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Assessing the global contribution of marine aerosols, terrestrial bioaerosols, and desert dust to ice-nucleating particle concentrations

CHATZIPARASCHOS, MARIOS; Myriokefalitakis, Stelios; Kalivitis, Nikos; Daskalakis, Nikos; Nenes, Athanasios; Gonçalves Ageitos, María; Costa-Surós, Montserrat; Pérez García-Pando, Carlos; Vrekoussis, Mihalis; Kanakidou, Maria

Abstract

Aerosol–cloud interactions, particularly ice processes in mixed-phase clouds (MPCs), remain a key source of uncertainty in climate change assessments. This study introduces state-of-the-art laboratory-based parameterizations into a global chemistry–transport model to investigate the contributions of mineral dust (specifically K-feldspar and quartz), marine primary organic aerosol (MPOA), and terrestrial primary biological aerosol particles (PBAPs) to ice-nucleating particles (INPs) in MPCs. The model suggests that INPs originating from PBAPs (INPPBAP) are the primary source of INPs at low altitudes between −10 and −20 °C, particularly in the tropics, with a pronounced peak in the Northern Hemisphere (NH) during the boreal summer. INPPBAP contributes over 40 % of the total simulated INP column burden at midlatitudes. Dust-derived INPs (INPD) are prominent at high altitudes across all seasons, dominating at temperatures below −20 °C, and they constitute over 89 % of the INP average column burden at high latitudes in the NH and about 74 % at high latitudes in the Southern Hemisphere (SH). MPOA-derived INPs (INPMPOA) prevail in the SH at low altitudes, particularly at subpolar and polar latitudes for temperatures above −20 °C, where they represent between 17 % and 36 % of the INP column population, depending on the season. When evaluated against available global observational INP data, the model achieves its highest predictability across all temperature ranges when both INPD and INPMPOA are included as independent INP sources. The addition of INPPBAP does not enhance the model's ability to reproduce the available observations; however, INPPBAP remains a key contributor to warm-temperature ice-nucleation events. Therefore, consideration of dust, marine aerosol, and terrestrial bioaerosols as distinct INP species is required to simulate ice nucleation in climate models.

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Supplement of Atmos. Chem. Phys., 25, 9085–9111, 2025 https://doi.org/10.5194/acp-25-9085-2025-supplement © Author(s) 2025. CC BY 4.0 License. Supplement of Assessing the global contribution of marine aerosols, terrestrial bioaerosols, and desert dust to ice-nucleating particle concentrations Marios Chatziparaschos et al. Correspondence to: Maria Kanakidou ([email protected]) The copyright of individual parts of the supplement might differ from the article licence. Chatziparaschos et al. ACP, 2025 1 Supplementary Figures Figure S1: Location of the data used for comparison in Figures 10, S6 and S7. For further information see Table S1 Chatziparaschos et al. ACP, 2025 2 Figure S2: Simulated concentrations of MPOA compared with Mace Head (green) and Amsterdam Island (violet) measurements. Figure S3: Seasonal variation of simulated number concentrations of PBAP compared to long-term (>4 weeks) FBAP observations compiled by Petersson Sjögren et al. (2023). Continuous lines are observations and dashed lines simulated number concentrations. Chatziparaschos et al. ACP, 2025 3 Figure S4: Seasonal percentage contribution of a) mineral dust, (b) fungal spores and bacteria and (c) marine organic aerosols calculated by TM4-ECPL where the total [INP] ambient concentration is larger than 0.01m −3 . The black contour lines represent seasonal mean isotherms in ο C. Chatziparaschos et al. ACP, 2025 4 Figure S5: Seasonal mean concentration of a) mineral dust, (b) fungal spores and bacteria and (c) marine organic aerosols calculated by TM4-ECPL where the total [INP] ambient concentration is larger than 0.01m −3 . The black contour lines represent seasonal mean isotherms in o C. Chatziparaschos et al. ACP, 2025 5 Figure S6: Order of magnitude / Logarithm of the deviation of simulated concentrations of INP types from total INP observations, as a function of binned temperatures in o C. INP Dust in yellow, INP PBAP in green, INP MPOA in blue. Figure S7: Comparison of INP concentrations calculated at the temperature of the measurements against total INP observations accounting for mineral dust (yellow), MPOA (blue), PBAP (green) separated in high, middle and low latitudes. Table S1: Data sets used for this study. Campaign/data Campaign/data set Location References Arctic station Barrow/Utqiagvik Arctic (Wex et al., 2019) Alert (Canadian Arctic Station) Arctic Arctic station Ny - Ålesund Arctic Station_Nord (Villum Research Station) Arctic Chatziparaschos et al. ACP, 2025 6 PS95 Atlantic Cruise 2015 Atlantic (Welti et al., 2020) KAD_Israel Tel Aviv (Ardon - Dryer and Levin, 2014) KAD_South_Pole South Pole (Ardon - Dryer et al., 2011) Conen_ Chaumont Jungfraujoch and Chaumont (Conen et al., 2015) CYPRUS BACCHUS/CHARMEX 2015 Forestry Department site, Agia Marina (Ansmann et al., 2019) BACCHUS_FRIDGE AMAZONAS Amazonian Tall Tower Observatory (Schrod et al., 2020) CalWater Coastal California, Airborne (Fan et al., 2014) Conen_JFJ Jungfraujoch (Conen et al., 2015) CLACE2014 Jungfraujoch (Lacher et al., 2021, 2018, 2017) (Boose et al., 2016) CLACE2013 Jungfraujoch CLACE2012 Jungfraujoch CalNex California (Wang et al., 2012) CALIMA 2014 Izana observatory, Tenerife (Boose et al., 2016) CALIMA 2013 Izana observatory, Tenerife (Boose et al., 2016) ISAC-CNR MaceHead BACCHUS Campaign Mace Head Observatory, Carna, Galway, Ireland (Rinaldi et al., 2016) ISAC-CNR SanPietro_Capofiume BACCHUS Campaign San Pietro Capofiume (BO, Italy) (Belosi et al., 2017) ISAC_CNR_MtCimone BACCHUS Campaign mountain observatory Mt. Cimone (Rinaldi et al., 2017) ISA C - CNR Antarctica BACCHUS Campaign Mario Zucchelli Station, Terranova Bay, Antarctica (Belosi et al., 2014) BACCHUS_FRIDGE_SVALBARD Campaign Zeppelin Observatory, Svalbard/Spitzbergen (Schrod et al., 2020) BACCHUS_FRIDGE_MARTINI QUE Volcanic and Seismologic Observatory, FondsSaint-Denis, Martinique, Caribbean (Schrod et al., 2020) CSU_CFDC_archive_BEACHON Manitou Experimental ForestObservatory (MEFO) (Tobo et al., 2013) Chatziparaschos et al. ACP, 2025 7 ETH_JFJ_2014 Jungfraujoch High Altitude Research Station (Lacher et al., 2017) ETH_JFJ_2016 Jungfraujoch High Altitude Research Station (Lacher et al., 2017, 2018) ETH_JFJ_2015 Jungfraujoch High Altitude Research Station (Lacher et al., 2017) TROPOS_Cyprus2016 Agia Marina, Xyliatou, Cyprus (Ansmann et al., 2019; Schrod et al., 2017) TROPOS_CV_IN Cape Verde (Welti et al., 2018) Yin_China China (Yin et al., 2012) NETCARE_2013 Coastal (West coast of Canada) (Mason et al. , 2015) Bigg_1969-1989 Australia, Southern Ocean, Argentina, Africa, India, Japan/Korea, Antarctica, Hawaii, Tasmania, https://www.bacchusenv.eu/in/ (Bigg, 1973, 1990) NETCARE Canadian Arctic (Irish et al., 2019) ACAPEX Bodega Bay (California) (DeMott and Hill, 2016) CAPRICORN South of Australia (McCluskey et al., 2018) ACE - SPACE Atlantic (Welti et al., 2020) Eq1. Modified normalised mean bias (MNMB) References: Ansmann, A., Mamouri, R. 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