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Effects of atmospheric conditions on ice nucleation activity of Pseudomonas

Although ice nuclei from bacterial origin are known to be efficient at the highest temperatures known for ice catalysts, quantitative data are still needed to assess their role in cloud processes. Here we studied the effects of three typical cloud conditions (i) acidic pH (ii) NO2 and O3 exposure and (iii) UV-A exposure on the ice nucleation activity (INA) of four Pseudomonas strains. Three of the Pseudomonas syringae strains were isolated from cloud water and the phyllosphere and Pseudomonas fluorescens strain CGina-01 was isolated from Antarctic glacier ice melt. Among the three conditions tested, acidic pH caused the most significant effects on INA likely due to denaturation of the ice nucleation protein complex. Exposure to NO2 and O3 gases had no significant or only weak effects on the INA of two P. syringae strains whereas the INA of P. fluorescens CGina-01 was significantly affected. The INA of the third P. syringae strain showed variable responses to NO2 and O3 exposure. These differences in the INA of different Pseudomonas suggest that the response to atmospheric conditions could be strain-specific. After UV-A exposure, a substantial loss of viability of all four strains was observed whereas their INA decreased only slightly. This corroborates the notion that under certain conditions dead bacterial cells can maintain their INA. Overall, the negative effects of the three environmental factors on INA were more significant at the warmer temperatures. Our results suggest that in clouds where temperatures are near 0 °C, the importance of bacterial ice nucleation in precipitation processes could be reduced by some environmental factors.
Sensitivity of cirrus and mixed-phase clouds to the ice nuclei spectra in McRAS-AC: single column model simulations

The salient features of mixed-phase and ice clouds in a GCM cloud scheme are examined using the ice nucleation parameterizations of Liu and Penner (LP) and Barahona and Nenes (BN). The performance of both parameterizations was assessed in the GEOS-5 AGCM using the McRAS-AC cloud microphysics framework in single column mode. Four dimensional assimilated data from the intensive observation period of ARM TWP-ICE campaign was used to drive the fluxes and lateral forcing. Simulation experiments were established to test the impact of each parameterization in the resulting cloud fields. Three commonly used IN spectra were utilized in the BN parameterization to describe the availability of IN for heterogeneous ice nucleation. The results showed large similarities in the cirrus cloud regime between all the schemes tested, in which ice crystal concentrations were within a factor of 10 regardless of the parameterization used. In mixed-phase clouds there were some persistent differences in cloud particle number concentration and size, as well as in cloud fraction, ice water mixing ratio, and ice water path. Contact freezing in the simulated mixed-phase clouds contributed to the effective transfer of liquid to ice, so that on average, the clouds were fully glaciated at T 260 K, irrespective of the ice nucleation parameterization used. Comparison of simulated ice water path to available satellite derived observations were also performed, finding that all the schemes tested with the BN parameterization predicted average values of IWP within ±15% of the observations.
Sea-spray geoengineering in the HadGEM2-ES earth-system model: radiative impact and climate response

The radiative impact and climate effects of geoengineering using sea-spray aerosols have been investigated in the HadGEM2-ES Earth system model using a fully prognostic treatment of the sea-spray aerosols and also including their direct radiative effect. Two different emission patterns were considered, one to maximise the direct effect in clear skies, the other to maximise the indirect effects of the sea-spray on low clouds; in both cases the emissions were limited to 10% of the ocean area. While the direct effect was found to be significant, the indirect effects on clouds were much more effective in reducing global mean temperature as well as having less of an impact on global mean precipitation per unit temperature reduction. The impact on the distribution of precipitation was found to be similar in character, but less in degree, to that simulated by a previous study using a much simpler treatment of this geoengineering process.
Artificial primary marine aerosol production: a laboratory study with varying water temperature, salinity, and succinic acid concentration

Primary marine aerosols are an important component of the climate system, especially in the remote marine environment. With diminishing sea-ice cover, better understanding of the role of sea spray aerosol on climate in the polar regions is required. As for Arctic Ocean water, laboratory experiments with NaCl water confirm that a few degrees change in the water temperature (Tw) gives a large change in the number of primary particles. Small particles with a dry diameter between 0.01 μm and 0.25 μm dominate the aerosol number density, but their relative dominance decreases with increasing water temperature from 0 °C where they represent 85–90% of the total aerosol number to 10 °C, where they represent 60–70% of the total aerosol number. This effect is most likely related to a change in physical properties and not to modification of sea water chemistry. A change of salinity between 15 g kg−1 and 35 g kg−1 did not influence the shape of a particle number size distribution. Although the magnitude of the size distribution for a water temperature change between 0 °C and 16 °C changed, the shape did not. An experiment where succinic acid was added to a NaCl water solution showed, that the number concentration of particles with 0.010 μm < Dp < 4.5 μm decreased on average by 10% when the succinic acid concentration in NaCl water at a water temperature of 0 °C was increased from 0 μmol L−1 to 94 μmol L−1. A shift to larger sizes in the particle number size distribution is observed from pure NaCl water to Arctic Ocean water. This is likely a consequence of organics and different inorganic salts present in Arctic Ocean water in addition to the NaCl.
Overview of the 2007 and 2008 campaigns conducted as part of the Greenland Summit Halogen-HOx Experiment (GSHOX)

From 10 May through 17 June 2007 and 6 June through 9 July 2008 intensive sampling campaigns at Summit, Greenland confirmed that active bromine chemistry is occurring in and above the snow pack at the highest part of the Greenland ice sheet (72°36´ N, 38°25´ W and 3.2 km above sea level). Direct measurements found BrO and soluble gas phase Br− mixing ratios in the low pptv range on many days (maxima < 10 pptv). Conversion of up to 200 pg m−3 of gaseous elemental mercury (GEM) to reactive gaseous mercury (RGM) and enhanced OH relative to HO2 plus RO2 confirm that active bromine chemistry is impacting chemical cycles even at such low abundances of reactive bromine species. However, it does not appear that Bry chemistry can fully account for observed perturbations to HOx partitioning, suggesting unknown additional chemical processes may be important in this unique environment, or that our understanding of coupled NOx-HOx-Bry chemistry above sunlit polar snow is incomplete. Rapid transport from the north Atlantic marine boundary layer occasionally caused enhanced BrO at Summit (just two such events observed during the 12 weeks of sampling over the two seasons). In general observed reactive bromine was linked to activation of bromide (Br−) in, and release of reactive bromine from, the snowpack. A coupled snow-atmosphere model simulated observed NO and BrO at Summit during a three day interval when winds were weak. The source of Br− in surface and near surface snow at Summit is not entirely clear, but concentrations were observed to increase when stronger vertical mixing brought free tropospheric air to the surface. Reactive Bry mixing ratios above the snow often increased in the day or two following increases in snow concentration, but this response was not consistent. On seasonal time scales concentrations of Br− in snow and reactive bromine in the air were directly related.
Mid-tropospheric δD observations from IASI/MetOp at high spatial and temporal resolution

In this paper we retrieve atmospheric HDO, H2O concentrations and their ratio δD from IASI radiances spectra. Our method relies on an existing radiative transfer model (Atmosphit) and an optimal estimation inversion scheme, but goes further than our previous work by explicitly considering correlations between the two species. A global HDO and H2O a priori profile together with a covariance matrix were built from daily LMDz-iso model simulations of HDO and H2O profiles over the whole globe and a whole year. The retrieval parameters are described and characterized in terms of errors. We show that IASI is mostly sensitive to δD in the middle troposphere and allows retrieving δD for an integrated 3–6 km column with an error of 38&permil; on an individual measurement basis. We examine the performance of the retrieval to capture the temporal (seasonal and short-term) and spatial variations of δD for one year of measurement at two dedicated sites (Darwin and Izaña) and a latitudinal band from −60° to 60° for a 15 day period in January. We report a generally good agreement between IASI and the model and indicate the capabilities of IASI to reproduce the large scale variations of δD (seasonal cycle and latitudinal gradient) with good accuracy. In particular, we show that there is no systematic significant bias in the retrieved δD values in comparison with the model, and that the retrieved variability is similar to the one in the model even though there are certain local differences. Moreover, the noticeable differences between IASI and the model are briefly examined and suggest modeling issues instead of retrieval effects. Finally, the results further reveal the unprecedented capabilities of IASI to capture short-term variations in δD, highlighting the added value of the sounder for monitoring hydrological processes.
The effect of model spatial resolution on Secondary Organic Aerosol predictions: a case study at Whistler, BC, Canada

A large fraction of submicron aerosol mass throughout the continental boundary layer consists of secondary organic aerosol (SOA) mass. As such, the ability of chemical transport models to accurately predict continental boundary layer aerosol greatly depends on their ability to predict SOA. Although there has been much recent effort to better describe SOA formation mechanisms in models, little attention has been paid to the effects of model spatial resolution on SOA predictions. The Whistler Aerosol and Cloud Study (WACS 2010), held between 22 June and 28 July 2010 and conducted at Whistler, BC, Canada provides a unique data set for testing simulated SOA predictions. The study consisted of intensive measurements of atmospheric trace gases and particles at several locations strongly influenced by biogenic sources in the region. We test the ability of the global chemical transport model GEOS-Chem to predict the aerosol concentrations during this event and throughout the campaign. Simulations were performed using three different resolutions of the model: 4° × 5° , 2° × 2.5° and 0.5° × 0.667°. Predictions of organic aerosol concentrations at Whistler were greatly dependent on the resolution; the 4° × 5° version of the model significantly under predicts organic aerosol, while the 2° × 2.5° and 0.5° × 0.667° versions are much more closely correlated with measurements. In addition, we performed a comparison between the 3 versions of the model across North America. Comparison simulations were run for both a summer case (July) and Winter case (January). For the summer case, 0.5° × 0.667° simulations predicted on average 19% more SOA than 2° × 2.5° and 32% more than 4° × 5° . For the winter case, the 0.5° × 0.667° simulations predicted 8% more SOA than the 2° × 2.5° and 23% more than the 4° × 5°. This increase in SOA with resolution is largely due to sub-grid variability of organic aerosol (OA) that leads to an increase in the partitioning of secondary organic matter to the aerosol phase at higher resolutions. SOA concentrations were further increased because the shift of secondary organic gases to SOA at higher resolutions increased the lifetime of secondary organic matter (secondary organic gases have a shorter deposition lifetime than SOA in the model). SOA precursor emissions also have smaller, but non-negligible, changes with resolution due to non-linear inputs to the MEGAN biogenic emissions scheme. These results suggest that a portion of the traditional under-prediction of SOA by global models may be due to the effects of coarse grid resolution.
Size distribution of particulate mercury in marine and coastal atmospheres

A study was conducted to determine the size distribution of particulate mercury (HgP) at a marine and coastal site, and to compare the seasonal variability at both sites. Data was collected during summer 2009 and 2010, winter 2010, and spring 2010. Two cascade impactors were used to collect HgP in ten size fractions ranging from > 10 μm to < 0.4 μm. During summer 2009, HgP was found mainly (50–60%) in coarse fractions, 1.1 to 5.8 μm, composed of sea salt particles at both our coastal site (Thompson Farm) and marine site (Appledore Island). In winter, HgP at Thompson Farm was dominated (65%) by fine particles, while in spring and summer 2010, at both sites, HgP was distributed across the coarse and fine fractions (40% each). Using bulk filters to collect total HgP, we show a diurnal cycle that matches that of gaseous elemental mercury. Finally, dry deposition rates of HgP were calculated to be 1.7–2.8 ng m−2 day−1 in the summer, 4.6 ng m−2 day−1 in the winter, and 2.5 ng m−2 day−1 in the spring.
A multi-instrument comparison of integrated water vapour measurements at a high latitude site

We compare measurements of integrated water vapour (IWV) over a subarctic site (Kiruna, Northern Sweden) from five different sensors and retrieval methods: Radiosondes, Global Positioning System (GPS), ground-based Fourier-transform infrared (FTIR) spectrometer, ground-based microwave radiometer, and satellite-based microwave radiometer (AMSU-B). Additionally, we compare also to ERA-Interim model reanalysis data. GPS-based IWV data have the highest temporal coverage and resolution and are chosen as reference data set. All datasets agree reasonably well, but the ground-based microwave instrument only if the data are cloud-filtered. We also address two issues that are general for such intercomparison studies, the impact of different lower altitude limits for the IWV integration, and the impact of representativeness error. We develop methods for correcting for the former, and estimating the random error contribution of the latter. A literature survey reveals that reported systematic differences between different techniques are study-dependent and show no overall consistent pattern. Further improving the absolute accuracy of IWV measurements and providing climate-quality time series therefore remain challenging problems.
A fast SEVIRI simulator for quantifying retrieval uncertainties in the CM SAF cloud physical property algorithm

The uncertainties in the cloud physical properties derived from satellite observations make it difficult to interpret model evaluation studies. In this paper, the uncertainties in the cloud water path (CWP) retrievals derived with the cloud physical properties retrieval algorithm (CPP) of the climate monitoring satellite application facility (CM SAF) are investigated. To this end, a numerical simulator of MSG-SEVIRI observations has been developed that calculates the reflectances at 0.64 and 1.63 μm for a wide range of cloud parameter values, satellite viewing geometries and surface albedos using a plane-parallel radiative transfer model. The reflectances thus obtained are used as input to CPP, and the retrieved values of CWP are compared to the original input of the simulator. Cloud parameters considered in this paper refer to e.g. sub-pixel broken clouds and the simultaneous occurrence of ice and liquid water clouds within one pixel. These configurations are not represented in the CPP algorithm and as such the associated retrieval uncertainties are potentially substantial. It is shown that the CWP retrievals are very sensitive to the assumptions made in the CPP code. The CWP retrieval errors are generally small for unbroken single-layer clouds with COT > 10, with retrieval errors of ~3% for liquid water clouds to ~10% for ice clouds. In a multi-layer cloud, when both liquid water and ice clouds are present in a pixel, the CWP retrieval errors increase dramatically; depending on the cloud, this can lead to uncertainties of 40–80%. CWP retrievals also become more uncertain when the cloud does not cover the entire pixel, leading to errors of ~50% for cloud fractions of 0.75 and even larger errors for smaller cloud fractions. Thus, the satellite retrieval of cloud physical properties of broken clouds as well as multi-layer clouds is complicated by inherent difficulties, and the proper interpretation of such retrievals requires extra care.