Abstract. The direct radiative effect (DRE) of aerosols, which is the instantaneous radiative impact of all atmospheric particles on the Earth's energy balance, is sometimes confused with the direct radiative forcing (DRF), which is the change in DRE from pre-industrial to present-day (not including climate feedbacks). In this study we couple a global chemical transport model (GEOS-Chem) with a radiative transfer model (RRTMG) to contrast these concepts. We estimate a global mean all-sky aerosol DRF of −0.36 Wm −2 and a DRE of −1.83 Wm −2 for 2010. Therefore, natural sources of aerosol (here including fire) affect the global energy balance over four times more than do present-day anthropogenic aerosols. If global anthropogenic emissions of aerosols and their precursors continue to decline as projected in recent scenarios due to effective pollution emission controls, the DRF will shrink (−0.22 Wm −2 for 2100). Secondary metrics, like DRE, that quantify temporal changes in both natural and anthropogenic aerosol burdens are therefore needed to quantify the total effect of aerosols on climate.

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[1] We use a global chemical transport model (GEOS-Chem) to interpret aircraft curtain observations of black carbon (BC) aerosol over the Pacific from 85°N to 67°S during the 2009-2011 HIAPER (High-Performance Instrumented Airborne Platform for Environmental Research) Pole-to-Pole Observations (HIPPO) campaigns. Observed concentrations are very low, implying much more efficient scavenging than is usually implemented in models. Our simulation with a global source of 6.5 Tg a À1 and mean tropospheric lifetime of 4.2 days (versus 6.8 ± 1.8 days for the Aerosol Comparisons between Observations and Models (AeroCom) models) successfully simulates BC concentrations in source regions and continental outflow and captures the principal features of the HIPPO data but is still higher by a factor of 2 (1.48 for column loads) over the Pacific. It underestimates BC absorbing aerosol optical depths (AAODs) from the Aerosol Robotic Network by 32% on a global basis. Only 8.7% of global BC loading in GEOS-Chem is above 5 km, versus 21 ± 11% for the AeroCom models, with important implications for radiative forcing estimates. Our simulation yields a global BC burden of 77 Gg, a global mean BC AAOD of 0.0017, and a top-of-atmosphere direct radiative forcing (TOA DRF) of 0.19 W m À2 , with a range of 0.17-0.31 W m À2 based on uncertainties in the BC atmospheric distribution. Our TOA DRF is lower than previous estimates (0.27 ± 0.06 W m À2 in AeroCom, 0.65-0.9 W m À2 in more recent studies). We argue that these previous estimates are biased high because of excessive BC concentrations over the oceans and in the free troposphere.

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Experimental and technoeconomic analysis of a catalytic process for the conversion of whole biomass into jet fuel.

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Aircraft emissions impact human health though degradation of air quality. The majority of previous analyses of air quality impacts from aviation have considered only landing and takeoff emissions. We show that aircraft cruise emissions impact human health over a hemispheric scale and provide the first estimate of premature mortalities attributable to aircraft emissions globally. We estimate ∼8000 premature mortalities per year are attributable to aircraft cruise emissions. This represents ∼80% of the total impact of aviation (where the total includes the effects of landing and takeoff emissions), and ∼1% of air quality-related premature mortalities from all sources. However, we note that the impact of landing and takeoff emissions is likely to be under-resolved. Secondary H(2)SO(4)-HNO(3)-NH(3) aerosols are found to dominate mortality impacts. Due to the altitude and region of the atmosphere at which aircraft emissions are deposited, the extent of transboundary air pollution is particularly strong. For example, we describe how strong zonal westerly winds aloft, the mean meridional circulation around 30-60°N, interaction of aircraft-attributable aerosol precursors with background ammonia, and high population densities in combination give rise to an estimated ∼3500 premature mortalities per year in China and India combined, despite their relatively small current share of aircraft emissions. Subsidence of aviation-attributable aerosol and aerosol precursors occurs predominantly around the dry subtropical ridge, which results in reduced wet removal of aviation-attributable aerosol. It is also found that aircraft NO(x) emissions serve to increase oxidation of nonaviation SO(2), thereby further increasing the air quality impacts of aviation. We recommend that cruise emissions be explicitly considered in the development of policies, technologies and operational procedures designed to mitigate the air quality impacts of air transportation.

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