The temporal variability of microphysical parameters of pyrolysis smoke, retrieved by inverting the characteristics of aerosol scattering and extinction, has been studied. The polarization scattering phase functions and spectral extinction coefficients were measured for 65 hours in smoke aerosols produced from thermal decomposition of pine wood during low-temperature pyrolysis in the Big Aerosol Chamber (BAC) of Institute of Atmospheric Optics, Siberian Branch, Russian Academy of Sciences. The microstructure parameters (volume concentration and mean radius of particles with division into fine and coarse fractions) and the complex refractive index of pyrolysis smoke are retrieved following the developed algorithm for inverting optical measurements. The real part of the refractive index is found to be in the vicinity of n = 1.55, and the imaginary part is in the range 0.007 < kappa < 0.009; the mean radius of fine particles varies in the narrow range 0.137-0.146 mu m. During smoke aging, the particle ensemble-mean radius monotonically increased from 0.19 to 0.6 mu m mainly due to a relative increase in the content of coarse aerosol. Results of this work are important for estimation of the radiative forcing of aerosol and improvement of climate models and algorithms of remote optical sounding.

According to the monitoring data of the optical and microphysical characteristics of smoke aerosol at AERONET stations during forest fires in the summer of 2019 in Alaska, the anomalous selective absorption of smoke aerosol has been detected in the visible and near-infrared spectral range from 440 to 1020 nm. With anomalous selective absorption, the imaginary part of the refractive index of smoke aerosol reached 0.315 at a wavelength of 1020 nm. A power-law approximation of the spectral dependence of the imaginary part of the refractive index with an exponent from 0.26 to 2.35 is proposed. It is shown that, for anomalous selective absorption, power-law approximations of the spectral dependences of the aerosol optical extinction and absorption depths are applicable with an angstrom ngstrom exponent from 0.96 to 1.65 for the aerosol optical extinction depth and from 0.97 to -0.89 for the aerosol optical absorption depth, which reached 0.72. Single scattering albedo varied from 0.62 to 0.96. In the size distribution of smoke aerosol particles with anomalous selective absorption, the fine fraction of particles of condensation origin dominated. The similarity of the fraction of particles distinguished by anomalous selective absorption with the fraction of tar balls (TBs) detected by electron microscopy in smoke aerosol, which, apparently, arise during the condensation of terpenes and their oxygen-containing derivatives, is noted.

Using a single column model with ground-based, aircraft, and satellite data sets we assess the combined role of smoke and dust aerosols, land degradation/aridization (LDA), and their impact on the planetary boundary layer (PBL) in influencing near-surface air temperature over the Sahel. Our study is unique because it assesses the combined role of smoke and dust aerosols on PBL evolution and near-surface air temperatures during both day and nighttime. More importantly, using a theoretical framework, we provide a careful explanation of the geophysical processes responsible for the changes in PBL and near-surface air temperature. Our results indicate that during northern hemisphere winter months, dust, and smoke over Sahel radiatively combine to impact the PBL. We show that aerosol mixtures dominated by dust modify PBL height in a manner that minimizes/maximizes surface layer cooling/warming at times when daytime maximum/nocturnal minimum temperatures occur. Furthermore, we find that increasing smoke contribution to total column aerosol optical extinction counteracts nighttime warming through daytime cooling. When smoke constitutes half or more of to the total column aerosol optical extinction, the ratio of longwave to shortwave radiative forcing is less than 10%, and nighttime cooling ensues. Minimum temperature is most sensitive to changes in mid-visible aerosol optical depth (AOD) values <1 and doubling of dust AOD within this range during the 1950-1980 Sahelian LDA event is estimated to have a nocturnal warming potential of 0.6 degrees C.

Australian wildfires burning from December 2019 to January 2020 injected approximately 0.9 Tg of smoke into the stratosphere; this is the largest amount observed in the satellite era. A comparison of numerical simulations to satellite observations of the plume rise suggests that the smoke mass contained 2.5% black carbon. Model calculations project a 1 K warming in the stratosphere of the Southern Hemisphere midlatitudes for more than 6 months following the injection of black-carbon containing smoke. The 2020 average global mean clear sky effective radiative forcing at top of atmosphere is estimated to be -0.03 W m(-2) with a surface value of -0.32 W m(-2). Assuming that smoke particles coat with sulfuric acid in the stratosphere and have similar heterogeneous reaction rates as sulfate aerosol, we estimate a smoke-induced chemical decrease in total column ozone of 10-20 Dobson units from August to December in mid-high southern latitudes.

Although the characteristics of biomass burning events and the ambient ecosystem determine emitted smoke composition, the conditions that modulate the partitioning of black carbon (BC) and brown carbon (BrC) formation are not well understood, nor are the spatial or temporal frequency of factors driving smoke particle evolution, such as hydration, coagulation, and oxidation, all of which impact smoke radiative forcing. In situ data from surface observation sites and aircraft field campaigns offer deep insight into the optical, chemical, and microphysical traits of biomass burning (BB) smoke aerosols, such as single scattering albedo (SSA) and size distribution, but cannot by themselves provide robust statistical characterization of both emitted and evolved particles. Data from the NASA Earth Observing System's Multi-Angle Imaging SpectroRadiometer (MISR) instrument can provide at least a partial picture of BB particle properties and their evolution downwind, once properly validated. Here we use in situ data from the joint NOAA/NASA 2019 Fire Influence on Regional to Global Environments Experiment-Air Quality (FIREX-AQ) field campaign to assess the strengths and limitations of MISR-derived constraints on particle size, shape, light-absorption, and its spectral slope, as well as plume height and associated wind vectors. Based on the satellite observations, we also offer inferences about aging mechanisms effecting downwind particle evolution, such as gravitational settling, oxidation, secondary particle formation, and the combination of particle aggregation and condensational growth. This work builds upon our previous study, adding confidence to our interpretation of the remote-sensing data based on an expanded suite of in situ measurements for validation. The satellite and in situ measurements offer similar characterizations of particle property evolution as a function of smoke age for the 06 August Williams Flats Fire, and most of the key differences in particle size and absorption can be attributed to differences in sampling and changes in the plume geometry between sampling times. Whereas the aircraft data provide validation for the MISR retrievals, the satellite data offer a spatially continuous mapping of particle properties over the plume, which helps identify trends in particle property downwind evolution that are ambiguous in the sparsely sampled aircraft transects. The MISR data record is more than two decades long, offering future opportunities to study regional wildfire plume behavior statistically, where aircraft data are limited or entirely lacking.

According to satellite monitoring data (MODIS/Terra), the spatial distribution of the aerosol optical depth (AOD) at a wavelength of 550 nm for the summer smog of 2007 over the North China Plain (NCP) and adjacent areas has been obtained. Areas over which the AOD is higher due to regional anthropogenic contamination sources near Beijing and Shanghai, as well as the smoke haze forming due to agricultural burning (the southwest part of the NCP), have been revealed. The similarity of optical and microphysical characteristics of aerosol in the smoke haze over the NCP and in the Russian territory has been found: (i) the decisive contribution to the optical characteristics of smoke aerosol is made by the fine mode and (ii) the attenuation spectra in the wavelength region 340-1020 nm are approximated (in logarithmic coordinates) by parabolas or fourth degree polynomials. The monitoring data at the AERONET Beijing site show that the single scattering albedo in the summer smog over the NCP is on average less (0.91) than in the smoke haze in the Russian territory (0.95-0.96). The radiative regimes of the atmosphere are significantly different: in the smog, the aerosol radiative forcing efficiency is lower approximately by 30% at the top of the atmosphere and higher by 30% at the bottom of the atmosphere than in the smoke haze.

We have investigated the variability of smoke aerosol absorbing ability with variations in the content of brown carbon (BrC) and black carbon (BC). Using monitoring data on radiative characteristics of smoke aerosol at AERONET stations and the spatial distribution of aerosol optical depth (AOD) obtained by the MODIS spectrometer (Terra satellite), we have detected large-scale smokes during boreal forest fires in Russia and Canada (1995-2012). The spatial distribution (50A degrees-70A degrees N, 95A degrees-125A degrees W) and temporal variability (at AERONET station Fort McMurray) of AOD during the smoking of a part of Canada in July 2012 have been analyzed. AOD probability distributions for July 14-18, 2012, and an estimate of aerosol radiative forcing of smoke aerosol at the upper boundary of the atmosphere have been obtained. We have proposed a technique for the diagnostics of BrC and BC in smoke aerosol particles from the spectral dependence of the imaginary part of the refractive index. At a wavelength of 440 nm, the contributions of BrC and BC to the smokeaerosol absorbing abitity can be comparable in magnitude. In many cases, the absorption spectra of smoke aerosol can be adequately approximated by either power or exponential functions. The presence of BrC in smoke-aerosol particles highly extends the variety of observed absorption spectra in a smoky atmosphere and spectral dependences of single scattering albedo. In the spectral range of 440-1020 nm, the radiative characteristics of smoke aerosol are largely contributed by its fine mode.

The impact of biomass burning (BB) on aerosol optical properties and radiative budget in the polar region following an intense boreal fire event in North America in July 2015 is explored in this paper. Presented data are obtained from the Navy Aerosol Analysis and Prediction System (NAAPS) reanalysis and the Fu-Liou radiative transfer model. NAAPS provides particle concentrations and aerosol optical depth (AOD) at 1 degrees x 1 degrees spatial and 6 hourly temporal resolution, its AOD and vertical profiles were validated with field measurements for this event. Direct aerosol radiative forcings (ARF) at the surface, the top of the atmosphere (TOA) and within the atmosphere are calculated for clear-sky and all-sky conditions, with the surface albedo and cloud properties constrained by satellite retrievals. The mean ARFs at the surface, the TOA, and within the atmosphere averaged for the north pole region (latitudes north of 75.5N) and the study period (July 5-15, 2015) are -13.1 +/- 2.7, 0.3 +/- 2.1, and 13.4 +/- 2.7 W/m(2) for clear-sky and -7.3 +/- 1.8, 5.0 +/- 2.6, and 12.3 +/- 1.6 W/m(2) for all-sky conditions respectively. Local ARFs can be a several times larger e.g. the clear-sky surface and TOA ARF reach over Alaska 85 and 30 W/m(2) and over Svalbard 41 and 20 W/m(2) respectively. The ARF is found negative at the surface (almost zero over high albedo region though) with the maximum forcing over the BB source region, and weaker forcing under all-sky conditions compared to the clear-sky conditions. Unlike the ARFs at the surface and within the atmosphere, which have consistent forcing signs all over the polar region, the ARF at the TOA changes signs from negative (cooling) over the source region (Alaska) to positive (heating) over bright surfaces (e.g., Greenland) because of strong surface albedo effect. NAAPS simulations also show that the transported BB particle over the Arctic are in the low-to-middle troposphere and above low-level clouds, resulting in little difference in ARFs at the TOA between clear- and all-sky conditions over the regions with high surface albedo. Over dark surfaces, the negative TOA forcing increases with AOD about 50% slower under all-sky conditions compared to clear-sky case. The boreal BB event resulted in large magnitude of ARFs and the high variabilities of the forcings over the polar region has a significant impact on the polar weather conditions and important implications for the polar climate.

The black carbon (BC) component of ambient particulate matter is an important marker for combustion sources and for its impact on human health and radiative forcing. Extensive data archives exist for the black smoke metric, the historic measure of ambient particle darkness. An expression presented in earlier publications (Quincey, 2007; Quincey et al., 2011) for estimating BC concentrations from traditional black smoke measurements is shown to have limitations that can be addressed by using a more systematic approach to the issue of corrections for increasing darkening of the filter. The form of the more general relationship is shown to be an off-axis parabola rather than the on-axis parabola of the earlier work. Existing data from co-located black smoke and aethalometer measurements at 5 UK sites are reanalysed in this context. At very low concentrations of dark particles (British Black Smoke index < similar to 10 mu g m(-3)) a simple linear relationship BC (/mu g m(-3)) = 0.27.BSIBRITISH will suffice. A parabolic relationship, [BC/mu g m(-3)) = root 5.2(-1.1)(+1.5) x BSIBRITISH + 62(-13)(+19) - 7.9(-0.9)(+1.1), quantitatively similar to the previously published relationship will be more reliable for BSIBRITISH values up to 20-25 mu g m(-3). The full set of data available was fitted empirically to the off-axis parabola over the range 0-80 mu g m(-3) as the quadratic: [BC/mu g m(-3)]= (0.27 +/- 0.03) . BSIBRITISH - (4.0 +/- 0.2) x 10(-4)(BSIBRITISH)(2), but this curve is highly dependent on the variations between the individual data sets. Adding the extra complexity of the full off-axis parabolic relationship is unlikely to be justified in practical situations. All expressions apply also to the OECD definition of black smoke with the substitution BSIBRITISH = 0.85.BSIOECD. However, in common with the previous approach, they apply only to black smoke values obtained from standard black smoke samplers with 25 mm diameter filters and similar to 2 m(3) day(-1) volumetric flow rate, and presume a value 16.6 m(2) g(-1) for the specific absorption of BC in ambient particulate matter measured by aethalometry. Fitting uncertainties correspond to imprecision in estimated BC of +/-5%, +/-12% and +/-18% at BSIBRITISH of 5, 20 and 80 mu g m(-3), respectively. Spatial and temporal variation in particle ensemble optical properties contributes to uncertainty in BC quantification. (C) 2012 Elsevier Ltd. All rights reserved.