[1] Black carbon aerosol plays a unique and important role in Earth's climate system. Black carbon is a type of carbonaceous material with a unique combination of physical properties. This assessment provides an evaluation of black-carbon climate forcing that is comprehensive in its inclusion of all known and relevant processes and that is quantitative in providing best estimates and uncertainties of the main forcing terms: direct solar absorption; influence on liquid, mixed phase, and ice clouds; and deposition on snow and ice. These effects are calculated with climate models, but when possible, they are evaluated with both microphysical measurements and field observations. Predominant sources are combustion related, namely, fossil fuels for transportation, solid fuels for industrial and residential uses, and open burning of biomass. Total global emissions of black carbon using bottom-up inventory methods are 7500 Gg yr À1 in the year 2000 with an uncertainty range of 2000 to 29000. However, global atmospheric absorption attributable to black

[1] A single-particle soot photometer (SP2) was flown on a NASA WB-57F high-altitude research aircraft in November 2004 from Houston, Texas. The SP2 uses laser-induced incandescence to detect individual black carbon (BC) particles in an air sample in the mass range of $3-300 fg ($0.15-0.7 mm volume equivalent diameter). Scattered light is used to size the remaining non-BC aerosols in the range of $0.17-0.7 mm diameter. We present profiles of both aerosol types from the boundary layer to the lower stratosphere from two midlatitude flights. Results for total aerosol amounts in the size range detected by the SP2 are in good agreement with typical particle spectrometer measurements in the same region. All ambient incandescing particles were identified as BC because their incandescence properties matched those of laboratory-generated BC aerosol. Approximately 40% of these BC particles showed evidence of internal mixing (e.g., coating). Throughout profiles between 5 and 18.7 km, BC particles were less than a few percent of total aerosol number, and black carbon aerosol (BCA) mass mixing ratio showed a constant gradient with altitude above 5 km. SP2 data was compared to results from the ECHAM4/MADE and LmDzT-INCA global aerosol models. The comparison will help resolve the important systematic differences in model aerosol processes that determine BCA loadings. Further intercomparisons of models and measurements as presented here will improve the accuracy of the radiative forcing contribution from BCA.Citation: Schwarz, J. P., et al. (2006), Single-particle measurements of midlatitude black carbon and light-scattering aerosols from the boundary layer to the lower stratosphere,

Biomass burning (BB) contributes large amounts of black carbon (BC) and particulate organic matter (POM) to the atmosphere and contributes significantly to the earth's radiation balance. BB particles can be a complicated optical system, with scattering and absorption contributions from BC, internal mixtures of BC and POM, and wavelength-dependent absorption of POM. Large amounts of POM can also be externally mixed. We report on the unique ability of multi-wavelength photo-acoustic measurements of dry and thermal-denuded absorption to deconstruct this complicated wavelength-dependent system of absorption and mixing. Optical measurements of BB particles from the Four Mile Canyon fire near Boulder, Colorado, showed that internal mixtures of BC and POM enhanced absorption by up to 70%. The data supports the assumption that the POM was very weakly absorbing at 532 nm. Enhanced absorption at 404 nm was in excess of 200% above BC absorption and varied as POM mass changed, indicative of absorbing POM. Absorption by internal mixing of BC and POM contributed 19ðAE8Þ% to total 404-nm absorption, while BC alone contributed 54ðAE16Þ%. Approximately 83% of POM mass was externally mixed, the absorption of which contributed 27ðAE15Þ% to total particle absorption (at 404 nm). The imaginary refractive index and mass absorption efficiency (MAE) of POM at 404 nm changed throughout the sampling period and were found to be 0.007 AE 0.005 and 0.82 AE 0.43 m 2 g −1 , respectively. Our analysis shows that the MAE of POM can be biased high by up to 50% if absorption from internal mixing of POM and BC is not included.forest fire | climate | tar balls P article emissions from biomass burning (BB) are a significant component of global combustion-sourced black carbon (BC) and primary particulate organic matter (POM), contributing approximately 63% and 94%, respectively (1). The radiative impact of BB emissions at regional and global scales are significant (2) and can create instantaneous top-of-atmosphere cooling or warming (up to AE10 s of Wm −2 ), depending on surface albedo (3, 4). BB emissions from northern Eurasia and North America are often efficiently transported into the Arctic (5, 6) and contribute to climate change in that region (7), including snow and ice melt following BC deposition (8).The radiative impacts of BB particle emissions are very different than those of particles emitted from relatively efficient (i.e., internal) fossil fuel (FF) combustion. Co-emission of strongly absorbing BC and non-or mildly absorbing POM contrast to the predominantly absorbing BC emissions of FF combustion (2, 9) and can lead to a dominance of light scattering from the POM.The co-emission of BC and POM can additionally lead to internal mixing, which can enhance BC absorption by serving as a radiation lens. Such lensing may increase absorption by a factor of two (10-12). BC particles can be associated with significant amounts of non-BC material in the atmosphere and enhancement of ambient BC absorption is expected (13-15). Studies of direct and i...

Particulate brown carbon (BrC) in the atmosphere absorbs light at subvisible wavelengths and has poorly constrained but potentially large climate forcing impacts. BrC from biomass burning has virtually unknown lifecycle and atmospheric stability. Here, BrC emitted from intense wildfires was measured in plumes transported over 2 days from two main fires, during the 2013 NASA SEAC4RS mission. Concurrent measurements of organic aerosol (OA) and black carbon (BC) mass concentration, BC coating thickness, absorption Ångström exponent, and OA oxidation state reveal that the initial BrC emitted from the fires was largely unstable. Using back trajectories to estimate the transport time indicates that BrC aerosol light absorption decayed in the plumes with a half‐life of 9 to 15 h, measured over day and night. Although most BrC was lost within a day, possibly through chemical loss and/or evaporation, the remaining persistent fraction likely determines the background BrC levels most relevant for climate forcing.

[1] In situ measurements of the mass, mixing state, and optical size of individual black-carbon (BC) particles in the fine mode (90 -600 nm) have been made in fresh emissions from urban and biomass burning sources with an airborne single-particle soot photometer. Contrasts between the two sources are significant and consistent. Urban BC tends to smaller sizes, fewer coated particles, thinner coatings, and less absorption per unit mass than biomass-burning BC. This suggests that urban BC may have a longer lifetime in the atmosphere and a different impact on BC radiative forcing in the first indirect effect than biomass-burning BC. These measurements bound the likely variability in the microphysical state of BC emissions from typical continental processes, and provide direct measurements of the size distribution and coating state of fine-mode BC for use in constraining climate and aerosol models. These results highlight the need for the integration of sourcespecific information into such models. Citation: Schwarz, J. P., et al. (2008), Measurement of the mixing state, mass, and optical size of individual black carbon particles in urban and biomass burning emissions, Geophys. Res. Lett., 35, L13810,

Interest in stratospheric aerosol and its role in climate have increased over the last decade due to the observed increase in stratospheric aerosol since 2000 and the potential for changes in the sulfur cycle induced by climate change. This review provides an overview about the advances in stratospheric aerosol research since the last comprehensive assessment of stratospheric aerosol was published in 2006. A crucial development since 2006 is the substantial improvement in the agreement between in situ and space-based inferences of stratospheric aerosol properties during volcanically quiescent periods. Furthermore, new measurement systems and techniques, both in situ and space based, have been developed for measuring physical aerosol properties with greater accuracy and for characterizing aerosol composition. However, these changes induce challenges to constructing a long-term stratospheric aerosol climatology. Currently, changes in stratospheric aerosol levels less than 20% cannot be confidently quantified. The volcanic signals tend to mask any nonvolcanically driven change, making them difficult to understand. While the role of carbonyl sulfide as a substantial and relatively constant source of stratospheric sulfur has been confirmed by new observations and model simulations, large uncertainties remain with respect to the contribution from anthropogenic sulfur dioxide emissions. New evidence has been provided that stratospheric aerosol can also contain small amounts of nonsulfate matter such as black carbon and organics. Chemistry-climate models have substantially increased in quantity and sophistication. In many models the implementation of stratospheric aerosol processes is coupled to radiation and/or stratospheric chemistry modules to account for relevant feedback processes.

[1] Black carbon (BC) is the dominant aerosol absorber of solar radiation in the atmosphere and is an important component of anthropogenic climate forcing. BC's role is strongly dependent on its physical state, which can influence the way that BC particles may act as ice and cloud nuclei, as well as the way they interact with solar radiation. In situ measurements made with a single-particle soot photometer flown on a NASA high-altitude research aircraft show the mass and size of individual BC particles in the tropics, as well as their propensity to be found mixed with additional materials. Mie theory was used to connect observed light scattering off BC particles to the optical effects of coatings on the particles. The observations indicate that as BC from ground-based emission sources rises in altitude to the lower stratosphere, coatings on BC particles become both thicker and more prevalent, while BC mass mixing ratios decrease dramatically from their values near the ground. Coatings enhance light absorption by the ambient BC column by at least 30%. These results reveal the microphysical state of BC in the atmosphere while providing important constraints for models evaluating BC's role in climate change.

We present an overview of the background, scientific goals, and execution of the Aerosol, Radiation, and Cloud Processes affecting Arctic Climate (ARCPAC) project of April 2008. We then summarize airborne measurements, made in the troposphere of the Alaskan Arctic, of aerosol particle size distributions, composition, and optical properties and discuss the sources and transport of the aerosols. The aerosol data were grouped into four categories based on gas-phase composition. First, the background troposphere contained a relatively diffuse, sulfate-rich aerosol extending from the top of the sea-ice inversion layer to 7.4 km altitude. Second, a region of depleted (relative to the background) aerosol was present within the surface inversion layer over sea-ice. Third, layers of dense, organic-rich smoke from open biomass fires in southern Russia and southeastern Siberia were frequently encountered at all altitudes from the top of the inversion layer to 7.1 km. Finally, some aerosol layers were dominated by components originating from fossil fuel combustion. <br></br> Of these four categories measured during ARCPAC, the diffuse background aerosol was most similar to the average springtime aerosol properties observed at a long-term monitoring site at Barrow, Alaska. The biomass burning (BB) and fossil fuel layers were present above the sea-ice inversion layer and did not reach the sea-ice surface during the course of the ARCPAC measurements. The BB aerosol layers were highly scattering and were moderately hygroscopic. On average, the layers produced a noontime net heating of ~0.1 K day^&minus;1 between 3 and 7 km and a slight cooling at the surface. The ratios of particle mass to carbon monoxide (CO) in the BB plumes, which had been transported over distances >5000 km, were comparable to the high end of literature values derived from previous measurements in wildfire smoke. These ratios suggest minimal precipitation scavenging and removal of the BB particles between the time they were emitted and the time they were observed in dense layers above the sea-ice inversion layer