Articles | Volume 18, issue 23
https://doi.org/10.5194/acp-18-17119-2018
© Author(s) 2018. This work is distributed under
the Creative Commons Attribution 4.0 License.
the Creative Commons Attribution 4.0 License.
https://doi.org/10.5194/acp-18-17119-2018
© Author(s) 2018. This work is distributed under
the Creative Commons Attribution 4.0 License.
the Creative Commons Attribution 4.0 License.
Research article
| 
04 Dec 2018
Research article |
| 04 Dec 2018
| 04 Dec 2018
On the thermodynamic and kinetic aspects of immersion ice nucleation
Donifan Barahona
CORRESPONDING AUTHOR
NASA Goddard Space Flight Center,
Greenbelt, MD, USA
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The Green's functions methodology offers a systematic, easy-to-implement, computationally cheap, scalable, and extendable method to tune uncertain parameters in models accounting for the dependent response of the model to a change in various parameters. Herein, we successfully show for the first time that long-term errors in earth system models can be considerably reduced using Green's functions methodology. The method can be easily applied to any model containing uncertain parameters.
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The study using the NASA Earth system model shows ~2.6 % increase in burning season gross primary production and ~1.5 % increase in annual net primary production across the Amazon Basin during 2010–2016 due to the change in surface downward direct and diffuse photosynthetically active radiation by biomass burning aerosols. Such an aerosol effect is strongly dependent on the presence of clouds. The cloud fraction at which aerosols switch from stimulating to inhibiting plant growth occurs at ~0.8.
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Increases in atmospheric aerosols affect the scattering and absorption of solar radiation by altering the macrophysical and microphysical processes of clouds. We analyzed aerosol–cloud interactions in response to degassing events from the Kilauea volcano in 2008 and 2018 by comparing satellite and simulated cloud properties. Results showed a threshold response to overcome meteorological effects that is largely controlled by aerosol concentration, composition, plume height, and ENSO state.
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Sara Bacer, Sylvia C. Sullivan, Vlassis A. Karydis, Donifan Barahona, Martina Krämer, Athanasios Nenes, Holger Tost, Alexandra P. Tsimpidi, Jos Lelieveld, and Andrea Pozzer
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We use the adjoint model of a cirrus parameterization to quantify sources of crystal variability for various ice-nucleating spectra and output from CAM5.
The sensitivities can be directly linked to nucleation regime and
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The lab-based spectrum calculates much higher INP efficiencies than field-based ones, owing to aerosol surface properties.
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Y. C. Sud, D. Lee, L. Oreopoulos, D. Barahona, A. Nenes, and M. J. Suarez
Geosci. Model Dev., 6, 57–79, https://doi.org/10.5194/gmd-6-57-2013, https://doi.org/10.5194/gmd-6-57-2013, 2013
Ehud Strobach, Andrea Molod, Donifan Barahona, Atanas Trayanov, Dimitris Menemenlis, and Gael Forget
Geosci. Model Dev., 15, 2309–2324, https://doi.org/10.5194/gmd-15-2309-2022, https://doi.org/10.5194/gmd-15-2309-2022, 2022
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The Green's functions methodology offers a systematic, easy-to-implement, computationally cheap, scalable, and extendable method to tune uncertain parameters in models accounting for the dependent response of the model to a change in various parameters. Herein, we successfully show for the first time that long-term errors in earth system models can be considerably reduced using Green's functions methodology. The method can be easily applied to any model containing uncertain parameters.
Huisheng Bian, Eunjee Lee, Randal D. Koster, Donifan Barahona, Mian Chin, Peter R. Colarco, Anton Darmenov, Sarith Mahanama, Michael Manyin, Peter Norris, John Shilling, Hongbin Yu, and Fanwei Zeng
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The study using the NASA Earth system model shows ~2.6 % increase in burning season gross primary production and ~1.5 % increase in annual net primary production across the Amazon Basin during 2010–2016 due to the change in surface downward direct and diffuse photosynthetically active radiation by biomass burning aerosols. Such an aerosol effect is strongly dependent on the presence of clouds. The cloud fraction at which aerosols switch from stimulating to inhibiting plant growth occurs at ~0.8.
Katherine H. Breen, Donifan Barahona, Tianle Yuan, Huisheng Bian, and Scott C. James
Atmos. Chem. Phys., 21, 7749–7771, https://doi.org/10.5194/acp-21-7749-2021, https://doi.org/10.5194/acp-21-7749-2021, 2021
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Increases in atmospheric aerosols affect the scattering and absorption of solar radiation by altering the macrophysical and microphysical processes of clouds. We analyzed aerosol–cloud interactions in response to degassing events from the Kilauea volcano in 2008 and 2018 by comparing satellite and simulated cloud properties. Results showed a threshold response to overcome meteorological effects that is largely controlled by aerosol concentration, composition, plume height, and ENSO state.
Jie Gong, Xiping Zeng, Dong L. Wu, S. Joseph Munchak, Xiaowen Li, Stefan Kneifel, Davide Ori, Liang Liao, and Donifan Barahona
Atmos. Chem. Phys., 20, 12633–12653, https://doi.org/10.5194/acp-20-12633-2020, https://doi.org/10.5194/acp-20-12633-2020, 2020
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This work provides a novel way of using polarized passive microwave measurements to study the interlinked cloud–convection–precipitation processes. The magnitude of differences between polarized radiances is found linked to ice microphysics (shape, size, orientation and density), mesoscale dynamic and thermodynamic structures, and surface precipitation. We conclude that passive sensors with multiple polarized channel pairs may serve as cheaper and useful substitutes for spaceborne radar sensors.
Sara Bacer, Sylvia C. Sullivan, Vlassis A. Karydis, Donifan Barahona, Martina Krämer, Athanasios Nenes, Holger Tost, Alexandra P. Tsimpidi, Jos Lelieveld, and Andrea Pozzer
Geosci. Model Dev., 11, 4021–4041, https://doi.org/10.5194/gmd-11-4021-2018, https://doi.org/10.5194/gmd-11-4021-2018, 2018
Short summary
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The complexity of ice nucleation mechanisms and aerosol--ice interactions makes their representation still challenging in atmospheric models. We have implemented a comprehensive ice crystal formation parameterization in the global chemistry-climate model EMAC to improve the representation of ice crystal number concentrations. The newly implemented parameterization takes into account processes which were previously neglected by the standard version of the model.
Sylvia C. Sullivan, Ricardo Morales Betancourt, Donifan Barahona, and Athanasios Nenes
Atmos. Chem. Phys., 16, 2611–2629, https://doi.org/10.5194/acp-16-2611-2016, https://doi.org/10.5194/acp-16-2611-2016, 2016
Short summary
Short summary
We use the adjoint model of a cirrus parameterization to quantify sources of crystal variability for various ice-nucleating spectra and output from CAM5.
The sensitivities can be directly linked to nucleation regime and
efficiency of various INP.
The lab-based spectrum calculates much higher INP efficiencies than field-based ones, owing to aerosol surface properties.
The sensitivity to temperature tends to be low, due to the compensating effects of temperature on INP spectrum parameters.
D. Barahona
Atmos. Chem. Phys., 15, 13819–13831, https://doi.org/10.5194/acp-15-13819-2015, https://doi.org/10.5194/acp-15-13819-2015, 2015
Short summary
Short summary
This paper describes the process of the transfer of water molecules between liquid and the ice during the early stages of ice formation. Using concepts of nonreversible thermodynamics, it is shown that the activation energy can be defined in terms of the bulk self-diffusivity of water and the probability of interface transfer. The application of this model to classical nucleation theory shows good agreement of measured nucleation rates with experimental results for temperatures as low as 190K.
D. Barahona, A. Molod, J. Bacmeister, A. Nenes, A. Gettelman, H. Morrison, V. Phillips, and A. Eichmann
Geosci. Model Dev., 7, 1733–1766, https://doi.org/10.5194/gmd-7-1733-2014, https://doi.org/10.5194/gmd-7-1733-2014, 2014
D. Barahona
Atmos. Chem. Phys., 14, 7665–7680, https://doi.org/10.5194/acp-14-7665-2014, https://doi.org/10.5194/acp-14-7665-2014, 2014
Y. C. Sud, D. Lee, L. Oreopoulos, D. Barahona, A. Nenes, and M. J. Suarez
Geosci. Model Dev., 6, 57–79, https://doi.org/10.5194/gmd-6-57-2013, https://doi.org/10.5194/gmd-6-57-2013, 2013
Related subject area
Subject: Aerosols | Research Activity: Atmospheric Modelling and Data Analysis | Altitude Range: Troposphere | Science Focus: Physics (physical properties and processes)
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Evaluating organosulfur (OS) hygroscopicity is important for assessing aerosol–cloud climate interactions in the post-fossil-fuel future, when SO2 emissions decrease and OS compounds become increasingly important. Here a state-of-the-art quantum-chemistry-based method was used to predict the hygroscopic growth factors (HGFs) of a group of atmospherically relevant OS compounds and their mixtures with (NH4)2SO4. A good agreement was observed between their model-estimated and experimental HGFs.
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Hengheng Zhang, Wei Huang, Xiaoli Shen, Ramakrishna Ramisetty, Junwei Song, Olga Kiseleva, Christopher Claus Holst, Basit Khan, Thomas Leisner, and Harald Saathoff
Atmos. Chem. Phys., 24, 10617–10637, https://doi.org/10.5194/acp-24-10617-2024, https://doi.org/10.5194/acp-24-10617-2024, 2024
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Giorgio Veratti, Alessandro Bigi, Michele Stortini, Sergio Teggi, and Grazia Ghermandi
Atmos. Chem. Phys., 24, 10475–10512, https://doi.org/10.5194/acp-24-10475-2024, https://doi.org/10.5194/acp-24-10475-2024, 2024
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In a study of two consecutive winter seasons, we used measurements and modelling tools to identify the levels and sources of black carbon pollution in a medium-sized urban area of the Po Valley, Italy. Our findings show that biomass burning and traffic-related emissions (especially from Euro 4 diesel cars) significantly contribute to BC concentrations. This research offers crucial insights for policymakers and urban planners aiming to improve air quality in cities.
Pascal Lemaitre, Arnaud Quérel, Alexis Dépée, Alice Guerra Devigne, Marie Monier, Thibault Hiron, Chloé Soto Minguez, Daniel Hardy, and Andrea Flossmann
Atmos. Chem. Phys., 24, 9713–9732, https://doi.org/10.5194/acp-24-9713-2024, https://doi.org/10.5194/acp-24-9713-2024, 2024
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A new in-cloud scavenging scheme is proposed. It is based on a microphysical model of cloud formation and may be applied to long-distance atmospheric transport models (> 100 km) and climatic models. This model is applied to the two most extreme precipitating cloud types in terms of both relative humidity and vertical extension: cumulonimbus and stratus.
Alex Rowell, James Brean, David C. S. Beddows, Tuukka Petäjä, Máté Vörösmarty, Imre Salma, Jarkko V. Niemi, Hanna E. Manninen, Dominik van Pinxteren, Thomas Tuch, Kay Weinhold, Zongbo Shi, and Roy M. Harrison
Atmos. Chem. Phys., 24, 9515–9531, https://doi.org/10.5194/acp-24-9515-2024, https://doi.org/10.5194/acp-24-9515-2024, 2024
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Different sources of airborne particles in the atmospheres of four European cities were distinguished by recognising their particle size distributions using a statistical procedure, positive matrix factorisation. The various sources responded differently to the changes in emissions associated with COVID-19 lockdowns, and the reasons are investigated. While traffic emissions generally decreased, particles formed from reactions of atmospheric gases decreased in some cities but increased in others.
Amy H. Peace, Ying Chen, George Jordan, Daniel G. Partridge, Florent Malavelle, Eliza Duncan, and Jim M. Haywood
Atmos. Chem. Phys., 24, 9533–9553, https://doi.org/10.5194/acp-24-9533-2024, https://doi.org/10.5194/acp-24-9533-2024, 2024
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Natural aerosols from volcanic eruptions can help us understand how anthropogenic aerosols modify climate. We use observations and model simulations of the 2014–2015 Holuhraun eruption plume to examine aerosol–cloud interactions in September 2014. We find a shift to clouds with smaller, more numerous cloud droplets in the first 2 weeks of the eruption. In the third week, the background meteorology and previous conditions experienced by air masses modulate the aerosol perturbation to clouds.
Hua Lu, Min Xie, Bingliang Zhuang, Danyang Ma, Bojun Liu, Yangzhihao Zhan, Tijian Wang, Shu Li, Mengmeng Li, and Kuanguang Zhu
Atmos. Chem. Phys., 24, 8963–8982, https://doi.org/10.5194/acp-24-8963-2024, https://doi.org/10.5194/acp-24-8963-2024, 2024
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To identify cloud, aerosol, and planetary boundary layer (PBL) interactions from an air quality perspective, we summarized two pollution patterns characterized by denser liquid cloud and by obvious cloud radiation interaction (CRI). Numerical simulation experiments showed CRI could cause a 50 % reduction in aerosol radiation interaction (ARI) under a low-trough system. The results emphasized the nonnegligible role of CRI and its inhibition of ARI under wet and cloudy pollution synoptic patterns.
Emilie Fons, Ann Kristin Naumann, David Neubauer, Theresa Lang, and Ulrike Lohmann
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Aerosols can modify the liquid water path (LWP) of stratocumulus and, thus, their radiative effect. We compare storm-resolving model and satellite data that disagree on the sign of LWP adjustments and diagnose this discrepancy with causal inference. We find that strong precipitation, the absence of wet scavenging, and cloud deepening under a weak inversion contribute to positive LWP adjustments to aerosols in the model, despite weak negative effects from cloud-top entrainment enhancement.
Muhammed Irfan, Thomas Kühn, Taina Yli-Juuti, Anton Laakso, Eemeli Holopainen, Douglas R. Worsnop, Annele Virtanen, and Harri Kokkola
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The study examines how the volatility of semi-volatile organic compounds affects secondary organic aerosol (SOA) formation and climate. Our simulations show that uncertainties in these volatilities influence aerosol mass and climate impacts. Accurate representation of these compounds in climate models is crucial for predicting global climate patterns.
Alkiviadis Kalisoras, Aristeidis K. Georgoulias, Dimitris Akritidis, Robert J. Allen, Vaishali Naik, Chaincy Kuo, Sophie Szopa, Pierre Nabat, Dirk Olivié, Twan van Noije, Philippe Le Sager, David Neubauer, Naga Oshima, Jane Mulcahy, Larry W. Horowitz, and Prodromos Zanis
Atmos. Chem. Phys., 24, 7837–7872, https://doi.org/10.5194/acp-24-7837-2024, https://doi.org/10.5194/acp-24-7837-2024, 2024
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Effective radiative forcing (ERF) is a metric for estimating how human activities and natural agents change the energy flow into and out of the Earth’s climate system. We investigate the anthropogenic aerosol ERF, and we estimate the contribution of individual processes to the total ERF using simulations from Earth system models within the Coupled Model Intercomparison Project Phase 6 (CMIP6). Our findings highlight that aerosol–cloud interactions drive ERF variability during the last 150 years.
Ryan Schmedding and Andreas Zuend
EGUsphere, https://doi.org/10.5194/egusphere-2024-1690, https://doi.org/10.5194/egusphere-2024-1690, 2024
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Four different approaches for computing the interfacial tension between liquid phases in aerosol particles were tested for particles with diameters from 10 nm to more than 5 μm. Antonov's rule led to the strongest reductions in the onset relative humidity of liquid–liquid phase separation and reproduced measured interfacial tensions for highly immiscible systems. A modified form of the Butler equation was able to best reproduce measured interfacial tensions in more miscible systems.
Qianqian Song, Paul Ginoux, María Gonçalves Ageitos, Ron L. Miller, Vincenzo Obiso, and Carlos Pérez García-Pando
Atmos. Chem. Phys., 24, 7421–7446, https://doi.org/10.5194/acp-24-7421-2024, https://doi.org/10.5194/acp-24-7421-2024, 2024
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We implement and simulate the distribution of eight dust minerals in the GFDL AM4.0 model. We found that resolving the eight minerals reduces dust absorption compared to the homogeneous dust used in the standard GFDL AM4.0 model that assumes a globally uniform hematite content of 2.7 % by volume. Resolving dust mineralogy results in significant impacts on radiation, land surface temperature, surface winds, and precipitation over North Africa in summer.
Mingxu Liu, Hitoshi Matsui, Douglas Hamilton, Sagar Rathod, Kara Lamb, and Natalie Mahowald
EGUsphere, https://doi.org/10.5194/egusphere-2024-1454, https://doi.org/10.5194/egusphere-2024-1454, 2024
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Atmospheric aerosol deposition provides iron to promote marine primary production, yet its amount remains highly uncertain. This study demonstrates that iron-containing particle size at emission is a critical factor in regulating their input to open oceans by performing global aerosol simulations. Further observational constraints on this are needed to reduce modelling uncertainties.
Ross J. Herbert, Alberto Sanchez-Marroquin, Daniel P. Grosvenor, Kirsty J. Pringle, Stephen R. Arnold, Benjamin J. Murray, and Kenneth S. Carslaw
EGUsphere, https://doi.org/10.5194/egusphere-2024-1538, https://doi.org/10.5194/egusphere-2024-1538, 2024
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Aerosol particles that help form ice in clouds vary in number and type around the world and with time. However, in many weather and climate models cloud ice is not linked to aerosol that are known to nucleate ice. Here we report the first steps towards representing ice-nucleating particles within the UK's Earth System Model. We conclude that in addition to ice nucleation by sea spray and mineral components of soil dust we also need to represent ice nucleation by the organic components of soils.
Senyi Kong, Zheng Wang, and Lei Bi
Atmos. Chem. Phys., 24, 6911–6935, https://doi.org/10.5194/acp-24-6911-2024, https://doi.org/10.5194/acp-24-6911-2024, 2024
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The retrieval of refractive indices of dust aerosols from laboratory optical measurements is commonly done assuming spherical particles. This paper aims to investigate the uncertainties in the shortwave refractive indices and corresponding optical properties by considering non-spherical and inhomogeneous models for dust samples. The study emphasizes the significance of using non-spherical models for simulating dust aerosols.
Wenxuan Hua, Sijia Lou, Xin Huang, Lian Xue, Ke Ding, Zilin Wang, and Aijun Ding
Atmos. Chem. Phys., 24, 6787–6807, https://doi.org/10.5194/acp-24-6787-2024, https://doi.org/10.5194/acp-24-6787-2024, 2024
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In this study, we diagnose uncertainties in carbon monoxide and organic carbon emissions from four inventories for seven major wildfire-prone regions. Uncertainties in vegetation classification methods, fire detection products, and cloud obscuration effects lead to bias in these biomass burning (BB) emission inventories. By comparing simulations with measurements, we provide certain inventory recommendations. Our study has implications for reducing uncertainties in emissions in further studies.
Léo Clauzel, Sandrine Anquetin, Christophe Lavaysse, Gilles Bergametti, Christel Bouet, Guillaume Siour, Rémy Lapere, Béatrice Marticorena, and Jennie Thomas
EGUsphere, https://doi.org/10.5194/egusphere-2024-1604, https://doi.org/10.5194/egusphere-2024-1604, 2024
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Solar energy production in West Africa is set to rise, needing accurate solar radiation estimates, which is affected by desert dust. This work analyses a March 2021 dust event using a modelling strategy incorporating desert dust. Results show that considering desert dust cut errors in solar radiation estimates by 75 % and reduces surface solar radiation by 18 %. This highlights the importance of incorporating dust aerosols into solar forecasting for better accuracy.
Chandrakala Bharali, Mary Barth, Rajesh Kumar, Sachin D. Ghude, Vinayak Sinha, and Baerbel Sinha
Atmos. Chem. Phys., 24, 6635–6662, https://doi.org/10.5194/acp-24-6635-2024, https://doi.org/10.5194/acp-24-6635-2024, 2024
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This study examines the role of atmospheric aerosols in winter fog over the Indo-Gangetic Plains of India using WRF-Chem. The increase in RH with aerosol–radiation feedback (ARF) is found to be important for fog formation as it promotes the growth of aerosols in the polluted environment. Aqueous-phase chemistry in the fog increases PM2.5 concentration, further affecting ARF. ARF and aqueous-phase chemistry affect the fog intensity and the timing of fog formation by ~1–2 h.
Wenxin Zhao, Yu Zhao, Yu Zheng, Dong Chen, Jinyuan Xin, Kaitao Li, Huizheng Che, Zhengqiang Li, Mingrui Ma, and Yun Hang
Atmos. Chem. Phys., 24, 6593–6612, https://doi.org/10.5194/acp-24-6593-2024, https://doi.org/10.5194/acp-24-6593-2024, 2024
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We evaluate the long-term (2000–2020) variabilities of aerosol absorption optical depth, black carbon emissions, and associated health risks in China with an integrated framework that combines multiple observations and modeling techniques. We demonstrate the remarkable emission abatement resulting from the implementation of national pollution controls and show how human activities affected the emissions with a spatiotemporal heterogeneity, thus supporting differentiated policy-making by region.
Peng Xian, Jeffrey S. Reid, Melanie Ades, Angela Benedetti, Peter R. Colarco, Arlindo da Silva, Tom F. Eck, Johannes Flemming, Edward J. Hyer, Zak Kipling, Samuel Rémy, Tsuyoshi Thomas Sekiyama, Taichu Tanaka, Keiya Yumimoto, and Jianglong Zhang
Atmos. Chem. Phys., 24, 6385–6411, https://doi.org/10.5194/acp-24-6385-2024, https://doi.org/10.5194/acp-24-6385-2024, 2024
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The study compares and evaluates monthly AOD of four reanalyses (RA) and their consensus (i.e., ensemble mean). The basic verification characteristics of these RA versus both AERONET and MODIS retrievals are presented. The study discusses the strength of each RA and identifies regions where divergence and challenges are prominent. The RA consensus usually performs very well on a global scale in terms of how well it matches the observational data, making it a good choice for various applications.
Roger Teoh, Zebediah Engberg, Ulrich Schumann, Christiane Voigt, Marc Shapiro, Susanne Rohs, and Marc E. J. Stettler
Atmos. Chem. Phys., 24, 6071–6093, https://doi.org/10.5194/acp-24-6071-2024, https://doi.org/10.5194/acp-24-6071-2024, 2024
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The radiative forcing (RF) due to aviation contrails is comparable to that caused by CO2. We estimate that global contrail net RF in 2019 was 62.1 mW m−2. This is ~1/2 the previous best estimate for 2018. Contrail RF varies regionally due to differences in conditions required for persistent contrails. COVID-19 reduced contrail RF by 54% in 2020 relative to 2019. Globally, 2 % of all flights account for 80 % of the annual contrail energy forcing, suggesting a opportunity to mitigate contrail RF.
Ragnhild Bieltvedt Skeie, Rachael Byrom, Øivind Hodnebrog, Caroline Jouan, and Gunnar Myhre
EGUsphere, https://doi.org/10.5194/egusphere-2024-1394, https://doi.org/10.5194/egusphere-2024-1394, 2024
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In 2020 new regulations by the International Maritime Organization of sulphur emissions came into force that reduced emissions of SO2 from the shipping sector by approximately 80 %. In this study, we use multiple models to calculate by how much the Earth energy balance changed due to the emission reduction, the so called effective radiative forcing. The calculated effective radiative forcing is weak, comparable to the effect of the increase in CO2 over the last two to three years.
Haotian Zu, Biwu Chu, Yiqun Lu, Ling Liu, and Xiuhui Zhang
Atmos. Chem. Phys., 24, 5823–5835, https://doi.org/10.5194/acp-24-5823-2024, https://doi.org/10.5194/acp-24-5823-2024, 2024
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The nucleation of iodic acid (HIO3) and iodous acid (HIO2) was proven to be critical in marine areas. However, HIO3–HIO2 nucleation cannot effectively derive the rapid nucleation in some polluted coasts. We find a significant enhancement of dimethylamine (DMA) on the HIO3–HIO2 nucleation in marine and polar regions with abundant DMA sources, which may establish reasonable connections between the HIO3–HIO2 nucleation and the rapid formation of new particles in polluted marine and polar regions.
Junghwa Lee, Patric Seifert, Tempei Hashino, Maximilian Maahn, Fabian Senf, and Oswald Knoth
Atmos. Chem. Phys., 24, 5737–5756, https://doi.org/10.5194/acp-24-5737-2024, https://doi.org/10.5194/acp-24-5737-2024, 2024
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Spectral bin model simulations of an idealized supercooled stratiform cloud were performed with the AMPS model for variable CCN and INP concentrations. We performed radar forward simulations with PAMTRA to transfer the simulations into radar observational space. The derived radar reflectivity factors were compared to observational studies of stratiform mixed-phase clouds. These studies report a similar response of the radar reflectivity factor to aerosol perturbations as we found in our study.
Masaru Yoshioka, Daniel P. Grosvenor, Ben B. B. Booth, Colin P. Morice, and Kenneth S. Carslaw
EGUsphere, https://doi.org/10.5194/egusphere-2024-1428, https://doi.org/10.5194/egusphere-2024-1428, 2024
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Sulfur emissions from shipping has been reduced by about 80 % as a result of the new regulation introduced in 2020. This has reduced aerosol in the atmosphere and its cooling effect through interactions with clouds. As a result, our coupled climate model simulations predict a global warming of 0.04 K averaged over three decades, potentially surpassing the Paris target of 1.5 K or contributing to recent temperature spikes, particularly notable in the Arctic with a mean warming of 0.15 K.
Basudev Swain, Marco Vountas, Aishwarya Singh, Nidhi L. Anchan, Adrien Deroubaix, Luca Lelli, Yanick Ziegler, Sachin S. Gunthe, Hartmut Bösch, and John P. Burrows
Atmos. Chem. Phys., 24, 5671–5693, https://doi.org/10.5194/acp-24-5671-2024, https://doi.org/10.5194/acp-24-5671-2024, 2024
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Arctic amplification (AA) accelerates the warming of the central Arctic cryosphere and affects aerosol dynamics. Limited observations hinder a comprehensive analysis. This study uses AEROSNOW aerosol optical density (AOD) data and GEOS-Chem simulations to assess AOD variability. Discrepancies highlight the need for improved observational integration into models to refine our understanding of aerosol effects on cloud microphysics, ice nucleation, and radiative forcing under evolving AA.
Vincenzo Obiso, María Gonçalves Ageitos, Carlos Pérez García-Pando, Jan P. Perlwitz, Gregory L. Schuster, Susanne E. Bauer, Claudia Di Biagio, Paola Formenti, Kostas Tsigaridis, and Ron L. Miller
Atmos. Chem. Phys., 24, 5337–5367, https://doi.org/10.5194/acp-24-5337-2024, https://doi.org/10.5194/acp-24-5337-2024, 2024
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We calculate the dust direct radiative effect (DRE) in an Earth system model accounting for regionally varying soil mineralogy through a new observationally constrained method. Linking dust absorption at solar wavelengths to the varying amount of specific minerals (i.e., iron oxides) improves the modeled range of dust single scattering albedo compared to observations and increases the global cooling by dust. Our results may contribute to improved estimates of the dust DRE and its climate impact.
Charlotte M. Beall, Po-Lun Ma, Matthew W. Christensen, Johannes Mülmenstädt, Adam Varble, Kentaroh Suzuki, and Takuro Michibata
Atmos. Chem. Phys., 24, 5287–5302, https://doi.org/10.5194/acp-24-5287-2024, https://doi.org/10.5194/acp-24-5287-2024, 2024
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Single-layer warm liquid clouds cover nearly one-third of the Earth's surface, and uncertainties regarding the impact of aerosols on their radiative properties pose a significant challenge to climate prediction. Here, we demonstrate how satellite observations can be used to constrain Earth system model estimates of the radiative forcing from the interactions of aerosols with clouds due to warm rain processes.
Xiaoli Wei, Qian Cui, Leiming Ma, Feng Zhang, Wenwen Li, and Peng Liu
Atmos. Chem. Phys., 24, 5025–5045, https://doi.org/10.5194/acp-24-5025-2024, https://doi.org/10.5194/acp-24-5025-2024, 2024
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A new aerosol-type classification algorithm has been proposed. It includes an optical database built by Mie scattering and a complex refractive index working as a baseline to identify different aerosol types. The new algorithm shows high accuracy and efficiency. Hence, a global map of aerosol types was generated to characterize aerosol types across the five continents. It will help improve the accuracy of aerosol inversion and determine the sources of aerosol pollution.
Zhiqiang Zhang, Ying Li, Haiyan Ran, Junling An, Yu Qu, Wei Zhou, Weiqi Xu, Weiwei Hu, Hongbin Xie, Zifa Wang, Yele Sun, and Manabu Shiraiwa
Atmos. Chem. Phys., 24, 4809–4826, https://doi.org/10.5194/acp-24-4809-2024, https://doi.org/10.5194/acp-24-4809-2024, 2024
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Secondary organic aerosols (SOAs) can exist in liquid, semi-solid, or amorphous solid states, which are rarely accounted for in current chemical transport models. We predict the phase state of SOA particles over China and find that in northwestern China SOA particles are mostly highly viscous or glassy solid. Our results indicate that the particle phase state should be considered in SOA formation in chemical transport models for more accurate prediction of SOA mass concentrations.
Alejandro Baró Pérez, Michael S. Diamond, Frida A.-M. Bender, Abhay Devasthale, Matthias Schwarz, Julien Savre, Juha Tonttila, Harri Kokkola, Hyunho Lee, David Painemal, and Annica M. L. Ekman
Atmos. Chem. Phys., 24, 4591–4610, https://doi.org/10.5194/acp-24-4591-2024, https://doi.org/10.5194/acp-24-4591-2024, 2024
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We use a numerical model to study interactions between humid light-absorbing aerosol plumes, clouds, and radiation over the southeast Atlantic. We find that the warming produced by the aerosols reduces cloud cover, especially in highly polluted situations. Aerosol impacts on drizzle play a minor role. However, aerosol effects on cloud reflectivity and moisture-induced changes in cloud cover dominate the climatic response and lead to an overall cooling by the biomass burning plumes.
Danny M. Leung, Jasper F. Kok, Longlei Li, David M. Lawrence, Natalie M. Mahowald, Simone Tilmes, and Erik Kluzek
EGUsphere, https://doi.org/10.5194/egusphere-2024-1124, https://doi.org/10.5194/egusphere-2024-1124, 2024
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This study derives a desert dust emission dataset for 1841–2000, by employing a combination of observed dust records from sedimentary cores as well as reanalyzed global dust cycle constraints. We evaluate the ability of global models to replicate the observed historical dust variability by using the emission dataset to force a historical simulation in an Earth system model. We show that prescribing our emissions forces the model to match better against observations than other mechanistic models.
Sampa Das, Peter R. Colarco, Huisheng Bian, and Santiago Gassó
Atmos. Chem. Phys., 24, 4421–4449, https://doi.org/10.5194/acp-24-4421-2024, https://doi.org/10.5194/acp-24-4421-2024, 2024
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The smoke aerosols emitted from vegetation burning can alter the regional energy budget via multiple pathways. We utilized detailed observations from the NASA ORACLES airborne campaign based in Namibia during September 2016 to improve the representation of smoke aerosol properties and lifetimes in our GEOS Earth system model. The improved model simulations are for the first time able to capture the observed changes in the smoke absorption during long-range plume transport.
Emilio Cuevas-Agulló, David Barriopedro, Rosa Delia García, Silvia Alonso-Pérez, Juan Jesús González-Alemán, Ernest Werner, David Suárez, Juan José Bustos, Gerardo García-Castrillo, Omaira García, África Barreto, and Sara Basart
Atmos. Chem. Phys., 24, 4083–4104, https://doi.org/10.5194/acp-24-4083-2024, https://doi.org/10.5194/acp-24-4083-2024, 2024
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During February–March (FM) 2020–2022, unusually intense dust storms from northern Africa hit the western Euro-Mediterranean (WEM). Using dust products from satellites and atmospheric reanalysis for 2003–2022, results show that cut-off lows and European blocking are key drivers of FM dust intrusions over the WEM. A higher frequency of cut-off lows associated with subtropical ridges is observed in the late 2020–2022 period.
Yahui Che, Bofu Yu, and Katherine Bracco
Atmos. Chem. Phys., 24, 4105–4128, https://doi.org/10.5194/acp-24-4105-2024, https://doi.org/10.5194/acp-24-4105-2024, 2024
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Dust events occur more frequently during the Austral spring and summer in dust regions, including central Australia, the southwest of Western Australia, and the northern and southern regions of eastern Australia using remote sensing and reanalysis datasets. High-concentration dust is distributed around central Australia and in the downwind northern and southern Australia. Typically, around 50 % of the dust lifted settles on Australian land, with the remaining half being deposited in the ocean.
Jonathan Elsey, Nicolas Bellouin, and Claire Ryder
Atmos. Chem. Phys., 24, 4065–4081, https://doi.org/10.5194/acp-24-4065-2024, https://doi.org/10.5194/acp-24-4065-2024, 2024
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Aerosols influence the Earth's energy balance. The uncertainty in this radiative forcing is large depending partly on uncertainty in measurements of aerosol optical properties. We have developed a freely available new framework of millions of radiative transfer simulations spanning aerosol uncertainty and assess the impact on radiative forcing uncertainty. We find that reducing these uncertainties would reduce radiative forcing uncertainty, but non-aerosol uncertainties must also be considered.
Jing Li, Nan Wu, Biwu Chu, An Ning, and Xiuhui Zhang
Atmos. Chem. Phys., 24, 3989–4000, https://doi.org/10.5194/acp-24-3989-2024, https://doi.org/10.5194/acp-24-3989-2024, 2024
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Iodic acid (HIO3) nucleates with iodous acid (HIO2) efficiently in marine areas; however, whether methanesulfonic acid (MSA) can synergistically participate in the HIO3–HIO2-based nucleation is unclear. We provide molecular-level evidence that MSA can efficiently promote the formation of HIO3–HIO2-based clusters using a theoretical approach. The proposed MSA-enhanced iodine nucleation mechanism may help us to deeply understand marine new particle formation events with bursts of iodine particles.
Hao Wang, Xiaohong Liu, Chenglai Wu, and Guangxing Lin
Atmos. Chem. Phys., 24, 3309–3328, https://doi.org/10.5194/acp-24-3309-2024, https://doi.org/10.5194/acp-24-3309-2024, 2024
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We quantified different global- and regional-scale drivers of biogenic volatile organic compound (BVOC) emission trends over the past 20 years. The results show that global greening trends significantly boost BVOC emissions and deforestation reduces BVOC emissions in South America and Southeast Asia. Elevated temperature in Europe and increased soil moisture in East and South Asia enhance BVOC emissions. The results deepen our understanding of long-term BVOC emission trends in hotspots.
Christof G. Beer, Johannes Hendricks, and Mattia Righi
Atmos. Chem. Phys., 24, 3217–3240, https://doi.org/10.5194/acp-24-3217-2024, https://doi.org/10.5194/acp-24-3217-2024, 2024
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Ice-nucleating particles (INPs) have important influences on cirrus clouds and the climate system; however, the understanding of their global impacts is still uncertain. We perform numerical simulations with a global aerosol–climate model to analyse INP-induced cirrus changes and the resulting climate impacts. We evaluate various sources of uncertainties, e.g. the ice-nucleating ability of INPs and the role of model dynamics, and provide a new estimate for the global INP–cirrus effect.
Jiawei Li, Zhiwei Han, Pingqing Fu, Xiaohong Yao, and Mingjie Liang
Atmos. Chem. Phys., 24, 3129–3161, https://doi.org/10.5194/acp-24-3129-2024, https://doi.org/10.5194/acp-24-3129-2024, 2024
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Organic aerosols of marine origin are important for aerosol climatic effects but are poorly understood. For the first time, an online coupled regional chemistry–climate model is applied to explore the characteristics of emission, distribution, and direct and indirect radiative effects of marine organic aerosols over the western Pacific, which reveals an important role of marine organic aerosols in perturbing cloud and radiation and promotes understanding of global aerosol climatic impact.
Yawen Liu, Yun Qian, Philip J. Rasch, Kai Zhang, Lai-yung Ruby Leung, Yuhang Wang, Minghuai Wang, Hailong Wang, Xin Huang, and Xiu-Qun Yang
Atmos. Chem. Phys., 24, 3115–3128, https://doi.org/10.5194/acp-24-3115-2024, https://doi.org/10.5194/acp-24-3115-2024, 2024
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Fire management has long been a challenge. Here we report that spring-peak fire activity over southern Mexico and Central America (SMCA) has a distinct quasi-biennial signal by measuring multiple fire metrics. This signal is initially driven by quasi-biennial variability in precipitation and is further amplified by positive feedback of fire–precipitation interaction at short timescales. This work highlights the importance of fire–climate interactions in shaping fires on an interannual scale.
Xu Feng, Loretta J. Mickley, Michelle L. Bell, Tianjia Liu, Jenny A. Fisher, and Maria Val Martin
Atmos. Chem. Phys., 24, 2985–3007, https://doi.org/10.5194/acp-24-2985-2024, https://doi.org/10.5194/acp-24-2985-2024, 2024
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During severe wildfire seasons, smoke can have a significant impact on air quality in Australia. Our study demonstrates that characterization of the smoke plume injection fractions greatly affects estimates of surface smoke PM2.5. Using the plume behavior predicted by the machine learning method leads to the best model agreement with observed surface PM2.5 in key cities across Australia, with smoke PM2.5 accounting for 5 %–52 % of total PM2.5 on average during fire seasons from 2009 to 2020.
Shiyi Lai, Ximeng Qi, Xin Huang, Sijia Lou, Xuguang Chi, Liangduo Chen, Chong Liu, Yuliang Liu, Chao Yan, Mengmeng Li, Tengyu Liu, Wei Nie, Veli-Matti Kerminen, Tuukka Petäjä, Markku Kulmala, and Aijun Ding
Atmos. Chem. Phys., 24, 2535–2553, https://doi.org/10.5194/acp-24-2535-2024, https://doi.org/10.5194/acp-24-2535-2024, 2024
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By combining in situ measurements and chemical transport modeling, this study investigates new particle formation (NPF) on the southeastern Tibetan Plateau. We found that the NPF was driven by the presence of biogenic gases and the transport of anthropogenic precursors. The NPF was vertically heterogeneous and shaped by the vertical mixing. This study highlights the importance of anthropogenic–biogenic interactions and meteorological dynamics in NPF in this climate-sensitive region.
Cited articles
Alpert, P. A., Aller, J. Y., and Knopf, D. A.: Ice nucleation from aqueous
NaCl droplets with and without marine diatoms, Atmos. Chem. Phys., 11,
5539–5555, https://doi.org/10.5194/acp-11-5539-2011, 2011. a, b, c
Anderson, D. M.: Ice nucleation and the substrate-ice interface, Nature, 216,
563–566, https://doi.org/10.1038/216563a0, 1967. a, b, c
Atkinson, J. D., Murray, B. J., Woodhouse, M. T., Whale, T. F., Baustian,
K. J., Carslaw, K. S., Dobbie, S., O'sullivan, D., and Malkin, T. L.: The
importance of feldspar for ice nucleation by mineral dust inmixed-phase
clouds, Nature, 498, 355–358, https://doi.org/10.1038/nature12278, 2013. a
Baker, M. and Baker, M.: A new look at homogeneous freezing of water,
Geophys. Res. Lett., 31, L19102, https://doi.org/10.1029/2004GL020483, 2004. a, b, c, d
Barahona, D. and Nenes, A.: Parameterization of cirrus formation in large
scale
models: Homogeneous nucleation, J. Geophys. Res., 113, D11211,
https://doi.org/10.1029/2007JD009355, 2008. a
Barahona, D. and Nenes, A.: Parameterizing the competition between
homogeneous and heterogeneous freezing in cirrus cloud formation –
monodisperse ice nuclei, Atmos. Chem. Phys., 9, 369–381,
https://doi.org/10.5194/acp-9-369-2009, 2009. a, b
Barahona, D., Molod, A., Bacmeister, J., Nenes, A., Gettelman, A., Morrison,
H., Phillips, V., and Eichmann, A.: Development of two-moment cloud
microphysics for liquid and ice within the NASA Goddard Earth Observing
System Model (GEOS-5), Geosci. Model Dev., 7, 1733–1766,
https://doi.org/10.5194/gmd-7-1733-2014, 2014. a, b, c, d
Barahona, D., Molod, A., and Kalesse, H.: Direct estimation of the global
distribution of vertical velocity within cirrus clouds, Sci. Rep. UK,
7, 6840, https://doi.org/10.1038/s41598-017-07038-6, 2017. a
Bellissent-Funel, M.-C.: Water near hydrophilic surfaces, J. Mol. Liquids,
96,
287–304, https://doi.org/10.1016/S0167-7322(01)00354-3, 2002. a
Bigg, E. K.: The formation of atmospheric ice crystals by the freezing of
droplets, Q. J. Roy. Meteor. Soc., 79, 510–519, https://doi.org/10.1002/qj.49707934207,
1953. a
Black, S.: Simulating nucleation of molecular solids, P. R. Soc. A, 463,
2799–2811, 2007. a
Broadley, S. L., Murray, B. J., Herbert, R. J., Atkinson, J. D., Dobbie, S.,
Malkin, T. L., Condliffe, E., and Neve, L.: Immersion mode heterogeneous ice
nucleation by an illite rich powder representative of atmospheric mineral
dust, Atmos. Chem. Phys., 12, 287–307,
https://doi.org/10.5194/acp-12-287-2012, 2012. a
Brukhno, A. V., Anwar, J., Davidchack, R., and Handel, R.: Challenges in
molecular simulation of homogeneous ice nucleation, J. Phys.-Condens. Mat., 20, 494243, https://doi.org/10.1088/0953-8984/20/49/494243, 2008. a
Bullock, G. and Molinero, V.: Low-density liquid water is the mother of ice:
on
the relation between mesostructure, thermodynamics and ice crystallization in
solutions, Faraday Discuss., https://doi.org/10.1039/C3FD00085K, 2013. a, b, c
Cahn, J. W. and Hilliard, J. E.: Free energy of a nonuniform system. I.
Interfacial free energy, J. Chem. Phys., 28, 258–267, 1958. a
Cooke, R. and Kuntz, I.: The properties of water in biological systems, Ann.
Review Biophys. Bioeng., 3, 95–126, 1974. a
Cox, S. J., Kathmann, S. M., Slater, B., and Michaelides, A.: Molecular
simulations of heterogeneous ice nucleation. I. Controlling ice nucleation
through surface hydrophilicity, J. Chem. Phys, 142, 184704,
https://doi.org/10.1063/1.4919714,
2015. a, b
Cziczo, D. J., Froyd, K. D., Hoose, C., Jensen, E. J., Diao, M., Zondlo,
M. A.,
Smith, J. B., Twohy, C. H., and Murphy, D. M.: Clarifying the Dominant
Sources and Mechanisms of Cirrus Cloud Formation, Science, 340, 1320–1324,
2013. a
De Gennes, P.-G.: Wetting: statics and dynamics, Rev. Modern Phys., 57,
827–863, https://doi.org/10.1103/RevModPhys.57.827, 1985. a
DeMott, P. J., Prenni, A. J., Liu, X., Kreidenweis, S. M., Petters, M. D.,
Twohy, C. H., Richardson, M. S., Eidhammer, T., and Rogers, D. C.: Predicting
global atmospheric ice nuclei distributions and their impacts on climate,
Proc. Natl. Acad. Sci. USA, 107, 11217–11222, https://doi.org/10.1073/pnas.0910818107, 2010. a
DeMott, P. J., Möhler, O., Stetzer, O., Vali, G., Levin, Z., Petters,
M. D., Murakami, M., Leisner, T., Bundke, U., Klein, H., et al.: Resurgence
in ice nuclei measurement research, B. Am. Meteorol. Soc., 92, 1623–1635, 2011. a
Diehl, K. and Wurzler, S.: Heterogeneous drop freezing in the immersion mode:
model calculations considering soluble and insoluble particles in the drops,
J. Atmos. Sci., 61, 2063–2072, 2004. a
Espinosa, J., Sanz, E., Valeriani, C., and Vega, C.: Homogeneous ice
nucleation
evaluated for several water models, J. Chem. Phys., 141, 18C529, https://doi.org/10.1063/1.4897524, 2014. a
Feibelman, P. J.: The first wetting layer on a solid, Physics today, 63, 34,
https://doi.org/10.1063/1.3326987, 2010. a, b
Fitzner, M., Sosso, G. C., Cox, S. J., and Michaelides, A.: The Many Faces of
Heterogeneous Ice Nucleation: Interplay Between Surface Morphology and
Hydrophobicity, J. Am. Chem. Soc., 137, 13658–13669,
https://doi.org/10.1021/jacs.5b08748, 2015. a
Fletcher, H.: On ice-crystal production by aerosol particles, J. Atmos. Sci.,
16, 173–180, 1959. a
Gettelman, A., Liu, X., Barahona, D., Lohmann, U., and Chen, C.: Climate
impacts of ice nucleation, J. Geophys. Res., 117, D20201, https://doi.org/10.1029/2012JD017950,
2012. a
Hiranuma, N., Augustin-Bauditz, S., Bingemer, H., Budke, C., Curtius, J.,
Danielczok, A., Diehl, K., Dreischmeier, K., Ebert, M., Frank, F., Hoffmann,
N., Kandler, K., Kiselev, A., Koop, T., Leisner, T., Möhler, O., Nillius,
B., Peckhaus, A., Rose, D., Weinbruch, S., Wex, H., Boose, Y., DeMott, P. J.,
Hader, J. D., Hill, T. C. J., Kanji, Z. A., Kulkarni, G., Levin, E. J. T.,
McCluskey, C. S., Murakami, M., Murray, B. J., Niedermeier, D., Petters, M.
D., O'Sullivan, D., Saito, A., Schill, G. P., Tajiri, T., Tolbert, M. A.,
Welti, A., Whale, T. F., Wright, T. P., and Yamashita, K.: A comprehensive
laboratory study on the immersion freezing behavior of illite NX particles: a
comparison of 17 ice nucleation measurement techniques, Atmos. Chem. Phys.,
15, 2489–2518, https://doi.org/10.5194/acp-15-2489-2015, 2015. a
Hoose, C. and Möhler, O.: Heterogeneous ice nucleation on atmospheric
aerosols: a review of results from laboratory experiments, Atmos. Chem.
Phys., 12, 9817–9854, https://doi.org/10.5194/acp-12-9817-2012, 2012. a, b, c, d
Hoose, C., Kristjansson, J., Chen, J.-C., and Hazra, A.: A
classical-theory-based parameterization of heterogeneous ice nucleation by
mineral dust, soot, and biological particles in a global climate model, J.
Atmos. Sci., 67, 2483–2503, https://doi.org/10.1175/2010JAS3425.1, 2010. a, b
Ickes, L., Welti, A., and Lohmann, U.: Classical nucleation theory of
immersion freezing: sensitivity of contact angle schemes to thermodynamic and
kinetic parameters, Atmos. Chem. Phys., 17, 1713–1739,
https://doi.org/10.5194/acp-17-1713-2017, 2017. a, b
Johari, G., Fleissner, G., Hallbrucker, A., and Mayer, E.: Thermodynamic
continuity between glassy and normal water, J. Phys. Chem., 98, 4719–4725,
1994. a
Johnston, J. C. and Molinero, V.: Crystallization, melting, and structure of
water nanoparticles at atmospherically relevant temperatures, JACS, 134,
6650–6659, https://doi.org/10.1021/ja210878c, 2012. a, b
Kalikmanov, V. I. and van Dongen, M. E. H.: Self-consistent cluster approach
to
the homogeneous kinetic nucleation theory, Phys. Rev. E, 47, 3532–3539,
https://doi.org/10.1103/PhysRevE.47.3532, 1993. a
Kärcher, B. and Lohmann, U.: A parameterization of cirrus cloud
formation:
Heterogeneous freezing, J. Geophys. Res., 108, 4402,
https://doi.org/10.1029/2002JD003220, 2003. a, b
Khvorostyanov, V. and Curry, J.: The theory of ice nucleation by
heterogeneous
freezing of deliquescent mixed CCN. Part II: parcel model simulations, J.
Atmos. Sci., 62, 261–285, 2005. a
Kiselev, A., Bachmann, F., Pedevilla, P., Cox, S. J., Michaelides, A.,
Gerthsen, D., and Leisner, T.: Active sites in heterogeneous ice
nucleation – the example of K-rich feldspars, Science, 355,
367–371, https://doi.org/10.1126/science.aai8034, 2017. a, b
Lance, S., Shupe, M. D., Feingold, G., Brock, C. A., Cozic, J., Holloway, J.
S., Moore, R. H., Nenes, A., Schwarz, J. P., Spackman, J. R., Froyd, K. D.,
Murphy, D. M., Brioude, J., Cooper, O. R., Stohl, A., and Burkhart, J. F.:
Cloud condensation nuclei as a modulator of ice processes in Arctic
mixed-phase clouds, Atmos. Chem. Phys., 11, 8003–8015,
https://doi.org/10.5194/acp-11-8003-2011, 2011. a
Li, K., Xu, S., Chen, J., Zhang, Q., Zhang, Y., Cui, D., Zhou, X., Wang, J.,
and Song, Y.: Viscosity of interfacial water regulates ice nucleation, App.
Phys. Lett., 104, 101605, https://doi.org/10.1063/1.4868255, 2014. a
Lohmann, U. and Feichter, J.: Global indirect aerosol effects: a review,
Atmos. Chem. Phys., 5, 715–737, https://doi.org/10.5194/acp-5-715-2005,
2005. a
Marcolli, C., Gedamke, S., Peter, T., and Zobrist, B.: Efficiency of
immersion mode ice nucleation on surrogates of mineral dust, Atmos. Chem.
Phys., 7, 5081–5091, https://doi.org/10.5194/acp-7-5081-2007, 2007. a
Matsumoto, M., Saito, S., and Ohmine, I.: Molecular dynamics simulation of
the
ice nucleation and growth process leading to water freezing, Nature, 416,
409–413, 2002. a
Meyers, M., DeMott, P., and Cotton, R.: New primary ice-nucleation
parameterization in an explicit cloud model, J. Appl. Meteorol., 31,
708–721, 1992. a
Michaelides, A. and Morgenstern, K.: Ice nanoclusters at hydrophobic metal
surfaces, Nat. Mater., 6, 597–601, https://doi.org/10.1038/nmat1940, 2007. a
Murphy, D. and Koop, T.: Review of the vapour pressures of ice and
supercooled
water for atmospheric applications, Q. J. Roy. Meteor. Soc., 131, 1539–1565,
2005. a
Myhre, G., Shindell, D., Breon, F.-M., Collins, W., Fuglestvedt, J., Huang,
J.,
Koch, D., Lamarque, J.-F., Lee, D., Mendoza, B., Nakajima, T., Robock, A.,
Stephens, G., Takemura, T., and Zhang, H.: Anthropogenic and Natural
Radiative Forcing. Climate Change 2013: The Physical Science Basis.
Contribution of Working Group I to the Fifth Assessment Report of the
Intergovernmental Panel on Climate Change, book section 8, 659–740,
Cambridge University Press, Cambridge, United Kingdom and New York, NY, USA,
https://doi.org/10.1017/CBO9781107415324.018,
2013. a
Niemand, M., Möhler, O., Vogel, B., Vogel, H., Hoose, C., Connolly, P.,
Klein, H., Bingemer, H., DeMott, P., Skrotzki, J., and Leisner, T.: A
particle-surface-area-based parameterization of immersion freezing on desert
dust particles, J. Atmos. Sci., 69, 3077–3092,
https://doi.org/10.1175/JAS-D-11-0249.1, 2012. a
O, K.-T. and Wood, R.: Exploring an approximation for the homogeneous
freezing temperature of water droplets, Atmos. Chem. Phys., 16, 7239–7249,
https://doi.org/10.5194/acp-16-7239-2016, 2016. a
Pauling, L.: The structure and entropy of ice and of other crystals with some
randomness of atomic arrangement, J. Am. Chem. Soc., 57, 2680–2684,
1935. a
Phillips, V. T., Demott, P. J., Andronache, C., Pratt, K. A., Prather, K. A.,
Subramanian, R., and Twohy, C.: Improvements to an Empirical Parameterization
of Heterogeneous Ice Nucleation and its Comparison with Observations, J. Atmos.
Sci., 70, 378–409, https://doi.org/10.1175/JAS-D-12-080.1, 2013. a
Rigg, Y. J., Alpert, P. A., and Knopf, D. A.: Immersion freezing of water and
aqueous ammonium sulfate droplets initiated by humic-like substances as a
function of water activity, Atmos. Chem. Phys., 13, 6603–6622,
https://doi.org/10.5194/acp-13-6603-2013, 2013. a, b, c
Rinnert, E., Carteret, C., Humbert, B., Fragneto-Cusani, G., Ramsay, J. D.,
Delville, A., Robert, J.-L., Bihannic, I., Pelletier, M., and Michot, L. J.:
Hydration of a synthetic clay with tetrahedral charges: a multidisciplinary
experimental and numerical study, J. Phys. Chem. B, 109, 23745–23759, 2005. a
Rusanov, A. I.: Surface thermodynamics revisited, Surf. Sc. Reports, 58,
111–239, 2005. a
Schmelzer, J. W., Boltachev, G. S., and Baidakov, V. G.: Classical and
generalized Gibbs' approaches and the work of critical cluster formation in
nucleation theory, J. Chem. Phys., 124, 194503, https://doi.org/10.1063/1.2196412, 2006. a
Seinfeld, J. H. and Pandis, S. N.: Atmospheric Chemistry and Physics, John
Wiley and Sons, New York, NY, USA, 1998. a
Snyder, P. W., Lockett, M. R., Moustakas, D. T., and Whitesides, G. M.: Is it
the shape of the cavity, or the shape of the water in the cavity?, The
European Physical Journal Special Topics, 223, 853–891,
https://doi.org/10.1140/epjst/e2013-01818-y, 2014. a, b
Tan, I., Storelvmo, T., and Zelinka, M. D.: Observational constraints on
mixed-phase clouds imply higher climate sensitivity, Science, 352, 224–227,
https://doi.org/10.1126/science.aad5300, 2016. a
Taylor, J. H. and Hale, B. N.: Monte Carlo simulations of water-ice layers on
a
model silver iodide substrate: A comparison with bulk ice systems, Physical
Rev. B, 47, 9732, 1993. a
Turnbull, D. and Fisher, J. C.: Rate of nucleation in condensed systems, J.
Chem. Phys., 17, 71–73, 1949. a
Vali, G.: Interpretation of freezing nucleation experiments: singular and
stochastic; sites and surfaces, Atmos. Chem. Phys., 14, 5271–5294,
https://doi.org/10.5194/acp-14-5271-2014, 2014. a
Vekilov, P. G.: The two-step mechanism of nucleation of crystals in solution,
Nanoscale, 2, 2346–2357, https://doi.org/10.1039/C0NR00628A, 2010. a, b
Wang, J., Kalinichev, A. G., and Kirkpatrick, R. J.: Effects of substrate
structure and composition on the structure, dynamics, and energetics of water
at mineral surfaces: A molecular dynamics modeling study, Geochim. Cosmochim. Ac., 70, 562–582, https://doi.org/10.1016/j.gca.2005.10.006, 2006. a
Wang, Q., Zhao, L., Li, C., and Cao, Z.: The decisive role of free water in
determining homogenous ice nucleation behavior of aqueous solutions,
Sci. Rep. UK, 6, 26831, https://doi.org/10.1038/srep26831, 2016. a
Warne, M., Allan, N., and Cosgrove, T.: Computer simulation of water
molecules
at kaolinite and silica surfaces, Phys. Chem. Chem. Phys., 2, 3663–3668,
2000. a
Wiacek, A., Peter, T., and Lohmann, U.: The potential influence of Asian and
African mineral dust on ice, mixed-phase and liquid water clouds, Atmos.
Chem. Phys., 10, 8649–8667, https://doi.org/10.5194/acp-10-8649-2010, 2010. a, b
Yu, C.-J., Evmenenko, G., Richter, A., Datta, A., Kmetko, J., and Dutta, P.:
Order in molecular liquids near solid–liquid interfaces, App. Surface Sci.,
182, 231–235, https://doi.org/10.1016/S0169-4332(01)00410-X, 2001. a, b, c
Zhang, Z., Lü, X., and Jiang, Q.: Finite size effect on melting enthalpy
and melting entropy of nanocrystals, Physica B, 270,
249–254, https://doi.org/10.1016/S0921-4526(99)00199-4, 1999. a, b
Zheng, J.-m., Chin, W.-C., Khijniak, E., Khijniak Jr, E., and Pollack, G. H.:
Surfaces and interfacial water: evidence that hydrophilic surfaces have
long-range impact, Adv. Colloid Interface Sc., 127, 19–27,
https://doi.org/10.1016/j.cis.2006.07.002, 2006. a
Zuberi, B., Bertram, A., Cassa, C., Molina, L., and Molina, M.: Heterogeneous
nucleation of ice in (NH4)2SO4-H2O particles with mineral dust immersions,
Geophys. Res. Lett., 29, 1504, https://doi.org/10.1029/2001GL014289, 2002. a
Short summary
This work develops a model for ice formation mediated by particles immersed within droplets. Ice nucleation is not only enhanced by the modification of the thermodynamic properties of the vicinal water but is also inhibited by decreased water mobility near the particle. The ice nucleation rate is thus determined by competing kinetic and thermodynamic factors during ice formation. A new regime where ice nucleation is mediated mainly by kinetics instead of thermodynamics is discovered.
This work develops a model for ice formation mediated by particles immersed within droplets. Ice...
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