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- ItemTropospheric and stratospheric wildfire smoke profiling with lidar: mass, surface area, CCN, and INP retrieval(Katlenburg-Lindau : European Geosciences Union, 2021) Ansmann, Albert; Ohneiser, Kevin; Mamouri, Rodanthi-Elisavet; Knopf, Daniel A.; Veselovskii, Igor; Baars, Holger; Engelmann, Ronny; Foth, Andreas; Jimenez, Cristofer; Seifert, Patric; Barja, BorisWe present retrievals of tropospheric and stratospheric height profiles of particle mass, volume, surface area, and number concentrations in the case of wildfire smoke layers as well as estimates of smoke-related cloud condensation nuclei (CCN) and ice-nucleating particle (INP) concentrations from backscatter lidar measurements on the ground and in space. Conversion factors used to convert the optical measurements into microphysical properties play a central role in the data analysis, in addition to estimates of the smoke extinction-to-backscatter ratios required to obtain smoke extinction coefficients. The set of needed conversion parameters for wildfire smoke is derived from AERONET observations of major smoke events, e.g., in western Canada in August 2017, California in September 2020, and southeastern Australia in January-February 2020 as well as from AERONET long-term observations of smoke in the Amazon region, southern Africa, and Southeast Asia. The new smoke analysis scheme is applied to CALIPSO observations of tropospheric smoke plumes over the United States in September 2020 and to ground-based lidar observation in Punta Arenas, in southern Chile, in aged Australian smoke layers in the stratosphere in January 2020. These case studies show the potential of spaceborne and ground-based lidars to document large-scale and long-lasting wildfire smoke events in detail and thus to provide valuable information for climate, cloud, and air chemistry modeling efforts performed to investigate the role of wildfire smoke in the atmospheric system. © 2021 Albert Ansmann et al.
- ItemPrimary versus secondary contributions to particle number concentrations in the European boundary layer(München : European Geopyhsical Union, 2011) Reddington, C.L.; Carslaw, K.S.; Spracklen, D.V.; Frontoso, M.G.; Collins, L.; Merikanto, J.; Minikin, A.; Hamburger, T.; Coe, H.; Kulmala, M.; Aalto, P.; Flentje, H.; Plass-Dülmer, C.; Birmili, W.; Wiedensohler, A.; Wehner, B.; Tuch, T.; Sonntag, A.; O'Dowd, C.D.; Jennings, S.G.; Dupuy, R.; Baltensperger, U.; Weingartner, E.; Hansson, H.-C.; Tunved, P.; Laj, P.; Sellegri, K.; Boulon, J.; Putaud, J.-P.; Gruening, C.; Swietlicki, E.; Roldin, P.; Henzing, J.S.; Moerman, M.; Mihalopoulos, N.; Kouvarakis, G.; Ždímal, V.; Zíková, N.; Marinoni, A.; Bonasoni, P.; Duchi, R.It is important to understand the relative contribution of primary and secondary particles to regional and global aerosol so that models can attribute aerosol radiative forcing to different sources. In large-scale models, there is considerable uncertainty associated with treatments of particle formation (nucleation) in the boundary layer (BL) and in the size distribution of emitted primary particles, leading to uncertainties in predicted cloud condensation nuclei (CCN) concentrations. Here we quantify how primary particle emissions and secondary particle formation influence size-resolved particle number concentrations in the BL using a global aerosol microphysics model and aircraft and ground site observations made during the May 2008 campaign of the European Integrated Project on Aerosol Cloud Climate Air Quality Interactions (EUCAARI). We tested four different parameterisations for BL nucleation and two assumptions for the emission size distribution of anthropogenic and wildfire carbonaceous particles. When we emit carbonaceous particles at small sizes (as recommended by the Aerosol Intercomparison project, AEROCOM), the spatial distributions of campaign-mean number concentrations of particles with diameter >50 nm (N50) and >100 nm (N100) were well captured by the model (R2≥0.8) and the normalised mean bias (NMB) was also small (−18% for N50 and −1% for N100). Emission of carbonaceous particles at larger sizes, which we consider to be more realistic for low spatial resolution global models, results in equally good correlation but larger bias (R2≥0.8, NMB = −52% and −29%), which could be partly but not entirely compensated by BL nucleation. Within the uncertainty of the observations and accounting for the uncertainty in the size of emitted primary particles, BL nucleation makes a statistically significant contribution to CCN-sized particles at less than a quarter of the ground sites. Our results show that a major source of uncertainty in CCN-sized particles in polluted European air is the emitted size of primary carbonaceous particles. New information is required not just from direct observations, but also to determine the "effective emission size" and composition of primary particles appropriate for different resolution models.
- ItemOzone depletion in the Arctic and Antarctic stratosphere induced by wildfire smoke(Katlenburg-Lindau : EGU, 2022) Ansmann, Albert; Ohneiser, Kevin; Chudnovsky, Alexandra; Knopf, Daniel A.; Eloranta, Edwin W.; Villanueva, Diego; Seifert, Patric; Radenz, Martin; Barja, Boris; Zamorano, Félix; Jimenez, Cristofer; Engelmann, Ronny; Baars, Holger; Griesche, Hannes; Hofer, Julian; Althausen, Dietrich; Wandinger, UllaA record-breaking stratospheric ozone loss was observed over the Arctic and Antarctica in 2020. Strong ozone depletion occurred over Antarctica in 2021 as well. The ozone holes developed in smoke-polluted air. In this article, the impact of Siberian and Australian wildfire smoke (dominated by organic aerosol) on the extraordinarily strong ozone reduction is discussed. The study is based on aerosol lidar observations in the North Pole region (October 2019-May 2020) and over Punta Arenas in southern Chile at 53.2°S (January 2020-November 2021) as well as on respective NDACC (Network for the Detection of Atmospheric Composition Change) ozone profile observations in the Arctic (Ny-Ålesund) and Antarctica (Neumayer and South Pole stations) in 2020 and 2021. We present a conceptual approach on how the smoke may have influenced the formation of polar stratospheric clouds (PSCs), which are of key importance in the ozone-depleting processes. The main results are as follows: (a) the direct impact of wildfire smoke below the PSC height range (at 10-12 km) on ozone reduction seems to be similar to well-known volcanic sulfate aerosol effects. At heights of 10-12 km, smoke particle surface area (SA) concentrations of 5-7 μm2 cm-3 (Antarctica, spring 2021) and 6-10 μm2 cm-3 (Arctic, spring 2020) were correlated with an ozone reduction in terms of ozone partial pressure of 0.4-1.2 mPa (about 30 % further ozone reduction over Antarctica) and of 2-3.5 mPa (Arctic, 20 %-30 % reduction with respect to the long-term springtime mean). (b) Within the PSC height range, we found indications that smoke was able to slightly increase the PSC particle number and surface area concentration. In particular, a smoke-related additional ozone loss of 1-2 mPa (10 %-20 % contribution to the total ozone loss over Antarctica) was observed in the 14-23 km PSC height range in September-October 2020 and 2021. Smoke particle number concentrations ranged from 10 to 100 cm-3 and were about a factor of 10 (in 2020) and 5 (in 2021) above the stratospheric aerosol background level. Satellite observations indicated an additional mean column ozone loss (deviation from the long-term mean) of 26-30 Dobson units (9 %-10 %, September 2020, 2021) and 52-57 Dobson units (17 %-20 %, October 2020, 2021) in the smoke-polluted latitudinal Antarctic belt from 70-80°S. Copyright:
- ItemHow the extreme 2019-2020 Australian wildfires affected global circulation and adjustments(Katlenburg-Lindau : EGU, 2023) Senf, Fabian; Heinold, Bernd; Kubin, Anne; Müller, Jason; Schrödner, Roland; Tegen, InaWildfires are a significant source of absorbing aerosols in the atmosphere. Extreme fires in particular, such as those during the 2019-2020 Australian wildfire season (Black Summer fires), can have considerable large-scale effects. In this context, the climate impact of extreme wildfires unfolds not only because of the emitted carbon dioxide but also due to smoke aerosol released up to an altitude of 17ĝ€¯km. The overall aerosol effects depend on a variety of factors, such as the amount emitted, the injection height, and the composition of the burned material, and is therefore subject to considerable uncertainty. In the present study, we address the global impact caused by the exceptionally strong and high-reaching smoke emissions from the Australian wildfires using simulations with a global aerosol-climate model. We show that the absorption of solar radiation by the black carbon contained in the emitted smoke led to a shortwave radiative forcing of more than +5ĝ€¯Wm-2 in the southern mid-latitudes of the lower stratosphere. Subsequent adjustment processes in the stratosphere slowed down the diabatically driven meridional circulation, thus redistributing the heating perturbation on a global scale. As a result of these stratospheric adjustments, a positive temperature perturbation developed in both hemispheres, leading to additional longwave radiation emitted back to space. According to the model results, this adjustment occurred in the stratosphere within the first 2 months after the event. At the top of the atmosphere (TOA), the net effective radiative forcing (ERF) averaged over the Southern Hemisphere was initially dominated by the instantaneous positive radiative forcing of about +0.5ĝ€¯Wm-2, for which the positive sign resulted mainly from the presence of clouds above the Southern Ocean. The longwave adjustments led to a compensation of the initially net positive TOA ERF, which is seen in the Southern Hemisphere, the tropics, and the northern mid-latitudes. The simulated changes in the lower stratosphere also affected the upper troposphere through a thermodynamic downward coupling. Subsequently, increased temperatures were also obtained in the upper troposphere, causing a global decrease in relative humidity, cirrus amount, and the ice water path of about 0.2ĝ€¯%. As a result, surface precipitation also decreased by a similar amount, which was accompanied by a weakening of the tropospheric circulation due to the given energetic constraints. In general, it appears that the radiative effects of smoke from single extreme wildfire events can lead to global impacts that affect the interplay of tropospheric and stratospheric budgets in complex ways. This emphasizes that future changes in extreme wildfires need to be included in projections of aerosol radiative forcing.
- ItemWildfires as a source of airborne mineral dust - Revisiting a conceptual model using large-eddy simulation (LES)(Göttingen : Copernicus GmbH, 2018) Wagner, R.; Jähn, M.; Schepanski, K.Airborne mineral dust is a key player in the Earth system and shows manifold impacts on atmospheric properties such as the radiation budget and cloud microphysics. Investigations of smoke plumes originating from wildfires found significant fractions of mineral dust within these plumes - most likely raised by strong, turbulent fire-related winds. This study presents and revisits a conceptual model describing the emission of mineral dust particles during wildfires. This is achieved by means of high-resolution large-eddy simulation (LES), conducted with the All Scale Atmospheric Model (ASAM). The impact of (a) different fire properties representing idealized grassland and shrubland fires, (b) different ambient wind conditions modulated by the fire's energy flux, and (c) the wind's capability to mobilize mineral dust particles was investigated. Results from this study illustrate that the energy release of the fire leads to a significant increase in near-surface wind speed, which consequently enhances the dust uplift potential. This is in particular the case within the fire area where vegetation can be assumed to be widely removed and uncovered soil is prone to wind erosion. The dust uplift potential is very sensitive to fire properties, such as fire size, shape, and intensity, but also depends on the ambient wind velocity. Although measurements already showed the importance of wildfires for dust emissions, pyro-convection is so far neglected as a dust emission process in atmosphere-aerosol models. The results presented in this study can be seen as the first step towards a systematic parameterization representing the connection between typical fire properties and related dust emissions.
- ItemWildfire smoke triggers cirrus formation: Lidar observations over the eastern Mediterranean(Katlenburg-Lindau : EGU, 2023) Mamouri, Rodanthi-Elisavet; Ansmann, Albert; Ohneiser, Kevin; Knopf, Daniel A.; Nisantzi, Argyro; Bühl, Johannes; Engelmann, Ronny; Skupin, Annett; Seifert, Patric; Baars, Holger; Ene, Dragos; Wandinger, Ulla; Hadjimitsis, DiofantosThe number of intense wildfires may increase further in upcoming years as a consequence of climate change. It is therefore necessary to improve our knowledge about the role of smoke in the climate system, with emphasis on the impact of smoke particles on the evolution of clouds, precipitation, and cloud radiative properties. Presently, one key aspect of research is whether or not wildfire smoke particles can initiate cirrus formation. In this study, we present lidar observations over Limassol, Cyprus, from 27 October to 3 November 2020, when extended wildfire smoke fields crossed the Mediterranean Basin from Portugal to Cyprus. We found strong evidence that aged smoke (organic aerosol particles) originating from wildfires in North America triggered significant ice nucleation at temperatures from -47 to -53° C and caused the formation of extended cirrus layers. The observations suggest that the ice crystals were nucleated just below the tropopause in the presence of smoke particles serving as ice-nucleating particles (INPs). The main part of the 2-3km thick smoke layer was, however, in the lower stratosphere just above the tropopause. With actual radiosonde observations of temperature and relative humidity and lidar-derived smoke particle surface area concentrations used as starting values, gravity wave simulations show that the lofting of air by 100-200m is sufficient to initiate significant ice nucleation on the smoke particles, leading to ice crystal number concentrations of 1-100L-1.
- ItemDepolarization and lidar ratios at 355, 532, and 1064 nm and microphysical properties of aged tropospheric and stratospheric Canadian wildfire smoke(Göttingen : Copernicus GmbH, 2018) Haarig, M.; Ansmann, A.; Baars, H.; Jimenez, C.; Veselovskii, I.; Engelmann, R.; Althausen, D.We present spectrally resolved optical and microphysical properties of western Canadian wildfire smoke observed in a tropospheric layer from 5-6.5 km height and in a stratospheric layer from 15-16 km height during a recordbreaking smoke event on 22 August 2017. Three polarization/ Raman lidars were run at the European Aerosol Research Lidar Network (EARLINET) station of Leipzig, Germany, after sunset on 22 August. For the first time, the linear depolarization ratio and extinction-to-backscatter ratio (lidar ratio) of aged smoke particles were measured at all three important lidar wavelengths of 355, 532, and 1064 nm. Very different particle depolarization ratios were found in the troposphere and in the stratosphere. The obviously compact and spherical tropospheric smoke particles caused almost no depolarization of backscattered laser radiation at all three wavelengths ( < 3 %), whereas the dry irregularly shaped soot particles in the stratosphere lead to high depolarization ratios of 22% at 355 nm and 18% at 532 nm and a comparably low value of 4% at 1064 nm. The lidar ratios were 40- 45 sr (355 nm), 65-80 sr (532 nm), and 80-95 sr (1064 nm) in both the tropospheric and stratospheric smoke layers indicating similar scattering and absorption properties. The strong wavelength dependence of the stratospheric depolarization ratio was probably caused by the absence of a particle coarse mode (particle mode consisting of particles with radius > 500nm). The stratospheric smoke particles formed a pronounced accumulation mode (in terms of particle volume or mass) centered at a particle radius of 350-400 nm. The effective particle radius was 0.32 μm. The tropospheric smoke particles were much smaller (effective radius of 0.17 μm). Mass concentrations were of the order of 5.5 μgm-3 (tropospheric layer) and 40 μgm-3 (stratospheric layer) in the night of 22 August 2017. The single scattering albedo of the stratospheric particles was estimated to be 0.74, 0.8, and 0.83 at 355, 532, and 1064 nm, respectively.
- ItemExtreme levels of Canadian wildfire smoke in the stratosphere over central Europe on 21-22 August 2017(Katlenburg-Lindau : EGU, 2018) Ansmann, Albert; Baars, Holger; Chudnovsky, Alexandra; Mattis, Ina; Veselovskii, Igor; Haarig, Moritz; Seifert, Patric; Engelmann, Ronny; Wandinger, UllaLight extinction coefficients of 500 Mm1, about 20 times higher than after the Pinatubo volcanic eruptions in 1991, were observed by European Aerosol Research Lidar Network (EARLINET) lidars in the stratosphere over central Europe on 21-22 August 2017. Pronounced smoke layers with a 1-2 km vertical extent were found 2-5 km above the local tropopause. Optically dense layers of Canadian wildfire smoke reached central Europe 10 days after their injection into the upper troposphere and lower stratosphere which was caused by rather strong pyrocumulonimbus activity over western Canada. The smoke-related aerosol optical thickness (AOT) identified by lidar was close to 1.0 at 532 nm over Leipzig during the noon hours on 22 August 2017. Smoke particles were found throughout the free troposphere (AOT of 0.3) and in the pronounced 2 km thick stratospheric smoke layer at an altitude of 14-16 km (AOT of 0.6). The lidar observations indicated peak mass concentrations of 70-100 μgm-3 in the stratosphere. In addition to the lidar profiles, we analyzed Moderate Resolution Imaging Spectroradiometer (MODIS) fire radiative power (FRP) over Canada, and the distribution of MODIS AOT and Ozone Monitoring Instrument (OMI) aerosol index across the North Atlantic. These instruments showed a similar pattern and a clear link between the western Canadian fires and the aerosol load over Europe. In this paper, we also present Aerosol Robotic Network (AERONET) sun photometer observations, compare photometer and lidar-derived AOT, and discuss an obvious bias (the smoke AOT is too low) in the photometer observations. Finally, we compare the strength of this recordbreaking smoke event (in terms of the particle extinction coefficient and AOT) with major and moderate volcanic events observed over the northern midlatitudes.
- ItemAn intercomparison study of analytical methods used for quantification of levoglucosan in ambient aerosol filter samples(München : European Geopyhsical Union, 2015) Yttri, K.E.; Schnelle-Kreis, J.; Maenhaut, W.; Abbaszade, G.; Alves, C.; Bjerke, A.; Bonnier, N.; Bossi, R.; Claeys, M.; Dye, C.; Evtyugina, M.; García-Gacio, D.; Hillamo, R.; Hoffer, A.; Hyder, M.; Iinuma, Y.; Jaffrezo, J.-L.; Kasper-Giebl, A.; Kiss, G.; López-Mahia, P.L.; Pio, C.; Piot, C.; Ramirez-Santa-Cruz, C.; Sciare, J.; Teinilä, K.; Vermeylen, R.; Vicente, A.; Zimmermann, R.The monosaccharide anhydrides (MAs) levoglucosan, galactosan and mannosan are products of incomplete combustion and pyrolysis of cellulose and hemicelluloses, and are found to be major constituents of biomass burning (BB) aerosol particles. Hence, ambient aerosol particle concentrations of levoglucosan are commonly used to study the influence of residential wood burning, agricultural waste burning and wildfire emissions on ambient air quality. A European-wide intercomparison on the analysis of the three monosaccharide anhydrides was conducted based on ambient aerosol quartz fiber filter samples collected at a Norwegian urban background site during winter. Thus, the samples' content of MAs is representative for BB particles originating from residential wood burning. The purpose of the intercomparison was to examine the comparability of the great diversity of analytical methods used for analysis of levoglucosan, mannosan and galactosan in ambient aerosol filter samples. Thirteen laboratories participated, of which three applied high-performance anion-exchange chromatography (HPAEC), four used high-performance liquid chromatography (HPLC) or ultra-performance liquid chromatography (UPLC) and six resorted to gas chromatography (GC). The analytical methods used were of such diversity that they should be considered as thirteen different analytical methods. All of the thirteen laboratories reported levels of levoglucosan, whereas nine reported data for mannosan and/or galactosan. Eight of the thirteen laboratories reported levels for all three isomers. The accuracy for levoglucosan, presented as the mean percentage error (PE) for each participating laboratory, varied from −63 to 20%; however, for 62% of the laboratories the mean PE was within ±10%, and for 85% the mean PE was within ±20%. For mannosan, the corresponding range was −60 to 69%, but as for levoglucosan, the range was substantially smaller for a subselection of the laboratories; i.e. for 33% of the laboratories the mean PE was within ±10%. For galactosan, the mean PE for the participating laboratories ranged from −84 to 593%, and as for mannosan 33% of the laboratories reported a mean PE within ±10%. The variability of the various analytical methods, as defined by their minimum and maximum PE value, was typically better for levoglucosan than for mannosan and galactosan, ranging from 3.2 to 41% for levoglucosan, from 10 to 67% for mannosan and from 6 to 364% for galactosan. For the levoglucosan to mannosan ratio, which may be used to assess the relative importance of softwood versus hardwood burning, the variability only ranged from 3.5 to 24 . To our knowledge, this is the first major intercomparison on analytical methods used to quantify monosaccharide anhydrides in ambient aerosol filter samples conducted and reported in the scientific literature. The results show that for levoglucosan the accuracy is only slightly lower than that reported for analysis of SO42- (sulfate) on filter samples, a constituent that has been analysed by numerous laboratories for several decades, typically by ion chromatography and which is considered a fairly easy constituent to measure. Hence, the results obtained for levoglucosan with respect to accuracy are encouraging and suggest that levels of levoglucosan, and to a lesser extent mannosan and galactosan, obtained by most of the analytical methods currently used to quantify monosaccharide anhydrides in ambient aerosol filter samples, are comparable. Finally, the various analytical methods used in the current study should be tested for other aerosol matrices and concentrations as well, the most obvious being summertime aerosol samples affected by wildfires and/or agricultural fires.
- ItemIs the near-spherical shape the "new black" for smoke?(Katlenburg-Lindau : EGU, 2020) Gialitaki, Anna; Tsekeri, Alexandra; Amiridis, Vassilis; Ceolato, Romain; Paulien, Lucas; Kampouri, Anna; Gkikas, Antonis; Solomos, Stavros; Marinou, Eleni; Haarig, Moritz; Baars, Holger; Ansmann, Albert; Lapyonok, Tatyana; Lopatin, Anton; Dubovik, Oleg; Groß, Silke; Wirth, Martin; Tsichla, Maria; Tsikoudi, Ioanna; Balis, DimitrisWe examine the capability of near-sphericalshaped particles to reproduce the triple-wavelength particle linear depolarization ratio (PLDR) and lidar ratio (LR) values measured over Europe for stratospheric smoke originating from Canadian wildfires. The smoke layers were detected both in the troposphere and the stratosphere, though in the latter case the particles presented PLDR values of almost 18% at 532 nm as well as a strong spectral dependence from the UV to the near-IR wavelength. Although recent simulation studies of rather complicated smoke particle morphologies have shown that heavily coated smoke aggregates can produce large PLDR, herein we propose a much simpler model of compact near-spherical smoke particles. This assumption allows for the reproduction of the observed intensive optical properties of stratospheric smoke, as well as their spectral dependence. We further examine whether an extension of the current Aerosol Robotic Network (AERONET) scattering model to include the near-spherical shapes could be of benefit to the AERONET retrieval for stratospheric smoke cases associated with enhanced PLDR. Results of our study illustrate the fact that triple-wavelength PLDR and LR lidar measurements can provide us with additional insight when it comes to particle characterization. © 2020 Author(s).