External particle mixing influences hygroscopicity in a sub-urban area

<p>Hygroscopicity strongly influences aerosol properties and multiphase chemistry, which is essential in several atmospheric processes. Although CCN (cloud condensation nuclei) properties are commonly measured, sub-saturated hygroscopicity measurements remain rare. During the ACROSS campaign (...

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Main Authors: S. Deshmukh, L. Poulain, B. Wehner, S. Henning, J.-E. Petit, P. Fombelle, O. Favez, H. Herrmann, M. Pöhlker
Format: Article
Language:English
Published: Copernicus Publications 2025-01-01
Series:Atmospheric Chemistry and Physics
Online Access:https://acp.copernicus.org/articles/25/741/2025/acp-25-741-2025.pdf
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author S. Deshmukh
L. Poulain
B. Wehner
S. Henning
J.-E. Petit
P. Fombelle
P. Fombelle
O. Favez
H. Herrmann
M. Pöhlker
M. Pöhlker
author_facet S. Deshmukh
L. Poulain
B. Wehner
S. Henning
J.-E. Petit
P. Fombelle
P. Fombelle
O. Favez
H. Herrmann
M. Pöhlker
M. Pöhlker
author_sort S. Deshmukh
collection DOAJ
description <p>Hygroscopicity strongly influences aerosol properties and multiphase chemistry, which is essential in several atmospheric processes. Although CCN (cloud condensation nuclei) properties are commonly measured, sub-saturated hygroscopicity measurements remain rare. During the ACROSS campaign (Atmospheric ChemistRy Of the Suburban foreSt, conducted in Paris in summer 2022), particles' hygroscopic growth rates at 90 % relative humidity (RH) and chemical composition were measured at the sub-urban site using a Hygroscopicity Tandem Differential Mobility Analyser (HTDMA, scanning at 100, 150, 200, and 250 nm) and an Aerodyne High-Resolution Time-of-Flight Aerosol Mass Spectrometer (HR-ToF-AMS). Growth factor probability density functions (GF-PDFs) revealed two distinct modes, namely hydrophobic and hygroscopic, suggesting a combination of internal and external particle mixing, with the split at GF 1.2. The prevalence of the hygroscopic mode increased with particle size, with mean hygroscopicity (<span class="inline-formula"><i>κ</i></span>) values of 0.23 and 0.38 for 100 and 200 nm particles, respectively. Using the Zdanovskii–Stokes–Robinson (ZSR) mixing rule, the agreement between measured and chemically derived hygroscopicity was approximately 51% for 100 nm particles, which declined for 200 and 250 nm. These emphasise the large effect of external particle mixing and its influence on predicting hygroscopicity. The ZSR approach proves to be unreliable in predicting the wide growth distribution of externally mixed particles. In this measurement, 80 %–90 % of the particles were externally mixed and influenced by fresh emission, which affected the hygroscopicity prediction by a factor of 2. A cluster analysis based on backward trajectories and meteorological conditions gives valuable insights into the chemical composition and variations in the hygroscopicity of different air masses.</p>
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spelling doaj-art-9da90f771dc1445392f1a7fdf36d2e112025-01-23T09:48:12ZengCopernicus PublicationsAtmospheric Chemistry and Physics1680-73161680-73242025-01-012574175810.5194/acp-25-741-2025External particle mixing influences hygroscopicity in a sub-urban areaS. Deshmukh0L. Poulain1B. Wehner2S. Henning3J.-E. Petit4P. Fombelle5P. Fombelle6O. Favez7H. Herrmann8M. Pöhlker9M. Pöhlker10Leibniz Institute for Tropospheric Research, e.V. (TROPOS), Permoserstrasse 15, 04318 Leipzig, GermanyLeibniz Institute for Tropospheric Research, e.V. (TROPOS), Permoserstrasse 15, 04318 Leipzig, GermanyLeibniz Institute for Tropospheric Research, e.V. (TROPOS), Permoserstrasse 15, 04318 Leipzig, GermanyLeibniz Institute for Tropospheric Research, e.V. (TROPOS), Permoserstrasse 15, 04318 Leipzig, GermanyLaboratoire des Sciences du Climat et de l'Environnement, CEA-CNRS-UVSQ, IPSL, Université Paris-Saclay, 91191 Gif-sur-Yvette, FranceLaboratoire des Sciences du Climat et de l'Environnement, CEA-CNRS-UVSQ, IPSL, Université Paris-Saclay, 91191 Gif-sur-Yvette, Francenow at: Université Clermont Auvergne, Laboratoire de Météorologie Physique, OPGC/CNRS UMR 6016, Clermont-Ferrand, FranceInstitut National de l'Environnement Industriel et des Risques, Parc Technologique ALATA, Verneuil-en-Halatte, FranceLeibniz Institute for Tropospheric Research, e.V. (TROPOS), Permoserstrasse 15, 04318 Leipzig, GermanyLeibniz Institute for Tropospheric Research, e.V. (TROPOS), Permoserstrasse 15, 04318 Leipzig, GermanyFaculty of Physics and Earth Sciences, Leipzig Institute for Meteorology, Leipzig University, 04103 Leipzig, Germany<p>Hygroscopicity strongly influences aerosol properties and multiphase chemistry, which is essential in several atmospheric processes. Although CCN (cloud condensation nuclei) properties are commonly measured, sub-saturated hygroscopicity measurements remain rare. During the ACROSS campaign (Atmospheric ChemistRy Of the Suburban foreSt, conducted in Paris in summer 2022), particles' hygroscopic growth rates at 90 % relative humidity (RH) and chemical composition were measured at the sub-urban site using a Hygroscopicity Tandem Differential Mobility Analyser (HTDMA, scanning at 100, 150, 200, and 250 nm) and an Aerodyne High-Resolution Time-of-Flight Aerosol Mass Spectrometer (HR-ToF-AMS). Growth factor probability density functions (GF-PDFs) revealed two distinct modes, namely hydrophobic and hygroscopic, suggesting a combination of internal and external particle mixing, with the split at GF 1.2. The prevalence of the hygroscopic mode increased with particle size, with mean hygroscopicity (<span class="inline-formula"><i>κ</i></span>) values of 0.23 and 0.38 for 100 and 200 nm particles, respectively. Using the Zdanovskii–Stokes–Robinson (ZSR) mixing rule, the agreement between measured and chemically derived hygroscopicity was approximately 51% for 100 nm particles, which declined for 200 and 250 nm. These emphasise the large effect of external particle mixing and its influence on predicting hygroscopicity. The ZSR approach proves to be unreliable in predicting the wide growth distribution of externally mixed particles. In this measurement, 80 %–90 % of the particles were externally mixed and influenced by fresh emission, which affected the hygroscopicity prediction by a factor of 2. A cluster analysis based on backward trajectories and meteorological conditions gives valuable insights into the chemical composition and variations in the hygroscopicity of different air masses.</p>https://acp.copernicus.org/articles/25/741/2025/acp-25-741-2025.pdf
spellingShingle S. Deshmukh
L. Poulain
B. Wehner
S. Henning
J.-E. Petit
P. Fombelle
P. Fombelle
O. Favez
H. Herrmann
M. Pöhlker
M. Pöhlker
External particle mixing influences hygroscopicity in a sub-urban area
Atmospheric Chemistry and Physics
title External particle mixing influences hygroscopicity in a sub-urban area
title_full External particle mixing influences hygroscopicity in a sub-urban area
title_fullStr External particle mixing influences hygroscopicity in a sub-urban area
title_full_unstemmed External particle mixing influences hygroscopicity in a sub-urban area
title_short External particle mixing influences hygroscopicity in a sub-urban area
title_sort external particle mixing influences hygroscopicity in a sub urban area
url https://acp.copernicus.org/articles/25/741/2025/acp-25-741-2025.pdf
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