (and variable) number of aerosol species can be treated (new species include sodium and chloride, and potentially magnesium, calcium, and potassium), (ii) the coupling of the aerosol microphysics to a choice of treatments of gas/aerosol partitioning to allow the treatment of semi-volatile aerosol, and, (iii) the implementation and evaluation of the developed submodel within the EMAC model of atmospheric chemistry. <br><br> Simulated concentrations of black carbon, particulate organic matter, dust, sea spray, sulfate and ammonium aerosol are shown to be in good agreement with observations (for all species at least 40% of modeled values are within a factor of 2 of the observations). The distribution of nitrate aerosol is compared to observations in both clean and polluted regions. Concentrations in polluted continental regions are simulated quite well, but there is a general tendency to overestimate nitrate, particularly in coastal regions (geometric mean of modelled values/geometric mean of observed data ≈2). In all regions considered more than 40% of nitrate concentrations are within a factor of two of the observations. Marine nitrate concentrations are well captured with 96% of modeled values within a factor of 2 of the observations

Reactive intermediates revealed in secondary organic aerosol formation from isoprene

Isoprene is a significant source of atmospheric organic aerosol; however, the oxidation pathways that lead to secondary organic aerosol (SOA) have remained elusive. Here, we identify the role of two key reactive intermediates, epoxydiols of isoprene (IEPOX = β-IEPOX + δ-IEPOX) and methacryloylperoxynitrate (MPAN), which are formed during isoprene oxidation under low- and high-NO_x conditions, respectively. Isoprene low-NO_x SOA is enhanced in the presence of acidified sulfate seed aerosol (mass yield 28.6%) over that in the presence of neutral aerosol (mass yield 1.3%). Increased uptake of IEPOX by acid-catalyzed particle-phase reactions is shown to explain this enhancement. Under high-NO_x conditions, isoprene SOA formation occurs through oxidation of its second-generation product, MPAN. The similarity of the composition of SOA formed from the photooxidation of MPAN to that formed from isoprene and methacrolein demonstrates the role of MPAN in the formation of isoprene high-NO_x SOA. Reactions of IEPOX and MPAN in the presence of anthropogenic pollutants (i.e., acidic aerosol produced from the oxidation of SO_2 and NO_2, respectively) could be a substantial source of “missing urban SOA” not included in current atmospheric models

Aerosol absorption over the clear-sky oceans deduced from POLDER-1 and AERONET observations

We estimate aerosol absorption over the clear-sky oceans using aerosol geophysical products from POLDER-1 space measurements and absorption properties from ground-based AERONET measurements. Our best estimate is 2.5 Wm-2 averaged over the 8-month lifetime of POLDER-1. Low and high absorption estimates are 2.2 and 3.1 Wm-2 based on the variability in aerosol single scattering albedo observed by AERONET. Main sources of uncertainties are the discrimation of the aerosol type from satellite measurements, and potential clear-sky bias induced by the cloud-screening procedure