Aerosol Burden Research Articles

Differing responses of the quasi-biennial oscillation to artificial SO<sub>2</sub> injections in two global models

Abstract. Artificial injections of sulfur dioxide (SO2) into the stratosphere show in several model studies an impact on stratospheric dynamics. The quasi-biennial oscillation (QBO) has been shown to slow down or even vanish under higher SO2 injections in the equatorial region. But the impact is only qualitatively but not quantitatively consistent across the different studies using different numerical models. The aim of this study is to understand the reasons behind the differences in the QBO response to SO2 injections between two general circulation models, the Whole Atmosphere Community Climate Model (WACCM-110L) and MAECHAM5-HAM. We show that the response of the QBO to injections with the same SO2 injection rate is very different in the two models, but similar when a similar stratospheric heating rate is induced by SO2 injections of different amounts. The reason for the different response of the QBO corresponding to the same injection rate is very different vertical advection in the two models, even in the control simulation. The stronger vertical advection in WACCM results in a higher aerosol burden and stronger heating of the aerosols and, consequently, in a vanishing QBO at lower injection rate than in simulations with MAECHAM5-HAM. The vertical velocity increases slightly in MAECHAM5-HAM when increasing the horizontal resolution. This study highlights the crucial role of dynamical processes and helps to understand the large uncertainties in the response of different models to artificial SO2 injections in climate engineering studies.

Comparisons and evaluation of aerosol burden and optical depth in CMIP5 simulations over East Asia

Aerosol plays an important role in the climate system by affecting the radiative and energy balances. Hence, in this paper, the spatial patterns of aerosol burden and aerosol optical properties (AOD) in four the Coupled Model Intercomparison Project phase 5 (CMIP5) models over East Asia during 2001–2005 are compared to quantify inter-model differences and to evaluate AOD simulations against observations. The evaluation of AOD against Moderate Resolution Imaging Spectroradiometer (MODIS) satellite retrievals shows that CMIP5 models can reproduce the spatial pattern of MODIS AOD reasonably well. The mean AOD over eastern China shows that NorESM1-M underestimates MODIS AOD by 40%, due to the lack of emissions of some aerosol components, such as nitrate, biogenic aerosol, and non-desert mineral dust. In contrast to that, CSIRO-Mk3.6.0 overestimates annual mean of MODIS AOD over eastern China by 20%, partially caused by larger aerosol emissions and burden. Compared to MODIS AOD, GFDL-CM3 performs the best in simulating AOD in eastern China, because ammonium and nitrate are included in this model. The comparisons of CMIP5 and Aerosol Robotic Network (AERONET) AOD show similar results. In addition, the simulated AOD values are closer to AERONET AOD in Mongolia, China, Japan and Korea than that in India. The results also reveal that there are some inter-model differences of aerosol burden over East Asia, caused by the inter-model differences of aerosol emissions, wet scavenging, and transport. Over eastern and northwestern China and the west Pacific, the inter-model differences of anthropogenic aerosol burden and spatial variabilities are smaller than that of natural aerosol burden.

Seasonal and interannual variations of atmospheric dust aerosols in mid and low latitudes of Asia – A comparative study

Although variations of atmospheric dust aerosols emitted from different sources within Asia have been studied separately in previous research, the characteristics and causes of these changes have not been fully explored. This study used the Modern-Era Retrospective Analysis for Research and Applications Version 2 (MERRA-2) data set for 1980–2016 to compare seasonal and interannual variations of atmospheric dust aerosols between mid- and low-latitude sources of Asia and explore the reasons for these variations. The seasonal variation of atmospheric dust aerosols in mid-latitude sources was different from that of low-latitude sources. The column burden of dust aerosols in the mid-latitude sources (including East and Central Asia) reached their maximum in spring, and accounted for about 37% and 33% of their annual total load, respectively. The maximum dust aerosols in spring in the Central Asia sources resulted from multiple factors such as soil wetness, snow depth, and vertical wind shear, but they were negatively correlated with soil wetness on the interannual scale (r = −0.65). The maximum dust aerosol burden in spring in the East Asia sources resulted from vertical wind shear in the lower troposphere, and showed a positive correlation with the interannual change of dust aerosols in this source region (r = 0.51). However, the column burden of dust aerosols in the low-latitude sources (including South and West Asia) reached their maximum in summer, and accounted for about 41% and 37% of their annual total load, respectively. The maximum dust aerosols of summer in the low-latitude sources also resulted from vertical wind shear in the lower troposphere with correlation coefficients of 0.50 and 0.73 in the South and West Asia sources, respectively. The present results may help in further understanding the formation and change of Asian dust aerosols.

Transformation and ageing of biomass burning carbonaceous aerosol over tropical South America from aircraft in situ measurements during SAMBBA

Abstract. We present a range of airborne in situ observations of biomass burning carbonaceous aerosol over tropical South America, including a case study of a large tropical forest wildfire and a series of regional survey flights across the Brazilian Amazon and Cerrado. The study forms part of the South American Biomass Burning Analysis (SAMBBA) project, which was conducted during September and October 2012. We find limited evidence for net increases in aerosol mass through atmospheric ageing combined with substantial changes in the chemical properties of organic aerosol (OA). Oxidation of the OA increases significantly and rapidly on the scale of 2.5–3 h based on our case study analysis and is consistent with secondary organic aerosol production. The observations of limited net enhancement in OA coupled with such changes in chemical composition imply that evaporation of OA is also occurring to balance these changes. We observe significant coatings on black carbon particles at source, but with limited changes with ageing in both particle core size and coating thickness. We quantify variability in the ratio of OA to carbon monoxide across our study as a key parameter representing both initial fire conditions and an indicator of net aerosol production with atmospheric ageing. We observe ratios of 0.075–0.13 µgsm-3ppbv-1 in the west of our study region over the Amazon tropical forest in air masses less influenced by precipitation and a value of 0.095 µgsm-3ppbv-1 over the Cerrado environment in the east (where sm−3 refers to standard metre cubed). Such values are consistent with emission factors used by numerical models to represent biomass burning OA emissions. Black carbon particle core sizes typically range from mean mass diameters of 250 to 290 nm, while coating thicknesses range from 40 to 110 nm in air masses less influenced by precipitation. The primary driver of the variability we observe appears to be related to changes at the initial fire source. A key lesson from our study is that simply aggregating our observations as a function of atmospheric ageing would have been misleading due to the complex nature of the regional aerosol and its drivers, due to the many conflating and competing factors that are present. Our study explores and quantifies key uncertainties in the evolution of biomass burning aerosol at both near-field and regional scales. Our results suggest that the initial conditions of the fire are the primary driver of carbonaceous aerosol physical and chemical properties over tropical South America, aside from significant oxidation of OA during atmospheric ageing. Such findings imply that uncertainties in the magnitude of the aerosol burden and its impact on weather, climate, health and natural ecosystems most likely lie in quantifying emission sources, alongside atmospheric dispersion, transport and removal rather than chemical enhancements in mass.

Re-examining Dust Chemical Aging and Its Impacts on Earth's Climate.

The impact of atmospheric particulate matter (i.e., aerosols) on Earth's radiative balance has been and continues to be the leading source of uncertainty with respect to predictions of future temperature increases due to climate change. Mineral dust particles transported from deserts and semiarid regions across the globe are a dominant contributor to the aerosol burden. Dust has many and diverse effects on Earth's climate: it directly scatters and/or absorbs incoming sunlight; it reacts with trace gases leading to impacts on the oxidizing capacity of the atmosphere that affect both the lifetime of the greenhouse gas methane in addition to concentrations of tropospheric ozone-a greenhouse gas and criteria air pollutant; it influences the production as well as the lifetime and radiative properties of clouds; and it deposits nutrients to aquatic and terrestrial ecosystems that can stimulate primary production and facilitate the sequestration of atmospheric carbon dioxide (CO2). This Account will focus on the last three effects. The ability of dust to affect clouds and biogeochemical cycles hinges upon the chemical nature of dust particles-in particular, whether the compounds found in dust particles are water-soluble. The solubility of nutrients found in dust is particularly critical for determining the impact of atmospheric deposition on ocean productivity. The traditional viewpoint is that dust is inherently insoluble but reactive toward trace acidic gases, a process herein referred to as chemical aging. These reactions are thought to affect the oxidizing capacity of the atmosphere while effectively transforming the chemical composition of dust by increasing its solubility. Consequently, chemical aging is hypothesized to substantially increase the impact of dust on cloud droplet formation and marine biogeochemical cycles.This Account presents recent advances in our understanding of the mechanisms that determine how efficiently dust undergoes chemical aging and what the consequences of these processes are for the different effects of dust on Earth's climate. This Account will re-examine the traditional viewpoint that dust chemical aging strongly impacts marine biogeochemical cycles as well as the ability of dust to nucleate cloud droplets. Laboratory studies on environmental samples are combined with chemical analysis of field samples collected at dust transport receptor sites to better understand chemical aging mechanisms and determine the impact of dust on tropospheric oxidants, clouds, and biogeochemical cycles. Our results highlight the important role that dust mineralogy plays in both the nucleation of clouds as well as the kinetics responsible for the chemical aging of dust. This Account will present cases where dust contains inherently soluble minerals and does not require chemical aging in order to efficiently nucleate clouds in the atmosphere. Lastly, this Account illustrates the critical role that nondust aerosols, namely, wildfire and combustion emissions, play as a supplier of soluble nutrients important for biogeochemical cycles, particularly in marine environments. This Account will discuss these findings and highlight future research directions and recommendations to better understand dust-climate interactions and the emerging role of biomass burning aerosol in marine biogeochemical cycles.

First direct observation of sea salt aerosol production from blowing snow above sea ice

Abstract. Two consecutive cruises in the Weddell Sea, Antarctica, in winter 2013 provided the first direct observations of sea salt aerosol (SSA) production from blowing snow above sea ice, thereby validating a model hypothesis to account for winter time SSA maxima in the Antarctic. Blowing or drifting snow often leads to increases in SSA during and after storms. For the first time it is shown that snow on sea ice is depleted in sulfate relative to sodium with respect to seawater. Similar depletion in bulk aerosol sized ∼0.3–6 µm above sea ice provided the evidence that most sea salt originated from snow on sea ice and not the open ocean or leads, e.g. >90 % during the 8 June to 12 August 2013 period. A temporally very close association of snow and aerosol particle dynamics together with the long distance to the nearest open ocean further supports SSA originating from a local source. A mass budget estimate shows that snow on sea ice contains even at low salinity (<0.1 psu) more than enough sea salt to account for observed increases in atmospheric SSA during storms if released by sublimation. Furthermore, snow on sea ice and blowing snow showed no or small depletion of bromide relative to sodium with respect to seawater, whereas aerosol was enriched at 2 m and depleted at 29 m, suggesting that significant bromine loss takes place in the aerosol phase further aloft and that SSA from blowing snow is a source of atmospheric reactive bromine, an important ozone sink, even during winter darkness. The relative increase in aerosol concentrations with wind speed was much larger above sea ice than above the open ocean, highlighting the importance of a sea ice source in winter and early spring for the aerosol burden above sea ice. Comparison of absolute increases in aerosol concentrations during storms suggests that to a first order corresponding aerosol fluxes above sea ice can rival those above the open ocean depending on particle size. Evaluation of the current model for SSA production from blowing snow showed that the parameterizations used can generally be applied to snow on sea ice. Snow salinity, a sensitive model parameter, depends to a first order on snowpack depth and therefore was higher above first-year sea ice (FYI) than above multi-year sea ice (MYI). Shifts in the ratio of FYI and MYI over time are therefore expected to change the seasonal SSA source flux and contribute to the variability of SSA in ice cores, which represents both an opportunity and a challenge for the quantitative interpretation of sea salt in ice cores as a proxy for sea ice.

The downstream air pollution impacts of the transition from coal to natural gas in the United States

The recent shift in the United States from coal to natural gas as a primary feedstock for the production of electric power has reduced the intensity of sectoral carbon dioxide emissions, but—due to gaps in monitoring—its downstream pollution-related effects have been less well understood. Here, I analyse old units that have been taken offline and new units that have come online to empirically link technology switches to observed aerosol and ozone changes and subsequent impacts on human health, crop yields and regional climate. Between 2005 and 2016 in the continental United States, decommissioning of a coal-fired unit was associated with reduced nearby pollution concentrations and subsequent reductions in mortality and increases in crop yield. In total during this period, the shutdown of coal-fired units saved an estimated 26,610 (5%–95% confidence intervals (CI), 2,725–49,680) lives and 570 million (249–878 million) bushels of corn, soybeans and wheat in their immediate vicinities; these estimates increase when pollution transport-related spillovers are included. Changes in primary and secondary aerosol burdens also altered regional atmospheric reflectivity, raising the average top of atmosphere instantaneous radiative forcing by 0.50 W m−2. Although there are considerable benefits of decommissioning older coal-fired units, the newer natural gas and coal-fired units that have supplanted them are not entirely benign. The recent shift in the United States from coal to natural gas for electric power has reduced the carbon dioxide emissions intensity of electric power production, but the other pollution-related impacts of this shift are not yet known. This study finds that, between 2005 and 2016, decommissioning coal-fired plants in the continental US saved an estimated 26,610 lives and 570 million bushels of corn, soybeans and wheat in their vicinities and also changed regional climate.

Reconciling atmospheric water uptake by hydrate forming salts.

Magnesium and calcium chloride salts contribute to the global atmospheric aerosol burden via emission of sea spray and mineral dust. Their influence on aerosol hygroscopicity and cloud forming potential is important but uncertain with ambiguities between results reported in the literature. To address this, we have conducted measurements of the hygroscopic growth and critical supersaturation of dried, size selected nano-particles made from aqueous solution droplets of MgCl2 and CaCl2, respectively, and compare experimentally derived values with results from state-of-the-art thermodynamic modelling. It is characteristic of both MgCl2 and CaCl2 salts that they bind water in the form of hydrates under a range of ambient conditions. We discuss how hydrate formation affects the particles' water uptake and provide an expression for hydrate correction factors needed in calculations of hygroscopic growth factors, critical super-saturations, and derived κ values of particles containing hydrate forming salts. We demonstrate the importance of accounting for hydrate forming salts when predicting hygroscopic properties of sea spray aerosol.

A New Satellite-Based Global Climatology of Dust Aerosol Optical Depth

AbstractBy mass, dust is the largest contributor to global aerosol burden, yet long-term observational records of dust, particularly over the ocean, are limited. Here, two nearly global observational datasets of dust aerosol optical depthτdare created primarily on the basis of optical measurements of the aerosol column from 1) the Moderate Resolution Imaging Spectroradiometer (MODIS) aboard theTerrasatellite spanning from 2001 to 2018 and 2) the Advanced Very High Resolution Radiometer (AVHRR) from 1981 to 2018. The quality of the new data is assessed by comparison with existing dust datasets that are spatially more limited. Between 2001 and 2018,τddecreased over Asia and increased significantly over the Sahara, Middle East, and parts of eastern Europe, with the largest increase found over the Aral Sea where emissive playa surfaces have been exposed. These daily, observational, and nearly global records of dust will allow for improvement in understanding the role of dust in climate variability.

Climate Forcing and Trends of Organic Aerosols in the Community Earth System Model (CESM2)

AbstractThe Community Earth System Model version 2 (CESM2) includes three main atmospheric configurations: the Community Atmosphere Model version 6 (CAM6) with simplified chemistry and a simplified organic aerosol (OA) scheme, CAM6 with comprehensive tropospheric and stratospheric chemistry representation (CAM6‐chem), and the Whole Atmosphere Community Climate Model version 6 (WACCM6). Both, CAM6‐chem and WACCM6 include a more comprehensive secondary organic aerosols (SOA) approach using the Volatility Basis Set (VBS) scheme and prognostic stratospheric aerosols. This paper describes the different OA schemes available in the different atmospheric configurations of CESM2 and discusses differences in aerosol burden and resulting climate forcings. Derived OA burden and trends differ due to differences in OA formation using the different approaches. Regional differences in Aerosol Optical Depth with larger values using the comprehensive approach occur over SOA source regions. Stronger increasing SOA trends between 1960 and 2015 in WACCM6 compared to CAM6 are due to increasing biogenic emissions aligned with increasing surface temperatures. Using the comprehensive SOA approach further leads to improved comparisons to aircraft observations and SOA formation of ≈143 Tg/yr. We further use WACCM6 to identify source contributions of OA from biogenic, fossil fuel, and biomass burning emissions, to quantify SOA amounts and trends from these sources. Increasing SOA trends between 1960 and 2015 are the result of increasing biogenic emissions aligned with increasing surface temperatures. Biogenic emissions are at least two thirds of the total SOA burden. In addition, SOA source contributions from fossil fuel emissions become more important, with largest values over Southeast Asia. The estimated total anthropogenic forcing of OA in WACCM6 for 1995–2010 conditions is −0.43 W/m2, mostly from the aerosol direct effect.

Evaluation of CNRM Earth System Model, CNRM‐ESM2‐1: Role of Earth System Processes in Present‐Day and Future Climate

AbstractThis study introduces CNRM‐ESM2‐1, the Earth system (ES) model of second generation developed by CNRM‐CERFACS for the sixth phase of the Coupled Model Intercomparison Project (CMIP6). CNRM‐ESM2‐1 offers a higher model complexity than the Atmosphere‐Ocean General Circulation Model CNRM‐CM6‐1 by adding interactive ES components such as carbon cycle, aerosols, and atmospheric chemistry. As both models share the same code, physical parameterizations, and grid resolution, they offer a fully traceable framework to investigate how far the represented ES processes impact the model performance over present‐day, response to external forcing and future climate projections. Using a large variety of CMIP6 experiments, we show that represented ES processes impact more prominently the model response to external forcing than the model performance over present‐day. Both models display comparable performance at replicating modern observations although the mean climate of CNRM‐ESM2‐1 is slightly warmer than that of CNRM‐CM6‐1. This difference arises from land cover‐aerosol interactions where the use of different soil vegetation distributions between both models impacts the rate of dust emissions. This interaction results in a smaller aerosol burden in CNRM‐ESM2‐1 than in CNRM‐CM6‐1, leading to a different surface radiative budget and climate. Greater differences are found when comparing the model response to external forcing and future climate projections. Represented ES processes damp future warming by up to 10% in CNRM‐ESM2‐1 with respect to CNRM‐CM6‐1. The representation of land vegetation and the CO2‐water‐stomatal feedback between both models explain about 60% of this difference. The remainder is driven by other ES feedbacks such as the natural aerosol feedback.

Black carbon aerosol quantification over north-west Himalayas: Seasonal heterogeneity, source apportionment and radiative forcing

Continuous measurements of Black Carbon (BC) aerosol mass concentrations were carried at Dehradun (30.33°N, 78.04°E, 700 m amsl), a semi-urban site in the foothills of north-westHimalayas, India during January 2011–December 2017. We reported both the BC seasonal variations as well as mass concentrations from fossil fuel combustion (BCff) and biomass burning (BCbb) sources. Annual mean BC exhibited a strong seasonal variability with maxima during winter (4.86 ± 0.78 μg m−3) followed by autumn (4.18 ± 0.54 μg m−3), spring (3.93 ± 0.75 μg m−3) and minima during summer (2.41 ± 0.66 μg m−3). Annual averaged BC mass concentrations were 3.85 ± 1.16 μg m−3 varying from 3.29 to 4.37 μg m−3 whereas BCff and BCbb ranged from 0.11 to 7.12 μg m−3 and 0.13–3.6 μg m−3. The percentage contributions from BCff and BCbb to total BC are 66% and 34% respectively, indicating relatively higher contribution from biomass burning as compared to other locations in India. This is explained using potential source contribution function (PSCF) and concentration weighted trajectories (CWT) analysis which reveals the potential sources of BC originating from the north-west and eastern parts of IGP and the western part of the Himalayas that are mostly crop residue burning and forest fire regions in India. The annual mean ARF at top-of-atmosphere (TOA), at surface (SUR), and within the atmosphere (ATM) were found to be −14.84 Wm−2, −43.41 Wm−2, and +28.57 Wm−2 respectively. To understand the impact of columnar aerosol burden on ARF, the radiative forcing efficiency (ARFE) was estimated and averaged values were −31.81, −91.63 and 59.82 Wm−2 τ−1 for TOA, SUR and ATM respectively. The high ARFE within the atmosphere indicates the dominance of absorbing aerosol (BC and dust) over Northwest Himalayas.

Absorption characteristics of aerosols over the central Himalayas and its adjacent foothills

Abstract The absorption characteristics and source processes of aerosols are investigated at two nearby distinct altitude sites: Nainital, located over the central Himalayas (~1958 m amsl) and Pantnagar, in the adjacent foothill region (~231 m amsl) in the Indo-Gangetic Plain region (IGP); based on in-situ measurements and model (GEOS-Chem) simulations. The study reveals the significant influence of biomass burning sources over both the locations during spring, indicating the efficiency of the vertical transport of biomass burning aerosols during the peak of the fire activity period over the northern Indian region. On the other hand, the dominance of fossil fuel emission sources is seen during most part of the year at the mountain site, while biomass/biofuel sources are prevalent at the foothill site. Simulations of different aerosol components in the GEOS-Chem model have revealed that dust aerosols, in addition to carbonaceous aerosols from fossil fuel and biomass burning sources, significantly influence aerosol burden over this broad region covering both high-altitude site Nainital and adjacent foothill site Pantnagar in IGP. Examination of dominant aerosol types and their contribution to the columnar abundance of aerosols is performed. During spring, the contribution of dust aerosols is as high as 22%, even though inorganic aerosols (42%), organic carbon (29%) play a dominant role in modulating aerosol absorption characteristics in the column over this region. This study highlights the importance of absorbing aerosol, their types and quantification for better estimates of radiative forcing of aerosols over this region. This might also provide valuable information for the regional impact assessment of aerosols over the Himalayan region.

Improved tropospheric and stratospheric sulfur cycle in the aerosol–chemistry–climate model SOCOL-AERv2

Abstract. SOCOL-AERv1 was developed as an aerosol–chemistry–climate model to study the stratospheric sulfur cycle and its influence on climate and the ozone layer. It includes a sectional aerosol model that tracks the sulfate particle size distribution in 40 size bins, between 0.39 nm and 3.2 µm. Sheng et al. (2015) showed that SOCOL-AERv1 successfully matched observable quantities related to stratospheric aerosol. In the meantime, SOCOL-AER has undergone significant improvements and more observational datasets have become available. In producing SOCOL-AERv2 we have implemented several updates to the model: adding interactive deposition schemes, improving the sulfate mass and particle number conservation, and expanding the tropospheric chemistry scheme. We compare the two versions of the model with background stratospheric sulfate aerosol observations, stratospheric aerosol evolution after Pinatubo, and ground-based sulfur deposition networks. SOCOL-AERv2 shows similar levels of agreement as SOCOL-AERv1 with satellite-measured extinctions and in situ optical particle counter (OPC) balloon flights. The volcanically quiescent total stratospheric aerosol burden simulated in SOCOL-AERv2 has increased from 109 Gg of sulfur (S) to 160 Gg S, matching the newly available satellite estimate of 165 Gg S. However, SOCOL-AERv2 simulates too high cross-tropopause transport of tropospheric SO2 and/or sulfate aerosol, leading to an overestimation of lower stratospheric aerosol. Due to the current lack of upper tropospheric SO2 measurements and the neglect of organic aerosol in the model, the lower stratospheric bias of SOCOL-AERv2 was not further improved. Model performance under volcanically perturbed conditions has also undergone some changes, resulting in a slightly shorter volcanic aerosol lifetime after the Pinatubo eruption. With the improved deposition schemes of SOCOL-AERv2, simulated sulfur wet deposition fluxes are within a factor of 2 of measured deposition fluxes at 78 % of the measurement stations globally, an agreement which is on par with previous model intercomparison studies. Because of these improvements, SOCOL-AERv2 will be better suited to studying changes in atmospheric sulfur deposition due to variations in climate and emissions.

Vapor-pressure pathways initiate but hydrolysis products dominate the aerosol estimated from organic nitrates.

Organic nitrates contribute significantly to the total organic aerosol burden. However, the formation and loss mechanisms of particulate organic nitrates (PONs) remain poorly understood. In this study, with the CMAQ modeling system, we implement a detailed biogenic volatile organic carbon gas phase oxidation mechanism and an explicit representation of multiphase organic nitrate formation and loss, including both aqueous-phase uptake and vapor-pressure driven partitioning into organic aerosol as well as condensed-phase reactions. We find vapor-pressure dependent partitioning is the leading mechanism for formation of PONs and hydrolysis is a major loss mechanism for PON resulting in substantial amounts of organic aerosol that originate as an organic nitrate. Partitioning and hydrolysis together can produce high concentrations (up to 5 μg/m3) of PON-derived aerosols over the southeast United States. The main source of PON-derived aerosols is monoterpene nitrates that have been chemically processed to lose their nitrate functionality through aqueous chemistry. In contrast, the major portion of aqueous aerosol and in-cloud PON, which retains its nitrate moiety, are soluble isoprene nitrates. We evaluate the model using the observations from the Southern Oxidant and Aerosol Study (SOAS) campaign in the Southeast US in summer 2013 and show implementing aerosol-phase pathways for organic nitrates dramatically improves the magnitude of total alkyl nitrates (ANs) in CMAQ. The contribution of PONs to the total ANs at the SOAS site is estimated to be ~20%, a value in the range of the measurements. The predicted AN composition is shifted from monoterpene to isoprene and anthropogenic organic nitrates.

Multitimescale variations in modeled stratospheric water vapor derived from three modern reanalysis products

Abstract. Stratospheric water vapor (SWV) plays important roles in the radiation budget and ozone chemistry and is a valuable tracer for understanding stratospheric transport. Meteorological reanalyses provide variables necessary for simulating this transport; however, even recent reanalyses are subject to substantial uncertainties, especially in the stratosphere. It is therefore necessary to evaluate the consistency among SWV distributions simulated using different input reanalysis products. In this study, we evaluate the representation of SWV and its variations on multiple timescales using simulations over the period 1980–2013. Our simulations are based on the Chemical Lagrangian Model of the Stratosphere (CLaMS) driven by horizontal winds and diabatic heating rates from three recent reanalyses: ERA-Interim, JRA-55 and MERRA-2. We present an intercomparison among these model results and observationally based estimates using a multiple linear regression method to study the annual cycle (AC), the quasi-biennial oscillation (QBO), and longer-term variability in monthly zonal-mean H2O mixing ratios forced by variations in the El Niño–Southern Oscillation (ENSO) and the volcanic aerosol burden. We find reasonable consistency among simulations of the distribution and variability in SWV with respect to the AC and QBO. However, the amplitudes of both signals are systematically weaker in the lower and middle stratosphere when CLaMS is driven by MERRA-2 than when it is driven by ERA-Interim or JRA-55. This difference is primarily attributable to relatively slow tropical upwelling in the lower stratosphere in simulations based on MERRA-2. Two possible contributors to the slow tropical upwelling in the lower stratosphere are suggested to be the large long-wave cloud radiative effect and the unique assimilation process in MERRA-2. The impacts of ENSO and volcanic aerosol on H2O entry variability are qualitatively consistent among the three simulations despite differences of 50 %–100 % in the magnitudes. Trends show larger discrepancies among the three simulations. CLaMS driven by ERA-Interim produces a neutral to slightly positive trend in H2O entry values over 1980–2013 (+0.01 ppmv decade−1), while both CLaMS driven by JRA-55 and CLaMS driven by MERRA-2 produce negative trends but with significantly different magnitudes (−0.22 and −0.08 ppmv decade−1, respectively).

Exploring accumulation-mode H<sub>2</sub>SO<sub>4</sub> versus SO<sub>2</sub> stratospheric sulfate geoengineering in a sectional aerosol–chemistry–climate model

Abstract. Stratospheric sulfate geoengineering (SSG) could contribute to avoiding some of the adverse impacts of climate change. We used the SOCOL-AER global aerosol–chemistry–climate model to investigate 21 different SSG scenarios, each with 1.83 Mt S yr−1 injected either in the form of accumulation-mode H2SO4 droplets (AM H2SO4), gas-phase SO2 or as combinations of both. For most scenarios, the sulfur was continuously emitted at an altitude of 50 hPa (≈20 km) in the tropics and subtropics. We assumed emissions to be zonally and latitudinally symmetric around the Equator. The spread of emissions ranged from 3.75∘ S–3.75∘ N to 30∘ S–30∘ N. In the SO2 emission scenarios, continuous production of tiny nucleation-mode particles results in increased coagulation, which together with gaseous H2SO4 condensation, produces coarse-mode particles. These large particles are less effective for backscattering solar radiation and have a shorter stratospheric residence time than AM H2SO4 particles. On average, the stratospheric aerosol burden and corresponding all-sky shortwave radiative forcing for the AM H2SO4 scenarios are about 37 % larger than for the SO2 scenarios. The simulated stratospheric aerosol burdens show a weak dependence on the latitudinal spread of emissions. Emitting at 30∘ N–30∘ S instead of 10∘ N–10∘ S only decreases stratospheric burdens by about 10 %. This is because a decrease in coagulation and the resulting smaller particle size is roughly balanced by faster removal through stratosphere-to-troposphere transport via tropopause folds. Increasing the injection altitude is also ineffective, although it generates a larger stratospheric burden, because enhanced condensation and/or coagulation leads to larger particles, which are less effective scatterers. In the case of gaseous SO2 emissions, limiting the sulfur injections spatially and temporally in the form of point and pulsed emissions reduces the total global annual nucleation, leading to less coagulation and thus smaller particles with increased stratospheric residence times. Pulse or point emissions of AM H2SO4 have the opposite effect: they decrease the stratospheric aerosol burden by increasing coagulation and only slightly decrease clear-sky radiative forcing. This study shows that direct emission of AM H2SO4 results in higher radiative forcing for the same sulfur equivalent mass injection strength than SO2 emissions, and that the sensitivity to different injection strategies varies for different forms of injected sulfur.

Transmission of bacteria in bronchiectasis and chronic obstructive pulmonary disease: Low burden of cough aerosols.

Aerosol transmission of Pseudomonas aeruginosa has been suggested as a possible mode of respiratory infection spread in patients with cystic fibrosis (CF); however, whether this occurs in other suppurative lung diseases is unknown. Therefore, we aimed to determine if (i) patients with bronchiectasis (unrelated to CF) or chronic obstructive pulmonary disease (COPD) can aerosolize P. aeruginosa during coughing and (ii) if genetically indistinguishable (shared) P. aeruginosa strains are present in these disease cohorts. People with bronchiectasis or COPD and P. aeruginosa respiratory infection were recruited for two studies. Aerosol study: Participants (n = 20) underwent cough testing using validated cough rigs to determine the survival of P. aeruginosa aerosols in the air over distance and duration. Genotyping study: P. aeruginosa sputum isolates (n = 95) were genotyped using the iPLEX20SNP platform, with a subset subjected to the enterobacterial repetitive intergenic consensus polymerase chain reaction (ERIC-PCR) assay to ascertain their genetic relatedness. Aerosol study: Overall, 7 of 20 (35%) participants released P. aeruginosa cough aerosols during at least one of the cough aerosol tests. These cough aerosols remained viable for 4 m from the source and for 15 min after coughing. The mean total aerosol count of P. aeruginosa at 2 m was two colony-forming units. Typing study: No shared P. aeruginosa strains were identified. Low viable count of P. aeruginosa cough aerosols and a lack of shared P. aeruginosa strains observed suggest that aerosol transmission of P. aeruginosa is an unlikely mode of respiratory infection spread in patients with bronchiectasis and COPD.

Background Conditions Influence the Estimated Cloud Radiative Effects of Anthropogenic Aerosol Emissions From Different Source Regions

AbstractUsing the Community Earth System Model, with the Community Atmosphere Model version 5.3, we investigate the cloud radiative effects of anthropogenic aerosols emitted from different source regions and global shipping. We also analyze aerosol burdens, cloud condensation nuclei concentration, liquid water path, and ice water path. Due to transboundary transport and sublinearity in the response of clouds to aerosols, the cloud radiative effects of emissions from a given source region are influenced by emissions from other source regions. For example, the shortwave cloud radiative effect of shipping is −0.39 ± 0.03 W/m2 when other anthropogenic emissions sources are present (the “present‐day background” assumption) compared with −0.60 ± 0.03 W/m2 when other anthropogenic emissions sources are absent (the “natural background” assumption). In general, the cloud radiative effects are weaker if present‐day background conditions are assumed compared with if natural background conditions are assumed. Assumptions about background conditions should be carefully considered when investigating the climate impacts of aerosol emissions from a given source region.

Droplet activation behaviour of atmospheric black carbon particles in fog as a function of their size and mixing state

Abstract. Among the variety of particle types present in the atmosphere, black carbon (BC), emitted by combustion processes, is uniquely associated with harmful effects to the human body and substantial radiative forcing of the Earth. Pure BC is known to be non-hygroscopic, but its ability to acquire a coating of hygroscopic organic and inorganic material leads to increased diameter and hygroscopicity, facilitating droplet activation. This affects BC radiative forcing through aerosol–cloud interactions (ACIs) and BC life cycle. To gain insights into these processes, we performed a field campaign in winter 2015–2016 in a residential area of Zurich which aimed at establishing relations between the size and mixing state of BC particles and their activation to form droplets in fog. This was achieved by operating a CCN counter (CCNC), a scanning mobility particle sizer (SMPS), a single-particle soot photometer (SP2) and an aerosol chemical speciation monitor (ACSM) behind a combination of a total- and an interstitial-aerosol inlet. Our results indicate that in the morning hours of weekdays, the enhanced traffic emissions caused peaks in the number fraction of externally mixed BC particles, which do not act as CCN within the CCNC. The very low effective peak supersaturations (SSpeak) occurring in fog (between approximately 0.03 % and 0.06 % during this campaign) restrict droplet activation to a minor fraction of the aerosol burden (around 0.5 % to 1 % of total particle number concentration between 20 and 593 nm) leading to very selective criteria on diameter and chemical composition. We show that bare BC cores are unable to activate to fog droplets at such low SSpeak, while BC particles surrounded by thick coating have very similar activation behaviour to BC-free particles. Using simplified κ-Köhler theory combined with the ZSR mixing rule assuming spherical core–shell particle geometry constrained with single-particle measurements of respective volumes, we found good agreement between the predicted and the directly observed size- and mixing-state-resolved droplet activation behaviour of BC-containing particles in fog. This successful closure demonstrates the predictability of their droplet activation in fog with a simplified theoretical model only requiring size and mixing state information, which can also be applied in a consistent manner in model simulations.