Search Results
Modelling winter organic aerosol at the European scale with CAMx: Evaluation and source apportionment with a VBS parameterization based on novel wood burning smog chamber experiments
2017, Ciarelli, Giancarlo, Aksoyoglu, Sebnem, El Haddad, Imad, Bruns, Emily A., Crippa, Monica, Poulain, Laurent, Äijälä, Mikko, Carbone, Samara, Freney, Evelyn, O'Dowd, Colin, Baltensperger, Urs, Prévôt, André S. H.
We evaluated a modified VBS (volatility basis set) scheme to treat biomass-burning-like organic aerosol (BBOA) implemented in CAMx (Comprehensive Air Quality Model with extensions). The updated scheme was parameterized with novel wood combustion smog chamber experiments using a hybrid VBS framework which accounts for a mixture of wood burning organic aerosol precursors and their further functionalization and fragmentation in the atmosphere. The new scheme was evaluated for one of the winter EMEP intensive campaigns (February-March 2009) against aerosol mass spectrometer (AMS) measurements performed at 11 sites in Europe. We found a considerable improvement for the modelled organic aerosol (OA) mass compared to our previous model application with the mean fractional bias (MFB) reduced from -61 to -29 %. We performed model-based source apportionment studies and compared results against positive matrix factorization (PMF) analysis performed on OA AMS data. Both model and observations suggest that OA was mainly of secondary origin at almost all sites. Modelled secondary organic aerosol (SOA) contributions to total OA varied from 32 to 88% (with an average contribution of 62 %) and absolute concentrations were generally under-predicted. Modelled primary hydrocarbon-like organic aerosol (HOA) and primary biomass-burning-like aerosol (BBPOA) fractions contributed to a lesser extent (HOA from 3 to 30 %, and BBPOA from 1 to 39 %) with average contributions of 13 and 25 %, respectively. Modelled BBPOA fractions were found to represent 12 to 64% of the total residential-heating-related OA, with increasing contributions at stations located in the northern part of the domain. Source apportionment studies were performed to assess the contribution of residential and non-residential combustion precursors to the total SOA. Non-residential combustion and road transportation sector contributed about 30-40% to SOA formation (with increasing contributions at urban and near industrialized sites), whereas residential combustion (mainly related to wood burning) contributed to a larger extent, around 60-70 %. Contributions to OA from residential combustion precursors in different volatility ranges were also assessed: our results indicate that residential combustion gas-phase precursors in the semivolatile range (SVOC) contributed from 6 to 30 %, with higher contributions predicted at stations located in the southern part of the domain. On the other hand, the oxidation products of higher-volatility precursors (the sum of intermediate-volatility compounds (IVOCs) and volatile organic compounds (VOCs)) contribute from 15 to 38% with no specific gradient among the stations. Although the new parameterization leads to a better agreement between model results and observations, it still underpredicts the SOA fraction, suggesting that uncertainties in the new scheme and other sources and/or formation mechanisms remain to be elucidated. Moreover, a more detailed characterization of the semivolatile components of the emissions is needed.
Doppler lidar studies of heat island effects on vertical mixing of aerosols during SAMUM-2
2017, Engelmann, Ronny, Ansmann, Albert, Horn, Stefan, Seifert, Patric, Althausen, Dietrich, Tesche, Matthias, Esselborn, Michael, Fruntke, Julia, Lieke, Kirsten, Freudenthaler, Volker, Gross, Silke
A wind Doppler lidar was deployed next to three aerosol lidars during the SAMUM–2 campaign on the main island of Cape Verde. The effects of the differential heating of the island and the surrounding ocean and the orographic impact of the capital island Santiago and the small island on its luv side, Maio, are investigated. Horizontal and vertical winds were measured in the disturbed maritime boundary layer and compared to local radiosoundings. Lidar measurements from the research aircraft Falcon and a 3-D Large Eddy Simulation (LES) model were used in addition to study the heating effects on the scale of the islands. Indications are found that these effects can widely control the downward mixing from greater heights to the surface of African aerosols, mainly Saharan dust and biomass-burning smoke, which were detected in a complex layering over the Cape Verde region.
Profiling of Saharan dust and biomass-burning smoke with multiwavelength polarization Raman lidar at Cape Verde
2017, Tesche, Matthias, Gross, Silke, Ansmann, Albert, Müller, Detlef, Althausen, Dietrich, Freudenthaler, Volker, Esselborn, Michael
Extensive lidar measurements of Saharan dust and biomass-burning smoke were performed with one airborne and three ground-based instruments in the framework of the second part of the SAharan Mineral dUst experiMent (SAMUM-2a) during January and February of 2008 at Cape Verde. Further lidar observations with one system only were conducted duringMay and June of 2008 (SAMUM-2b). The active measurements were supported by Sun photometer observations. During winter, layers of mineral dust from the Sahara and biomass-burning smoke from southern West Africa pass Cape Verde on their way to South America while pure dust layers cross the Atlantic on their way to the Caribbean during summer. The mean 500-nm aerosol optical thickness (AOT) observed during SAMUM-2a was 0.35 ± 0.18. SAMUM-2a observations showed transport of pure dust within the lowermost 1.5 km of the atmospheric column. In the height range from 1.5 to 5.0 km, mixed dust/smoke layers with mean lidar ratios of 67 ± 14 sr at 355 and 532 nm, respectively, prevailed. Within these layers, wavelength-independent linear particle depolarization ratios of 0.12–0.18 at 355, 532, and 710 nm indicate a large contribution (30–70%) of mineral dust to the measured optical properties. Ångstr¨om exponents for backscatter and extinction of around 0.7 support this finding. Mean extinction coefficients in the height range between 2 and 4 km were 66 ± 6 Mm−1 at 355 nm and 48 ± 5 Mm−1 at 532 nm. Comparisons with airborne high-spectral-resolution lidar observations show good agreement within the elevated layers. 3–5 km deep dust layers where observed during SAMUM-2b. These layers showed optical properties similar to the ones of SAMUM-1 in Morocco with a mean 500-nm AOT of 0.4 ± 0.2. Dust extinction coefficients were about 80 ± 6 Mm−1 at 355 and 532 nm. Dust lidar ratios were 53 ± 10 sr at 355 and 532 nm, respectively. Dust depolarization ratios showed an increase with wavelength from 0.31 ± 0.10 at 532 nm to 0.37 ± 0.07 at 710 nm.
Regional modelling of Saharan dust and biomass-burning smoke, Part I: Model description and evaluation
2017, Heinold, Bernd, Tegen, Ina, Schepanski, Kerstin, Tesche, Matthias, Esselborn, Michael, Freudenthaler, Volker, Gross, Silke, Kandler, Konrad, Knippertz, Peter, Müller, Detlef, Schladitz, Alexander, Toledano, Carlos, Weinzierl, Bernadett, Ansmann, Albert, Althausen, Dietrich, Müller, Thomas, Petzold, Andreas, Wiedensohler, Alfred
The spatio-temporal evolution of the Saharan dust and biomass-burning plume during the SAMUM-2 field campaign in January and February 2008 is simulated at 28 km horizontal resolution with the regional model-system COSMOMUSCAT. The model performance is thoroughly tested using routine ground-based and space-borne remote sensing and local field measurements. Good agreement with the observations is found in many cases regarding transport patterns, aerosol optical thicknesses and the ratio of dust to smoke aerosol. The model also captures major features of the complex aerosol layering. Nevertheless, discrepancies in the modelled aerosol distribution occur, which are analysed in detail. The dry synoptic dynamics controlling dust uplift and transport during the dry season are well described by the model, but surface wind peaks associated with the breakdown of nocturnal low-level jets are not always reproduced. Thus, a strong dust outbreak is underestimated. While dust emission modelling is a priori more challenging, since strength and placement of dust sources depend on on-line computed winds, considerable inaccuracies also arise in observation-based estimates of biomass-burning emissions. They are caused by cloud and spatial errors of satellite fire products and uncertainties in fire emission parameters, and can lead to unrealistic model results of smoke transport.
Microphysical characterization of long-range transported biomass burning particles from North America at three EARLINET stations
2017, Ortiz-Amezcua, Pablo, Guerrero-Rascado, Juan Luis, Granados-Muñoz, María José, Benavent-Oltra, José Antonio, Böckmann, Christine, Samaras, Stefanos, Stachlewska, Iwona S., Janicka, Łucja, Baars, Holger, Bohlmann, Stephanie, Alados-Arboledas, Lucas
Strong events of long-range transported biomass burning aerosol were detected during July 2013 at three EARLINET (European Aerosol Research Lidar Network) stations, namely Granada (Spain), Leipzig (Germany) and Warsaw (Poland). Satellite observations from MODIS (Moderate Resolution Imaging Spectroradiometer) and CALIOP (Cloud-Aerosol Lidar with Orthogonal Polarization) instruments, as well as modeling tools such as HYSPLIT (Hybrid Single-Particle Lagrangian Integrated Trajectory) and NAAPS (Navy Aerosol Analysis and Prediction System), have been used to estimate the sources and transport paths of those North American forest fire smoke particles. A multiwavelength Raman lidar technique was applied to obtain vertically resolved particle optical properties, and further inversion of those properties with a regularization algorithm allowed for retrieving microphysical information on the studied particles. The results highlight the presence of smoke layers of 1-2 km thickness, located at about 5 km a.s.l. altitude over Granada and Leipzig and around 2.5 km a.s.l. at Warsaw. These layers were intense, as they accounted for more than 30 % of the total AOD (aerosol optical depth) in all cases, and presented optical and microphysical features typical for different aging degrees: Color ratio of lidar ratios (LR532/LR355) around 2, α-related ängström exponents of less than 1, effective radii of 0.3 μm and large values of single scattering albedos (SSA), nearly spectrally independent. The intensive microphysical properties were compared with columnar retrievals form co-located AERONET (Aerosol Robotic Network) stations. The intensity of the layers was also characterized in terms of particle volume concentration, and then an experimental relationship between this magnitude and the particle extinction coefficient was established.
Airborne spectral radiation measurements to derive solar radiative forcing of Saharan dust mixed with biomass burning smoke particles
2017, Bauer, S., Bierwirth, E., Esselborn, M., Petzold, A., Macke, A., Trautmann, T., Wendisch, M.
Airborne measurements of upward solar spectral irradiances were performed during the second Saharan Mineral dUst experiMent (SAMUM-2) campaign based on the Cape Verde Islands. Additionally, airborne high resolution lidar measurements of vertical profiles of particle extinction coefficients were collected in parallel to the radiation data. Aerosol layers of Saharan dust, partly mixed with biomass-burning smoke, were probed. With corresponding radiative transfer simulations the single scattering albedo and the asymmetry parameter of the aerosol particles were derived although with high uncertainty. The broad-band aerosol solar radiative forcing at the top of atmosphere was calculated and examined as a function of the aerosol types. However, due to uncertainties in both the measurements and the calculations the chemical composition cannot be identified. In addition, a mostly measurement-based method to derive the broad-band aerosol solar radiative forcing was used. This approach revealed clear differences of broad-band net irradiances as a function of the aerosol optical depth. The data were used to identify different aerosol types from different origins. Higher portions of biomass-burning smoke lead to larger broad-band net irradiances.
Regional modelling of Saharan dust and biomass-burning smoke, Part 2: Direct radiative forcing and atmospheric dynamic response
2017, Heinold, Bernd, Tegen, Ina, Bauer, Stefan, Wendisch, Manfred
The direct radiative forcing and dynamic atmospheric response due to Saharan dust and biomass-burning aerosol particles are presented for a case study during the SAMUM-2 field campaign in January and February 2008. The regional model system COSMO-MUSCAT is used. It allows online interaction of the computed dust and smoke load with the solar and terrestrial radiation and with the model dynamics. Model results of upward solar irradiances are evaluated against airborne radiation measurements in the Cape Verde region. The comparison shows a good agreement for the case of dust and smoke mixture. Dust and smoke particles influence the atmospheric dynamics by changing the radiative heating rates. The related pressure perturbations modify local and synoptic scale air-flow patterns. In the radiative feedback simulations, the Hadley circulation is enhanced and convergence zones occur along the Guinea coast. Thus, the smoke particles spread more than 5◦ further north and the equatorward transport is reduced. Within the convergence zones, Saharan dust and biomass-burning material are more effectively advected towards the Cape Verdes. Given the model uncertainties, the agreement between the modelled and observed aerosol distribution is locally improved when aerosol–radiation interaction is considered.
Optical properties of aerosol mixtures derived from sun-sky radiometry during SAMUM-2
2017, Toledano, C., Wiegner, M., Groß, S., Freudenthaler, V., Gasteiger, J., Müller, D., Müller, T., Schladitz, A., Weinzierl, B., Torres, B., O’neill, N.T.
The SAMUM-2 experiment took place in the Cape Verde is lands in January–February 2008. The colocated ground-based and airborne instruments allow the study of desert dust optical and microphysical properties in a closure experiment. The Meteorological Institute of the University of Munich deployed one sun-sky photometer and two tropospheric lidar systems. A travelling AERONET-Cimel sun-sky radiometer was also deployed. During the measurement period the aerosol scenario over Cape Verde mostly consisted of a dust layer below 2 km and a smoke-dust layer above 2–4 km a.s.l. The Saharan dust arrived at the site from the NE, whereas the smoke originated in the African equatorial region. This paper describes the main results of the Sun photometer observations, supported by lidar information. An analysis of the variations in the aerosol optical depth (AOD) in the range 340–1550 nm, the Ångström exponent, volume size distributions and single scattering albedo is presented. The aerosol mixtures are analysed by means of the fine mode fraction of the AOD provided by the sun-sky inversion data and the Spectral Deconvolution Algorithm. The mean AOD (500 nm) was 0.31, with associated low ångström exponent of 0.46. Several types of events were detected within the data set, with prevalence of dust or mixtures as characterized by the Ångstr¨om exponents of extinction and absorption and the fine mode fraction. Aerosol properties derived from sunphotometry were compared to in situ measurements of size distribution, effective radius and single scattering albedo.
Optical and microphysical properties of smoke over Cape Verde inferred from multiwavelength lidar measurements
2017, Tesche, Matthias, Müller, Detlef, Gross, Silke, Ansmann, Albert, Althausen, Dietrich, Freudenthaler, Volker, Weinzierl, Bernadett, Veira, Andreas, Petzold, Andreas
Lidar measurements of mixed dust/smoke plumes over the tropical Atlantic ocean were carried out during the winter campaign of SAMUM-2 at Cape Verde. Profiles of backscatter and extinction coefficients, lidar ratios, and Ångstr¨om exponents related to pure biomass-burning aerosol from southern West Africa were extracted from these observations. Furthermore, these findings were used as input for an inversion algorithm to retrieve microphysical properties of pure smoke. Seven measurement days were found suitable for the procedure of aerosol-type separation and successive inversion of optical data that describe biomass-burning smoke. We inferred high smoke lidar ratios of 87 ± 17 sr at 355 nm and 79 ± 17 sr at 532 nm. Smoke lidar ratios and Ångstr¨om exponents are higher compared to the ones for the dust/smoke mixture. These numbers indicate higher absorption and smaller sizes for pure smoke particles compared to the dust/smoke mixture. Inversion of the smoke data set results in mean effective radii of 0.22 ± 0.08 μm with individual results varying between 0.10 and 0.36 μm. The single-scattering albedo for pure biomass-burning smoke was found to vary between 0.63 and 0.89 with a very low mean value of 0.75 ± 0.07. This is in good agreement with findings of airborne in situ measurements which showed values of 0.77 ± 0.03. Effective radii from the inversion were similar to the ones found for the fine mode of the in situ size distributions.
Dust mobilization and aerosol transport from West Africa to Cape Verde - a meteorological overview of SAMUM-2
2017, Knippertz, Peter, Tesche, Matthias, Heinold, Bernd, Kandler, Konrad, Toledano, Carlos, Esselborn, Michael
The second field campaign of the SAharan Mineral dUst experiMent (SAMUM-2) was performed between 15 January and 14 February 2008 at the airport of Praia, Cape Verde, and provided valuable information to study the westward transport of Saharan dust and the mixing with biomass-burning smoke and sea-salt aerosol. Here lidar, meteorological, and particle measurements at Praia, together with operational analyses, trajectories, and satellite and synoptic station data are used to give an overview of the meteorological conditions and to place other SAMUM-2 measurements into a large-scale context. It is demonstrated that wintertime dust conditions at Cape Verde are closely related to the movement and intensification of mid-latitude high-pressure systems and the associated pressure gradients at their southern flanks. These cause dust emission over Mauritania, Mali, and Niger, and subsequent westward transport to Cape Verde within about 1–5 d. Dust emissions often peak around midday, suggesting a relation to daytime mixing of momentum from nocturnal low-level jets to the surface. The dust layer over Cape Verde is usually restricted to the lowest 1.5 km of the atmosphere. During periods with near-surface wind speeds about 5.5 ms−1, a maritime aerosol layer develops which often mixes with dust from above. On most days, the middle levels up to about 5 km additionally contain smoke that can be traced back to sources in southernWest Africa. Above this layer, clean air masses are transported to Cape Verde with the westerly flow at the southern side of the subtropical jet. The penetration of extra-tropical disturbances to low latitudes can bring troposphere-deep westerly flow and unusually clean conditions to the region.