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Transport and chemistry of isoprene and its oxidation products in deep convective clouds
Stockholm University, Faculty of Science, Department of Meteorology .
Stockholm University, Faculty of Science, Department of Environmental Science.ORCID iD: 0000-0001-9085-2319
Stockholm University, Faculty of Science, Department of Environmental Science.ORCID iD: 0000-0002-9384-9702
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2021 (English)In: Tellus. Series B, Chemical and physical meteorology, ISSN 0280-6509, E-ISSN 1600-0889, Vol. 73, no 1, p. 1-21Article in journal (Refereed) Published
Abstract [en]

Deep convective clouds can transport trace gases from the planetary boundary layer into the upper troposphere where subsequent chemistry may impact aerosol particle formation and growth. In this modelling study, we investigate processes that affect isoprene and its oxidation products injected into the upper troposphere by an isolated deep convective cloud in the Amazon. We run a photochemical box model with coupled cloud microphysics along hundreds of individual air parcel trajectories sampled from a cloud-resolving model simulation of a convective event. The box model simulates gas-phase chemical reactions, gas scavenging by liquid and ice hydrometeors, and turbulent dilution inside a deep convective cloud. The results illustrate the potential importance of gas uptake to anvil ice in regulating the intensity of the isoprene oxidation and associated low volatility organic vapour concentrations in the outflow. Isoprene transport and fate also depends on the abundance of lightning-generated nitrogen oxide radicals (NOx = NO + NO2). If gas uptake on ice is efficient and lightning activity is low, around 30% of the boundary layer isoprene will survive to the cloud outflow after approximately one hour of transport, while all the low volatile oxidation products will be scavenged by the cloud hydrometeors. If lightning NOx is abundant and gas uptake by ice is inefficient, then all isoprene will be oxidised during transport or in the immediate outflow region, while several low volatility isoprene oxidation products will have elevated concentrations in the cloud outflow. Reducing uncertainties associated with the uptake of vapours on ice hydrometeors, especially HO2 and oxygenated organics, is essential to improve predictions of isoprene and its oxidation products in deep convective outflows and their potential contribution to new particle formation and growth.

Place, publisher, year, edition, pages
2021. Vol. 73, no 1, p. 1-21
Keywords [en]
Convective transport of isoprene, deep convective cloud trajectories, photochemical box model
National Category
Meteorology and Atmospheric Sciences
Identifiers
URN: urn:nbn:se:su:diva-197760DOI: 10.1080/16000889.2021.1979856ISI: 000702561000001OAI: oai:DiVA.org:su-197760DiVA, id: diva2:1603188
Available from: 2021-10-14 Created: 2021-10-14 Last updated: 2025-02-07Bibliographically approved
In thesis
1. Transport and chemical processing of trace gases in deep convective clouds
Open this publication in new window or tab >>Transport and chemical processing of trace gases in deep convective clouds
2021 (English)Doctoral thesis, comprehensive summary (Other academic)
Abstract [en]

Deep convective clouds can efficiently transport trace gases from the planetary boundary layer to the upper troposphere. Once there, some gases will contribute to new particle formation and growth, eventually producing aerosols that are large enough to influence cloud properties, the radiative budget of the Earth, and climate. The magnitude and exact pathways of the convective transport of many organic and inorganic compounds are, however, still unclear. This dissertation presents a framework to study vertical transport of gas mixtures by deep convective clouds. The method consists of a chemical box model that is driven by cloud air parcel trajectory data generated by large-eddy simulation. This combination allows us to examine detailed gas-cloud interactions as well as complex systems of gas-phase chemical reactions. A large ensemble of simulated cloud trajectories was used to identify and characterize convective up- and downdrafts in the Amazon region. The analysis showed that air parcels starting close to the surface (at 0.5 km) experienced a substantially larger probability of reaching the upper troposphere (above 10 km) than parcels starting at the top of the boundary layer. Furthermore, the framework was used to estimate the vertical transport of isoprene, isoprene oxidation products, ammonia, and several non-reactive trace gases. We found that a typical Amazonian deep convective cloud can transport around 30% of the boundary layer isoprene to the cloud outflow if the efficiency of the gas uptake on ice is high and there is no lightning within the cloud. If the efficiency of gas uptake on ice is low and lightning within the cloud is extensive, all isoprene will be oxidized. Several low-volatility isoprene oxidation products will then have relatively high concentrations in the outflow, which potentially could lead to new particle formation and growth. Another result was that up to 10% of the boundary layer ammonia can reach the cloud outflow, where it in some environments can nucleate synergistically with nitric and sulfuric acid. A key uncertainty in our estimates is the efficiency of gas uptake by ice particles.

Place, publisher, year, edition, pages
Stockholm: Department of Meteorology, Stockholm University, 2021. p. 32
Keywords
gas transport, atmospheric chemistry, convective cloud, box model, new particle formation
National Category
Meteorology and Atmospheric Sciences
Research subject
Atmospheric Sciences and Oceanography
Identifiers
urn:nbn:se:su:diva-197903 (URN)978-91-7911-656-9 (ISBN)978-91-7911-657-6 (ISBN)
Public defence
2021-12-08, Vivi Täckholmsalen (Q-salen), NPQ-huset, Svante Arrhenius väg 20, Stockholm, 13:00 (English)
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Available from: 2021-11-15 Created: 2021-10-18 Last updated: 2025-02-07Bibliographically approved

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Bardakov, RomanRiipinen, IlonaKrejci, RadovanEkman, Annica M. L.

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