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Observations and analysis of organic aerosol evolution in some prescribed fire smoke plumes

Open biomass burning is a significant source of primary air pollutants such as particulate matter (PM) and non-methane organic gases (NMOG). However, the physical and chemical atmospheric processing of these emissions during transport is poorly understood. Atmospheric transformations of biomass burning emissions have been investigated in environmental chambers, but there have been limited opportunities to investigate these transformations in the atmosphere. In this study, we deployed a suite of real-time instrumentation on a Twin Otter aircraft to sample smoke from prescribed fires in South Carolina, conducting measurements at both the source and downwind to characterize smoke evolution with atmospheric aging. Organic aerosol (OA) within the smoke plumes was quantified using an aerosol mass spectrometer (AMS); refractory black carbon (rBC) was quantified using a single-particle soot photometer, and carbon monoxide (CO) and carbon dioxide (CO2) were measured using a cavity ring-down spectrometer. During the two fires for which we were able to obtain aerosol aging data, normalized excess mixing ratios and "export factors" of conserved species (rBC, CO, CO2) suggested that changes in emissions at the source did not account for most of the differences observed in samples of increasing age. An investigation of AMS mass fragments indicated that the in-plume fractional contribution (fm/z) to OA of the primary fragment (m/z 60) decreased downwind, while the fractional contribution of the secondary fragment (m/z 44) increased. Increases in f44 are typically interpreted as indicating chemical aging of OA. Likewise, we observed an increase in the O : C elemental ratio downwind, which is usually associated with aerosol aging. However, the rapid mixing of these plumes into the background air suggests that these chemical transformations may be attributable to the different volatilities of the compounds that fragment to these m/z in the AMS. The gas–particle partitioning behavior of the bulk OA observed during the study was consistent with the predictions from a parameterization developed for open biomass burning emissions in the laboratory. Furthermore, we observed no statistically significant increase in total organic mass with atmospheric transport. Hence, our results suggest that dilution-driven evaporation likely dominated over the chemical production of secondary organic aerosol (SOA) within our smoke plumes, presumably due to the fast dilution and limited aging times (< ~ 5 h) that we could sample.
The role of organic condensation on ultrafine particle growth during nucleation events

A new aerosol dynamics model (DMANx) has been developed that simulates aerosol size/composition distribution and includes the condensation of organic vapors on nanoparticles through the implementation of the recently developed volatility basis set framework. Simulations were performed for Hyytiälä (Finland) and Finokalia (Greece), two locations with different organic sources where detailed measurements were available to constrain the new model. We investigate the effect of condensation of organics and chemical aging reactions of secondary organic aerosol (SOA) precursors on ultrafine particle growth and particle number concentration during a typical springtime nucleation event in both locations. This work highlights the importance of the pathways of oxidation of biogenic volatile organic compounds and the production of extremely low volatility organics. At Hyytiälä, organic condensation dominates the growth process of new particles. The low-volatility SOA contributes to particle growth during the early growth stage, but after a few hours most of the growth is due to semi-volatile SOA. At Finokalia, simulations show that organics have a complementary role in new particle growth, contributing 45% to the total mass of new particles. Condensation of organics increases the number concentration of particles that can act as CCN (cloud condensation nuclei) (N100) by 13% at Finokalia and 25% at Hyytiälä during a typical spring day with nucleation. The sensitivity of our results to the surface tension used is discussed.
Impacts of 20th century aerosol emissions on the South Asian monsoon in the CMIP5 models

Comparison of single-forcing varieties of 20th century historical experiments in a subset of models from the Fifth Coupled Model Intercomparison Project (CMIP5) reveals that South Asian summer monsoon rainfall increases towards the present day in Greenhouse Gas (GHG)-only experiments with respect to pre-industrial levels, while it decreases in anthropogenic aerosol-only experiments. Comparison of these single-forcing experiments with the all-forcings historical experiment suggests aerosol emissions have dominated South Asian monsoon rainfall trends in recent decades, especially during the 1950s to 1970s. The variations in South Asian monsoon rainfall in these experiments follows approximately the time evolution of inter-hemispheric temperature gradient over the same period, suggesting a contribution from the large-scale background state relating to the asymmetric distribution of aerosol emissions about the equator. By examining the 24 available all-forcings historical experiments, we show that models including aerosol indirect effects dominate the negative rainfall trend. Indeed, models including only the direct radiative effect of aerosol show an increase in monsoon rainfall, consistent with the dominance of increasing greenhouse gas emissions and planetary warming on monsoon rainfall in those models. For South Asia, reduced rainfall in the models with indirect effects is related to decreased evaporation at the land surface rather than from anomalies in horizontal moisture flux, suggesting the impact of indirect effects on local aerosol emissions. This is confirmed by examination of aerosol loading and cloud droplet number trends over the South Asia region. Thus, while remote aerosols and their asymmetric distribution about the equator play a role in setting the inter-hemispheric temperature distribution on which the South Asian monsoon, as one of the global monsoons, operates, the addition of indirect aerosol effects acting on very local aerosol emissions also plays a role in declining monsoon rainfall. The disparity between the response of monsoon rainfall to increasing aerosol emissions in models containing direct aerosol effects only and those also containing indirect effects needs to be urgently investigated since the suggested future decline in Asian anthropogenic aerosol emissions inherent to the representative concentration pathways (RCPs) used for future climate projection may turn out to be optimistic. In addition, both groups of models show declining rainfall over China, also relating to local aerosol mechanisms. We hypothesize that aerosol emissions over China are large enough, in the CMIP5 models, to cause declining monsoon rainfall even in the absence of indirect aerosol effects. The same is not true for India.
Survival and ice nucleation activity of bacteria as aerosols in a cloud simulation chamber

The residence time of bacterial cells in the atmosphere is predictable by numerical models. However, estimations of their aerial dispersion as living entities are limited by a lack of information concerning survival rates and behavior in relation to atmospheric water. Here we investigate the viability and ice nucleation (IN) activity of typical atmospheric ice nucleation active bacteria (Pseudomonas syringae and P. fluorescens) when airborne in a cloud simulation chamber (AIDA, Karlsruhe, Germany). Cell suspensions were sprayed into the chamber and aerosol samples were collected by impingement at designated times over a total duration of up to 18 h, and at some occasions after dissipation of a cloud formed by depressurization. Aerosol concentration was monitored simultaneously by online instruments. The cultivability of airborne cells decreased exponentially over time with a half-life time of 250 ± 30 min (about 3.5 to 4.5 h). In contrast, IN activity remained unchanged for several hours after aerosolization, demonstrating that IN activity was maintained after cell death. Interestingly, the relative abundance of IN active cells still airborne in the chamber was strongly decreased after cloud formation and dissipation. This illustrates the preferential precipitation of IN active cells by wet processes. Our results indicate that from 106 cells aerosolized from a surface, one would survive the average duration of its atmospheric journey estimated at 3.4 days. Statistically, this corresponds to the emission of 1 cell that achieves dissemination every ~ 33 min m−2 of cultivated crops fields, a strong source of airborne bacteria. Based on the observed survival rates, depending on wind speed, the trajectory endpoint could be situated several hundreds to thousands of kilometers from the emission source. These results should improve the representation of the aerial dissemination of bacteria in numeric models.
Tropical, oceanic, deep convective cloud morphology as observed by CloudSat

An investigation into the physical shape and size of mature, oceanic, tropical, deep convective clouds is conducted. A previously developed CloudSat data-partitioning methodology is used that separates components of cloud objects and measures their various length scales. In particular, the cloud objects are divided into a lower "pedestal" region on which the upper-level "anvil" region sits. Mean cloud objects are discussed in the framework of this morphological partitioning. For single-core clouds, the mean cloud has an anvil width of 95 km, a pedestal width of 11 km, and an anvil thickness of 6.4 km. The number of identified convective cores within the pedestal correlates positively with certain cloud length scales and morphological attributes of cloud objects such as anvil width. As the number of cores increases, the width of cloud objects is observed to grow. Pedestal width is shown to regress linearly to anvil width when a 2/3rd power scaling is applied to pedestal width. This result implies a decrease in the anvil width to pedestal width ratio with growing pedestals and an equivalence between the mass convected through the pedestal top and that into the anvil. Taller clouds are found to be wider. Some of the results obtained using the CloudSat methodology are also examined with a large-domain radiative-convective equilibrium numerical simulation and are found to exhibit similar trends when modeled. Finally, various CloudSat sampling issues are discussed in several appendices.
A 12-year observation of water-soluble ions in TSP aerosols collected at a remote marine location in the western North Pacific: an outflow region of Asian dust

In order to characterize the long-term trend of remote marine aerosols, a 12-year observation was conducted for water-soluble ions in TSP (total suspended particulate) aerosols collected from 2001 to 2012 in the Asian outflow region at Chichijima Island in the western North Pacific. We found a clear difference in chemical composition between the continentally affected and marine background air masses over the observation site. Asian continental air masses are delivered from late autumn to spring, whereas marine air masses were dominated in summer. Concentrations of non-sea salt (nss-) SO42−, NO3−, NH4+, nss-K+ and nss-Ca2+ are high in winter and spring and low in summer. On the other hand, MSA− (methanesulfonate) exhibits higher concentrations during spring and winter, probably due to springtime dust bloom or due to the direct continental transport of MSA− to the observation site. We could not find any clear decadal trend for Na+, Cl−, Mg2+ and nss-Ca2+ in all seasons, although there exists a clear seasonal trend. However, concentrations of nss-SO42− continuously decreased from 2007 to 2012, probably due to the decreased SO2 emissions in East Asia especially in China. In contrast, nss-K+ and MSA− concentrations continuously increased from 2001 to 2012 during winter and spring seasons, demonstrating that biomass burning and/or terrestrial biological emissions in East Asia are being increasingly transported from the Asian continent to the western North Pacific. This study also demonstrates that Asian dusts can act as an important source of nutrients for phytoplankton and thus sea-to-air emission of dimethyl sulfide over the western North Pacific.
Particulate emissions from residential wood combustion in Europe – revised estimates and an evaluation

Currently residential wood combustion (RWC) is increasing in Europe because of rising fossil fuel prices but also due to climate change mitigation policies. However, especially in small-scale applications, RWC may cause high emissions of particulate matter (PM). Recently we have developed a new high-resolution (7 × 7 km) anthropogenic carbonaceous aerosol emission inventory for Europe. The inventory indicated that about half of the total PM2.5 emission in Europe is carbonaceous aerosol and identified RWC as the largest organic aerosol source in Europe. The inventory was partly based on national reported PM emissions. Use of this organic aerosol inventory as input for two chemical transport models (CTMs), PMCAMx and EMEP MSC-W, revealed major underestimations of organic aerosol in winter time, especially for regions dominated by RWC. Interestingly, this was not universal but appeared to differ by country. In the present study we constructed a revised bottom-up emission inventory for RWC accounting for the semivolatile components of the emissions. The revised RWC emissions are higher than those in the previous inventory by a factor of 2–3 but with substantial inter-country variation. The new emission inventory served as input for the CTMs and a substantially improved agreement between measured and predicted organic aerosol was found. The revised RWC inventory improves the model-calculated organic aerosol significantly. Comparisons to Scandinavian source apportionment studies also indicate substantial improvements in the modelled wood-burning component of organic aerosol. This suggests that primary organic aerosol emission inventories need to be revised to include the semivolatile organic aerosol that is formed almost instantaneously due to dilution and cooling of the flue gas or exhaust. Since RWC is a key source of fine PM in Europe, a major revision of the emission estimates as proposed here is likely to influence source–receptor matrices and modelled source apportionment. Since usage of biofuels in small combustion units is a globally significant source, the findings presented here are also relevant for regions outside of Europe.
Regional differences in Chinese SO2 emission control efficiency and policy implications

SO2 emission control has been one of the most important air pollution policies in China since 2000. In this study, we assess regional differences in SO2 emission control efficiencies in China through the modeling analysis of four scenarios of SO2 emissions, all of which aim to reduce the national total SO2 emissions by 8% or 2.3 Tg below the 2010 emissions level, the target set by the current twelfth Five-Year Plan (FYP; 2011–2015), but differ in spatial implementation. The GEOS-Chem chemical transport model is used to evaluate the efficiency of each scenario on the basis of four impact metrics: surface SO2 and sulfate concentrations, population-weighted sulfate concentration (PWC), and sulfur export flux from China to the western Pacific. The efficiency of SO2 control (β) is defined as the relative change of each impact metric to a 1% reduction in SO2 emissions from the 2010 baseline. The S1 scenario, which adopts a spatially uniform reduction in SO2 emissions in China, gives a β of 0.99, 0.71, 0.83, and 0.67 for SO2 and sulfate concentrations, PWC, and export flux, respectively. By comparison, the S2 scenario, which implements all the SO2 emissions reduction over North China (NC), is found most effective in reducing national mean surface SO2 and sulfate concentrations and sulfur export fluxes, with β being 1.0, 0.76, and 0.95 respectively. The S3 scenario of implementing all the SO2 emission reduction over South China (SC) has the highest β in reducing PWC (β = 0.98) because SC has the highest correlation between population density and sulfate concentration. Reducing SO2 emissions over Southwest China (SWC) is found to be least efficient on the national scale, albeit with large benefits within the region. The difference in β by scenario is attributable to the regional difference in SO2 oxidation pathways and the source–receptor relationship. Among the three regions examined here, NC shows the largest proportion of sulfate formation through gas-phase oxidation, which is more sensitive to SO2 emissions change than aqueous oxidation. In addition, NC makes the largest contribution to inter-regional transport of sulfur within China and to the transport fluxes to the western Pacific. The policy implication of this is that China needs to carefully design a regionally specific implementation plan of realizing its SO2 emissions reduction target in order to maximize the resulting air quality benefits, not only for China but for the downwind regions, with emphasis on reducing emissions from NC, where SO2 emissions have decreased at a slower rate than national total emissions in the previous FYP period.
Potential source regions and processes of aerosol in the summer Arctic

Sub-micrometer particle size distributions measured during four summer cruises of the Swedish icebreaker Oden 1991, 1996, 2001, and 2008 were combined with dimethyl sulfide gas data, back trajectories, and daily maps of pack ice cover in order to investigate source areas and aerosol formation processes of the boundary layer aerosol in the central Arctic. With a clustering algorithm, potential aerosol source areas were explored. Clustering of particle size distributions together with back trajectories delineated five potential source regions and three different aerosol types that covered most of the Arctic Basin: marine, newly formed and aged particles over the pack ice. Most of the pack ice area with < 15% of open water under the trajectories exhibited the aged aerosol type with only one major mode around 40 nm. For newly formed particles to occur, two conditions had to be fulfilled over the pack ice: the air had spent 10 days while traveling over ever more contiguous ice and had traveled over less than 30% open water during the last 5 days. Additionally, the air had experienced more open water (at least twice as much as in the cases of aged aerosol) during the last 4 days before arrival in heavy ice conditions at Oden. Thus we hypothesize that these two conditions were essential factors for the formation of ultrafine particles over the central Arctic pack ice. In a comparison the Oden data with summer size distribution data from Alert, Nunavut, and Mt. Zeppelin, Spitsbergen, we confirmed the Oden findings with respect to particle sources over the central Arctic. Future more frequent broken-ice or open water patches in summer will spur biological activity in surface water promoting the formation of biological particles. Thereby low clouds and fogs and subsequently the surface energy balance and ice melt may be affected.
Modelling the impact of climate change on the atmospheric transport and the fate of persistent organic pollutants in the Arctic

The Danish Eulerian Hemispheric Model (DEHM) was applied to investigate how projected climate changes will affect the atmospheric transport of 13 persistent organic pollutants (POPs) to the Arctic and their environmental fate within the Arctic. Three sets of simulations were performed, one with present day emissions and initial environmental concentrations from a 20-year spin-up simulation, one with present day emissions and with initial environmental concentrations set to zero and one without emissions but with initial environmental concentrations from the 20-year spin-up simulation. Each set of simulations consisted of two 10-year time slices representing the present (1990–2000) and future (2090–2100) climate conditions. DEHM was driven using meteorological input from the global circulation model, ECHAM/MPI-OM, simulating the SRES (Special Report on Emissions Scenarios) A1B climate scenario. Under the applied climate and emission scenarios, the total mass of all compounds was predicted to be up to 55 % lower across the Northern Hemisphere at the end of the 2090s than in the 1990s. The mass of HCHs within the Arctic was predicted to be up to 38 % higher, whereas the change in mass of the PCBs was predicted to range from 38 % lower to 17 % higher depending on the congener and the applied initial environmental concentrations. The results of this study also indicate that contaminants with no or a short emission history will be more rapidly transported to and build up in the arctic environment in a future warmer climate. The process that dominates the environmental behaviour of POPs in the Arctic under a future warmer climate scenario is the shift in mass of POPs from the surface media to the atmosphere induced by the higher mean temperature. This is to some degree counteracted by higher degradation rates also following the higher mean temperature. The more dominant of these two processes depends on the physical-chemical properties of the compounds. Previous model studies have predicted that the effect of a changed climate on the transport of POPs to the Arctic is moderate relative to the effect of proposed changes in emissions, which is confirmed in this study. However, the model studies do not agree on whether climate change acts to reduce or increase environmental concentrations of POPs in the Arctic, and further work is needed to resolve this matter.