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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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.
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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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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.
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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
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 | Altitude Range: Troposphere | Science Focus: Physics (physical properties and processes)
Role of K-feldspar and quartz in global ice nucleation by mineral dust in mixed-phase clouds
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Ice formation is enabled by ice-nucleating particles (INP) at higher temperatures than homogeneous formation and can profoundly affect the properties of clouds. Our global model results show that K-feldspar is the most important contributor to INP concentrations globally, affecting mid-level mixed-phase clouds. However, quartz can significantly contribute and dominates the lowest and the highest altitudes of dust-derived INP, affecting mainly low-level and high-level mixed-phase clouds.
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Rémy Lapere, Nicolás Huneeus, Sylvain Mailler, Laurent Menut, and Florian Couvidat
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Glaciers in the Andes of central Chile are shrinking rapidly in response to global warming. This melting is accelerated by the deposition of opaque particles onto snow and ice. In this work, model simulations quantify typical deposition rates of soot on glaciers in summer and winter months and show that the contribution of emissions from Santiago is not as high as anticipated. Additionally, the combination of regional- and local-scale meteorology explains the seasonality in deposition.
Ju Liang and Jim Haywood
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The recent record-breaking flood events in China during the summer of 2021 highlight the importance of mitigating the risks from future changes in high-impact weather systems under global warming. Based on a state-of-the-art Earth system model, we demonstrate a pilot study on the responses of atmospheric rivers and extreme precipitation over East Asia to anthropogenically induced climate warming and an unconventional mitigation strategy – stratospheric aerosol injection.
Azad Madhu, Myoseon Jang, and David Deacon
Atmos. Chem. Phys., 23, 1661–1675, https://doi.org/10.5194/acp-23-1661-2023, https://doi.org/10.5194/acp-23-1661-2023, 2023
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SOA formation is simulated using the UNIPAR model for series of linear alkanes. The inclusion of autoxidation reactions within the explicit gas mechanisms of C9–C12 was found to significantly improve predictions. Available product distributions were extrapolated with an incremental volatility coefficient (IVC) to predict SOA formation of alkanes without explicit mechanisms. These product distributions were used to simulate SOA formation from C13 and C15 and had good agreement with chamber data.
Jianbing Jin, Bas Henzing, and Arjo Segers
Atmos. Chem. Phys., 23, 1641–1660, https://doi.org/10.5194/acp-23-1641-2023, https://doi.org/10.5194/acp-23-1641-2023, 2023
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Aerosol models and satellite retrieval algorithms rely on different aerosol size assumptions. In practice, differences between simulations and observations do not always reflect the difference in aerosol amount. To avoid inconsistencies, we designed a hybrid assimilation approach. Different from a standard aerosol optical depth (AOD) assimilation that directly assimilates AODs, the hybrid one estimates aerosol size parameters by assimilating Ängström observations before assimilating the AODs.
Je-Yun Chun, Robert Wood, Peter Blossey, and Sarah J. Doherty
Atmos. Chem. Phys., 23, 1345–1368, https://doi.org/10.5194/acp-23-1345-2023, https://doi.org/10.5194/acp-23-1345-2023, 2023
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Nora L. S. Fahrenbach and Massimo A. Bollasina
Atmos. Chem. Phys., 23, 877–894, https://doi.org/10.5194/acp-23-877-2023, https://doi.org/10.5194/acp-23-877-2023, 2023
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We studied the monthly-scale climate response to COVID-19 aerosol emission reductions during January–May 2020 using climate models. Our results show global temperature and rainfall anomalies driven by circulation changes. The climate patterns reverse polarity from JF to MAM due to a shift in the main SO2 reduction region from China to India. This real-life example of rapid climate adjustments to abrupt, regional aerosol emission reduction has large implications for future climate projections.
Seoung Soo Lee, Junshik Um, Won Jun Choi, Kyung-Ja Ha, Chang Hoon Jung, Jianping Guo, and Youtong Zheng
Atmos. Chem. Phys., 23, 273–286, https://doi.org/10.5194/acp-23-273-2023, https://doi.org/10.5194/acp-23-273-2023, 2023
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This paper elaborates on process-level mechanisms regarding how the interception of radiation by aerosols interacts with the surface heat fluxes and atmospheric instability in warm cumulus clouds. This paper elucidates how these mechanisms vary with the location or altitude of an aerosol layer. This elucidation indicates that the location of aerosol layers should be taken into account for parameterizations of aerosol–cloud interactions.
Meredith Schervish and Manabu Shiraiwa
Atmos. Chem. Phys., 23, 221–233, https://doi.org/10.5194/acp-23-221-2023, https://doi.org/10.5194/acp-23-221-2023, 2023
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Secondary organic aerosols (SOAs) can exhibit complex non-ideal behavior and adopt an amorphous semisolid state. We simulate condensation of semi-volatile compounds into a phase-separated particle to investigate the effect of non-ideality and particle phase state on the equilibration timescale of SOA partitioning. Our results provide useful insights into the interpretation of experimental observations and the description and treatment of SOA in aerosol models.
Christof G. Beer, Johannes Hendricks, and Mattia Righi
Atmos. Chem. Phys., 22, 15887–15907, https://doi.org/10.5194/acp-22-15887-2022, https://doi.org/10.5194/acp-22-15887-2022, 2022
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Ice-nucleating particles (INPs) have important influences on cirrus clouds and the climate system; however, their global atmospheric distribution in the cirrus regime is still very uncertain. We present a global climatology of INPs under cirrus conditions derived from model simulations, considering the mineral dust, soot, crystalline ammonium sulfate, and glassy organics INP types. The comparison of respective INP concentrations indicates the large importance of ammonium sulfate particles.
Mykhailo Savenets, Larysa Pysarenko, Svitlana Krakovska, Alexander Mahura, and Tuukka Petäjä
Atmos. Chem. Phys., 22, 15777–15791, https://doi.org/10.5194/acp-22-15777-2022, https://doi.org/10.5194/acp-22-15777-2022, 2022
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The paper explores the spatio-temporal variability of black carbon during a wildfire in August 2010, with a focus on Ukraine. As a research tool, the seamless Enviro-HIRLAM modelling system is used for investigating the atmospheric transport of aerosol particles emitted by wildfires from remote and local sources. The results of this study improve our understanding of the physical and chemical processes and the interactions of aerosols in the atmosphere.
Huilin Huang, Yun Qian, Ye Liu, Cenlin He, Jianyu Zheng, Zhibo Zhang, and Antonis Gkikas
Atmos. Chem. Phys., 22, 15469–15488, https://doi.org/10.5194/acp-22-15469-2022, https://doi.org/10.5194/acp-22-15469-2022, 2022
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Using a clustering method developed in the field of artificial neural networks, we identify four typical dust transport patterns across the Sierra Nevada, associated with the mesoscale and regional-scale wind circulations. Our results highlight the connection between dust transport and dominant weather patterns, which can be used to understand dust transport in a changing climate.
Anbao Zhu, Haiming Xu, Jiechun Deng, Jing Ma, and Shaofeng Hua
Atmos. Chem. Phys., 22, 15425–15447, https://doi.org/10.5194/acp-22-15425-2022, https://doi.org/10.5194/acp-22-15425-2022, 2022
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This study demonstrates the instant and delayed effects of biomass burning (BB) aerosols on precipitation over the Indochina Peninsula (ICP). The convection suppression due to the BB aerosol-induced stabilized atmosphere dominates over the favorable water-vapor condition induced by large-scale circulation responses, leading to an overall reduced precipitation in March, while the delayed effect promotes precipitation from early April to mid April due to the anomalous atmospheric circulations.
Wenjie Zhang, Hong Wang, Xiaoye Zhang, Liping Huang, Yue Peng, Zhaodong Liu, Xiao Zhang, and Huizheng Che
Atmos. Chem. Phys., 22, 15207–15221, https://doi.org/10.5194/acp-22-15207-2022, https://doi.org/10.5194/acp-22-15207-2022, 2022
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Aerosol–cloud interaction (ACI) is first implemented in the atmospheric chemistry system GRAPES_Meso5.1/CUACE. ACI can improve the simulated cloud, temperature, and precipitation under haze pollution conditions in Jing-Jin-Ji in China. This paper demonstrates the critical role of ACI in current numerical weather prediction over the severely polluted region.
Santeri Tuovinen, Runlong Cai, Veli-Matti Kerminen, Jingkun Jiang, Chao Yan, Markku Kulmala, and Jenni Kontkanen
Atmos. Chem. Phys., 22, 15071–15091, https://doi.org/10.5194/acp-22-15071-2022, https://doi.org/10.5194/acp-22-15071-2022, 2022
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We compare observed survival probabilities of atmospheric particles from Beijing, China, with survival probabilities based on analytical formulae and model simulations. We find observed survival probabilities under polluted conditions at smaller sizes to be higher, while at larger sizes they are lower than or similar to theoretical survival probabilities. Uncertainties in condensation sink and growth rate are unlikely to explain higher-than-predicted survival probabilities at smaller sizes.
Stephanie Woodward, Alistair A. Sellar, Yongming Tang, Marc Stringer, Andrew Yool, Eddy Robertson, and Andy Wiltshire
Atmos. Chem. Phys., 22, 14503–14528, https://doi.org/10.5194/acp-22-14503-2022, https://doi.org/10.5194/acp-22-14503-2022, 2022
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We describe the dust scheme in the UKESM1 Earth system model and show generally good agreement with observations. Comparing with the closely related HadGEM3-GC3.1 model, we show that dust differences are not only due to inter-model differences but also to the dust size distribution. Under climate change, HadGEM3-GC3.1 dust hardly changes, but UKESM1 dust decreases because that model includes the vegetation response which, in our models, has a bigger impact on dust than climate change itself.
Yang Yang, Liangying Zeng, Hailong Wang, Pinya Wang, and Hong Liao
Atmos. Chem. Phys., 22, 14489–14502, https://doi.org/10.5194/acp-22-14489-2022, https://doi.org/10.5194/acp-22-14489-2022, 2022
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Using an aerosol–climate model, dust pollution in China affected by different spatial and temporal types of El Niño are examined. Both eastern and central Pacific El Niño and short-duration El Niño increase winter dust concentrations over northern China, while long-duration El Niño decreases concentrations. Only long-duration El Niño events can significantly affect dust over China in the following spring. This study has profound implications for air pollution control and dust storm prediction.
Ruth Price, Andrea Baccarini, Julia Schmale, Paul Zieger, Ian M. Brooks, Paul Field, and Ken S. Carslaw
EGUsphere, https://doi.org/10.5194/egusphere-2022-1079, https://doi.org/10.5194/egusphere-2022-1079, 2022
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Arctic clouds can control how much energy is absorbed by the surface or reflected back to space. Using a computer model of the atmosphere, we investigated the formation of atmospheric particles that allow cloud droplets to form. We found that particles formed aloft are transported to the lowest part of the Arctic atmosphere and that this is a key source of particles. Our results have implications for the way Arctic clouds will behave in the future as climate change continues to impact the region.
Robin Stevens, Andrei Ryjkov, Mahtab Majdzadeh, and Ashu Dastoor
Atmos. Chem. Phys., 22, 13527–13549, https://doi.org/10.5194/acp-22-13527-2022, https://doi.org/10.5194/acp-22-13527-2022, 2022
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Absorbing particles like black carbon can be coated with other matter. How much radiation these particles absorb depends on the coating thickness. The removal of these particles by clouds and rain depends on the coating composition. These effects are important for both climate and air quality. We implement a more detailed representation of these particles in an air quality model which accounts for both coating thickness and composition. We find a significant effect on particle concentrations.
Fan Wang, Gregory R. Carmichael, Jing Wang, Bin Chen, Bo Huang, Yuguo Li, Yuanjian Yang, and Meng Gao
Atmos. Chem. Phys., 22, 13341–13353, https://doi.org/10.5194/acp-22-13341-2022, https://doi.org/10.5194/acp-22-13341-2022, 2022
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Unprecedented urbanization in China has led to serious urban heat island (UHI) issues, exerting intense heat stress on urban residents. We find diverse influences of aerosol pollution on urban heat island intensity (UHII) under different circulations. Our results also highlight the role of black carbon in aggravating UHI, especially during nighttime. It could thus be targeted for cooperative management of heat islands and aerosol pollution.
Qianqian Song, Zhibo Zhang, Hongbin Yu, Jasper F. Kok, Claudia Di Biagio, Samuel Albani, Jianyu Zheng, and Jiachen Ding
Atmos. Chem. Phys., 22, 13115–13135, https://doi.org/10.5194/acp-22-13115-2022, https://doi.org/10.5194/acp-22-13115-2022, 2022
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This study developed a dataset that enables us to efficiently calculate dust direct radiative effect (DRE, i.e., cooling or warming our planet) for any given dust size distribution in addition to three sets of dust mineral components and two dust shapes. We demonstrate and validate the method of using this dataset to calculate dust DRE. Moreover, using this dataset we found that dust mineral composition is a more important factor in determining dust DRE than dust size and shape.
Eleni Drakaki, Vassilis Amiridis, Alexandra Tsekeri, Antonis Gkikas, Emmanouil Proestakis, Sotirios Mallios, Stavros Solomos, Christos Spyrou, Eleni Marinou, Claire L. Ryder, Demetri Bouris, and Petros Katsafados
Atmos. Chem. Phys., 22, 12727–12748, https://doi.org/10.5194/acp-22-12727-2022, https://doi.org/10.5194/acp-22-12727-2022, 2022
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State-of-the-art atmospheric dust models have limitations in accounting for a realistic dust size distribution (emission, transport). We modify the parameterization of the mineral dust cycle by including particles with diameter >20 μm, as indicated by observations over deserts. Moreover, we investigate the effects of reduced settling velocities of dust particles. Model results are evaluated using airborne and spaceborne dust measurements above Cabo Verde.
Christopher D. Wells, Matthew Kasoar, Nicolas Bellouin, and Apostolos Voulgarakis
EGUsphere, https://doi.org/10.5194/egusphere-2022-919, https://doi.org/10.5194/egusphere-2022-919, 2022
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The climate is altered by greenhouse gases and air pollutant particles, and such emissions are likely to change drastically in the future over Africa. Air pollutants do not travel far, so their climate effect depends on where they are emitted. This study uses a climate model to find the climate impacts of future African pollutant emissions being either high or low. The particles absorb and scatter sunlight, causing the ground nearby to be cooler, but elsewhere the increased heat causes warming.
Chenguang Tian, Xu Yue, Jun Zhu, Hong Liao, Yang Yang, Yadong Lei, Xinyi Zhou, Hao Zhou, Yimian Ma, and Yang Cao
Atmos. Chem. Phys., 22, 12353–12366, https://doi.org/10.5194/acp-22-12353-2022, https://doi.org/10.5194/acp-22-12353-2022, 2022
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We quantify the impacts of fire aerosols on climate through direct, indirect, and albedo effects. In atmosphere-only simulations, we find global fire aerosols cause surface cooling and rainfall inhibition over many land regions. These fast atmospheric perturbations further lead to a reduction in regional leaf area index and lightning activities. By considering the feedback of fire aerosols on humidity, lightning, and leaf area index, we predict a slight reduction in fire emissions.
Yanxing Wu, Run Liu, Yanzi Li, Junjie Dong, Zhijiong Huang, Junyu Zheng, and Shaw Chen Liu
Atmos. Chem. Phys., 22, 11945–11955, https://doi.org/10.5194/acp-22-11945-2022, https://doi.org/10.5194/acp-22-11945-2022, 2022
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Multiple linear regression (MLR) analyses often interpret the correlation coefficient (r2) as the contribution of an independent variable to the dependent variable. Since a good correlation does not imply a causal relationship, we propose that r2 should be interpreted as the maximum possible contribution. Moreover, MLR results are sensitive to the length of time analyzed; long-term analysis gives a more accurate assessment because of its additional constraints.
Mengying Li, Shaocai Yu, Xue Chen, Zhen Li, Yibo Zhang, Zhe Song, Weiping Liu, Pengfei Li, Xiaoye Zhang, Meigen Zhang, Yele Sun, Zirui Liu, Caiping Sun, Jingkun Jiang, Shuxiao Wang, Benjamin N. Murphy, Kiran Alapaty, Rohit Mathur, Daniel Rosenfeld, and John H. Seinfeld
Atmos. Chem. Phys., 22, 11845–11866, https://doi.org/10.5194/acp-22-11845-2022, https://doi.org/10.5194/acp-22-11845-2022, 2022
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This study constructed an emission inventory of condensable particulate matter (CPM) in China with a focus on organic aerosols (OAs), based on collected CPM emission information. The results show that OA emissions are enhanced twofold for the years 2014 and 2017 after the inclusion of CPM in the new inventory. Sensitivity cases demonstrated the significant contributions of CPM emissions from stationary combustion and mobile sources to primary, secondary, and total OA concentrations.
Petri Räisänen, Joonas Merikanto, Risto Makkonen, Mikko Savolahti, Alf Kirkevåg, Maria Sand, Øyvind Seland, and Antti-Ilari Partanen
Atmos. Chem. Phys., 22, 11579–11602, https://doi.org/10.5194/acp-22-11579-2022, https://doi.org/10.5194/acp-22-11579-2022, 2022
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A climate model is used to evaluate how the radiative forcing (RF) associated with black carbon (BC) emissions depends on the latitude, longitude, and seasonality of emissions. It is found that both the direct RF (BC absorption of solar radiation in air) and snow RF (BC absorption in snow/ice) depend strongly on the emission region and season. The results suggest that, for a given mass of BC emitted, climatic impacts are likely to be largest for high-latitude emissions due to the large snow RF.
Xipeng Jin, Xuhui Cai, Mingyuan Yu, Yu Song, Xuesong Wang, Hongsheng Zhang, and Tong Zhu
Atmos. Chem. Phys., 22, 11409–11427, https://doi.org/10.5194/acp-22-11409-2022, https://doi.org/10.5194/acp-22-11409-2022, 2022
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Meteorological discontinuities in the vertical direction define the lowest atmosphere as the boundary layer, while in the horizontal direction it identifies the contrast zone as the internal boundary. Both of them determine the polluted air mass dimension over the North China Plain. This study reveals the boundary layer structures under three categories of internal boundaries, modified by thermal, dynamical, and blending effects. It provides a new insight to understand regional pollution.
Lichao Yang, Wansuo Duan, Zifa Wang, and Wenyi Yang
Atmos. Chem. Phys., 22, 11429–11453, https://doi.org/10.5194/acp-22-11429-2022, https://doi.org/10.5194/acp-22-11429-2022, 2022
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The initial meteorological state has a great impact on PM2.5 forecasts. Assimilating additional observations is an effective way to improve the accuracy of the initial meteorological state. Here we used an advanced optimization approach to identify where we should preferentially place the meteorological observations associated with PM2.5 forecasts in the Beijing–Tianjin–Hebei region of China. We provide evidence that the target observation strategy is effective for improving PM2.5 forecasts.
Anthony C. Jones, Adrian Hill, John Hemmings, Pascal Lemaitre, Arnaud Quérel, Claire L. Ryder, and Stephanie Woodward
Atmos. Chem. Phys., 22, 11381–11407, https://doi.org/10.5194/acp-22-11381-2022, https://doi.org/10.5194/acp-22-11381-2022, 2022
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As raindrops fall to the ground, they capture aerosol (i.e. below-cloud scavenging or BCS). Many different BCS schemes are available to climate models, and it is unclear what the impact of selecting one scheme over another is. Here, various BCS models are outlined and then applied to mineral dust in climate model simulations. We find that dust concentrations are highly sensitive to the BCS scheme, with dust atmospheric lifetimes ranging from 5 to 44 d.
Peng Wang, Ruhan Zhang, Shida Sun, Meng Gao, Bo Zheng, Dan Zhang, Yangli Zhang, Gregory R. Carmichael, and Hongliang Zhang
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2022-577, https://doi.org/10.5194/acp-2022-577, 2022
Revised manuscript accepted for ACP
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In China, vehicles have jumped significantly in the recent decade. This caused severe traffic congestion and aggravated air pollution. In this study, we developed a new temporal-allocation approach to quantify the impacts of traffic congestion. We found that traffic congestion worsens air quality and health burden across China, especially in the urban clusters. More effective and comprehensive vehicle emission control policies should be implemented to improve air quality in China.
Zhicong Yin, Mingkeng Duan, Yuyan Li, Tianbao Xu, and Huijun Wang
Atmos. Chem. Phys., 22, 11173–11185, https://doi.org/10.5194/acp-22-11173-2022, https://doi.org/10.5194/acp-22-11173-2022, 2022
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The PM2.5 concentration has been greatly reduced in recent years in China and has entered a crucial stage that required fine seasonal prediction. However, there is still no study aimed at predicting gridded PM2.5 concentration. A model for seasonal prediction of gridded winter PM2.5 concentration in the east of China was developed by analyzing the contributions of emissions and climate variability, which could provide scientific support for air pollution control at the regional and city levels.
Qirui Zhong, Nick Schutgens, Guido van der Werf, Twan van Noije, Kostas Tsigaridis, Susanne E. Bauer, Tero Mielonen, Alf Kirkevåg, Øyvind Seland, Harri Kokkola, Ramiro Checa-Garcia, David Neubauer, Zak Kipling, Hitoshi Matsui, Paul Ginoux, Toshihiko Takemura, Philippe Le Sager, Samuel Rémy, Huisheng Bian, Mian Chin, Kai Zhang, Jialei Zhu, Svetlana G. Tsyro, Gabriele Curci, Anna Protonotariou, Ben Johnson, Joyce E. Penner, Nicolas Bellouin, Ragnhild B. Skeie, and Gunnar Myhre
Atmos. Chem. Phys., 22, 11009–11032, https://doi.org/10.5194/acp-22-11009-2022, https://doi.org/10.5194/acp-22-11009-2022, 2022
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Aerosol optical depth (AOD) errors for biomass burning aerosol (BBA) are evaluated in 18 global models against satellite datasets. Notwithstanding biases in satellite products, they allow model evaluations. We observe large and diverse model biases due to errors in BBA. Further interpretations of AOD diversities suggest large biases exist in key processes for BBA which require better constraining. These results can contribute to further model improvement and development.
Marje Prank, Juha Tonttila, Jaakko Ahola, Harri Kokkola, Thomas Kühn, Sami Romakkaniemi, and Tomi Raatikainen
Atmos. Chem. Phys., 22, 10971–10992, https://doi.org/10.5194/acp-22-10971-2022, https://doi.org/10.5194/acp-22-10971-2022, 2022
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Aerosols and clouds persist as the dominant sources of uncertainty in climate projections. In this modelling study, we investigate the role of marine aerosols in influencing the lifetime of low-level clouds. Our high resolution simulations show that sea spray can both extend and shorten the lifetime of the cloud layer depending on the model setup. The impact of the primary marine organics is relatively limited while secondary aerosol from monoterpenes can have larger impact.
Roger Teoh, Ulrich Schumann, Edward Gryspeerdt, Marc Shapiro, Jarlath Molloy, George Koudis, Christiane Voigt, and Marc E. J. Stettler
Atmos. Chem. Phys., 22, 10919–10935, https://doi.org/10.5194/acp-22-10919-2022, https://doi.org/10.5194/acp-22-10919-2022, 2022
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Aircraft condensation trails (contrails) contribute to over half of the climate forcing attributable to aviation. This study uses historical air traffic and weather data to simulate contrails in the North Atlantic over 5 years, from 2016 to 2021. We found large intra- and inter-year variability in contrail radiative forcing and observed a 66 % reduction due to COVID-19. Most warming contrails predominantly result from night-time flights in winter.
Haochi Che, Philip Stier, Duncan Watson-Parris, Hamish Gordon, and Lucia Deaconu
Atmos. Chem. Phys., 22, 10789–10807, https://doi.org/10.5194/acp-22-10789-2022, https://doi.org/10.5194/acp-22-10789-2022, 2022
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Extensive stratocumulus clouds over the south-eastern Atlantic (SEA) can lead to a cooling effect on the climate. A key pathway by which aerosols affect cloud properties is by acting as cloud condensation nuclei (CCN). Here, we investigated the source attribution of CCN in the SEA as well as the cloud responses. Our results show that aerosol nucleation contributes most to CCN in the marine boundary layer. In terms of emissions, anthropogenic sources contribute most to the CCN and cloud droplets.
Aditya Kumar, R. Bradley Pierce, Ravan Ahmadov, Gabriel Pereira, Saulo Freitas, Georg Grell, Chris Schmidt, Allen Lenzen, Joshua P. Schwarz, Anne E. Perring, Joseph M. Katich, John Hair, Jose L. Jimenez, Pedro Campuzano-Jost, and Hongyu Guo
Atmos. Chem. Phys., 22, 10195–10219, https://doi.org/10.5194/acp-22-10195-2022, https://doi.org/10.5194/acp-22-10195-2022, 2022
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We use the WRF-Chem model with new implementations of GOES-16 wildfire emissions and plume rise based on fire radiative power (FRP) to interpret aerosol observations during the 2019 NASA–NOAA FIREX-AQ field campaign and perform model evaluations. The model shows significant improvements in simulating the variety of aerosol loading environments sampled during FIREX-AQ. Our results also highlight the importance of accurate wildfire diurnal cycle and aerosol chemical mechanisms in models.
Golnaz Roudsari, Olli H. Pakarinen, Bernhard Reischl, and Hanna Vehkamäki
Atmos. Chem. Phys., 22, 10099–10114, https://doi.org/10.5194/acp-22-10099-2022, https://doi.org/10.5194/acp-22-10099-2022, 2022
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We use atomistic simulations to study heterogeneous ice nucleation on silver iodide surfaces in slit and wedge geometries at low supercooling which serve as a model of irregularities on real atmospheric aerosol particle surfaces. The revealed microscopic ice nucleation mechanisms in confined geometries strongly support the experimental evidence for the importance of surface features such as cracks or pits functioning as active sites for ice nucleation in the atmosphere.
Carlton Xavier, Metin Baykara, Robin Wollesen de Jonge, Barbara Altstädter, Petri Clusius, Ville Vakkari, Roseline Thakur, Lisa Beck, Silvia Becagli, Mirko Severi, Rita Traversi, Radovan Krejci, Peter Tunved, Mauro Mazzola, Birgit Wehner, Mikko Sipilä, Markku Kulmala, Michael Boy, and Pontus Roldin
Atmos. Chem. Phys., 22, 10023–10043, https://doi.org/10.5194/acp-22-10023-2022, https://doi.org/10.5194/acp-22-10023-2022, 2022
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The focus of this work is to study and improve our understanding of processes involved in the formation and growth of new particles in a remote Arctic marine environment. We run the 1D model ADCHEM along air mass trajectories arriving at Ny-Ålesund in May 2018. The model finds that ion-mediated H2SO4–NH3 nucleation can explain the observed new particle formation at Ny-Ålesund. The growth of particles is driven via H2SO4 condensation and formation of methane sulfonic acid in the aqueous phase.
Tuuli Miinalainen, Harri Kokkola, Antti Lipponen, Antti-Pekka Hyvärinen, Vijay Kumar Soni, Kari E. J. Lehtinen, and Thomas Kühn
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2022-513, https://doi.org/10.5194/acp-2022-513, 2022
Revised manuscript accepted for ACP
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We simulated the effects of aerosol emission mitigation on both global and regional radiative forcing and city-level air quality with a global-scale climate model. We used a machine learning downscaling approach to bias-correct the PM2.5 values obtained from the global model for the Indian mega-city New Delhi. Our results indicate that aerosol mitigation could result in both improved air quality and less radiative heating for India.
Kai Zhang, Wentao Zhang, Hui Wan, Philip J. Rasch, Steven J. Ghan, Richard C. Easter, Xiangjun Shi, Yong Wang, Hailong Wang, Po-Lun Ma, Shixuan Zhang, Jian Sun, Susannah M. Burrows, Manish Shrivastava, Balwinder Singh, Yun Qian, Xiaohong Liu, Jean-Christophe Golaz, Qi Tang, Xue Zheng, Shaocheng Xie, Wuyin Lin, Yan Feng, Minghuai Wang, Jin-Ho Yoon, and L. Ruby Leung
Atmos. Chem. Phys., 22, 9129–9160, https://doi.org/10.5194/acp-22-9129-2022, https://doi.org/10.5194/acp-22-9129-2022, 2022
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Here we analyze the effective aerosol forcing simulated by E3SM version 1 using both century-long free-running and short nudged simulations. The aerosol forcing in E3SMv1 is relatively large compared to other models, mainly due to the large indirect aerosol effect. Aerosol-induced changes in liquid and ice cloud properties in E3SMv1 have a strong correlation. The aerosol forcing estimates in E3SMv1 are sensitive to the parameterization changes in both liquid and ice cloud processes.
Seoung Soo Lee, Jinho Choi, Goun Kim, Kyung-Ja Ha, Kyong-Hwan Seo, Chang Hoon Jung, Junshik Um, Youtong Zheng, Jianping Guo, Sang-Keun Song, Yun Gon Lee, and Nobuyuki Utsumi
Atmos. Chem. Phys., 22, 9059–9081, https://doi.org/10.5194/acp-22-9059-2022, https://doi.org/10.5194/acp-22-9059-2022, 2022
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This study investigates how aerosols affect clouds and precipitation and how the aerosol effects vary with varying types of clouds that are characterized by cloud depth in two metropolitan areas in East Asia. As cloud depth increases, the enhancement of precipitation amount transitions to no changes in precipitation amount with increasing aerosol concentrations. This indicates that cloud depth needs to be considered for a comprehensive understanding of aerosol-cloud interactions.
Karine Sartelet, Youngseob Kim, Florian Couvidat, Maik Merkel, Tuukka Petäjä, Jean Sciare, and Alfred Wiedensohler
Atmos. Chem. Phys., 22, 8579–8596, https://doi.org/10.5194/acp-22-8579-2022, https://doi.org/10.5194/acp-22-8579-2022, 2022
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A methodology is defined to estimate number emissions from an inventory providing mass emissions. Number concentrations are simulated over Greater Paris using different nucleation parameterisations (binary, ternary involving sulfuric acid and ammonia, and heteromolecular involving sulfuric acid and extremely low-volatility organics, ELVOCs). The comparisons show that ternary nucleation may not be a dominant process for new particle formation in cities, but they stress the role of ELVOCs.
Zhaochen Liu, Xianmei Lang, and Dabang Jiang
Atmos. Chem. Phys., 22, 7667–7680, https://doi.org/10.5194/acp-22-7667-2022, https://doi.org/10.5194/acp-22-7667-2022, 2022
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Stratospheric aerosol intervention geoengineering is considered a potential means to counteract global warming. Here the impact of stratospheric aerosol intervention geoengineering on surface air temperature over China and related physical processes are investigated. Results show that the increased stratospheric aerosols cause surface cooling over China. The temperature responses vary with models, regions, and seasons and are largely related to net surface shortwave radiation changes.
Jie Luo, Zhengqiang Li, Chenchong Zhang, Qixing Zhang, Yongming Zhang, Ying Zhang, Gabriele Curci, and Rajan K. Chakrabarty
Atmos. Chem. Phys., 22, 7647–7666, https://doi.org/10.5194/acp-22-7647-2022, https://doi.org/10.5194/acp-22-7647-2022, 2022
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The fractal black carbon was applied to re-evaluate the regional impacts of morphologies on aerosol–radiation interactions (ARIs), and the effects were compared between the US and China. The regional-mean clear-sky ARI is significantly affected by the BC morphology, and relative differences of 17.1 % and 38.7 % between the fractal model with a Df of 1.8 and the spherical model were observed in eastern China and the northwest US, respectively.
Suvarna Fadnavis, Prashant Chavan, Akash Joshi, Sunil M. Sonbawne, Asutosh Acharya, Panuganti C. S. Devara, Alexandru Rap, Felix Ploeger, and Rolf Müller
Atmos. Chem. Phys., 22, 7179–7191, https://doi.org/10.5194/acp-22-7179-2022, https://doi.org/10.5194/acp-22-7179-2022, 2022
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We show that large amounts of anthropogenic aerosols are transported from South Asia to the northern Indian Ocean. These aerosols are then lifted into the UTLS by the ascending branch of the Hadley circulation. They are further transported to the Southern Hemisphere and downward via westerly ducts over the tropical Atlantic and Pacific. These aerosols increase tropospheric heating, resulting in an increase in water vapor, which is then transported to the UTLS.
Kevin Ohneiser, Albert Ansmann, Jonas Witthuhn, Hartwig Deneke, Alexandra Chudnovsky, and Gregor Walter
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2022-343, https://doi.org/10.5194/acp-2022-343, 2022
Revised manuscript accepted for ACP
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This study shows that smoke layers can reach the tropopause via the self-lofting effect within 3–7 days in the absence of pyroCB convection if the AOT is larger than approximately 2 for a longer time period. In the stratosphere it can further self-loft if the AOT is larger than 0.01. When reaching the stratosphere, wildfire smoke can sensitively influence the stratospheric composition on a hemispheric scale and thus can affect the Earth’s climate and the ozone layer.
Xiadong An, Wen Chen, Peng Hu, Shangfeng Chen, and Lifang Sheng
Atmos. Chem. Phys., 22, 6507–6521, https://doi.org/10.5194/acp-22-6507-2022, https://doi.org/10.5194/acp-22-6507-2022, 2022
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The intraseasonal NAAA usually establishes quickly on day −3 with a life span of 8 days. Further results revealed that the probability of regional PM2.5 pollution related to the NAAA for at least 2 days in the NCP is 80% in NDJ period 2000–2021. Particularly, air quality in the NCP tends to deteriorate on day 2 prior to the peak day of the NAAA and reaches a peak on day −1 with a life cycle of 4 days. The corresponding meteorological conditions support these conclusions.
Jianbing Jin, Mijie Pang, Arjo Segers, Wei Han, Li Fang, Baojie Li, Haochuan Feng, Hai Xiang Lin, and Hong Liao
Atmos. Chem. Phys., 22, 6393–6410, https://doi.org/10.5194/acp-22-6393-2022, https://doi.org/10.5194/acp-22-6393-2022, 2022
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Super dust storms reappeared in East Asia last spring after being absent for one and a half decades. Accurate simulation of such super sandstorms is valuable, but challenging due to imperfect emissions. In this study, the emissions of these dust storms are estimated by assimilating multiple observations. The results reveal that emissions originated from both China and Mongolia. However, for northern China, long-distance transport from Mongolia contributes much more dust than Chinese deserts.
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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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