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.

, and extinction (light attenuation within an optical cavity). The study covered an experimental matrix consisting of 318 runs that systematically tested the performance of instruments across a range of parameters including: fuel equivalence ratio (1.8 ≤ φ ≤ 5), particle shape (mass-mobility exponent ( D f m ), 2.0 ≤ D f m ≤ 3.0), particle mobility size (30 ≤ d m ≤ 300 nm), black carbon mass (0.07 ≤ m BC ≤ 4.2 fg) and particle chemical composition. In selected runs, particles were coated with sulfuric acid or dioctyl sebacate (DOS) (0.5 ≤ r ve ≤ 201 nm) where r ve is the change in the volume equivalent radius due to the coating material. SOOT PARTICLE INSTRUMENT INTER-COMPARISON 593The effect of non-absorbing coatings on instrument response was determined. Changes in the morphology of fractal soot particles were monitored during coating and denuding processes and the effect of particle shape on instrument response was determined. The combination of optical and mass based measurements was used to determine the mass specific absorption coefficient for denuded soot particles. The single scattering albedo of the particles was also measured. An overview of the experiments and sample results are presented.

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.

Observations from June to October 2016, from a surface‐based ARM Mobile Facility deployment on Ascension Island (8°S, 14.5°W) indicate that refractory black carbon (rBC) is almost always present within the boundary layer. The rBC mass concentrations, light absorption coefficients, and cloud condensation nuclei concentrations vary in concert and synoptically, peaking in August. Light absorption coefficients at three visible wavelengths as a function of rBC mass are approximately double that calculated from black carbon in lab studies. A spectrally‐flat absorption angstrom exponent suggests most of the light absorption is from lens‐coated black carbon. The single‐scattering‐albedo increases systematically from August to October in both 2016 and 2017, with monthly means of 0.78 ± 0.02 (August), 0.81 ± 0.03 (September), and 0.83 ± 0.03 (October) at the green wavelength. Boundary layer aerosol loadings are only loosely correlated with total aerosol optical depth, with smoke more likely to be present in the boundary layer earlier in the biomass burning season, evolving to smoke predominantly present above the cloud layers in September–October, typically resting upon the cloud top inversion. The time period with the campaign‐maximum near‐surface light absorption and column aerosol optical depth, on 13–16 August 2016, is investigated further. Backtrajectories that indicate more direct boundary layer transport westward from the African continent is central to explaining the elevated surface aerosol loadings.

[1] The large uncertainty associated with black carbon (BC) direct forcing is due, in part, to the dependence of light absorption of BC-containing particles on the position of the BC within the particle. It is predicted that this absorption will be greatest for an idealized core-shell configuration in which the BC is a sphere at the center of the particle whereas much less absorption should be observed for particles in which the BC is located near or on the surface. Such microphysical information on BC-containing particles has previously been provided only by labor-intensive microscopy techniques, thus often requiring that climate modelers make assumptions about the location of the BC within the particle that are based more on mathematical simplicity than physical reality. The present paper describes a novel analysis method that utilizes the temporal behavior of the scattering and incandescence signals from individual particles containing refractory BC (rBC) measured by the Single-Particle Soot Photometer (SP2) to distinguish particles with rBC near the surface from those that have structures more closely resembling the core-shell configuration. This approach permits collection of a high-time-resolution data set of the fraction of rBCcontaining particles with rBC near the surface. By application of this method to a plume containing tracers for biomass burning, it was determined that this fraction was greater than 60%. Such a data set will not only provide previously unavailable information to the climate modeling community, allowing greater accuracy in calculating rBC radiative forcing, but also will yield insight into aerosol processes.