The Earth’s atmosphere is a complex system with many layers, but the troposphere is where 85% of its air resides. Understanding the atmospheric chemistry that drives changes in the troposphere’s composition is crucial. One area of particular importance is the formation and prevalence of secondary organic aerosols (SOAs), which can have significant impacts on the planet’s radiation balance, air quality, and human health.

An international team of researchers, led by the U.S. Department of Energy’s (DOE) Argonne National Laboratory, Sandia National Laboratories, and NASA’s Jet Propulsion Laboratory (JPL), has made groundbreaking discoveries that are shedding light on the formation of SOAs. In a new paper published in Nature Geosciences, the team detailed their findings, which are based on the study of a class of compounds known as Criegee intermediates (CIs).

Criegee intermediates are believed to play a crucial role in the formation of SOAs through a process called oligomerization. However, until now, no one had directly identified the chemical signatures of this process in the field. By using advanced methods for detecting gas-phase molecules and aerosols in the atmosphere, the team conducted field measurements in the Amazon rainforest, a key area for SOA formation. They were able to find clear evidence consistent with reactions of a Criegee intermediate compound containing carbon, hydrogen, and oxygen (CH2OO).

Rebecca L. Caravan, an assistant chemist at Argonne and the first author of the paper, emphasized the significance of this discovery. The team was able to establish direct connections between what was observed in the field, anticipated reactions with oligomerization of CIs, and characterizations made in the lab. Their findings suggest that CI chemistry may have a larger impact on altering the troposphere’s composition than current atmospheric models acknowledge, potentially by an order of magnitude.

While the discoveries made by the research team represent significant progress in understanding atmospheric chemistry, there are still challenges ahead. Carl Percival, a researcher at NASA’s JPL, highlighted the need for further research to fully define the role of CI reactions in the troposphere. The updated modeling based on their work indicated that there may be unidentified chemical mechanisms at play, driving even more transformation within the troposphere. As such, there is still much work to be done in unraveling the complexities of atmospheric chemistry and its implications for our planet.


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