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Abstract. Secondary organic aerosol (SOA) accounts for a significant fraction of ambient tropospheric aerosol and a detailed knowledge of the formation, properties and transformation of SOA is therefore required to evaluate its impact on atmospheric processes, climate and human health. The chemical and physical processes associated with SOA formation are complex and varied, and, despite considerable progress in recent years, a quantitative and predictive understanding of SOA formation does not exist and therefore represents a major research challenge in atmospheric science. This review begins with an update on the current state of knowledge on the global SOA budget and is followed by an overview of the atmospheric degradation mechanisms for SOA precursors, gas-particle partitioning theory and the analytical techniques used to determine the chemical composition of SOA. A survey of recent laboratory, field and modeling studies is also presented. The following topical and emerging issues are highlighted and discussed in detail: molecular characterization of biogenic SOA constituents, condensed phase reactions and oligomerization, the interaction of atmospheric organic components with sulfuric acid, the chemical and photochemical processing of organics in the atmospheric aqueous phase, aerosol formation from real plant emissions, interaction of atmospheric organic components with water, thermodynamics and mixtures in atmospheric models. Finally, the major challenges ahead in laboratory, field and modeling studies of SOA are discussed and recommendations for future research directions are proposed.

Abstract. Reactive gases and aerosols are produced by terrestrial ecosystems, processed within plant canopies, and can then be emitted into the above-canopy atmosphere. Estimates of the above-canopy fluxes are needed for quantitative earth system studies and assessments of past, present and future air quality and climate. The Model of Emissions of Gases and Aerosols from Nature (MEGAN) is described and used to quantify net terrestrial biosphere emission of isoprene into the atmosphere. MEGAN is designed for both global and regional emission modeling and has global coverage with ~1 km2 spatial resolution. Field and laboratory investigations of the processes controlling isoprene emission are described and data available for model development and evaluation are summarized. The factors controlling isoprene emissions include biological, physical and chemical driving variables. MEGAN driving variables are derived from models and satellite and ground observations. Tropical broadleaf trees contribute almost half of the estimated global annual isoprene emission due to their relatively high emission factors and because they are often exposed to conditions that are conducive for isoprene emission. The remaining flux is primarily from shrubs which have a widespread distribution. The annual global isoprene emission estimated with MEGAN ranges from about 500 to 750 Tg isoprene (440 to 660 Tg carbon) depending on the driving variables which include temperature, solar radiation, Leaf Area Index, and plant functional type. The global annual isoprene emission estimated using the standard driving variables is ~600 Tg isoprene. Differences in driving variables result in emission estimates that differ by more than a factor of three for specific times and locations. It is difficult to evaluate isoprene emission estimates using the concentration distributions simulated using chemistry and transport models, due to the substantial uncertainties in other model components, but at least some global models produce reasonable results when using isoprene emission distributions similar to MEGAN estimates. In addition, comparison with isoprene emissions estimated from satellite formaldehyde observations indicates reasonable agreement. The sensitivity of isoprene emissions to earth system changes (e.g., climate and land-use) demonstrates the potential for large future changes in emissions. Using temperature distributions simulated by global climate models for year 2100, MEGAN estimates that isoprene emissions increase by more than a factor of two. This is considerably greater than previous estimates and additional observations are needed to evaluate and improve the methods used to predict future isoprene emissions.

Abstract. The present paper reviews existing knowledge with regard to Organic Aerosol (OA) of importance for global climate modelling and defines critical gaps needed to reduce the involved uncertainties. All pieces required for the representation of OA in a global climate model are sketched out with special attention to Secondary Organic Aerosol (SOA): The emission estimates of primary carbonaceous particles and SOA precursor gases are summarized. The up-to-date understanding of the chemical formation and transformation of condensable organic material is outlined. Knowledge on the hygroscopicity of OA and measurements of optical properties of the organic aerosol constituents are summarized. The mechanisms of interactions of OA with clouds and dry and wet removal processes parameterisations in global models are outlined. This information is synthesized to provide a continuous analysis of the flow from the emitted material to the atmosphere up to the point of the climate impact of the produced organic aerosol. The sources of uncertainties at each step of this process are highlighted as areas that require further studies.

Abstract. Aerosols affect the climate system by changing cloud characteristics in many ways. They act as cloud condensation and ice nuclei, they may inhibit freezing and they could have an influence on the hydrological cycle. While the cloud albedo enhancement (Twomey effect) of warm clouds received most attention so far and traditionally is the only indirect aerosol forcing considered in transient climate simulations, here we discuss the multitude of effects. Different approaches how the climatic implications of these aerosol effects can be estimated globally as well as improvements that are needed in global climate models in order to better represent indirect aerosol effects are discussed in this paper.

Abstract. Many atmospheric chemicals occur in the gas phase as well as in liquid cloud droplets and aerosol particles. Therefore, it is necessary to understand the distribution between the phases. According to Henry's law, the equilibrium ratio between the abundances in the gas phase and in the aqueous phase is constant for a dilute solution. Henry's law constants of trace gases of potential importance in environmental chemistry have been collected and converted into a uniform format. The compilation contains 17 350 values of Henry's law constants for 4632 species, collected from 689 references. It is also available at http://www.henrys-law.org.

Abstract. We present and discuss a new dataset of gridded emissions covering the historical period (1850–2000) in decadal increments at a horizontal resolution of 0.5° in latitude and longitude. The primary purpose of this inventory is to provide consistent gridded emissions of reactive gases and aerosols for use in chemistry model simulations needed by climate models for the Climate Model Intercomparison Program #5 (CMIP5) in support of the Intergovernmental Panel on Climate Change (IPCC) Fifth Assessment report (AR5). Our best estimate for the year 2000 inventory represents a combination of existing regional and global inventories to capture the best information available at this point; 40 regions and 12 sectors are used to combine the various sources. The historical reconstruction of each emitted compound, for each region and sector, is then forced to agree with our 2000 estimate, ensuring continuity between past and 2000 emissions. Simulations from two chemistry-climate models are used to test the ability of the emission dataset described here to capture long-term changes in atmospheric ozone, carbon monoxide and aerosol distributions. The simulated long-term change in the Northern mid-latitudes surface and mid-troposphere ozone is not quite as rapid as observed. However, stations outside this latitude band show much better agreement in both present-day and long-term trend. The model simulations indicate that the concentration of carbon monoxide is underestimated at the Mace Head station; however, the long-term trend over the limited observational period seems to be reasonably well captured. The simulated sulfate and black carbon deposition over Greenland is in very good agreement with the ice-core observations spanning the simulation period. Finally, aerosol optical depth and additional aerosol diagnostics are shown to be in good agreement with previously published estimates and observations.

Abstract. A new inventory of air pollutant emissions in Asia in the year 2006 is developed to support the Intercontinental Chemical Transport Experiment-Phase B (INTEX-B) funded by the National Aeronautics and Space Administration (NASA). Emissions are estimated for all major anthropogenic sources, excluding biomass burning. We estimate total Asian anthropogenic emissions in the year 2006 as follows: 47.1 Tg SO2, 36.7 Tg NOx, 298.2 Tg CO, 54.6 Tg NMVOC, 29.2 Tg PM10, 22.2 Tg PM2.5, 2.97 Tg BC, and 6.57 Tg OC. We emphasize emissions from China because they dominate the Asia pollutant outflow to the Pacific and the increase of emissions from China since 2000 is of great concern. We have implemented a series of improved methodologies to gain a better understanding of emissions from China, including a detailed technology-based approach, a dynamic methodology representing rapid technology renewal, critical examination of energy statistics, and a new scheme of NMVOC speciation for model-ready emissions. We estimate China's anthropogenic emissions in the year 2006 to be as follows: 31.0 Tg SO2, 20.8 Tg NOx, 166.9 Tg CO, 23.2 Tg NMVOC, 18.2 Tg PM10, 13.3 Tg PM2.5, 1.8 Tg BC, and 3.2 Tg OC. We have also estimated 2001 emissions for China using the same methodology and found that all species show an increasing trend during 2001–2006: 36% increase for SO2, 55% for NOx, 18% for CO, 29% for VOC, 13% for PM10, and 14% for PM2.5, BC, and OC. Emissions are gridded at a resolution of 30 min×30 min and can be accessed at our web site (http://mic.greenresource.cn/intex-b2006).

Abstract. To tackle the problem of severe air pollution, China has implemented active clean air policies in recent years. As a consequence, the emissions of major air pollutants have decreased and the air quality has substantially improved. Here, we quantified China's anthropogenic emission trends from 2010 to 2017 and identified the major driving forces of these trends by using a combination of bottom-up emission inventory and index decomposition analysis (IDA) approaches. The relative change rates of China's anthropogenic emissions during 2010–2017 are estimated as follows: −62 % for SO2, −17 % for NOx, +11 % for nonmethane volatile organic compounds (NMVOCs), +1 % for NH3, −27 % for CO, −38 % for PM10, −35 % for PM2.5, −27 % for BC, −35 % for OC, and +16 % for CO2. The IDA results suggest that emission control measures are the main drivers of this reduction, in which the pollution controls on power plants and industries are the most effective mitigation measures. The emission reduction rates markedly accelerated after the year 2013, confirming the effectiveness of China's Clean Air Action that was implemented since 2013. We estimated that during 2013–2017, China's anthropogenic emissions decreased by 59 % for SO2, 21 % for NOx, 23 % for CO, 36 % for PM10, 33 % for PM2.5, 28 % for BC, and 32 % for OC. NMVOC emissions increased and NH3 emissions remained stable during 2010–2017, representing the absence of effective mitigation measures for NMVOCs and NH3 in current policies. The relative contributions of different sectors to emissions have significantly changed after several years' implementation of clean air policies, indicating that it is paramount to introduce new policies to enable further emission reductions in the future.

Abstract. This article, the second in the series, presents kinetic and photochemical data evaluated by the IUPAC Subcommittee on Gas Kinetic Data Evaluation for Atmospheric Chemistry. It covers the gas phase and photochemical reactions of Organic species, which were last published in 1999, and were updated on the IUPAC website in late 2002, and subsequently during the preparation of this article. The article consists of a summary table of the recommended rate coefficients, containing the recommended kinetic parameters for the evaluated reactions, and eight appendices containing the data sheets, which provide information upon which the recommendations are made.

Abstract. Biomass burning represents an important source of atmospheric aerosols and greenhouse gases, yet little is known about its interannual variability or the underlying mechanisms regulating this variability at continental to global scales. Here we investigated fire emissions during the 8 year period from 1997 to 2004 using satellite data and the CASA biogeochemical model. Burned area from 2001–2004 was derived using newly available active fire and 500 m. burned area datasets from MODIS following the approach described by Giglio et al. (2006). ATSR and VIRS satellite data were used to extend the burned area time series back in time through 1997. In our analysis we estimated fuel loads, including organic soil layer and peatland fuels, and the net flux from terrestrial ecosystems as the balance between net primary production (NPP), heterotrophic respiration (Rh), and biomass burning, using time varying inputs of precipitation (PPT), temperature, solar radiation, and satellite-derived fractional absorbed photosynthetically active radiation (fAPAR). For the 1997–2004 period, we found that on average approximately 58 Pg C year−1 was fixed by plants as NPP, and approximately 95% of this was returned back to the atmosphere via Rh. Another 4%, or 2.5 Pg C year−1 was emitted by biomass burning; the remainder consisted of losses from fuel wood collection and subsequent burning. At a global scale, burned area and total fire emissions were largely decoupled from year to year. Total carbon emissions tracked burning in forested areas (including deforestation fires in the tropics), whereas burned area was largely controlled by savanna fires that responded to different environmental and human factors. Biomass burning emissions showed large interannual variability with a range of more than 1 Pg C year−1, with a maximum in 1998 (3.2 Pg C year−1) and a minimum in 2000 (2.0 Pg C year−1).