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- ItemBiomass burning and urban emission impacts in the Andes Cordillera region based on in situ measurements from the Chacaltaya observatory, Bolivia (5240a.s.l.)(Katlenburg-Lindau : EGU, 2019) Chauvigné, Aurélien; Aliaga, Diego; Sellegri, Karine; Montoux, Nadège; Krejci, Radovan; Močnik, Griša; Moreno, Isabel; Müller, Thomas; Pandolfi, Marco; Velarde, Fernando; Weinhold, Kay; Ginot, Patrick; Wiedensohler, Alfred; Andrade, Marcos; Laj, PaoloThis study documents and analyses a 4-year continuous record of aerosol optical properties measured at the Global Atmosphere Watch (GAW) station of Chacaltaya (CHC; 5240a.s.l.), in Bolivia. Records of particle light scattering and particle light absorption coefficients are used to investigate how the high Andean Cordillera is affected by both long-range transport and by the fast-growing agglomeration of La Paz-El Alto, located approximately 20km away and 1.5km below the sampling site. The extended multi-year record allows us to study the properties of aerosol particles for different air mass types, during wet and dry seasons, also covering periods when the site was affected by biomass burning in the Bolivian lowlands and the Amazon Basin. The absorption, scattering, and extinction coefficients (median annual values of 0.74, 12.14, and 12.96Mm-1 respectively) show a clear seasonal variation with low values during the wet season (0.57, 7.94, and 8.68Mm-1 respectively) and higher values during the dry season (0.80, 11.23, and 14.51Mm-1 respectively). The record is driven by variability at both seasonal and diurnal scales. At a diurnal scale, all records of intensive and extensive aerosol properties show a pronounced variation (daytime maximum, night-time minimum), as a result of the dynamic and convective effects. The particle light absorption, scattering, and extinction coefficients are on average 1.94, 1.49, and 1.55 times higher respectively in the turbulent thermally driven conditions than the more stable conditions, due to more efficient transport from the boundary layer. Retrieved intensive optical properties are significantly different from one season to the other, reflecting the changing aerosol emission sources of aerosol at a larger scale. Using the wavelength dependence of aerosol particle optical properties, we discriminated between contributions from natural (mainly mineral dust) and anthropogenic (mainly biomass burning and urban transport or industries) emissions according to seasons and local circulation. The main sources influencing measurements at CHC are from the urban area of La Paz-El Alto in the Altiplano and from regional biomass burning in the Amazon Basin. Results show a 28% to 80% increase in the extinction coefficients during the biomass burning season with respect to the dry season, which is observed in both tropospheric dynamic conditions. From this analysis, long-term observations at CHC provide the first direct evidence of the impact of biomass burning emissions of the Amazon Basin and urban emissions from the La Paz area on atmospheric optical properties at a remote site all the way to the free troposphere. © Author(s) 2019.
- ItemMultidecadal trend analysis of in situ aerosol radiative properties around the world(Katlenburg-Lindau : EGU, 2020) Collaud Coen, Martine; Andrews, Elisabeth; Alastuey, Andrés; Petkov Arsov, Todor; Backman, John; Brem, Benjamin T.; Bukowiecki, Nicolas; Couret, Cédric; Eleftheriadis, Konstantinos; Flentje, Harald; Fiebig, Markus; Gysel-Beer, Martin; Hand, Jenny L.; Hoffer, András; Hooda, Rakesh; Hueglin, Christoph; Joubert, Warren; Keywood, Melita; Eun Kim, Jeong; Kim, Sang-Woo; Labuschagne, Casper; Lin, Neng-Huei; Lin, Yong; Lund Myhre, Cathrine; Luoma, Krista; Lyamani, Hassan; Marinoni, Angela; Mayol-Bracero, Olga L.; Mihalopoulos, Nikos; Pandolfi, Marco; Prats, Natalia; Prenni, Anthony J.; Putaud, Jean-Philippe; Ries, Ludwig; Reisen, Fabienne; Sellegri, Karine; Sharma, Sangeeta; Sheridan, Patrick; Sherman, James Patrick; Sun, Junying; Titos, Gloria; Torres, Elvis; Tuch, Thomas; Weller, Rolf; Wiedensohler, Alfred; Zieger, Paul; Laj, PaoloIn order to assess the evolution of aerosol parameters affecting climate change, a long-term trend analysis of aerosol optical properties was performed on time series from 52 stations situated across five continents. The time series of measured scattering, backscattering and absorption coefficients as well as the derived single scattering albedo, backscattering fraction, scattering and absorption Ångström exponents covered at least 10 years and up to 40 years for some stations. The non-parametric seasonal Mann-Kendall (MK) statistical test associated with several pre-whitening methods and with Sen's slope was used as the main trend analysis method. Comparisons with general least mean square associated with autoregressive bootstrap (GLS/ARB) and with standard least mean square analysis (LMS) enabled confirmation of the detected MK statistically significant trends and the assessment of advantages and limitations of each method. Currently, scattering and backscattering coefficient trends are mostly decreasing in Europe and North America and are not statistically significant in Asia, while polar stations exhibit a mix of increasing and decreasing trends. A few increasing trends are also found at some stations in North America and Australia. Absorption coefficient time series also exhibit primarily decreasing trends. For single scattering albedo, 52 % of the sites exhibit statistically significant positive trends, mostly in Asia, eastern/northern Europe and the Arctic, 22 % of sites exhibit statistically significant negative trends, mostly in central Europe and central North America, while the remaining 26 % of sites have trends which are not statistically significant. In addition to evaluating trends for the overall time series, the evolution of the trends in sequential 10-year segments was also analyzed. For scattering and backscattering, statistically significant increasing 10-year trends are primarily found for earlier periods (10-year trends ending in 2010-2015) for polar stations and Mauna Loa. For most of the stations, the present-day statistically significant decreasing 10-year trends of the single scattering albedo were preceded by not statistically significant and statistically significant increasing 10-year trends. The effect of air pollution abatement policies in continental North America is very obvious in the 10-year trends of the scattering coefficient - there is a shift to statistically significant negative trends in 2009-2012 for all stations in the eastern and central USA. This long-term trend analysis of aerosol radiative properties with a broad spatial coverage provides insight into potential aerosol effects on climate changes. © 2020 Royal Society of Chemistry. All rights reserved.
- ItemProfiles of cloud condensation nuclei, dust mass concentration, and ice-nucleating-particle-relevant aerosol properties in the Saharan Air Layer over Barbados from polarization lidar and airborne in situ measurements(Katlenburg-Lindau : EGU, 2019) Haarig, Moritz; Walser, Adrian; Ansmann, Albert; Dollner, Maximilian; Althausen, Dietrich; Sauer, Daniel; Farrell, David; Weinzierl, BernadettThe present study aims to evaluate lidar retrievals of cloud-relevant aerosol properties by using polarization lidar and coincident airborne in situ measurements in the Saharan Air Layer (SAL) over the Barbados region. Vertical profiles of the number concentration of cloud condensation nuclei (CCN), large particles (diameter d > 500 nm), surface area, mass, and ice-nucleating particle (INP) concentration are derived from the lidar measurements and compared with CCN concentrations and the INP-relevant aerosol properties measured in situ with aircraft. The measurements were performed in the framework of the Saharan Aerosol Longrange Transport and Aerosol-Cloud-Interaction Experiment (SALTRACE) in summer 2013. The CCN number concentrations derived from lidar observations were up to a factor of 2 higher than the ones measured in situ aboard the research aircraft Falcon. Possible reasons for the difference are discussed. The number concentration of particles with a dry radius of more than 250 nm and the surface-area concentration obtained from the lidar observations and used as input for the INP parameterizations agreed well (< 30 %-50 % deviation) with the aircraft measurements. In a pronounced lofted dust layer during summer (10 July 2013), the lidar retrieval yielded 100-300 CCN per cubic centimeter at 0.2 % water supersaturation and 10-200 INPs per liter at-25?C. Excellent agreement was also obtained in the comparison of mass concentration profiles. During the SALTRACE winter campaign (March 2014), the dust layer from Africa was mixed with smoke particles which dominated the CCN number concentration. This example highlights the unique lidar potential to separate smoke and dust contributions to the CCN reservoir and thus to identify the sensitive role of smoke in trade wind cumuli developments over the tropical Atlantic during the winter season. © 2017 Georg Thieme Verlag. All rights reserved.
- ItemEstimation of cloud condensation nuclei number concentrations and comparison to in situ and lidar observations during the HOPE experiments(Katlenburg-Lindau : EGU, 2020) Genz, Christa; Schrödner, Roland; Heinold, Bernd; Henning, Silvia; Baars, Holger; Spindler, Gerald; Tegen, InaAtmospheric aerosol particles are the precondition for the formation of cloud droplets and therefore have large influence on the microphysical and radiative properties of clouds. In this work, four different methods to derive or measure number concentrations of cloud condensation nuclei (CCN) were analyzed and compared for presentday aerosol conditions: (i) a model parameterization based on simulated particle concentrations, (ii) the same parameterization based on gravimetrical particle measurements, (iii) direct CCN measurements with a CCN counter, and (iv) lidarderived and in situ measured vertical CCN profiles. In order to allow for sensitivity studies of the anthropogenic impact, a scenario to estimate the maximum CCN concentration under peak aerosol conditions of the mid-1980s in Europe was developed as well. In general, the simulations are in good agreement with the observations. At ground level, average values between 0.7 and 1:5 × 109 CCNm-3 at a supersaturation of 0.2 % were found with the different methods under present-day conditions. The discrimination of the chemical species revealed an almost equal contribution of ammonium sulfate and ammonium nitrate to the total number of CCN for present-day conditions. This was not the case for the peak aerosol scenario, in which it was assumed that no ammonium nitrate was formed while large amounts of sulfate were present, consuming all available ammonia during ammonium sulfate formation. The CCN number concentration at five different supersaturation values has been compared to the measurements. The discrepancies between model and in situ observations were lowest for the lowest (0.1 %) and highest supersaturations (0.7 %). For supersaturations between 0.3 % and 0.5 %, the model overestimated the potentially activated particle fraction by around 30 %. By comparing the simulation with observed profiles, the vertical distribution of the CCN concentration was found to be overestimated by up to a factor of 2 in the boundary layer. The analysis of the modern (year 2013) and the peak aerosol scenario (expected to be representative of the mid-1980s over Europe) resulted in a scaling factor, which was defined as the quotient of the average vertical profile of the peak aerosol and present-day CCN concentration. This factor was found to be around 2 close to the ground, increasing to around 3.5 between 2 and 5 km and approaching 1 (i.e., no difference between present-day and peak aerosol conditions) with further increasing height. © 2020 Author(s).