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Importance of size representation and morphology in modelling optical properties of black carbon: comparison between laboratory measurements and model simulations

2022, Romshoo, Baseerat, Pöhlker, Mira, Wiedensohler, Alfred, Pfeifer, Sascha, Saturno, Jorge, Nowak, Andreas, Ciupek, Krzysztof, Quincey, Paul, Vasilatou, Konstantina, Ess, Michaela N., Gini, Maria, Eleftheriadis, Konstantinos, Robins, Chris, Gaie-Levrel, François, Müller, Thomas

Black carbon (BC) from incomplete combustion of biomass or fossil fuels is the strongest absorbing aerosol component in the atmosphere. Optical properties of BC are essential in climate models for quantification of their impact on radiative forcing. The global climate models, however, consider BC to be spherical particles, which causes uncertainties in their optical properties. Based on this, an increasing number of model-based studies provide databases and parameterization schemes for the optical properties of BC, using more realistic fractal aggregate morphologies. In this study, the reliability of the different modelling techniques of BC was investigated by comparing them to laboratory measurements. The modelling techniques were examined for bare BC particles in the first step and for BC particles with organic material in the second step. A total of six morphological representations of BC particles were compared, three each for spherical and fractal aggregate morphologies. In general, the aggregate representation performed well for modelling the particle light absorption coefficient σabs, single-scattering albedo SSA, and mass absorption cross-section MACBC for laboratory-generated BC particles with volume mean mobility diameters dp,V larger than 100nm. However, for modelling Ångström absorption exponent AAE, it was difficult to suggest a method due to size dependence, although the spherical assumption was in better agreement in some cases. The BC fractal aggregates are usually modelled using monodispersed particles, since their optical simulations are computationally expensive. In such studies, the modelled optical properties showed a 25% uncertainty in using the monodisperse size method. It is shown that using the polydisperse size distribution in combination with fractal aggregate morphology reduces the uncertainty in measured σabs to 10% for particles with dp,V between 60-160nm. Furthermore, the sensitivities of the BC optical properties to the various model input parameters such as the real and imaginary parts of the refractive index (mre and mim), the fractal dimension (Df), and the primary particle radius (app) of an aggregate were investigated. When the BC particle is small and rather fresh, the change in the Df had relatively little effect on the optical properties. There was, however, a significant relationship between app and the particle light scattering, which increased by a factor of up to 6 with increasing total particle size. The modelled optical properties of BC are well aligned with laboratory-measured values when the following assumptions are used in the fractal aggregate representation: mre between 1.6 and 2, mim between 0.50 and 1, Df from 1.7 to 1.9, and app between 10 and 14nm. Overall, this study provides experimental support for emphasizing the importance of an appropriate size representation (polydisperse size method) and an appropriate morphological representation for optical modelling and parameterization scheme development of BC.

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The potential of elastic and polarization lidars to retrieve extinction profiles

2020, Giannakaki, Elina, Kokkalis, Panos, Marinou, Eleni, Bartsotas, Nikolaos S., Amiridis, Vassilis, Ansmann, Albert, Komppula, Mika

A new method, called ElEx (elastic extinction), is proposed for the estimation of extinction coefficient lidar profiles using only the information provided by the elastic and polarization channels of a lidar system. The method is applicable to lidar measurements both during daytime and nighttime under well-defined aerosol mixtures. ElEx uses the particle backscatter profiles at 532 nm and the vertically resolved particle linear depolarization ratio measurements at the same wavelength. The particle linear depolarization ratio and the lidar ratio values of pure aerosol types are also taken from literature. The total extinction profile is then estimated and compared well with Raman retrievals. In this study, ElEx was applied in an aerosol mixture of marine and dust particles at Finokalia station during the CHARADMExp campaign. Any difference between ElEx and Raman extinction profiles indicates that the nondust component could be probably attributed to polluted marine or polluted continental aerosols. Comparison with sun photometer aerosol optical depth observations is performed as well during daytime. Differences in the total aerosol optical depth are varying between 1.2 % and 72 %, and these differences are attributed to the limited ability of the lidar to correctly represent the aerosol optical properties in the near range due to the overlap problem. © 2020 Author(s).

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Application of the shipborne remote sensing supersite OCEANET for profiling of Arctic aerosols and clouds during Polarstern cruise PS106

2020, Griesche, Hannes J., Seifer, Patric, Ansmann, Albert, Baars, Holger, Velasco, Carola Barrientos, Bühl, Johannes, Engelmann, Ronny, Radenz, Martin, Zhenping, Yin, Macke, Andreas

From 25 May to 21 July 2017, the research vessel Polarstern performed the cruise PS106 to the high Arctic in the region north and northeast of Svalbard. The mobile remote-sensing platform OCEANET was deployed aboard Polarstern. Within a single container, OCEANET houses state-of-the-art remote-sensing equipment, including a multiwavelength Raman polarization lidar PollyXT and a 14-channel microwave radiometer HATPRO (Humidity And Temperature PROfiler). For the cruise PS106, the measurements were supplemented by a motion-stabilized 35 GHz cloud radar Mira-35. This paper describes the treatment of technical challenges which were immanent during the deployment of OCEANET in the high Arctic. This includes the description of the motion stabilization of the cloud radar Mira-35 to ensure vertical-pointing observations aboard the moving Polarstern as well as the applied correction of the vessels heave rate to provide valid Doppler velocities. The correction ensured a leveling accuracy of ±0.5◦ during transits through the ice and an ice floe camp. The applied heave correction reduced the signal induced by the vertical movement of the cloud radar in the PSD of the Doppler velocity by a factor of 15. Low-level clouds, in addition, frequently prevented a continuous analysis of cloud conditions from synergies of lidar and radar within Cloudnet, because the technically determined lowest detection height of Mira-35 was 165 m above sea level. To overcome this obstacle, an approach for identification of the cloud presence solely based on data from the near-field receiver of PollyXT at heights from 50 m and 165 m above sea level is presented. We found low-level stratus clouds, which were below the lowest detection range of most automatic ground-based remote-sensing instruments during 25 % of the observation time. We present case studies of aerosol and cloud studies to introduce the capabilities of the data set. In addition, new approaches for ice crystal effective radius and eddy dissipation rates from cloud radar measurements and the retrieval of aerosol optical and microphysical properties from the observations of PollyXT are introduced. © Author(s) 2020. This work is distributed under the Creative Commons Attribution 4.0 License.