Wildfire smoke, Arctic haze, and aerosol effects on mixed-phase and cirrus clouds over the North Pole region during MOSAiC: an introduction Atmospheric Chemistry and Physics DOI 10.5194/acp-21-13397-2021 27 October 2021 A Raman lidar was operated aboard the icebreaker Polarstern during MOSAiC and monitored aerosol and cloud layers in the central Arctic up to 30 km height. The article provides an overview of the spectrum of aerosol profiling observations and shows aerosol–cloud interaction studies for liquid-water and ice clouds. A highlight was the detection of a 10 km deep wildfire smoke layer over the North Pole up to 17 km height from the fire season of 2019, which persisted over the whole winter period. Read more
Predicting gas–particle partitioning coefficients of atmospheric molecules with machine learning Atmospheric Chemistry and Physics DOI 10.5194/acp-21-13227-2021 22 October 2021 The study of climate change relies on climate models, which require an understanding of aerosol formation. We train a machine-learning model to predict the partitioning coefficients of atmospheric molecules, which govern condensation into aerosols. The model can make instant predictions based on molecular structures with accuracy surpassing that of standard computational methods. This will allow the screening of low-volatility molecules that contribute most to aerosol formation. Read more
Opinion: The germicidal effect of ambient air (open-air factor) revisited Atmospheric Chemistry and Physics DOI 10.5194/acp-21-13011-2021 18 October 2021 The term open-air factor was coined in the 1960s, establishing that rural air had powerful germicidal properties possibly resulting from immediate products of the reaction of ozone with alkenes, unsaturated compounds ubiquitously present in natural and polluted environments. We have re-evaluated those early experiments, applying the recently substantially improved knowledge, and put them into the context of the lifetime of aerosol-borne pathogens that are so important in the Covid-19 pandemic. Read more
Opinion: Papers that shaped tropospheric chemistry Atmospheric Chemistry and Physics DOI 10.5194/acp-21-12909-2021 6 October 2021 Which published papers have transformed our understanding of the chemical processes in the troposphere and shaped the field of atmospheric chemistry? We explore how these papers have shaped the development of the field of atmospheric chemistry and identify the major landmarks in the field of atmospheric chemistry through the lens of those papers’ impact on science, legislation and environmental events. Read more
The long-term transport and radiative impacts of the 2017 British Columbia pyrocumulonimbus smoke aerosols in the stratosphere Atmospheric Chemistry and Physics DOI 10.5194/acp-21-12069-2021 22 September 2021 Interactions of extreme fires with weather systems can produce towering smoke plumes that inject aerosols at very high altitudes (> 10 km). Three such major injections, largest at the time in terms of emitted aerosol mass, took place over British Columbia, Canada, in August 2017. We model the transport and impacts of injected aerosols on the radiation balance of the atmosphere. Our model results match the satellite-observed plume transport and residence time at these high altitudes very closely. Read more
Better representation of dust can improve climate models with too weak an African monsoon Atmospheric Chemistry and Physics DOI 10.5194/acp-21-11423-2021 6 September 2021 Earth system models have persistent biases that impinge on our ability to make robust future regional predictions of precipitation. For the last 15 years, there has been little improvement in these biases. This work presents an accurate representation of dust absorption based upon observed dust mineralogical composition and size distribution. The striking result is that this more accurate representation improves tropical precipitations for climate models with too weak an African monsoon. Read more
Disparities in particulate matter (PM10) origins and oxidative potential at a city scale (Grenoble, France) – Part 2. Atmospheric Chemistry and Physics DOI 10.5194/acp-21-9719-2021 11 August 2021 With an enhanced source apportionment obtained in a companion paper, this paper acquires more understanding of the spatiotemporal associations of the sources of PM to oxidative potential (OP), an emerging health-based metric. Multilayer perceptron neural network analysis was used to apportion OP from PM sources. Results showed that such a methodology is as robust as the linear classical inversion and permits an improvement in the OP prediction when local features or non-linear effects occur. Read more
Investigations on the anthropogenic reversal of the natural ozone gradient between northern and southern midlatitudes Atmospheric Chemistry and Physics DOI 10.5194/acp-21-9669-2021 6 August 2021 The few ozone measurements made before the 1980s indicate that industrial development increased ozone concentrations by a factor of ~ 2 at northern midlatitudes, which are now larger than at southern midlatitudes. This difference was much smaller, and likely reversed, in the pre-industrial atmosphere. Earth system models find similar increases, but not higher pre-industrial ozone in the south. This disagreement may indicate that modeled natural ozone sources and/or deposition loss are inadequate. Read more
Smoke-charged vortices in the stratosphere generated by wildfires and their behaviour in both hemispheres: comparing Australia 2020 to Canada 2017 Atmospheric Chemistry and Physics DOI 10.5194/acp-21-7113-2021 30 June 2021 Following the 2020 Australian fires, it was recently discovered that stratospheric wildfire smoke plumes self-organize as anticyclonic vortices that persist for months and rise by 10 km due to the radiative heating from the absorbing smoke. In this study, we show that smoke-charged vortices previously occurred in the aftermath of the 2017 Canadian fires. We use meteorological analysis to characterize this new object in geophysical fluid dynamics, which likely impacts radiation and climate. Read more
Heterogeneous interactions between SO2 and organic peroxides in submicron aerosol Atmospheric Chemistry and Physics DOI 10.5194/acp-21-6647-2021 21 June 2021 Discrepancies between atmospheric modeling and field observations, especially in highly polluted cities, have highlighted the lack of understanding of sulfate formation mechanisms and kinetics. Here, we directly quantify the reactive uptake coefficient of SO2 onto organic peroxides and study the important governing factors. The SO2 uptake rate was observed to depend on RH, peroxide amount and reactivity, pH, and ionic strength, which provides a framework to better predict sulfate formation. Read more