Less atmospheric radiative heating due to aspherical dust with coarser size

Mineral dust aerosols cool and warm the atmosphere by scattering and absorbing both solar (short-wave: SW) and thermal (long-wave: LW) radiation. However, large uncertainties remain in dust radiative effects, largely due to differences in the dust size distribution and optical properties simulated in Earth system models. Here, we improve the simulated dust properties with datasets that leverage measurements of size-resolved dust concentration and asphericity factor (improved simulation) in a coupled global chemical transport model (IMPACT) with a radiative transfer module (RRTMG) (default simulation). The global and annual average of dust aerosol optical depth at 550 nm (DAOD550) from the improved simulation (0.029) falls within the range of a semi-observation-based estimate (0.030 ± 0.005), in contrast to that (0.023) of the default simulation. Improved agreement against semi-observation-based estimate of the radiative effect efficiency was obtained using less absorptive SW and more absorptive LW dust refractive indices. Our sensitivity simulations reveal that the improved simulation leads to a similar net global dust radiative effect at the Top Of Atmosphere (TOA) on a global scale to the default simulation (−0.08 vs. −0.09 W ·m−2) but results in less cooling at the surface (−0.23 vs. −0.88 W ·m−2), because of enhanced LW warming by coarser aspherical dust. Our results thus suggest less atmospheric radiative heating due to aspherical dust with coarser size over the major source regions (0.15 vs. 0.79 W ·m−2 on a global scale).

Regional and intercontinental pollution signatures on modeled and measured PAN at northern mid-latitude mountain sites

Peroxy acetyl nitrate (PAN) is the most important reservoir species for nitrogen oxides (NOx) in the remote troposphere. Upon decomposition in remote regions, PAN promotes efficient ozone production. We evaluate monthly mean PAN abundances from global chemical transport model simulations (HTAP1) for 2001 with measurements from five northern mid-latitude mountain sites (four European and one North American). The multi-model mean generally captures the observed monthly mean PAN but individual models simulate a factor of ~ 4–8 range in monthly abundances. We quantify PAN source-receptor relationships at the measurement sites with sensitivity simulations that decrease regional anthropogenic emissions of PAN (and ozone) precursors by 20 % from North America (NA), Europe (EU), and East Asia (EA). The HTAP1 models attribute more of the observed PAN at Jungfraujoch (Switzerland) to emissions in NA and EA, and less to EU, than a prior trajectory-based estimate. The trajectory-based and modeling approaches agree that EU emissions play a role in the observed springtime PAN maximum at Jungfraujoch. The signal from anthropogenic emissions on PAN is strongest at Jungfraujoch and Mount Bachelor (Oregon, U.S.A.) during April. In this month, PAN source-receptor relationships correlate both with model differences in regional anthropogenic volatile organic compound (AVOC) emissions and with ozone source-receptor relationships. PAN observations at mountaintop sites can thus provide key information for evaluating models, including links between PAN and ozone production and source-receptor relationships. Establishing routine, long-term, mountaintop measurements is essential given the large observed interannual variability in PAN.

Characteristics of intercontinental transport of tropospheric ozone from Africa to Asia

Based on 20-year simulations using a global chemical transport model, GEOS-Chem, and a trajectory model, HYSPLIT, the transport of ozone produced in the African troposphere to Asia is investigated. The study shows that the influence of African ozone on Asia varies largely in time and space. In the middle and upper troposphere, the inflow of African ozone to Asia peaks around 25° N, being the largest in boreal winter and early spring (> 10 ppbv) and the lowest in boreal summer (

The impact of snow nitrate photolysis on boundary layer chemistry and the recycling and redistribution of reactive nitrogen across Antarctica and Greenland in a global chemical transport model

The formation and recycling of reactive nitrogen (NO, NO2, HONO) at the air–snow interface has implications for air quality and the oxidation capacity of the atmosphere in snow-covered regions. Nitrate (NO3−) photolysis in snow provides a source of oxidants (e.g., hydroxyl radical) and oxidant precursors (e.g., nitrogen oxides) to the overlying boundary layer, and alters the concentration and isotopic (e.g., δ15N) signature of NO3− preserved in ice cores. We have incorporated an idealized snowpack with a NO3− photolysis parameterization into a global chemical transport model (Goddard Earth Observing System (GEOS) Chemistry model, GEOS-Chem) to examine the implications of snow NO3− photolysis for boundary layer chemistry, the recycling and redistribution of reactive nitrogen, and the preservation of ice-core NO3− in ice cores across Antarctica and Greenland, where observations of these parameters over large spatial scales are difficult to obtain. A major goal of this study is to examine the influence of meteorological parameters and chemical, optical, and physical snow properties on the magnitudes and spatial patterns of snow-sourced NOx fluxes and the recycling and redistribution of reactive nitrogen across Antarctica and Greenland. Snow-sourced NOx fluxes are most influenced by temperature-dependent quantum yields of NO3− photolysis, photolabile NO3− concentrations in snow, and concentrations of light-absorbing impurities (LAIs) in snow. Despite very different assumptions about snowpack properties, the range of model-calculated snow-sourced NOx fluxes are similar in Greenland (0.5–11 × 108 molec cm−2 s−1) and Antarctica (0.01–6.4 × 108 molec cm−2 s−1) due to the opposing effects of higher concentrations of both photolabile NO3− and LAIs in Greenland compared to Antarctica. Despite the similarity in snow-sourced NOx fluxes, these fluxes lead to smaller factor increases in mean austral summer boundary layer mixing ratios of total nitrate (HNO3+ NO3−), NOx, OH, and O3 in Greenland compared to Antarctica because of Greenland's proximity to pollution sources. The degree of nitrogen recycling in the snow is dependent on the relative magnitudes of snow-sourced NOx fluxes versus primary NO3− deposition. Recycling of snow NO3− in Greenland is much less than in Antarctica Photolysis-driven loss of snow NO3− is largely dependent on the time that NO3− remains in the snow photic zone (up to 6.5 years in Antarctica and 7 months in Greenland), and wind patterns that redistribute snow-sourced reactive nitrogen across Antarctica and Greenland. The loss of snow NO3− is higher in Antarctica (up to 99 %) than in Greenland (up to 83 %) due to deeper snow photic zones and lower snow accumulation rates in Antarctica. Modeled enrichments in ice-core δ15N(NO3−) due to photolysis-driven loss of snow NO3− ranges from 0 to 363 ‰ in Antarctica and 0 to 90 ‰ in Greenland, with the highest fraction of NO3− loss and largest enrichments in ice-core δ15N(NO3−) at high elevations where snow accumulation rates are lowest. There is a strong relationship between the degree of photolysis-driven loss of snow NO3− and the degree of nitrogen recycling between the air and snow throughout all of Greenland and in Antarctica where snow accumulation rates are greater than 130 kg m−2 a−1 in the present day.

Estimates of black carbon emissions in the western United States using the GEOS-Chem adjoint model

We estimate black carbon (BC) emissions in the western United States for July–September 2006 by inverting surface BC concentrations from the Interagency Monitoring of Protected Visual Environments (IMPROVE) network using a global chemical transport model (GEOS-Chem) and its adjoint. Our best estimate of the BC emissions is 49.9 Gg at 2° × 2.5° (a factor of 2.1 increase) and 47.3 Gg at 0.5° × 0.667° (1.9 times increase). Model results now capture the observed major fire episodes with substantial bias reductions (~ 35 % at 2° × 2.5° and ~ 15 % at 0.5° × 0.667°). The emissions are ~ 20–50 % larger than those from our earlier analytical inversions (Mao et al., 2014). The discrepancy is especially drastic in the partitioning of anthropogenic versus biomass burning emissions. The August biomass burning BC emissions are 4.6–6.5 Gg and anthropogenic BC emissions 8.6–12.8 Gg, varying with the model resolution, error specifications, and subsets of observations used. On average both anthropogenic and biomass burning emissions in the adjoint inversions increase 2-fold relative to the respective {a priori} emissions, in distinct contrast to the halving of the anthropogenic and tripling of the biomass burning emissions in the analytical inversions. We attribute these discrepancies to the inability of the adjoint inversion system, with limited spatiotemporal coverage of the IMPROVE observations, to effectively distinguish collocated anthropogenic and biomass burning emissions on model grid scales. This calls for concurrent measurements of other tracers of biomass burning and fossil fuel combustion (e.g., carbon monoxide and carbon isotopes). We find that the adjoint inversion system as is has sufficient information content to constrain the total emissions of BC on the model grid scales.