Incomplete mass closure in atmospheric nanoparticle growth

Abstract Nucleation and subsequent growth of new aerosol particles in the atmosphere is a major source of cloud condensation nuclei and persistent large uncertainty in climate models. Newly formed particles need to grow rapidly to avoid scavenging by pre-existing aerosols and become relevant for the...

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Main Authors: Dominik Stolzenburg, Nina Sarnela, Federico Bianchi, Jing Cai, Runlong Cai, Yafang Cheng, Lubna Dada, Neil M. Donahue, Hinrich Grothe, Sebastian Holm, Veli-Matti Kerminen, Katrianne Lehtipalo, Tuukka Petäjä, Juha Sulo, Paul M. Winkler, Chao Yan, Juha Kangasluoma, Markku Kulmala
Format: Article
Language:English
Published: Nature Portfolio 2025-02-01
Series:npj Climate and Atmospheric Science
Online Access:https://doi.org/10.1038/s41612-025-00893-5
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author Dominik Stolzenburg
Nina Sarnela
Federico Bianchi
Jing Cai
Runlong Cai
Yafang Cheng
Lubna Dada
Neil M. Donahue
Hinrich Grothe
Sebastian Holm
Veli-Matti Kerminen
Katrianne Lehtipalo
Tuukka Petäjä
Juha Sulo
Paul M. Winkler
Chao Yan
Juha Kangasluoma
Markku Kulmala
author_facet Dominik Stolzenburg
Nina Sarnela
Federico Bianchi
Jing Cai
Runlong Cai
Yafang Cheng
Lubna Dada
Neil M. Donahue
Hinrich Grothe
Sebastian Holm
Veli-Matti Kerminen
Katrianne Lehtipalo
Tuukka Petäjä
Juha Sulo
Paul M. Winkler
Chao Yan
Juha Kangasluoma
Markku Kulmala
author_sort Dominik Stolzenburg
collection DOAJ
description Abstract Nucleation and subsequent growth of new aerosol particles in the atmosphere is a major source of cloud condensation nuclei and persistent large uncertainty in climate models. Newly formed particles need to grow rapidly to avoid scavenging by pre-existing aerosols and become relevant for the climate and air quality. In the continental atmosphere, condensation of oxygenated organic molecules is often the dominant mechanism for rapid growth. However, the huge variety of different organics present in the continental boundary layer makes it challenging to predict nanoparticle growth rates from gas-phase measurements. Moreover, recent studies have shown that growth rates of nanoparticles derived from particle size distribution measurements show surprisingly little dependency on potentially condensable vapors observed in the gas phase. Here, we show that the observed nanoparticle growth rates in the sub-10 nm size range can be predicted in the boreal forest only for springtime conditions, even with state-of-the-art mass spectrometers and particle sizing instruments. We find that, especially under warmer conditions, observed growth is slower than predicted from gas-phase condensation. We show that only a combination of simple particle-phase reaction schemes, phase separation due to non-ideal solution behavior, or particle-phase diffusion limitations can explain the observed lower growth rates. Our analysis provides first insights as to why atmospheric nanoparticle growth rates above 10 nm h−1 are rarely observed. Ultimately, a reduction of experimental uncertainties and improved sub-10 nm particle hygroscopicity and chemical composition measurements are needed to further investigate the occurrence of such a growth rate-limiting process.
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spelling doaj-art-e1f4a1f4394e497bb2b3df18b42ecdaa2025-08-20T03:04:18ZengNature Portfolionpj Climate and Atmospheric Science2397-37222025-02-01811910.1038/s41612-025-00893-5Incomplete mass closure in atmospheric nanoparticle growthDominik Stolzenburg0Nina Sarnela1Federico Bianchi2Jing Cai3Runlong Cai4Yafang Cheng5Lubna Dada6Neil M. Donahue7Hinrich Grothe8Sebastian Holm9Veli-Matti Kerminen10Katrianne Lehtipalo11Tuukka Petäjä12Juha Sulo13Paul M. Winkler14Chao Yan15Juha Kangasluoma16Markku Kulmala17Institute of Materials Chemistry, TU WienInstitute for Atmospheric and Earth System Research/Physics, University of HelsinkiInstitute for Atmospheric and Earth System Research/Physics, University of HelsinkiInstitute for Atmospheric and Earth System Research/Physics, University of HelsinkiInstitute for Atmospheric and Earth System Research/Physics, University of HelsinkiMinerva Research Group, Max Planck Institute for ChemistryInstitute for Atmospheric and Earth System Research/Physics, University of HelsinkiCenter for Atmospheric Particle Studies, Carnegie Mellon UniversityInstitute of Materials Chemistry, TU WienInstitute for Atmospheric and Earth System Research/Physics, University of HelsinkiInstitute for Atmospheric and Earth System Research/Physics, University of HelsinkiInstitute for Atmospheric and Earth System Research/Physics, University of HelsinkiInstitute for Atmospheric and Earth System Research/Physics, University of HelsinkiInstitute for Atmospheric and Earth System Research/Physics, University of HelsinkiFaculty of Physics, University of ViennaInstitute for Atmospheric and Earth System Research/Physics, University of HelsinkiInstitute for Atmospheric and Earth System Research/Physics, University of HelsinkiInstitute for Atmospheric and Earth System Research/Physics, University of HelsinkiAbstract Nucleation and subsequent growth of new aerosol particles in the atmosphere is a major source of cloud condensation nuclei and persistent large uncertainty in climate models. Newly formed particles need to grow rapidly to avoid scavenging by pre-existing aerosols and become relevant for the climate and air quality. In the continental atmosphere, condensation of oxygenated organic molecules is often the dominant mechanism for rapid growth. However, the huge variety of different organics present in the continental boundary layer makes it challenging to predict nanoparticle growth rates from gas-phase measurements. Moreover, recent studies have shown that growth rates of nanoparticles derived from particle size distribution measurements show surprisingly little dependency on potentially condensable vapors observed in the gas phase. Here, we show that the observed nanoparticle growth rates in the sub-10 nm size range can be predicted in the boreal forest only for springtime conditions, even with state-of-the-art mass spectrometers and particle sizing instruments. We find that, especially under warmer conditions, observed growth is slower than predicted from gas-phase condensation. We show that only a combination of simple particle-phase reaction schemes, phase separation due to non-ideal solution behavior, or particle-phase diffusion limitations can explain the observed lower growth rates. Our analysis provides first insights as to why atmospheric nanoparticle growth rates above 10 nm h−1 are rarely observed. Ultimately, a reduction of experimental uncertainties and improved sub-10 nm particle hygroscopicity and chemical composition measurements are needed to further investigate the occurrence of such a growth rate-limiting process.https://doi.org/10.1038/s41612-025-00893-5
spellingShingle Dominik Stolzenburg
Nina Sarnela
Federico Bianchi
Jing Cai
Runlong Cai
Yafang Cheng
Lubna Dada
Neil M. Donahue
Hinrich Grothe
Sebastian Holm
Veli-Matti Kerminen
Katrianne Lehtipalo
Tuukka Petäjä
Juha Sulo
Paul M. Winkler
Chao Yan
Juha Kangasluoma
Markku Kulmala
Incomplete mass closure in atmospheric nanoparticle growth
npj Climate and Atmospheric Science
title Incomplete mass closure in atmospheric nanoparticle growth
title_full Incomplete mass closure in atmospheric nanoparticle growth
title_fullStr Incomplete mass closure in atmospheric nanoparticle growth
title_full_unstemmed Incomplete mass closure in atmospheric nanoparticle growth
title_short Incomplete mass closure in atmospheric nanoparticle growth
title_sort incomplete mass closure in atmospheric nanoparticle growth
url https://doi.org/10.1038/s41612-025-00893-5
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