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Colorado air quality impacted by long-range-transported aerosol: a set of case studies during the 2015 Pacific Northwest fires

Biomass burning plumes containing aerosols from forest fires can be transported long distances, which can ultimately impact climate and air quality in regions far from the source. Interestingly, these fires can inject aerosols other than smoke into the atmosphere, which very few studies have evidenced. Here, we demonstrate a set of case studies of long-range transport of mineral dust aerosols in addition to smoke from numerous fires (including predominantly forest fires and a few grass/shrub fires) in the Pacific Northwest to Colorado, US. These aerosols were detected in Boulder, Colorado, along the Front Range using beta-ray attenuation and energy-dispersive X-ray fluorescence spectroscopy, and corroborated with satellite-borne lidar observations of smoke and dust. Further, we examined the transport pathways of these aerosols using air mass trajectory analysis and regional- and synoptic-scale meteorological dynamics. Three separate events with poor air quality and increased mass concentrations of metals from biomass burning (S and K) and minerals (Al, Si, Ca, Fe, and Ti) occurred due to the introduction of smoke and dust from regional- and synoptic-scale winds. Cleaner time periods with good air quality and lesser concentrations of biomass burning and mineral metals between the haze events were due to the advection of smoke and dust away from the region. Dust and smoke present in biomass burning haze can have diverse impacts on visibility, health, cloud formation, and surface radiation. Thus, it is important to understand how aerosol populations can be influenced by long-range-transported aerosols, particularly those emitted from large source contributors such as wildfires.
Global impacts of tropospheric halogens (Cl, Br, I) on oxidants and composition in GEOS-Chem

We present a simulation of the global present-day composition of the troposphere which includes the chemistry of halogens (Cl, Br, I). Building on previous work within the GEOS-Chem model we include emissions of inorganic iodine from the oceans, anthropogenic and biogenic sources of halogenated gases, gas phase chemistry, and a parameterised approach to heterogeneous halogen chemistry. Consistent with Schmidt et al. (2016) we do not include sea-salt debromination. Observations of halogen radicals (BrO, IO) are sparse but the model has some skill in reproducing these. Modelled IO shows both high and low biases when compared to different datasets, but BrO concentrations appear to be modelled low. Comparisons to the very sparse observations dataset of reactive Cl species suggest the model represents a lower limit of the impacts of these species, likely due to underestimates in emissions and therefore burdens. Inclusion of Cl, Br, and I results in a general improvement in simulation of ozone (O3) concentrations, except in polar regions where the model now underestimates O3 concentrations. Halogen chemistry reduces the global tropospheric O3 burden by 18.6 %, with the O3 lifetime reducing from 26 to 22 days. Global mean OH concentrations of 1.28  ×  106 molecules cm−3 are 8.2 % lower than in a simulation without halogens, leading to an increase in the CH4 lifetime (10.8 %) due to OH oxidation from 7.47 to 8.28 years. Oxidation of CH4 by Cl is small (∼  2 %) but Cl oxidation of other VOCs (ethane, acetone, and propane) can be significant (∼  15–27 %). Oxidation of VOCs by Br is smaller, representing 3.9 % of the loss of acetaldehyde and 0.9 % of the loss of formaldehyde.
Controlled meteorological (CMET) free balloon profiling of the Arctic atmospheric boundary layer around Spitsbergen compared to ERA-Interim and Arctic System Reanalyses

Observations from CMET (Controlled Meteorological) balloons are analysed to provide insights into tropospheric meteorological conditions (temperature, humidity, wind) around Svalbard, European High Arctic. Five Controlled Meteorological (CMET) balloons were launched from Ny-Ålesund in Svalbard (Spitsbergen) over 5–12 May 2011 and measured vertical atmospheric profiles over coastal areas to both the east and west. One notable CMET flight achieved a suite of 18 continuous soundings that probed the Arctic marine boundary layer (ABL) over a period of more than 10 h. Profiles from two CMET flights are compared to model output from ECMWF Era-Interim reanalysis (ERA-I) and to a high-resolution (15 km) Arctic System Reanalysis (ASR) product. To the east of Svalbard over sea ice, the CMET observed a stable ABL profile with a temperature inversion that was reproduced by ASR but not captured by ERA-I. In a coastal ice-free region to the west of Svalbard, the CMET observed a stable ABL with strong wind shear. The CMET profiles document increases in ABL temperature and humidity that are broadly reproduced by both ASR and ERA-I. The ASR finds a more stably stratified ABL than observed but captured the wind shear in contrast to ERA-I. Detailed analysis of the coastal CMET-automated soundings identifies small-scale temperature and humidity variations with a low-level flow and provides an estimate of local wind fields. We demonstrate that CMET balloons are a valuable approach for profiling the free atmosphere and boundary layer in remote regions such as the Arctic, where few other in situ observations are available for model validation.
Mineralogical properties and internal structures of individual fine particles of Saharan dust

Mineral dust interacts with incoming/outgoing radiation, gases, other aerosols, and clouds. The assessment of its optical and chemical impacts requires knowledge of the physical and chemical properties of bulk dust and single particles. Despite the existence of a large body of data from field measurements and laboratory analyses, the internal properties of single dust particles have not been defined precisely. Here, we report on the mineralogical organization and internal structures of individual fine ( <  5 µm) Saharan dust particles sampled at Tenerife, Canary Islands. The bulk of Tenerife dust was composed of clay minerals (81 %), followed by quartz (10 %), plagioclase (3 %), and K-feldspar (2 %). Cross-sectional slices of Saharan dust particles prepared by the focused ion beam technique were analyzed by transmission electron microscopy (TEM) to probe the particle interiors. TEM analysis showed that the most common particle type was clay-rich agglomerate, dominated by illite–smectite series clay minerals with subordinate kaolinite. Submicron grains of iron (hydr)oxides (goethite and hematite) were commonly dispersed through the clay-rich particles. The median total volume of the iron (hydr)oxide grains included in the dust particles was estimated to be about 1.5 % vol. The average iron content of clay minerals, assuming 14 wt % H2O, was determined to be 5.0 wt %. Coarse mineral cores, several micrometers in size, were coated with thin layers of clay-rich agglomerate. Overall, the dust particles were roughly ellipsoidal, with an average axial ratio of 1.4 : 1.0 : 0.5. The mineralogical and structural properties of single Saharan dust particles provide a basis for the modeling of dust radiative properties. Major iron-bearing minerals, such as illite–smectite series clay minerals and iron (hydr)oxides, were commonly submicron- to nano-sized, possibly enhancing their biogeochemical availability to remote marine ecosystems lacking micronutrients.
What controls the low ice number concentration in the upper troposphere?

Cirrus clouds in the tropical tropopause play a key role in regulating the moisture entering the stratosphere through their dehydrating effect. Low ice number concentrations ( <  200 L−1) and high supersaturations (150–160 %) have been observed in these clouds. Different mechanisms have been proposed to explain these low ice number concentrations, including the inhibition of homogeneous freezing by the deposition of water vapour onto pre-existing ice crystals, heterogeneous ice formation on glassy organic aerosol ice nuclei (IN), and limiting the formation of ice number from high-frequency gravity waves. In this study, we examined the effect from three different representations of updraft velocities, the effect from pre-existing ice crystals, the effect from different water vapour deposition coefficients (α  =  0.1 or 1), and the effect of 0.1 % of the total secondary organic aerosol (SOA) particles acting as IN. Model-simulated ice crystal numbers are compared against an aircraft observational dataset. Including the effect from water vapour deposition on pre-existing ice particles can effectively reduce simulated in-cloud ice number concentrations for all model setups. A larger water vapour deposition coefficient (α  =  1) can also efficiently reduce ice number concentrations at temperatures below 205 K, but less so at higher temperatures. SOA acting as IN is most effective at reducing ice number concentrations when the effective updraft velocities are moderate ( ∼  0.05–0.2 m s−1). However, the effects of including SOA as IN and using (α  =  1) are diminished when the effect from pre-existing ice is included. When a grid-resolved large-scale updraft velocity ( <  0.1 m s−1) is used, the ice nucleation parameterization with homogeneous freezing only or with both homogeneous freezing and heterogeneous nucleation is able to generate low ice number concentrations in good agreement with observations for temperatures below 205 K as long as the pre-existing ice effect is included. For the moderate updraft velocity ( ∼  0.05–0.2 m s−1), simulated ice number concentrations in good agreement with observations at temperatures below 205 K can be achieved if effects from pre-existing ice, a larger water vapour deposition coefficient (α  =  1), and SOA IN are all included. Using the sub-grid-scale turbulent kinetic energy (TKE)-based updraft velocity ( ∼  0–2 m s−1) always overestimates the ice number concentrations at temperatures below 205 K but compares well with observations at temperatures above 205 K when the pre-existing ice effect is included.
Global tropospheric hydroxyl distribution, budget and reactivity

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

This study investigates the Reynolds-number dependence of turbulence enhancement on the collision growth of cloud droplets. The Onishi turbulent coagulation kernel proposed in Onishi et al. (2015) is updated by using the direct numerical simulation (DNS) results for the Taylor-microscale-based Reynolds number (Reλ) up to 1140. The DNS results for particles with a small Stokes number (St) show a consistent Reynolds-number dependence of the so-called clustering effect with the locality theory proposed by Onishi et al. (2015). It is confirmed that the present Onishi kernel is more robust for a wider St range and has better agreement with the Reynolds-number dependence shown by the DNS results. The present Onishi kernel is then compared with the Ayala–Wang kernel (Ayala et al., 2008a; Wang et al., 2008). At low and moderate Reynolds numbers, both kernels show similar values except for r2 ∼ r1, for which the Ayala–Wang kernel shows much larger values due to its large turbulence enhancement on collision efficiency. A large difference is observed for the Reynolds-number dependences between the two kernels. The Ayala–Wang kernel increases for the autoconversion region (r1, r2 < 40 µm) and for the accretion region (r1 < 40 and r2 > 40 µm; r1 > 40 and r2 < 40 µm) as Reλ increases. In contrast, the Onishi kernel decreases for the autoconversion region and increases for the rain–rain self-collection region (r1, r2 > 40 µm). Stochastic collision–coalescence equation (SCE) simulations are also conducted to investigate the turbulence enhancement on particle size evolutions. The SCE with the Ayala–Wang kernel (SCE-Ayala) and that with the present Onishi kernel (SCE-Onishi) are compared with results from the Lagrangian Cloud Simulator (LCS; Onishi et al., 2015), which tracks individual particle motions and size evolutions in homogeneous isotropic turbulence. The SCE-Ayala and SCE-Onishi kernels show consistent results with the LCS results for small Reλ. The two SCE simulations, however, show different Reynolds-number dependences, indicating possible large differences in atmospheric turbulent clouds with large Reλ.
Monthly and spatially resolved black carbon emission inventory of India: uncertainty analysis

Black carbon (BC) emissions from India for the year 2011 are estimated to be 901.11 ± 151.56 Gg yr−1 based on a new ground-up, GIS-based inventory. The grid-based, spatially resolved emission inventory includes, in addition to conventional sources, emissions from kerosene lamps, forest fires, diesel-powered irrigation pumps and electricity generators at mobile towers. The emissions have been estimated at district level and were spatially distributed onto grids at a resolution of 40 × 40 km2. The uncertainty in emissions has been estimated using a Monte Carlo simulation by considering the variability in activity data and emission factors. Monthly variation of BC emissions has also been estimated to account for the seasonal variability. To the total BC emissions, domestic fuels contributed most significantly (47 %), followed by industry (22 %), transport (17 %), open burning (12 %) and others (2 %). The spatial and seasonal resolution of the inventory will be useful for modeling BC transport in the atmosphere for air quality, global warming and other process-level studies that require greater temporal resolution than traditional inventories.
Current and future levels of mercury atmospheric pollution on a global scale

An assessment of current and future emissions, air concentrations, and atmospheric deposition of mercury worldwide is presented on the basis of results obtained during the performance of the EU GMOS (Global Mercury Observation System) project. Emission estimates for mercury were prepared with the main goal of applying them in models to assess current (2013) and future (2035) air concentrations and atmospheric deposition of this contaminant. The combustion of fossil fuels (mainly coal) for energy and heat production in power plants and in industrial and residential boilers, as well as artisanal and small-scale gold mining, is one of the major anthropogenic sources of Hg emissions to the atmosphere at present. These sources account for about 37 and 25 % of the total anthropogenic Hg emissions globally, estimated to be about 2000 t. Emissions in Asian countries, particularly in China and India, dominate the total emissions of Hg. The current estimates of mercury emissions from natural processes (primary mercury emissions and re-emissions), including mercury depletion events, were estimated to be 5207 t year−1, which represents nearly 70 % of the global mercury emission budget. Oceans are the most important sources (36 %), followed by biomass burning (9 %). A comparison of the 2035 anthropogenic emissions estimated for three different scenarios with current anthropogenic emissions indicates a reduction of these emissions in 2035 up to 85 % for the best-case scenario. Two global chemical transport models (GLEMOS and ECHMERIT) have been used for the evaluation of future mercury pollution levels considering future emission scenarios. Projections of future changes in mercury deposition on a global scale simulated by these models for three anthropogenic emissions scenarios of 2035 indicate a decrease in up to 50 % deposition in the Northern Hemisphere and up to 35 % in Southern Hemisphere for the best-case scenario. The EU GMOS project has proved to be a very important research instrument for supporting the scientific justification for the Minamata Convention and monitoring of the implementation of targets of this convention, as well as the EU Mercury Strategy. This project provided the state of the art with regard to the development of the latest emission inventories for mercury, future emission scenarios, dispersion modelling of atmospheric mercury on a global and regional scale, and source–receptor techniques for mercury emission apportionment on a global scale.
Chemical ionization of clusters formed from sulfuric acid and dimethylamine or diamines

Chemical ionization (CI) mass spectrometers are used to study atmospheric nucleation by detecting clusters produced by reactions of sulfuric acid and various basic gases. These instruments typically use nitrate to deprotonate and thus chemically ionize the clusters. In this study, we compare cluster concentrations measured using either nitrate or acetate. Clusters were formed in a flow reactor from vapors of sulfuric acid and dimethylamine, ethylene diamine, tetramethylethylene diamine, or butanediamine (also known as putrescine). These comparisons show that nitrate is unable to chemically ionize clusters with high base content. In addition, we vary the ion–molecule reaction time to probe ion processes which include proton-transfer, ion–molecule clustering, and decomposition of ions. Ion decomposition upon deprotonation by acetate/nitrate was observed. More studies are needed to quantify to what extent ion decomposition affects observed cluster content and concentrations, especially those chemically ionized with acetate since it deprotonates more types of clusters than nitrate. Model calculations of the neutral and ion cluster formation pathways are also presented to better identify the cluster types that are not efficiently deprotonated by nitrate. Comparison of model and measured clusters indicate that sulfuric acid dimers with two diamines and sulfuric acid trimers with two or more base molecules are not efficiently chemical ionized by nitrate. We conclude that acetate CI provides better information on cluster abundancies and their base content than nitrate CI.