Simon Rosanka

Bio: Simon Rosanka is an academic researcher from Forschungszentrum Jülich. The author has contributed to research in topics: Atmospheric chemistry & Troposphere. The author has an hindex of 5, co-authored 12 publications receiving 119 citations.

Ubiquitous atmospheric production of organic acids mediated by cloud droplets.

Abstract: Atmospheric acidity is increasingly determined by carbon dioxide and organic acids1–3. Among the latter, formic acid facilitates the nucleation of cloud droplets4 and contributes to the acidity of clouds and rainwater1,5. At present, chemistry–climate models greatly underestimate the atmospheric burden of formic acid, because key processes related to its sources and sinks remain poorly understood2,6–9. Here we present atmospheric chamber experiments that show that formaldehyde is e ciently converted to gaseous formic acid via a multiphase pathway that involves its hydrated form, methanediol. In warm cloud droplets, methanediol undergoes fast outgassing but slow dehydration. Using a chemistry–climate model, we estimate that the gas-phase oxidation of methanediol produces up to four times more formic acid than all other known chemical sources combined. Our ndings reconcile model predictions and measurements of formic acid abundance. The additional formic acid burden increases atmospheric acidity by reducing the pH of clouds and rainwater by up to 0.3. The diol mechanism presented here probably applies to other aldehydes and may help to explain the high atmospheric levels of other organic acids that a ect aerosol growth and cloud evolution.

Importance of isomerization reactions for OH radical regeneration from the photo-oxidation of isoprene investigated in the atmospheric simulation chamber SAPHIR

Abstract: . Theoretical, laboratory, and chamber studies have shown fast regeneration of the hydroxyl radical (OH) in the photochemistry of isoprene, largely due to unimolecular reactions which were previously thought not to be important under atmospheric conditions. Based on early field measurements, nearly complete regeneration was hypothesized for a wide range of tropospheric conditions, including areas such as the rainforest where slow regeneration of OH radicals is expected due to low concentrations of nitric oxide (NO). In this work the OH regeneration in isoprene oxidation is directly quantified for the first time through experiments covering a wide range of atmospherically relevant NO levels (between 0.15 and 2 ppbv – parts per billion by volume) in the atmospheric simulation chamber SAPHIR. These conditions cover remote areas partially influenced by anthropogenic NO emissions, giving a regeneration efficiency of OH close to 1, and areas like the Amazonian rainforest with very low NO, resulting in a surprisingly high regeneration efficiency of 0.5, i.e. a factor of 2 to 3 higher than explainable in the absence of unimolecular reactions. The measured radical concentrations were compared to model calculations, and the best agreement was observed when at least 50 % of the total loss of isoprene peroxy radicals conformers (weighted by their abundance) occurs via isomerization reactions for NO lower than 0.2 ppbv. For these levels of NO, up to 50 % of the OH radicals are regenerated from the products of the 1,6 α -hydroxy-hydrogen shift (1,6-H shift) of Z- δ - RO2 radicals through the photolysis of an unsaturated hydroperoxy aldehyde (HPALD) and/or through the fast aldehydic hydrogen shift (rate constant ∼10 s −1 at 300 K) in di-hydroperoxy carbonyl peroxy radicals (di-HPCARP- RO2 ), depending on their relative yield. The agreement between all measured and modelled trace gases (hydroxyl, hydroperoxy, and organic peroxy radicals, carbon monoxide, and the sum of methyl vinyl ketone, methacrolein, and hydroxyl hydroperoxides) is nearly independent of the adopted yield of HPALD and di-HPCARP- RO2 as both degrade relatively fast ( h), forming the OH radical and CO among other products. Taking into consideration this and earlier isoprene studies, considerable uncertainties remain on the distribution of oxygenated products, which affect radical levels and organic aerosol downwind of unpolluted isoprene-dominated regions.

Atmospheric chemical loss processes of isocyanic acid (HNCO): a combined theoretical kinetic and global modelling study

Abstract: . Isocyanic acid (HNCO) is a chemical constituent suspected to be harmful to humans if ambient concentrations exceed ∼1 ppbv. HNCO is mainly emitted by combustion processes but is also inadvertently released by NOx mitigation measures in flue gas treatments. With increasing biomass burning and more widespread usage of catalytic converters in car engines, good prediction of HNCO atmospheric levels with global models is desirable. Little is known directly about the chemical loss processes of HNCO, which limits the implementation in global Earth system models. This study aims to close this knowledge gap by combining a theoretical kinetic study on the major oxidants reacting with HNCO with a global modelling study. The potential energy surfaces of the reactions of HNCO with OH and NO3 radicals, Cl atoms, and ozone were studied using high-level CCSD(T)/CBS(DTQ)//M06-2X/aug-cc-pVTZ quantum chemical methodologies, followed by transition state theory (TST) theoretical kinetic predictions of the rate coefficients at temperatures of 200–3000 K . It was found that the reactions are all slow in atmospheric conditions, with k ( 300 K ) ≤ 7 × 10 - 16 cm 3 molecule - 1 s - 1 , and that product formation occurs predominantly by H abstraction; the predictions are in good agreement with earlier experimental work, where available. The reverse reactions of NCO radicals with H2O , HNO3 , and HCl, of importance mostly in combustion, were also examined briefly. The findings are implemented into the atmospheric model EMAC (ECHAM/MESSy Atmospheric Chemistry) to estimate the importance of each chemical loss process on a global scale. The EMAC predictions confirm that the gas-phase chemical loss of HNCO is a negligible process, contributing less than 1 % and leaving heterogeneous losses as the major sinks. The removal of HNCO by clouds and precipitation contributes about 10 % of the total loss, while globally dry deposition is the main sink, accounting for ∼90 %. The global simulation also shows that due to its long chemical lifetime in the free troposphere, HNCO can be efficiently transported into the UTLS by deep convection events. Daily-average mixing ratios of ground-level HNCO are found to regularly exceed 1 ppbv in regions dominated by biomass burning events, but rarely exceed levels above 10 ppt in other areas of the troposphere, though locally instantaneous toxic levels are expected.

Simulation of organics in the atmosphere: evaluation of EMACv2.54 with the Mainz Organic Mechanism (MOM) coupled to the ORACLE (v1.0) submodel

Abstract: . An updated and expanded representation of organics in the chemistry general circulation model EMAC (ECHAM5/MESSy for Atmospheric Chemistry) has been evaluated. First, the comprehensive Mainz Organic Mechanism (MOM) in the submodel MECCA (Module Efficiently Calculating the Chemistry of the Atmosphere) was activated with explicit degradation of organic species up to five carbon atoms and a simplified mechanism for larger molecules. Second, the ORACLE submodel (version 1.0) considers now condensation on aerosols for all organics in the mechanism. Parameterizations for aerosol yields are used only for the lumped species that are not included in the explicit mechanism. The simultaneous usage of MOM and ORACLE allows an efficient estimation, not only of the chemical degradation of the simulated volatile organic compounds, but also of the contribution of organics to the growth and fate of (organic) aerosol, with a complexity of the mechanism largely increased compared to EMAC simulations with more simplified chemistry. The model evaluation presented here reveals that the OH concentration is well reproduced globally, while significant biases for observed oxygenated organics are present. We also investigate the general properties of the aerosols and their composition, showing that the more sophisticated and process-oriented secondary aerosol formation does not degrade the good agreement of previous model configurations with observations at the surface, allowing further research in the field of gas-aerosol interactions.

This is How the Discussion Started

Abstract: A copy of Guangbo jiemu bao [Broadcast Program Report] was being passed from hand to hand among a group of young people eager to be the first to read the article introducing the program "What Is Revolutionary Love?" It said: "… Young friends, you are certainly very concerned about this problem'. So, we would like you to meet the young women workers Meng Xiaoyu and Meng Yamei and the older cadre Miss Feng. They are the three leading characters in the short story ‘The Place of Love.’ Through the description of the love lives of these three, the story induces us to think deeply about two questions that merit further examination.

On the Radiative Forcing by Contrails

Abstract: A parametric study of the instantaneous radiative impact of contrails is presented using three different radiative transfer models for a series of model atmospheres and cloud parameters. Contrails are treated as geometrically and optically thin plane parallel homogeneous cirrus layers in a static atmosphere. The ice water content is varied as a function of ambient temperature. The model atmospheres include tropical, mid-latitude, and subarctic summer and winter atmospheres. Optically thin contrails cause a positive net forcing at top of the atmosphere. At the surface the radiative forcing is negative during daytime. The forcing increases with the optical depth and the amount of contrail cover. At the top of the atmosphere, a mean contrail cover of 0.1% with average optical depth of 0.2 to 0.5 causes about 0.01 to 0.03 Wm−2 daily mean instantaneous radiative forcing. Contrails cool the surface during the day and heat the surface during the night, and hence reduce the daily temperature amplitude. The net effect depends strongly on the daily variation of contrail cloud cover. The indirect radiative forcing due to particle changes in natural cirrus clouds may be of the same magnitude as the direct one due to additional cover.

Evaluating the climate impact of aviation emission scenarios towards the Paris agreement including COVID-19 effects.

Abstract: Aviation is an important contributor to the global economy, satisfying society’s mobility needs. It contributes to climate change through CO2 and non-CO2 effects, including contrail-cirrus and ozone formation. There is currently significant interest in policies, regulations and research aiming to reduce aviation’s climate impact. Here we model the effect of these measures on global warming and perform a bottom-up analysis of potential technical improvements, challenging the assumptions of the targets for the sector with a number of scenarios up to 2100. We show that although the emissions targets for aviation are in line with the overall goals of the Paris Agreement, there is a high likelihood that the climate impact of aviation will not meet these goals. Our assessment includes feasible technological advancements and the availability of sustainable aviation fuels. This conclusion is robust for several COVID-19 recovery scenarios, including changes in travel behaviour.