Self-consistent global transport of metallic ions with WACCM-X Atmospheric Chemistry and Physics DOI 10.5194/acp-21-15619-2021 3 January 2022 Metal layers occur in the MLT region (80–120 km) from the ablation of cosmic dust. The latest lidar observations show these metals can reach a height approaching 200 km, which is challenging to explain. We have developed the first global simulation incorporating the full life cycle of metal atoms and ions. The model results compare well with lidar and satellite observations of the seasonal and diurnal variation of the metals and demonstrate the importance of ion mass and ion-neutral coupling. WACCM-X">Read more
Direct estimates of biomass burning NOx emissions and lifetimes using daily observations from TROPOMI Atmospheric Chemistry and Physics DOI 10.5194/acp-21-15569-2021 31 December 2021 We describe direct estimates of NOx emissions and lifetimes for biomass burning plumes using daily TROPOMI retrievals of NO2. Satellite-derived NOx emission factors are consistent with those from in situ measurements. We observe decreasing NOx lifetime with fire intensity, which is due to the increase in NOx abundance and radical production. Our findings suggest promise for applying space-based observations to track the emissions and chemical evolution of reactive nitrogen from wildfires. TROPOMI">Read more
How alkaline compounds control atmospheric aerosol particle acidity Atmospheric Chemistry and Physics DOI 10.5194/acp-21-14983-2021 22 December 2021 Aerosol particle pH is well-buffered by alkaline compounds, notably NH3 and crustal elements. NH3 is found to supply remarkable buffering capacity on a global scale, from the polluted continents to the remote oceans. Potential future changes in agricultural NH3 must be accompanied by strong reductions of SO2 and NOx to avoid particles becoming highly acidic, with implications for human health (aerosol toxicity), ecosystems (acid deposition), clouds, and climate (aerosol hygroscopicity). Read more
Aerosol–cloud interactions: the representation of heterogeneous ice activation in cloud models Atmospheric Chemistry and Physics DOI 10.5194/acp-21-15213-2021 20 December 2021 Aerosol–cloud interactions play an important role in climate change. Simulations of the competition between homogeneous solution droplet freezing and heterogeneous ice nucleation can be compromised by the misapplication of ice-active particle fractions frequently derived from laboratory measurements or parametrizations. Our study frames the problem and establishes a solution that is easy to implement in cloud models. Read more
Ambient aerosol properties in the remote atmosphere from global-scale in situ measurements Atmospheric Chemistry and Physics DOI 10.5194/acp-21-15023-2021 15 December 2021 The Atmospheric Tomography Mission was an airborne study that mapped the chemical composition of the remote atmosphere. From this, we developed a comprehensive description of aerosol properties that provides a unique, global-scale dataset against which models can be compared. The data show the polluted nature of the remote atmosphere in the Northern Hemisphere and quantify the contributions of sea salt, dust, soot, biomass burning particles, and pollution particles to the haziness of the sky. Read more
The driving factors of new particle formation and growth in the polluted boundary layer Atmospheric Chemistry and Physics DOI 10.5194/acp-21-14275-2021 19 November 2021 Experiments at CLOUD show that in polluted environments new particle formation (NPF) is largely driven by the formation of sulfuric acid–base clusters, stabilized by amines, high ammonia concentrations or lower temperatures. While oxidation products of aromatics can nucleate, they play a minor role in urban NPF. Our experiments span 4 orders of magnitude variation of observed NPF rates in ambient conditions. We provide a framework based on NPF and growth rates to interpret ambient observations. Read more
Heterogeneity and chemical reactivity of the remote troposphere defined by aircraft measurements Atmospheric Chemistry and Physics DOI 10.5194/acp-21-13729-2021 3 November 2021 The NASA Atmospheric Tomography (ATom) mission built a climatology of the chemical composition of tropospheric air parcels throughout the middle of the Pacific and Atlantic oceans. The level of detail allows us to reconstruct the photochemical budgets of O3 and CH4 over these vast, remote regions. We find that most of the chemical heterogeneity is captured at the resolution used in current global chemistry models and that the majority of reactivity occurs in the “hottest” 20 % of parcels. Read more
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