The impact of historical land use change from 1850 to 2000 on particulate matter and ozone

Anthropogenic land use change (LUC) since pre-industrial (1850) has altered the vegetation distribution and density around the world. We use a global model (GEOS-Chem) to assess the attendant changes in surface air quality and the direct radiative forcing (DRF). We focus our analysis on secondary particulate matter and tropospheric ozone formation. The general trend of expansion of managed ecosystems (croplands and pasturelands) at the expense of natural ecosystems has led to an 11 % decline in global mean biogenic volatile organic compound emissions. Concomitant growth in agricultural activity has more than doubled ammonia emissions and increased emissions of nitrogen oxides from soils by more than 50 %. Conversion to croplands has also led to a widespread increase in ozone dry deposition velocity. Together these changes in biosphere-atmosphere exchange have led to a 14 % global mean increase in biogenic secondary organic aerosol (BSOA) surface concentrations, a doubling of surface aerosol nitrate concentrations, and local changes in surface ozone of up to 8.5 ppb. We assess a global mean LUC-DRF of +0.017 Wm−2, −0.071 Wm−2, and −0.01 Wm−2 for BSOA, nitrate, and tropospheric ozone, respectively. We conclude that the DRF and the perturbations in surface air quality associated with LUC are substantial and should be considered alongside changes in anthropogenic emissions and climate feedbacks in chemistry-climate studies.https://www.atmos-chem-phys.net/16/14997/2016/acp-16-14997-2016.pdfhttps://www.atmos-chem-phys.net/16/14997/2016/acp-16-14997-2016.pdfPublished versio

Global modeling of secondary organic aerosol formation from aromatic hydrocarbons: high- vs low-yield pathways

Formation of SOA from the aromatic species toluene, xylene, and, for the first time, benzene, is added to a global chemical transport model. A simple mechanism is presented that accounts for competition between low and high-yield pathways of SOA formation, wherein secondary gas-phase products react further with either nitrogen oxide (NO) or hydroperoxy radical (HO2) to yield semi- or non-volatile products, respectively. Aromatic species yield more SOA when they react with OH in regions where the [NO]/[HO2] ratios are lower. The SOA yield thus depends upon the distribution of aromatic emissions, with biomass burning emissions being in areas with lower [NO]/[HO2] ratios, and the reactivity of the aromatic with respect to OH, as a lower initial reactivity allows transport away from industrial source regions, where [NO]/[HO2] ratios are higher, to more remote regions, where this ratio is lower and, hence, the ultimate yield of SOA is higher. As a result, benzene is estimated to be the most important aromatic species with regards to formation of SOA, with a total production nearly equal that of toluene and xylene combined. In total, while only 39% percent of the aromatic species react via the low-NOx pathway, 72% of the aromatic SOA is formed via this mechanism. Predicted SOA concentrations from aromatics in the Eastern United States and Eastern Europe are actually largest during the summer, when the [NO]/[HO2] ratio is lower. Global production of SOA from aromatic sources is estimated at 3.5 Tg/yr, resulting in a global burden of 0.08 Tg, twice as large as previous estimates. The contribution of these largely anthropogenic sources to global SOA is still small relative to biogenic sources, which are estimated to comprise 90% of the global SOA burden, about half of which comes from isoprene. Compared to recent observations, it would appear there are additional pathways beyond those accounted for here for production of anthropogenic SOA. However, owing to differences in spatial distributions of sources and seasons of peak production, there are still regions in which aromatic SOA produced via the mechanisms identified here are predicted to contribute substantially to, and even dominate, the local SOA concentrations, such as outflow regions from North America and South East Asia during the wintertime, though total SOA concentrations there are small (~0.1 μg/m^³)

The Parkes HI Zone of Avoidance Survey

A blind HI survey of the extragalactic sky behind the southern Milky Way has been conducted with the multibeam receiver on the 64-m Parkes radio telescope. The survey covers the Galactic longitude range 212 < l < 36 and Galactic latitudes |b| < 5, and yields 883 galaxies to a recessional velocity of 12,000 km/s. The survey covers the sky within the HIPASS area to greater sensitivity, finding lower HI-mass galaxies at all distances, and probing more completely the large-scale structures at and beyond the distance of the Great Attractor. Fifty-one percent of the HI detections have an optical/NIR counterpart in the literature. A further 27% have new counterparts found in existing, or newly obtained, optical/NIR images. The counterpart rate drops in regions of high foreground stellar crowding and extinction, and for low-HI mass objects. Only 8% of all counterparts have a previous optical redshift measurement. A notable new galaxy is HIZOA J1353-58, a possible companion to the Circinus galaxy. Merging this catalog with the similarly-conducted northern extension (Donley et al. 2005), large-scale structures are delineated, including those within the Puppis and Great Attractor regions, and the Local Void. Several newly-identified structures are revealed here for the first time. Three new galaxy concentrations (NW1, NW2 and NW3) are key in confirming the diagonal crossing of the Great Attractor Wall between the Norma cluster and the CIZA J1324.7-5736 cluster. Further contributors to the general mass overdensity in that area are two new clusters (CW1 and CW2) in the nearer Centaurus Wall, one of which forms part of the striking 180 deg (100/h Mpc) long filament that dominates the southern sky at velocities of ~3000 km/s, and the suggestion of a further Wall at the Great Attractor distance at slightly higher longitudes.Comment: Published in Astronomical Journal 9 February 2016 (accepted 26 September 2015); 42 pages, 7 tables, 18 figures, main figures data tables only available in the on-line version of journa

Investigating the observed sensitivities of air-quality extremes to meteorological drivers via quantile regression

Air pollution variability is strongly dependent on meteorology. However, quantifying the impacts of changes in regional climatology on pollution extremes can be difficult due to the many non-linear and competing meteorological influences on the production, transport, and removal of pollutant species. Furthermore, observed pollutant levels at many sites show sensitivities at the extremes that differ from those of the overall mean, indicating relationships that would be poorly characterized by simple linear regressions. To address this challenge, we apply quantile regression to observed daily ozone (O[subscript 3]) and fine particulate matter (PM[subscript 2.5]) levels and reanalysis meteorological fields in the USA over the past decade to specifically identify the meteorological sensitivities of higher pollutant levels. From an initial set of over 1700 possible meteorological indicators (including 28 meteorological variables with 63 different temporal options), we generate reduced sets of O[subscript 3] and PM[subscript 2.5] indicators for both summer and winter months, analyzing pollutant sensitivities to each for response quantiles ranging from 2 to 98 %. Primary covariates connected to high-quantile O[subscript 3] levels include temperature and relative humidity in the summer, while winter O[subscript 3] levels are most commonly associated with incoming radiation flux. Covariates associated with summer PM[subscript 2.5] include temperature, wind speed, and tropospheric stability at many locations, while stability, humidity, and planetary boundary layer height are the key covariates most frequently associated with winter PM[subscript 2.5]. We find key differences in covariate sensitivities across regions and quantiles. For example, we find nationally averaged sensitivities of 95th percentile summer O[subscript 3] to changes in maximum daily temperature of approximately 0.9 ppb °C[superscript −1], while the sensitivity of 50th percentile summer O[subscript 3] (the annual median) is only 0.6 ppb °C[superscript −1]. This gap points to differing sensitivities within various percentiles of the pollutant distribution, highlighting the need for statistical tools capable of identifying meteorological impacts across the entire response spectrum.United States. Environmental Protection Agency (Grant/Cooperative Agreement RD-83522801

A decadal satellite analysis of the origins and impacts of smoke in Colorado

We analyze the record of aerosol optical depth (AOD) measured by the MODerate resolution Imaging Spectroradiometer (MODIS) aboard the Terra satellite in combination with surface PM[subscript 2.5] to investigate the impact of fires on aerosol loading and air quality over Colorado from 2000 to 2012, and to evaluate the contribution of local versus transported smoke. Fire smoke contributed significantly to the AOD levels observed over Colorado. During the worst fire seasons of 2002 and 2012, average MODIS AOD over the Colorado Front Range corridor were 20–50% larger than the other 11 yr studied. Surface PM[subscript 2.5] was also unusually elevated during fire events and concentrations were in many occasions above the daily National Ambient Air Quality Standard (35 μg m[superscript −3]) and even reached locally unhealthy levels (> 100 μg m[superscript −3]) over populated areas during the 2012 High Park fire and the 2002 Hayman fire. Over the 13 yr examined, long-range transport of smoke from northwestern US and even California (> 1500 km distance) occurred often and affected AOD and surface PM[subscript 2.5]. During most of the transport events, MODIS AOD and surface PM[subscript 2.5] were reasonable correlated (r[superscript 2] = 0.2–0.9), indicating that smoke subsided into the Colorado boundary layer and reached surface levels. However, that is not always the case since at least one event of AOD enhancement was disconnected from the surface (r[superscript 2]<0.01 and low PM[subscript 2.5] levels). Observed plume heights from the Multi-angle Imaging SpectroRadiometer (MISR) satellite instrument and vertical aerosol profiles measured by the space-based Cloud-Aerosol LIdar with Orthogonal Polarization (CALIOP) showed a complex vertical distribution of smoke emitted by the High Park fire in 2012. Smoke was detected from a range of 1.5 to 7.5 km altitude at the fire origin and from ground levels to 12.3 km altitude far away from the source. The variability of smoke altitude as well as the local meteorology were key in determining the aerosol loading and air quality over the Colorado Front Range region. Our results underline the importance of accurate characterization of the vertical distribution of smoke for estimating the air quality degradation associated with fire activity and its link to human health.United States. National Park Service (Grant H2370 094000/J2350103006

How emissions, climate, and land use change will impact mid-century air quality over the United States: A focus on effects at national parks

We use a global coupled chemistry-climate-land model (CESM) to assess the integrated effect of climate, emissions and land use changes on annual surface O3 and PM2.5 in the United States with a focus on national parks (NPs) and wilderness areas, using the RCP4.5 and RCP8.5 projections. We show that, when stringent domestic emission controls are applied, air quality is predicted to improve across the US, except surface O3 over the western and central US under RCP8.5 conditions, where rising background ozone counteracts domestic emission reductions. Under the RCP4.5 scenario, surface O3 is substantially reduced (about 5 ppb), with daily maximum 8 h averages below the primary US Environmental Protection Agency (EPA) National Ambient Air Quality Standards (NAAQS) of 75 ppb (and even 65 ppb) in all the NPs. PM2.5 is significantly reduced in both scenarios (4 μg m-3; ~50%), with levels below the annual US EPA NAAQS of 12 μg m-3 across all the NPs; visibility is also improved (10-15 dv; >75 km in visibility range), although some western US parks with Class I status (40-74 % of total sites in the US) are still above the 2050 planned target level to reach the goal of natural visibility conditions by 2064. We estimate that climate-driven increases in fire activity may dominate summertime PM2.5 over the western US, potentially offsetting the large PM2.5 reductions from domestic emission controls, and keeping visibility at present-day levels in many parks. Our study indicates that anthropogenic emission patterns will be important for air quality in 2050. However, climate and land use changes alone may lead to a substantial increase in surface O3 (2-3 ppb) with important consequences for O3 air quality and ecosystem degradation at the US NPs. Our study illustrates the need to consider the effects of changes in climate, vegetation, and fires in future air quality management and planning and emission policy making

Investigating organic aerosol loading in the remote marine environment

Aerosol loading in the marine environment is investigated using aerosol composition measurements from several research ship campaigns (ICEALOT, MAP, RHaMBLe, VOCALS and OOMPH), observations of total AOD column from satellite (MODIS) and ship-based instruments (Maritime Aerosol Network, MAN), and a global chemical transport model (GEOS-Chem). This work represents the most comprehensive evaluation of oceanic OM emission inventories to date, by employing aerosol composition measurements obtained from campaigns with wide spatial and temporal coverage. The model underestimates AOD over the remote ocean on average by 0.02 (21 %), compared to satellite observations, but provides an unbiased simulation of ground-based Maritime Aerosol Network (MAN) observations. Comparison with cruise data demonstrates that the GEOS-Chem simulation of marine sulfate, with the mean observed values ranging between 0.22 μg m−3 and 1.34 μg m−3, is generally unbiased, however surface organic matter (OM) concentrations, with the mean observed concentrations between 0.07 μg m−3 and 0.77 μg m−3, are underestimated by a factor of 2–5 for the standard model run. Addition of a sub-micron marine OM source of approximately 9 TgC yr−1 brings the model into agreement with the ship-based measurements, however this additional OM source does not explain the model underestimate of marine AOD. The model underestimate of marine AOD is therefore likely the result of a combination of satellite retrieval bias and a missing marine aerosol source (which exhibits a different spatial pattern than existing aerosol in the model)