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Organic matter matters for ice nuclei of agricultural soil origin

Heterogeneous ice nucleation is a crucial process for forming ice-containing clouds and subsequent ice-induced precipitation. The importance for ice nucleation by airborne desert soil dusts composed predominantly of minerals is widely acknowledged. However, the potential influence of agricultural soil dusts on ice nucleation has been poorly recognized, despite recent estimates that they may account for up to 20–25% of the global atmospheric dust load. We have conducted freezing experiments with various dusts, including agricultural soil dusts derived from the largest dust-source region in North America. Here we show evidence for the significant role of soil organic matter (SOM) in particles acting as ice nuclei (IN) under mixed-phase cloud conditions. We find that the ice-nucleating ability of the agricultural soil dusts is similar to that of desert soil dusts, but is clearly reduced after either H2O2 digestion or dry heating to 300 °C. In addition, based on chemical composition analysis, we demonstrate that organic-rich particles are more important than mineral particles for the ice-nucleating ability of the agricultural soil dusts at temperatures warmer than about −36 °C. Finally, we suggest that such organic-rich particles of agricultural origin (namely, SOM particles) may contribute significantly to the ubiquity of organic-rich IN in the global atmosphere.
Uncertainties in assessing the environmental impact of amine emissions from a CO2 capture plant

In this study, a new model framework that couples the atmospheric chemistry transport model system Weather Research and Forecasting–European Monitoring and Evaluation Programme (WRF-EMEP) and the multimedia fugacity level III model was used to assess the environmental impact of in-air amine emissions from post-combustion carbon dioxide capture. The modelling framework was applied to a typical carbon capture plant artificially placed at Mongstad, on the west coast of Norway. The study region is characterized by high precipitation amounts, relatively few sunshine hours, predominantly westerly winds from the North Atlantic and complex topography. Mongstad can be considered as moderately polluted due to refinery activities. WRF-EMEP enables a detailed treatment of amine chemistry in addition to atmospheric transport and deposition. Deposition fluxes of WRF-EMEP simulations were used as input to the fugacity model in order to derive concentrations of nitramines and nitrosamine in lake water. Predicted concentrations of nitramines and nitrosamines in ground-level air and drinking water were found to be highly sensitive to the description of amine chemistry, especially of the night-time chemistry with the nitrate (NO3) radical. Sensitivity analysis of the fugacity model indicates that catchment characteristics and chemical degradation rates in soil and water are among the important factors controlling the fate of these compounds in lake water. The study shows that realistic emission of commonly used amines result in levels of the sum of nitrosamines and nitramines in ground-level air (0.6–10 pg m−3) and drinking water (0.04–0.25 ng L−1) below the current safety guideline for human health that is enforced by the Norwegian Environment Agency. The modelling framework developed in this study can be used to evaluate possible environmental impacts of emissions of amines from post-combustion capture in other regions of the world.
A climatology of dust emission events from northern Africa using long-term surface observations

Long-term (1984–2012) surface observations from 70 stations in the Sahara and Sahel are used to explore the diurnal, seasonal and geographical variations in dust emission events and thresholds. The frequency of dust emission (FDE) is calculated using the present weather codes of SYNOP reports. Thresholds are estimated as the wind speed for which there is a 50% probability of dust emission and are then used to calculate strong wind frequency (SWF) and dust uplift potential (DUP), where the latter is an estimate of the dust-generating power of winds. Stations are grouped into six coherent geographical areas for more in-depth analysis. FDE is highest at stations in Sudan and overall peaks in spring north of 23° N. South of this, where stations are directly influenced by the summer monsoon, the annual cycle in FDE is more variable. Thresholds are highest in northern Algeria, lowest in the latitude band 16–21° N and have greatest seasonal variations in the Sahel. Spatial variability in thresholds partly explain spatial variability in frequency of dust emission events on an annual basis. However, seasonal variations in thresholds for the six grouped areas are not the main control on seasonal variations in FDE. This is demonstrated by highly correlated seasonal cycles of FDE and SWF which are not significantly changed by using a fixed, or seasonally varying, threshold. The likely meteorological mechanisms generating these patterns such as low-level jets and haboobs are discussed.
Characterisation of bioaerosol emissions from a Colorado pine forest: results from the BEACHON-RoMBAS experiment

The behaviour of primary biological aerosols (PBAs) at an elevated, un-polluted North American forest site was studied using an ultra violet-light induced fluorescence (UV-LIF) measurement technique in conjunction with hierarchical agglomerative cluster analysis (HA-CA). Contemporaneous UV-LIF measurements were made with two wide-band integrated bioaerosol spectrometers, WIBS-3 and WIBS-4, which sampled close to the forest floor and via a continuous vertical profiling system, respectively. Additionally, meteorological parameters were recorded at various heights throughout the forest and used to estimate PBAP (Primary Biological Aerosol Particle) fluxes. HA-CA using data from the two, physically separated WIBS instruments independently yielded very similar cluster solutions. All fluorescent clusters displayed a diurnal minimum at midday at the forest floor with maximum concentration occurring at night. Additionally, the number concentration of each fluorescent cluster was enhanced, to different degrees, during wet periods. A cluster that displayed the greatest enhancement and highest concentration during sustained wet periods appears consistent with behaviour reported for fungal spores. A cluster that appears to be behaviourally consistent with bacteria dominated during dry periods. Fluorescent particle concentrations were found to be greater within the forest canopy than at the forest floor, indicating that the canopy was the main source of these particles rather than the minimal surface vegetation, which appeared to contribute little to overall PBA concentrations at this site. Fluorescent particle concentration was positively correlated with relative humidity (RH), and parameterisations of the aerosol response during dry and wet periods are reported. The aforementioned fungal spore-like cluster displayed a strong positive response to increasing RH. The bacteria-like cluster responded more strongly to direct rain-fall events than other PBA types. Peak concentrations of this cluster are shown to be linearly correlated to the log of peak rainfall rates. Parallel studies by Huffman et al. (2013) and Prenni et al. (2013) showed that the fluorescent particle concentrations correlated linearly with ice nuclei (IN) concentrations at this site during rain events. We discuss this result in conjunction with our cluster analysis to appraise the candidate IN.
EARLINET dust observations vs. BSC-DREAM8b modeled profiles: 12-year-long systematic comparison at Potenza, Italy

In this paper, we report the first systematic comparison of 12-year modeled dust extinction profiles vs. Raman lidar measurements. We use the BSC-DREAM8b model, one of the most widely used dust regional models in the Mediterranean, and Potenza EARLINET lidar profiles for Saharan dust cases, the largest one-site database of dust extinction profiles. A total of 310 dust cases were compared for the May 2000–July 2012 period. The model reconstructs the measured layers well: profiles are correlated within 5% of significance for 60% of the cases and the dust layer center of mass as measured by lidar and modeled by BSC-DREAM8b differ on average 0.3 ± 1.0 km. Events with a dust optical depth lower than 0.1 account for 70% of uncorrelated profiles. Although there is good agreement in terms of profile shape and the order of magnitude of extinction values, the model overestimates the occurrence of dust layer top above 10 km. Comparison with extinction profiles measured by the Raman lidar shows that BSC-DREAM8b typically underestimates the dust extinction coefficient, in particular below 3 km. Lowest model–observation differences (below 17%) correspond to a lidar ratio at 532 nm and Ångström exponent at 355/532 nm of 60 ± 13 and 0.1 ± 0.6 sr, respectively. These are in agreement with values typically observed and modeled for pure desert dust. However, the highest differences (higher than 85%) are typically related to greater Ångström values (0.5 ± 0.6), denoting smaller particles. All these aspects indicate that the level of agreement decreases with an increase in mixing/modification processes.
Diagnosing the average spatio-temporal impact of convective systems – Part 2: A model intercomparison using satellite data

The representation of the effect of tropical deep convective (DC) systems on upper-tropospheric moist processes and outgoing longwave radiation is evaluated in the EC-Earth3, ECHAM6, and CAM5 (Community Atmosphere Model) climate models using satellite-retrieved data. A composite technique is applied to thousands of deep convective systems that are identified using local rain rate maxima in order to focus on the temporal evolution of the deep convective processes in the model and satellite-retrieved data. The models tend to over-predict the occurrence of rain rates that are less than ≈ 3 mm h−1 compared to Tropical Rainfall Measurement Mission (TRMM) Multi-satellite Precipitation Analysis (TMPA). While the diurnal distribution of oceanic rain rate maxima in the models is similar to the satellite-retrieved data, the land-based maxima are out of phase. Despite having a larger climatological mean upper-tropospheric relative humidity, models closely capture the satellite-derived moistening of the upper troposphere following the peak rain rate in the deep convective systems. Simulated cloud fractions near the tropopause are larger than in the satellite data, but the ice water contents are smaller compared with the satellite-retrieved ice data. The models capture the evolution of ocean-based deep convective systems fairly well, but the land-based systems show significant discrepancies. Over land, the diurnal cycle of rain is too intense, with deep convective systems occurring at the same position on subsequent days, while the satellite-retrieved data vary more in timing and geographical location. Finally, simulated outgoing longwave radiation anomalies associated with deep convection are in reasonable agreement with the satellite data, as well as with each other. Given the fact that there are strong disagreements with, for example, cloud ice water content, and cloud fraction, between the models, this study supports the hypothesis that such agreement with satellite-retrieved data is achieved in the three models due to different representations of deep convection processes and compensating errors.
On the submicron aerosol distributions and CCN number concentrations in and around the Korean Peninsula

Total number concentrations of particles having a diameter larger than 10 nm (NCN), cloud condensation nuclei at several supersaturation (S) values (NCCN) and number size distributions of particles with 10–414 nm diameter were measured in Seoul between 2004 and 2010. Overall average values of NCN and geometric mean diameter were 17 811 ± 5581 cm−3 and 48 ± 6 nm. Average NCCN at 0.4, 0.6 and 0.8% S were 4145 ± 2016, 5323 ± 2453 and 6067 ± 2780 cm−3 and corresponding NCCN / NCN were 0.26 ± 0.11, 0.33 ± 0.11 and 0.37 ± 0.12. There is a clear seasonal variation in aerosol concentration, which seems to be due to the monsoon. NCN and NCCN are also found to depend on the volume of traffic and the height of the planetary boundary layer, respectively. During aircraft campaigns in 2009 and 2011, NCN and NCCN at 0.6% S (N0.6%) were measured in and around the Korean Peninsula. During the 2011 campaign, the aerosol scattering coefficient was also measured. NCN and N0.6% in the lower altitudes were generally higher than at higher altitudes, except for cases when particle formation and growth events were thought to occur at higher altitudes. NCN and N0.6% generally show a positive correlation with aerosol scattering coefficients but this correspondence tends to vary with altitude. Occasional instances of low (< 0.3) N0.6% / NCN in the boundary layer are demonstrated to be associated with particle formation and growth events. With the support of ground measurements, it is confirmed that a particle formation and growth event did indeed occur over the Yellow Sea on a flight day, and the areal extent of this event is estimated to be greater than 100 km × 450 km. With the combination of the current and several relevant previous studies, a composite map of NCN and NCCN in and around the Korean Peninsula is produced. Overall, the exhibited concentrations are typical of values measured over polluted regions elsewhere on the globe. Moreover, there is a generally decreasing trend from west to east over the region, implying that the region is constantly under the dominant influence of continental outflow.
Observation and modelling of HOx radicals in a boreal forest

Measurements of OH and HO2 radicals were conducted in a pine-dominated forest in southern Finland during the HUMPPA-COPEC-2010 (Hyytiälä United Measurements of Photochemistry and Particles in Air – Comprehensive Organic Precursor Emission and Concentration study) field campaign in summer 2010. Simultaneous side-by-side measurements of hydroxyl radicals were conducted with two instruments using chemical ionization mass spectrometry (CIMS) and laser-induced fluorescence (LIF), indicating small systematic disagreement, OHLIF / OHCIMS = (1.31 ± 0.14). Subsequently, the LIF instrument was moved to the top of a 20 m tower, just above the canopy, to investigate the radical chemistry at the ecosystem–atmosphere interface. Comprehensive measurements including observations of many volatile organic compounds (VOCs) and the total OH reactivity were conducted and analysed using steady-state calculations as well as an observationally constrained box model. Production rates of OH calculated from measured OH precursors are consistent with those derived from the steady-state assumption and measured total OH loss under conditions of moderate OH reactivity. The primary photolytic sources of OH contribute up to one-third to the total OH production. OH recycling, which occurs mainly by HO2 reacting with NO and O3, dominates the total hydroxyl radical production in this boreal forest. Box model simulations agree with measurements for hydroxyl radicals (OHmod. / OHobs. = 1.00 ± 0.16), while HO2 mixing ratios are significantly under-predicted (HO2mod. / HO2obs. = 0.3 ± 0.2), and simulated OH reactivity does not match the observed OH reactivity. The simultaneous under-prediction of HO2 and OH reactivity in periods in which OH concentrations were simulated realistically suggests that the missing OH reactivity is an unaccounted-for source of HO2. Detailed analysis of the HOx production, loss, and recycling pathways suggests that in periods of high total OH reactivity there are additional recycling processes forming OH directly, not via reaction of HO2 with NO or O3, or unaccounted-for primary HOx sources. Under conditions of moderate observed OH reactivity and high actinic flux, an additional RO2 source of approximately 1 × 106 molec cm−3 s−1 would be required to close the radical budget. Nevertheless, a major fraction of the OH recycling occurs via the reaction of HO2 with NO and O3 in this terpene-dominated environment.
Investigation of the "elevated heat pump" hypothesis of the Asian monsoon using satellite observations

The "elevated heat pump" (EHP) hypothesis has been a topic of intensive research and controversy. It postulates that aerosol-induced anomalous mid- and upper-tropospheric warming in the Himalayan foothills and above the Tibetan Plateau leads to an early onset and intensification of Asian monsoon rainfall. This finding is primarily based on results from a NASA finite-volume general circulation model run with and without radiative forcing from different types of aerosols. In particular, black carbon emissions from sources in northern India and dust from Western China, Afghanistan, Pakistan, the Thar Desert, and the Arabian Peninsula drive the modeled anomalous heating. Since the initial discussion of the EHP hypothesis in 2006, the aerosol–monsoon relationship has been investigated using various modeling and observational techniques. The current study takes a novel observational approach to detect signatures of the "elevated heat pump" effect on convection, precipitation, and temperature for contrasting aerosol content years during the period of 2000–2012. The analysis benefits from unique high-resolution convection information inferred from Meteosat-5 observations as available through 2005. Additional data sources include temperature data from the NCEP/NCAR Reanalysis and the European Reanalysis (ERA-Interim) precipitation data from the Global Precipitation Climatology Project (GPCP), aerosol optical depth from the Multi-angle Imaging Spectroradiometer (MISR) and the Moderate Resolution Imaging Spectroradiometer (MODIS), and aerosol optical properties from the Modern-Era Retrospective Analysis for Research and Applications (MERRA) aerosol reanalysis. Anomalous upper-tropospheric warming and the early onset and intensification of the Indian monsoon were not consistently observed during the years with high loads of absorbing aerosols. Possibly, model assumptions and/or unaccounted semi-direct aerosol effects caused the disagreement between observed and hypothesized behavior.
Ice nucleation by fungal spores from the classes Agaricomycetes, Ustilaginomycetes, and Eurotiomycetes, and the effect on the atmospheric transport of these spores

We studied the ice nucleation properties of 12 different species of fungal spores chosen from three classes: Agaricomycetes, Ustilaginomycetes, and Eurotiomycetes. Agaricomycetes include many types of mushroom species and are widely distributed over the globe. Ustilaginomycetes are agricultural pathogens and have caused widespread damage to crops. Eurotiomycetes are found on all types of decaying material and include important human allergens. We focused on these classes because they are thought to be abundant in the atmosphere and because there is very little information on the ice nucleation ability of these classes of spores in the literature. All of the fungal spores investigated contained some fraction of spores that serve as ice nuclei at temperatures warmer than homogeneous freezing. The cumulative number of ice nuclei per spore was 0.001 at temperatures between −19 °C and −29 °C, 0.01 between −25.5 °C and −31 °C, and 0.1 between −26 °C and −31.5 °C. On average, the order of ice nucleating ability for these spores is Ustilaginomycetes > Agaricomycetes ≃ Eurotiomycetes. The freezing data also suggests that, at temperatures ranging from −20 °C to −25 °C, all of the fungal spores studied here are less efficient ice nuclei compared to Asian mineral dust on a per surface area basis. We used our new freezing results together with data in the literature to compare the freezing temperatures of spores from the phyla Basidiomycota and Ascomycota, which together make up 98% of known fungal species found on Earth. The data show that within both phyla (Ascomycota and Basidiomycota), there is a wide range of freezing properties, and also that the variation within a phylum is greater than the variation between the average freezing properties of the phyla. Using a global chemistry–climate transport model, we investigated whether ice nucleation on the studied spores, followed by precipitation, can influence the transport and global distributions of these spores in the atmosphere. Simulations suggest that inclusion of ice nucleation scavenging of these fungal spores in mixed-phase clouds can decrease the annual mean concentrations of fungal spores in near-surface air over the oceans and polar regions, and decrease annual mean concentrations in the upper troposphere.