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The Pagami Creek smoke plume after long-range transport to the upper troposphere over Europe – Aerosol properties and black carbon mixing state

2014, Dahlkötter, F., Gysel, M., Sauer, D., Minikin, A., Baumann, R., Seifert, P., Ansmann, A., Fromm, M., Voigt, C., Weinzierl, B.

During the CONCERT 2011 field experiment with the DLR research aircraft Falcon, an enhanced aerosol layer with particle linear depolarization ratios of 6–8% at 532 nm was observed at altitudes above 10 km over northeast Germany on 16 September 2011. Dispersion simulations with HYSPILT suggest that the elevated aerosol layer originated from the Pagami Creek forest fire in Minnesota, USA, which caused pyro-convective uplift of particles and gases. The 3–4 day-old smoke plume had high total refractory black carbon (rBC) mass concentrations of 0.03–0.35 μg m−3 at standard temperature and pressure (STP) with rBC mass equivalent diameter predominantly smaller than 130 nm. Assuming a core-shell particle structure, the BC cores exhibit very thick (median: 105–136 nm) BC-free coatings. A large fraction of the BC-containing particles disintegrated into a BC-free fragment and a BC fragment while passing through the laser beam of the Single Particle Soot Photometer (SP2). In this study, the disintegration is a result of very thick coatings around the BC cores. This is in contrast to a previous study in a forest-fire plume, where it was hypothesized to be a result of BC cores being attached to a BC-free particle. For the high-altitude forest-fire aerosol layer observed in this study, increased mass specific light-absorption cross sections of BC can be expected due to the very thick coatings around the BC cores, while this would not be the case for the attached-type morphology. We estimate the BC mass import from the Pagami Creek forest fire into the upper troposphere/lower stratosphere (UTLS) region (best estimate: 25 Mg rBC). A comparison to black carbon emission rates from aviation underlines the importance of pyro-convection on the BC load in the UTLS region. Our study provides detailed information on the microphysics and the mixing state of BC in the forest-fire aerosol layer in the upper troposphere that can be used to better understand and investigate the radiative impact of such upper tropospheric aerosol layers.

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Surface matters: Limitations of CALIPSO V3 aerosol typing in coastal regions

2014, Kanitz, T., Ansmann, A., Foth, A., Seifert, P., Wandinger, U., Engelmann, R., Baars, H., Althausen, D., Casiccia, C., Zamorano, F.

In the CALIPSO data analysis, surface type (land/ocean) is used to augment the aerosol characterization. However, this surface-dependent aerosol typing prohibits a correct classification of marine aerosol over land that is advected from ocean to land. This might result in a systematic overestimation of the particle extinction coefficient and of the aerosol optical thickness (AOT) of up to a factor of 3.5 over land in coastal areas. We present a long-term comparison of CALIPSO and ground-based lidar observations of the aerosol conditions in the coastal environment of southern South America (Punta Arenas, Chile, 53° S), performed in December 2009–April 2010. Punta Arenas is almost entirely influenced by marine particles throughout the year, indicated by a rather low AOT of 0.02–0.04. However, we found an unexpectedly high fraction of continental aerosol in the aerosol types inferred by means of CALIOP observations and, correspondingly, too high values of particle extinction. Similar features of the CALIOP data analysis are presented for four other coastal areas around the world. Since CALIOP data serve as important input for global climate models, the influence of this systematic error was estimated by means of simplified radiative-transfer calculations.

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Four-year long-path monitoring of ambient aerosol extinction at a central European urban site: Dependence on relative humidity

2016, Skupin, A., Ansmann, A., Engelmann, R., Seifert, P., Müller, T.

The ambient aerosol particle extinction coefficient is measured with the Spectral Aerosol Extinction Monitoring System (SÆMS) along a 2.84 km horizontal path at 30–50 m height above ground in the urban environment of Leipzig (51.3° N, 12.4° E), Germany, since 2009. The dependence of the particle extinction coefficient (wavelength range from 300 to 1000 nm) on relative humidity up to almost 100 % was investigated. The main results are presented. For the wavelength of 550 nm, the mean extinction enhancement factor was found to be 1.75 ± 0.4 for an increase of relative humidity from 40 to 80 %. The respective 4-year mean extinction enhancement factor is 2.8 ± 0.6 for a relative-humidity increase from 40 to 95 %. A parameterization of the dependency of the urban particle extinction coefficient on relative humidity is presented. A mean hygroscopic exponent of 0.46 for the 2009–2012 period was determined. Based on a backward trajectory cluster analysis, the dependence of several aerosol optical properties for eight air flow regimes was investigated. Large differences were not found, indicating that local pollution sources widely control the aerosol conditions over the urban site. The comparison of the SÆMS extinction coefficient statistics with respective statistics from ambient AERONET sun photometer observations yields good agreement. Also, time series of the particle extinction coefficient computed from in situ-measured dry particle size distributions and humidity-corrected SÆMS extinction values (for 40 % relative humidity) were found in good overall consistency, which verifies the applicability of the developed humidity parameterization scheme. The analysis of the spectral dependence of particle extinction (Ångström exponent) revealed an increase of the 390–881 nm Ångström exponent from, on average, 0.3 (at 30 % relative humidity) to 1.3 (at 95 % relative humidity) for the 4-year period.