Heterogeneous nucleation drives particle size segregation in sequential ozone and nitrate radical oxidation of catechol

Secondary organic aerosol formation via condensation of organic vapors onto existing aerosol transforms the chemical composition and size distribution of ambient aerosol, with implications for air quality and Earth's radiative balance. Gas-to-particle conversion is generally thought to occur on a continuum between equilibrium-driven partitioning of semivolatile molecules to the pre-existing mass size distribution and kinetic-driven condensation of low volatility molecules to the pre-existing surface area size distribution. However, we offer experimental evidence in contrast to this framework. When catechol is sequentially oxidized by O-3 and NO3 in the presence of (NH4)(2)SO4 seed particles with a single size mode, we observe a bimodal organic aerosol mass size distribution with two size modes of distinct chemical composition with nitrocatechol from NO3 oxidation preferentially condensing onto the large end of the pre-existing size distribution (similar to 750 nm). A size-resolved chemistry and microphysics model reproduces the evolution of the two distinct organic aerosol size modes-heterogeneous nucleation to an independent, nitrocatechol-rich aerosol phase.

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Author Garofalo, L. A.
He, Y.
Jathar, S. H.
Pierce, J. R.
Fredrickson, C. D.
Palm, B. B.
Thornton, J. A.
Mahrt, F.
Crescenzo, G. V.
Bertram, A. K.
Draper, D. C.
Fry, Juliane
Orlando, John J.
Zhang, Xuan
Farmer, D. K.
Publisher UCAR/NCAR - Library
Publication Date 2021-12-07T00:00:00
Digital Object Identifier (DOI) Not Assigned
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Topic Category geoscientificInformation
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Metadata Date 2025-07-11T16:09:07.651521
Metadata Record Identifier edu.ucar.opensky::articles:25177
Metadata Language eng; USA
Suggested Citation Garofalo, L. A., He, Y., Jathar, S. H., Pierce, J. R., Fredrickson, C. D., Palm, B. B., Thornton, J. A., Mahrt, F., Crescenzo, G. V., Bertram, A. K., Draper, D. C., Fry, Juliane, Orlando, John J., Zhang, Xuan, Farmer, D. K.. (2021). Heterogeneous nucleation drives particle size segregation in sequential ozone and nitrate radical oxidation of catechol. UCAR/NCAR - Library. https://n2t.org/ark:/85065/d74q7zkg. Accessed 03 August 2025.

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