Abstract. Aerosols affect the Earth's energy budget directly by scattering and absorbing radiation and indirectly by acting as cloud condensation nuclei and, thereby, affecting cloud properties. However, large uncertainties exist in current estimates of aerosol forcing because of incomplete knowledge concerning the distribution and the physical and chemical properties of aerosols as well as aerosol-cloud interactions. In recent years, a great deal of effort has gone into improving measurements and datasets. It is thus feasible to shift the estimates of aerosol forcing from largely model-based to increasingly measurement-based. Our goal is to assess current observational capabilities and identify uncertainties in the aerosol direct forcing through comparisons of different methods with independent sources of uncertainties. Here we assess the aerosol optical depth (τ ), direct radiative effect (DRE) by natural and anthropogenic aerosols, and direct climate forcing (DCF) by anthropogenic aerosols, focusing on satellite and ground-based measurements supplemented by global chemical transport modelCorrespondence to: H. Yu (hyu@climate.gsfc.nasa.gov) (CTM) simulations. The multi-spectral MODIS measures global distributions of aerosol optical depth (τ ) on a daily scale, with a high accuracy of ±0.03±0.05τ over ocean. The annual average τ is about 0.14 over global ocean, of which about 21%±7% is contributed by human activities, as estimated by MODIS fine-mode fraction. The multiangle MISR derives an annual average AOD of 0.23 over global land with an uncertainty of ∼20% or ±0.05. These high-accuracy aerosol products and broadband flux measurements from CERES make it feasible to obtain observational constraints for the aerosol direct effect, especially over global the ocean. A number of measurement-based approaches estimate the clear-sky DRE (on solar radiation) at the top-of-atmosphere (TOA) to be about −5.5±0.2 Wm −2 (median ± standard error from various methods) over the global ocean. Accounting for thin cirrus contamination of the satellite derived aerosol field will reduce the TOA DRE to −5.0 Wm −2 . Because of a lack of measurements of aerosol absorption and difficulty in characterizing land surface reflection, estimates of DRE over land and at the ocean surface are currently realized through a combination of satellite Published by Copernicus GmbH on behalf of the European Geosciences Union. 614H. Yu et al.: Measurement-based aerosol direct forcing retrievals, surface measurements, and model simulations, and are less constrained. Over the oceans the surface DRE is estimated to be −8.8±0.7 Wm −2 . Over land, an integration of satellite retrievals and model simulations derives a DRE of −4.9±0.7 Wm −2 and −11.8±1.9 Wm −2 at the TOA and surface, respectively. CTM simulations derive a wide range of DRE estimates that on average are smaller than the measurement-based DRE by about 30-40%, even after accounting for thin cirrus and cloud contamination.A number of issues remain. Current estimates of the aerosol direct effect ...

Published by Copernicus Publications on behalf of the European Geosciences Union. 8340 X. Lu et al.: Exploring 2016-2017 surface ozone pollution over ChinaBVOC ozone enhancements) and ozone chemical production, increase the thermal decomposition of peroxyacetyl nitrate (PAN), and further decrease ozone dry deposition velocity. More stringent emission control measures are thus required to offset the adverse effects of unfavorable meteorology, such as high temperature, on surface ozone air quality.

.[1] The aerosol direct solar effect under clear sky is assessed by (1) combining multiple aerosol characterizations and (2) using the satellite-retrieved land surface albedo. The aerosol characterization is made through an integration of the MODerate resolution Imaging Spectroradiometer (MODIS) retrievals and the Georgia Tech/Goddard Global Ozone Chemistry Aerosol Radiation and Transport (GOCART) model simulations. The spectral and bidirectional albedo of land surface is derived from MODIS. On a global average, the solar forcing at the top of atmosphere (TOA) DF TOA is À4.5 Wm À2 , of which about 1/3 is contributed by a sum of natural and anthropogenic sulfate and carbonaceous aerosols. Though the optical depth is about 50% higher over land than over ocean, no significant land-ocean contrast in this TOA forcing is observed. It is reduced by larger aerosol absorption and higher surface albedo over land. As a result of absorption by soot and dust, a much larger surface cooling and substantial atmospheric absorption coexist over land and adjacent oceans. Globally, the surface cooling DF SFC is about À9.9 Wm À2 , and the atmospheric absorption DF AIR is about 5.4 Wm À2 , suggesting that more than half of the surface cooling results from the atmospheric absorption. Sensitivity tests show that an inclusion of MODIS-derived anisotropy of land surface reflection reduces the diurnal variation of TOA solar forcing, because of aerosol-induced changes in the fraction of direct beam and hence in the effective reflection from the surface. Constraining the GOCART dust absorption with recent measurements reduces DF AIR and DF SFC by 1.3 Wm À2 and 0.9 Wm À2 , respectively, and increases the TOA cooling by 0.4 Wm À2 .

Abstract. Aerosols affect the Earth's energy budget ''directly'' by scattering and absorbing radiation and ''indirectly'' by acting as cloud condensation nuclei and, thereby, affecting cloud properties. However, large uncertainties exist in current estimates of aerosol forcing because of incomplete knowledge concerning the distribution and the physical and chemical properties of aerosols as well as aerosol-cloud interactions. In recent years, a great deal of effort has gone into improving measurements and datasets. It is thus feasible to shift the estimates of aerosol forcing from largely model-based to increasingly measurement-based. Here we assess the aerosol optical depth, direct radiative effect (DRE) by natural and anthropogenic aerosols, and direct climate forcing (DCF) by anthropogenic aerosols, focusing on satellite and ground-based measurements supplemented by global chemical transport model (CTM) simulations. The multi-spectral MODIS measures global distributions of aerosol optical thickness (τ) on a daily scale, with a high accuracy of ±0.03±0.05τ over ocean. The annual average τ is about 0.14 over global ocean, of which about 21% is contributed by human activities, as determined by MODIS fine-mode fraction. The multi-angle MISR derives an annual average AOT of 0.23 over global land with an uncertainty of ~20% or ± 0.05. These high-accuracy aerosol products and broadband flux measurements from CERES make it feasible to obtain observational constraints for the aerosol direct effect, especially over global ocean. A number of measurement-based approaches estimate the clear-sky DRE (on solar radiation) at the top-of-atmosphere (TOA) to be about −5.5±0.2 Wm−2 (median ± standard error) over global ocean. Accounting for thin cirrus contamination of the satellite derived aerosol field will reduce the TOA DRE to −5.0 Wm−2. Because of a lack of measurements of aerosol absorption and difficulty in characterizing land surface reflection, estimates of DRE over land and at the ocean surface are currently realized through a combination of satellite retrievals, surface measurements, and model simulations, and are less constrained. Over the ocean surface, the DRE is estimated to be −8.8±0.4 Wm-2. Over land, an integration of satellite retrievals and model simulations derives a DRE of −4.9±0.7 Wm−2 and −11.8±1.9 Wm−2 at the TOA and surface, respectively. CTM simulations derive a wide range of DRE estimates that on average are smaller than the measurement-based DRE by about 30–40%, even after accounting for thin cirrus and cloud contamination. Despite these achievements, a number of issues remain open and more efforts are required to address them. Current estimates of the aerosol direct effect over land are poorly constrained. Uncertainties of DRE estimates are also larger on regional scales than on a global scale and large discrepancies exist between different approaches. The characterization of aerosol absorption and vertical distribution remains challenging. The aerosol direct effect in the thermal infrared range and under cloudy condition remains relatively unexplored and quite uncertain, because of a lack of global systematic aerosol vertical profile measurements. A coordinated research strategy needs to be developed for integration and assimilation of satellite measurements into models to constrain model simulations. Hopefully, enhanced measurement capabilities in the next few years and high-level scientific cooperation, will further advance our knowledge.

Intensive agricultural activities in the North China Plain (NCP) lead to substantial emissions of nitrogen oxides (NOx) from soil, while the role of this source on local severe ozone pollution is unknown. Here we use a mechanistic parameterization of soil NOx emissions combined with two atmospheric chemistry models to investigate the issue. We find that the presence of soil NOx emissions in the NCP significantly reduces the sensitivity of ozone to anthropogenic emissions. The maximum ozone air quality improvements in July 2017, as can be achieved by controlling all domestic anthropogenic emissions of air pollutants, decrease by 30% due to the presence of soil NOx. This effect causes an emission control penalty such that large additional emission reductions are required to achieve ozone regulation targets. As NOx emissions from fuel combustion are being controlled, the soil emission penalty would become increasingly prominent and shall be considered in emission control strategies.