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- ItemModel simulations of chemical effects of sprites in relation with observed HO2 enhancements over sprite-producing thunderstorms(Katlenburg-Lindau : European Geosciences Union, 2021) Winkler, Holger; Yamada, Takayoshi; Kasai, Yasuko; Berger, Uwe; Notholt, JustusRecently, measurements by the Superconducting Submillimeter-Wave Limb Emission Sounder (SMILES) satellite instrument have been presented which indicate an increase in mesospheric HO2 above sprite-producing thunderstorms. The aim of this paper is to compare these observations to model simulations of chemical sprite effects. A plasma chemistry model in combination with a vertical transport module was used to simulate the impact of a streamer discharge in the altitude range 70–80 km, corresponding to one of the observed sprite events. Additionally, a horizontal transport and dispersion model was used to simulate advection and expansion of the sprite air masses. The model simulations predict a production of hydrogen radicals mainly due to reactions of proton hydrates formed after the electrical discharge. The net effect is a conversion of water molecules into H+OH. This leads to increasing HO2 concentrations a few hours after the electric breakdown. Due to the modelled long-lasting increase in HO2 after a sprite discharge, an accumulation of HO2 produced by several sprites appears possible. However, the number of sprites needed to explain the observed HO2 enhancements is unrealistically large. At least for the lower measurement tangent heights, the production mechanism of HO2 predicted by the model might contribute to the observed enhancements.
- ItemImpact of water uptake and mixing state on submicron particle deposition in the human respiratory tract (HRT) based on explicit hygroscopicity measurements at HRT-like conditions(Katlenburg-Lindau : EGU, 2022) Man, Ruiqi; Wu, Zhijun; Zong, Taomou; Voliotis, Aristeidis; Qiu, Yanting; Größ, Johannes; van Pinxteren, Dominik; Zeng, Limin; Herrmann, Hartmut; Wiedensohler, Alfred; Hu, MinParticle hygroscopicity plays a key role in determining the particle deposition in the human respiratory tract (HRT). In this study, the effects of hygroscopicity and mixing state on regional and total deposition doses on the basis of the particle number concentration for children, adults, and the elderly were quantified using the Multiple-Path Particle Dosimetry model, based on the size-resolved particle hygroscopicity measurements at HRT-like conditions (relative humidity = 98 %) performed in the North China Plain. The measured particle population with an external mixing state was dominated by hygroscopic particles (number fraction = (91.5 ± 5.7) %, mean ± standard deviation (SD); the same below). Particle hygroscopic growth in the HRT led to a reduction by around 24 % in the total doses of submicron particles for all age groups. Such a reduction was mainly caused by the growth of hygroscopic particles and was more pronounced in the pulmonary and tracheobronchial regions. Regardless of hygroscopicity, the elderly group of people had the highest total dose among three age groups, while children received the maximum total deposition rate. With 270 nm in diameter as the boundary, the total deposition doses of particles smaller than this diameter were overestimated, and those of larger particles were underestimated, assuming no particle hygroscopic growth in the HRT. From the perspective of the daily variation, the deposition rates of hygroscopic particles with an average of (2.88 ± 0.81) × 109 particles h-1 during the daytime were larger than those at night ((2.32 ± 0.24) × 109 particles h-1). On the contrary, hydrophobic particles interpreted as freshly emitted soot and primary organic aerosols exhibited higher deposition rates at nighttime ((3.39 ± 1.34) × 108 particles h-1) than those in the day ((2.58 ± 0.76) × 108 particles h-1). The traffic emissions during the rush hours enhanced the deposition rate of hydrophobic particles. This work provides a more explicit assessment of the impact of hygroscopicity and mixing state on the deposition pattern of submicron particles in the HRT. Copyright:
- ItemEvaluated kinetic and photochemical data for atmospheric chemistry: Volume VII-Criegee intermediates(Katlenburg-Lindau : EGU, 2020) Cox, R. Anthony; Ammann, Markus; Crowley, John N.; Herrmann, Hartmut; Jenkin, Michael E.; Faye McNeill, V.; Mellouki, Abdelwahid; Troe, Jürgen; Wallington, Timothy J.This article, the seventh in the series, presents kinetic and photochemical data sheets evaluated by the IUPAC Task Group on Atmospheric Chemical Kinetic Data Evaluation. It covers an extension of the gas-phase and photochemical reactions related to Criegee intermediates previously published in Atmospheric Chemistry and Physics (ACP) in 2006 and implemented on the IUPAC website up to 2020. The article consists of an introduction, description of laboratory measurements, a discussion of rate coefficients for reactions of O3 with alkenes producing Criegee intermediates, rate coefficients of unimolecular and bimolecular reactions and photochemical data for reactions of Criegee intermediates, and an overview of the atmospheric chemistry of Criegee intermediates. Summary tables of the recommended kinetic and mechanistic parameters for the evaluated reactions are provided. Data sheets summarizing information upon which the recommendations are based are given in two files, provided as a Supplement to this article. © Author(s) 2020.