Wildfires emit significant amounts of pollutants that degrade air quality. Plumes from three wildfires in the western U.S. were measured from aircraft during the Studies of Emissions and Atmospheric Composition, Clouds and Climate Coupling by Regional Surveys (SEAC4RS) and the Biomass Burning Observation Project (BBOP), both in summer 2013. This study reports an extensive set of emission factors (EFs) for over 80 gases and 5 components of submicron particulate matter (PM1) from these temperate wildfires. These include rarely, or never before, measured oxygenated volatile organic compounds and multifunctional organic nitrates. The observed EFs are compared with previous measurements of temperate wildfires, boreal forest fires, and temperate prescribed fires. The wildfires emitted high amounts of PM1 (with organic aerosol (OA) dominating the mass) with an average EF that is more than 2 times the EFs for prescribed fires. The measured EFs were used to estimate the annual wildfire emissions of carbon monoxide, nitrogen oxides, total nonmethane organic compounds, and PM1 from 11 western U.S. states. The estimated gas emissions are generally comparable with the 2011 National Emissions Inventory (NEI). However, our PM1 emission estimate (1530 ± 570 Gg yr−1) is over 3 times that of the NEI PM2.5 estimate and is also higher than the PM2.5 emitted from all other sources in these states in the NEI. This study indicates that the source of OA from biomass burning in the western states is significantly underestimated. In addition, our results indicate that prescribed burning may be an effective method to reduce fine particle emissions.

Abstract. The VAMOS 1 Ocean-Cloud-Atmosphere-Land Study Regional Experiment (VOCALS-REx) was an international field program designed to make observations of poorly understood but critical components of the coupled climate system of the southeast Pacific. This region is characterized by strong coastal upwelling, the coolest SSTs in the tropi- cal belt, and is home to the largest subtropical stratocumulus deck on Earth. The field intensive phase of VOCALSREx took place during October and November 2008 and constitutes a critical part of a broader CLIVAR program (VOCALS) designed to develop and promote scientific activities leading to improved understanding, model simulations, and predictions of the southeastern Pacific (SEP) coupled ocean-atmosphere-land system, on diurnal to interannual timescales. The other major components of VOCALS are a modeling program with a model hierarchy ranging from the local to global scales, and a suite of extended observations from regular research cruises, instrumented moorings, Published by Copernicus Publications on behalf of the European Geosciences Union. R. Wood et al.: VOCALS operationsand satellites. The two central themes of VOCALS-REx focus upon (a) links between aerosols, clouds and precipitation and their impacts on marine stratocumulus radiative properties, and (b) physical and chemical couplings between the upper ocean and the lower atmosphere, including the role that mesoscale ocean eddies play. A set of hypotheses designed to be tested with the combined field, monitoring and modeling work in VOCALS is presented here. A further goal of VOCALS-REx is to provide datasets for the evaluation and improvement of large-scale numerical models. VOCALSREx involved five research aircraft, two ships and two surface sites in northern Chile. We describe the instrument payloads and key mission strategies for these platforms and give a summary of the missions conducted.

Abstract. The time evolution of aerosol concentration and chemical composition in a megacity urban plume was determined based on 8 flights of the DOE G-1 aircraft in and downwind of Mexico City during the March 2006 MILAGRO field campaign. A series of selection criteria are imposed to eliminate data points with non-urban emission influences. Biomass burning has urban and non-urban sources that are distinguished on the basis of CH3CN and CO. In order to account for dilution in the urban plume, aerosol concentrations are normalized to CO which is taken as an inert tracer of urban emission, proportional to the emissions of aerosol precursors. Time evolution is determined with respect to photochemical age defined as −Log10 (NOx/NOy). The geographic distribution of photochemical age and CO is examined, confirming the picture that Mexico City is a source region and that pollutants become more dilute and aged as they are advected towards T1 and T2, surface sites that are located at the fringe of the City and 35 km to the NE, respectively. Organic aerosol (OA) per ppm CO is found to increase 7 fold over the range of photochemical ages studied, corresponding to a change in NOx/NOy from nearly 100% to 10%. In the older samples the nitrate/CO ratio has leveled off suggesting that evaporation and formation of aerosol nitrate are in balance. In contrast, OA/CO increases with age in older samples, indicating that OA is still being formed. The amount of carbon equivalent to the deduced change in OA/CO with age is 56 ppbC per ppm CO. At an aerosol yield of 5% and 8% for low and high yield aromatic compounds, it is estimated from surface hydrocarbon observations that only ~9% of the OA formation can be accounted for. A comparison of OA/CO in Mexico City and the eastern U.S. gives no evidence that aerosol yields are higher in a more polluted environment.

In support of the first Tropospheric Ozone Assessment Report (TOAR) a relational database of global surface ozone observations has been developed and populated with hourly measurement data and enhanced metadata. A comprehensive suite of ozone data products including standard statistics, health and vegetation impact metrics, and trend information, are made available through a common data portal and a web interface. These data form the basis of the TOAR analyses focusing on human health, vegetation, and climate relevant ozone issues, which are part of this special feature.Cooperation among many data centers and individual researchers worldwide made it possible to build the world's largest collection of in-situ hourly surface ozone data covering the period from 1970 to 2015. By combining the data from almost 10,000 measurement sites around the world with global metadata information, new analyses of surface ozone have become possible, such as the first globally consistent characterisations of measurement sites as either urban or rural/remote. Exploitation of these global metadata allows for new insights into the global distribution, and seasonal and long-term changes of tropospheric ozone and they enable TOAR to perform the first, globally consistent analysis of present-day ozone concentrations and recent ozone changes with relevance to health, agriculture, and climate.Considerable effort was made to harmonize and synthesize data formats and metadata information from various networks and individual data submissions. Extensive quality control was applied to identify questionable and erroneous data, including changes in apparent instrument offsets or calibrations. Such data were excluded from TOAR data products. Limitations of a posteriori data quality assurance are discussed. As a result of the work presented here, global coverage of surface ozone data for scientific analysis has been significantly extended. Yet, large gaps remain in the surface observation network both in Schultz et al: Tropospheric Ozone Assessment Report Art. 58, page 2 of 26 terms of regions without monitoring, and in terms of regions that have monitoring programs but no public access to the data archive. Therefore future improvements to the database will require not only improved data harmonization, but also expanded data sharing and increased monitoring in data-sparse regions.

Abstract. The radiative impact of organic aerosols (OA) is a large source of uncertainty in estimating the global direct radiative effect (DRE) of aerosols. This radiative impact includes not only light scattering but also light absorption from a subclass of OA referred to as brown carbon (BrC). However, the absorption properties of BrC are poorly understood, leading to large uncertainties in modeling studies. To obtain observational constraints from measurements, a simple absorption Ångström exponent (AAE) method is often used to separate the contribution of BrC absorption from that of black carbon (BC). However, this attribution method is based on assumptions regarding the spectral dependence of BC that are often violated in the ambient atmosphere. Here we develop a new AAE method which improves upon previous approaches by using the information from the wavelengthdependent measurements themselves and by allowing for an atmospherically relevant range of BC properties, rather than fixing these at a single assumed value. We note that constraints on BC optical properties and mixing state would help further improve this method. We apply this method to multiwavelength absorption aerosol optical depth (AAOD) measurements at AERONET sites worldwide and surface aerosol absorption measurements at multiple ambient sites. We estimate that BrC globally contributes up to 40 % of the seasonally averaged absorption at 440 nm. We find that the mass absorption coefficient of OA (OA-MAC) is positively correlated with the BC / OA mass ratio. Based on the variability in BC properties and BC / OA emission ratio, we estimate a range of 0.05-1.5 m 2 g −1 for OA-MAC at 440 nm. Using the combination of AERONET and OMI UV absorption observations we estimate that the AAE 388/440 nm for BrC is generally ∼ 4 worldwide, with a smaller value in Europe (< 2). Our analyses of observations at two surface sites (Cape Cod, to the southeast of Boston, and the GoAmazon2014/5 T3 site, to the west of Manaus, Brazil) reveal no significant relationship between BrC absorptivity and photochemical aging in urban-influenced conditions. However, the absorption of BrC measured during the biomass burning season near Manaus is found to decrease with photochemical aging with a lifetime of ∼ 1 day. This lifetime is comparable to previous observations within a biomass burning plume but much slower than estimated from laboratory studies. Given the large uncertainties associated with AERONET retrievals of AAOD, the most challenging aspect of our analysis is that an accurate, globally distributed, multiple-wavelength aerosol absorption measurement dataset is unavailable at present. Thus, achieving a better understanding of the properties, evolution, and impacts of global BrC will rely on the future deployment of accurate multiple-wavelength absorption measurements toPublished by Copernicus Publications on behalf of the European Geosciences Union.