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Creators/Authors contains: "Mutzel, Anke"

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  1. Knowledge of the viscosity of particles containing secondary organic material (SOM) is useful for predicting reaction rates and diffusion in SOM particles. In this study we investigate the viscosity of SOM particles as a function of relative humidity and SOM particle mass concentration, during SOM synthesis. The SOM was generated via the ozonolysis of α-pinene at < 5 % relative humidity (RH). Experiments were carried out using the poke-and-flow technique, which measures the experimental flow time (τexp, flow) of SOM after poking the material with a needle. In the first set of experiments, we show that τexp, flow increased by a factor of 3600 as the RH increased from < 0.5 RH to 50 % RH, for SOM with a production mass concentration of 121 µg m−3. Based on simulations, the viscosities of the particles were between 6  ×  105 and 5  ×  107 Pa s at < 0.5 % RH and between 3  ×  102 and 9  ×  103 Pa s at 50 % RH. In the second set of experiments we show that under dry conditions τexp, flow decreased by a factor of 45 as the production mass concentration increased from 121 to 14 000 µg m−3. From simulations of the poke-and-flow experiments, the viscosity of SOM with a production mass concentration of 14 000 µg m−3 was determined to be between 4  ×  104 and 1.5  ×  106 Pa s compared to between 6  ×  105 and 5  ×  107 Pa s for SOM with a production mass concentration of 121 µg m−3. The results can be rationalized by a dependence of the chemical composition of SOM on production conditions. These results emphasize the shifting characteristics of SOM, not just with RH and precursor type, but also with the production conditions, and suggest that production mass concentration and the RH at which the viscosity was determined should be considered both when comparing laboratory results and when extrapolating these results to the atmosphere. 
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  2. Abstract. Oxidation of biogenic volatile organic compounds (BVOC) by the nitrate radical (NO3) represents one of the important interactions between anthropogenic emissions related to combustion and natural emissions from the biosphere. This interaction has been recognized for more than 3 decades, during which time a large body of research has emerged from laboratory, field, and modeling studies. NO3-BVOC reactions influence air quality, climate and visibility through regional and global budgets for reactive nitrogen (particularly organic nitrates), ozone, and organic aerosol. Despite its long history of research and the significance of this topic in atmospheric chemistry, a number of important uncertainties remain. These include an incomplete understanding of the rates, mechanisms, and organic aerosol yields for NO3-BVOC reactions, lack of constraints on the role of heterogeneous oxidative processes associated with the NO3 radical, the difficulty of characterizing the spatial distributions of BVOC and NO3 within the poorly mixed nocturnal atmosphere, and the challenge of constructing appropriate boundary layer schemes and non-photochemical mechanisms for use in state-of-the-art chemical transport and chemistry–climate models. This review is the result of a workshop of the same title held at the Georgia Institute of Technology in June 2015. The first half of the review summarizes the current literature on NO3-BVOC chemistry, with a particular focus on recent advances in instrumentation and models, and in organic nitrate and secondary organic aerosol (SOA) formation chemistry. Building on this current understanding, the second half of the review outlines impacts of NO3-BVOC chemistry on air quality and climate, and suggests critical research needs to better constrain this interaction to improve the predictive capabilities of atmospheric models. 
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