CaltechAUTHORS
Published June 8, 2023 | Version Published + Supplemental Material
Journal Article Open

NO at low concentration can enhance the formation of highly oxygenated biogenic molecules in the atmosphere

Creators

  • 1. ROR icon Nanjing University
  • 2. ROR icon University of Helsinki
  • 3. ROR icon Lund University
  • 4. ROR icon Goethe University Frankfurt
  • 5. ROR icon Paul Scherrer Institute
  • 6. ROR icon University of California, Irvine
  • 7. ROR icon Swiss Federal Institute for Forest, Snow and Landscape Research
  • 8. ROR icon University of Vienna
  • 9. ROR icon University of Colorado Boulder
  • 10. ROR icon University of Lisbon
  • 11. ROR icon California Institute of Technology
  • 12. ROR icon Universität Innsbruck
  • 13. ROR icon Carnegie Mellon University
  • 14. ROR icon Cyprus Institute
  • 15. ROR icon Pusan National University
  • 16. ROR icon Finnish Meteorological Institute
  • 17. ROR icon National Research Council Canada
  • 18. ROR icon P.N. Lebedev Physical Institute of the Russian Academy of Sciences
  • 19. ROR icon Moscow Institute of Physics and Technology
  • 20. ROR icon University of Beira Interior
  • 21. ROR icon Fudan University
  • 22. ROR icon European Organization for Nuclear Research
  • 23. ROR icon Aerodyne Research

Abstract

The interaction between nitrogen monoxide (NO) and organic peroxy radicals (RO2) greatly impacts the formation of highly oxygenated organic molecules (HOM), the key precursors of secondary organic aerosols. It has been thought that HOM production can be significantly suppressed by NO even at low concentrations. Here, we perform dedicated experiments focusing on HOM formation from monoterpenes at low NO concentrations (0 – 82 pptv). We demonstrate that such low NO can enhance HOM production by modulating the RO₂ loss and favoring the formation of alkoxy radicals that can continue to autoxidize through isomerization. These insights suggest that HOM yields from typical boreal forest emissions can vary between 2.5%-6.5%, and HOM formation will not be completely inhibited even at high NO concentrations. Our findings challenge the notion that NO monotonically reduces HOM yields by extending the knowledge of RO₂-NO interactions to the low-NO regime. This represents a major advance towards an accurate assessment of HOM budgets, especially in low-NO environments, which prevails in the pre-industrial atmosphere, pristine areas, and the upper boundary layer.

Additional Information

© The Author(s) 2023. This article is licensed under a Creative Commons Attribution 4.0 International License, which permits use, sharing, adaptation, distribution and reproduction in any medium or format, as long as you give appropriate credit to the original author(s) and the source, provide a link to the Creative Commons license, and indicate if changes were made. The images or other third party material in this article are included in the article's Creative Commons license, unless indicated otherwise in a credit line to the material. If material is not included in the article's Creative Commons license and your intended use is not permitted by statutory regulation or exceeds the permitted use, you will need to obtain permission directly from the copyright holder. To view a copy of this license, visit http://creativecommons.org/licenses/by/4.0/. We thank CERN for supporting CLOUD with technical and financial resources. We thank the tofTools team for providing programs for data analysis of mass spectrometry. We thank Lei Wang and Duzitian Li for analyzing the NOₓ data of SORPES and SMEAR II stations. This work was supported by the National Natural Science Foundation of China (NSFC) project (92044301, 42220104006, 42075101 and 41975154), the Jiangsu Provincial Collaborative Innovation Center of Climate Change, the Academy of Finland (grant nos. 317380, 320094 and 323255), the Fundamental Research Funds for the Centra Universities, the Swedish Research Council VR (project nr. 2019-05006), the Swedish Research Council FORMAS (project nr. 2018-01745), the strategic research area MERGE hosted by Lund University, US National Science Foundation (nos. AGS-1801574, AGS-1801897, and AGS-2132089), the H2020 European Research Council (CHAPAs (grant no. 850614). These authors contributed equally: Wei Nie, Chao Yan. Contributions. W.N., C.Y., A.D., M.E. and N.M.D. designed the study; W.N., C.Y., L.Y., P.R. and Y.L. analyzed the data; W.N., C.Y., L.Y., A.D., M.E. and N.M.D. wrote the manuscript; A.V., D.S., H.F., A.A., F.B., J.C., L.D., D.D., J.Du., A.H., X-C.H., V.H., T.J., C.K., K.L., L.N., R.M., V.M., B.M., A.M-O., L.L.Q., S.S., M.S., C.T., A.T., R.V., A.C.W., R.W., M. W., P.Y., H.L., W.H., X.Q., S.L., T.L. and X.C. collected the data and contributed to the analysis; U.M., T.P., J.Do., U.B., I.E.H., J.K., D.W. and M.K. contributed to data interpretation and editing of manuscript. Data availability. The observation data that support the main findings of this study are available at figshare (https://doi.org/10.6084/m9.figshare.22724648.v1). Code availability. Data processing techniques are available on request from the corresponding author. The authors declare no competing interests.

Attached Files

Published - s41467-023-39066-4.pdf

Supplemental Material - 41467_2023_39066_MOESM1_ESM.pdf

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Additional details

Identifiers

PMCID
PMC10250349
Eprint ID
121956
Resolver ID
CaltechAUTHORS:20230615-129171000.11

Related works

Describes
10.6084/m9.figshare.22724648.v1 (DOI)

Funding

CERN
National Natural Science Foundation of China
92044301
National Natural Science Foundation of China
42075101
National Natural Science Foundation of China
42220104006
National Natural Science Foundation of China
41975154
Jiangsu Provincial Collaborative Innovation Center of Climate Change
Academy of Finland
317380
Academy of Finland
320094
Academy of Finland
323255
Fundamental Research Funds for the Central Universities
Swedish Research Council
2019-05006
Swedish Research Council
2018-01745-COBACCA
Lund University
NSF
AGS-1801574
NSF
AGS-1801897
NSF
AGS-2132089
European Research Council (ERC)
850614

Dates

Created
2023-06-27
Created from EPrint's datestamp field
Updated
2023-06-27
Created from EPrint's last_modified field