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Creators/Authors contains: "Leisner, Thomas"

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  1. Abstract. Indole (ind) is a nitrogen-containing heterocyclic volatile organic compound commonly emitted from animal husbandry and from different plants like maize with global emissions of 0.1 Tg yr−1. The chemical composition and optical properties of indole secondary organic aerosol (SOA) and brown carbon (BrC) are still not well understood. To address this, environmental chamber experiments were conducted to investigate the oxidation of indole at atmospherically relevant concentrations of selected oxidants (OH radicals and O3) with or without NO2. In the presence of NO2, the SOA yields decreased by more than a factor of 2, but the mass absorption coefficient at 365 nm (MAC365) of ind-SOA was 4.3 ± 0.4 m2 g−1, which was 5 times higher than that in experiments without NO2. In the presence of NO2, C8H6N2O2 (identified as 3-nitroindole) contributed 76 % to all organic compounds detected by a chemical ionization mass spectrometer, contributing ∼ 50 % of the light absorption at 365 nm (Abs365). In the absence of NO2, the dominating chromophore was C8H7O3N, contributing to 20 %–30 % of Abs365. Indole contributes substantially to the formation of secondary BrC and its potential impact on the atmospheric radiative transfer is further enhanced in the presence of NO2, as it significantly increases the specific light absorption of ind-SOA by facilitating the formation of 3-nitroindole. This work provides new insights into an important process of brown carbon formation by interaction of two pollutants, NO2 and indole, mainly emitted by anthropogenic activities. 
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  2. null (Ed.)
    Abstract. Ice crystal submicron structures have a large impact on the opticalproperties of cirrus clouds and consequently on their radiative effect.Although there is growing evidence that atmospheric ice crystals are rarelypristine, direct in situ observations of the degree of ice crystal complexityare largely missing. Here we show a comprehensive in situ data set of icecrystal complexity coupled with measurements of the cloud angular scatteringfunctions collected during a number of observational airborne campaigns atdiverse geographical locations. Our results demonstrate that an overwhelmingfraction (between 61 % and 81 %) of atmospheric ice crystals sampledin the different regions contain mesoscopic deformations and, as aconsequence, a similar flat and featureless angular scattering function isobserved. A comparison between the measurements and a database of opticalparticle properties showed that severely roughened hexagonal aggregatesoptimally represent the measurements in the observed angular range. Based onthis optical model, a new parameterization of the cloud bulk asymmetry factorwas introduced and its effects were tested in a global climate model. Themodelling results suggest that, due to ice crystal complexity, ice-containingclouds can induce an additional short-wave cooling effect of−1.12 W m2 on the top-of-the-atmosphere radiative budget that hasnot yet been considered. 
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