Articles | Volume 15, issue 14
https://doi.org/10.5194/acp-15-8217-2015
© Author(s) 2015. This work is distributed under
the Creative Commons Attribution 3.0 License.
the Creative Commons Attribution 3.0 License.
Special issue:
https://doi.org/10.5194/acp-15-8217-2015
© Author(s) 2015. This work is distributed under
the Creative Commons Attribution 3.0 License.
the Creative Commons Attribution 3.0 License.
Particulate matter, air quality and climate: lessons learned and future needs
Istituto di Scienze dell'Atmosfera e del Clima, Consiglio Nazionale delle Ricerche, Bologna, Italy
U. Baltensperger
Laboratory of Atmospheric Chemistry, Paul Scherrer Institute, Villigen, Switzerland
K. Carslaw
Institute for Climate and Atmospheric Science, School of Earth and Environment, University of Leeds, Leeds, UK
S. Decesari
Istituto di Scienze dell'Atmosfera e del Clima, Consiglio Nazionale delle Ricerche, Bologna, Italy
H. Denier van der Gon
TNO, Department of Climate, Air and Sustainability, Utrecht, the Netherlands
M. C. Facchini
Istituto di Scienze dell'Atmosfera e del Clima, Consiglio Nazionale delle Ricerche, Bologna, Italy
D. Fowler
Centre for Ecology and Hydrology, Edinburgh, UK
Department of Earth and Planetary Sciences, Weizmann Institute of Science, Rehovot, Israel
B. Langford
Centre for Ecology and Hydrology, Edinburgh, UK
U. Lohmann
ETH, Institute for Atmospheric and Climate Science, Zurich, Switzerland
E. Nemitz
Centre for Ecology and Hydrology, Edinburgh, UK
S. Pandis
Department of Chemical Engineering, University of Patras, Patras, Greece
I. Riipinen
Department of Applied Environmental Science, Stockholm University, Stockholm, Sweden
Y. Rudich
Department of Earth and Planetary Sciences, Weizmann Institute of Science, Rehovot, Israel
M. Schaap
TNO, Department of Climate, Air and Sustainability, Utrecht, the Netherlands
J. G. Slowik
Laboratory of Atmospheric Chemistry, Paul Scherrer Institute, Villigen, Switzerland
D. V. Spracklen
Institute for Climate and Atmospheric Science, School of Earth and Environment, University of Leeds, Leeds, UK
E. Vignati
European Commission, Joint Research Center, Institute for Environment and Sustainability, Ispra, Italy
ETH, Institute for Atmospheric and Climate Science, Zurich, Switzerland
M. Williams
Environmental Research Group, King's College London, London, UK
S. Gilardoni
Istituto di Scienze dell'Atmosfera e del Clima, Consiglio Nazionale delle Ricerche, Bologna, Italy
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This preprint is open for discussion and under review for Atmospheric Chemistry and Physics (ACP).
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This preprint is open for discussion and under review for Atmospheric Chemistry and Physics (ACP).
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EGUsphere, https://doi.org/10.5194/egusphere-2024-1989, https://doi.org/10.5194/egusphere-2024-1989, 2024
This preprint is open for discussion and under review for Atmospheric Chemistry and Physics (ACP).
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Atmos. Chem. Phys., 24, 8205–8223, https://doi.org/10.5194/acp-24-8205-2024, https://doi.org/10.5194/acp-24-8205-2024, 2024
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Revised manuscript under review for GMD
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Mark D. Tarn, Bethany V. Wyld, Naama Reicher, Matan Alayof, Daniella Gat, Alberto Sanchez-Marroquin, Sebastien N. F. Sikora, Alexander D. Harrison, Yinon Rudich, and Benjamin J. Murray
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Nadja Omanovic, Sylvaine Ferrachat, Christopher Fuchs, Jan Henneberger, Anna J. Miller, Kevin Ohneiser, Fabiola Ramelli, Patric Seifert, Robert Spirig, Huiying Zhang, and Ulrike Lohmann
Atmos. Chem. Phys., 24, 6825–6844, https://doi.org/10.5194/acp-24-6825-2024, https://doi.org/10.5194/acp-24-6825-2024, 2024
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We present simulations with a high-resolution numerical weather prediction model to study the growth of ice crystals in low clouds following glaciogenic seeding. We show that the simulated ice crystals grow slower than observed and do not consume as many cloud droplets as measured in the field. This may have implications for forecasting precipitation, as the ice phase is crucial for precipitation at middle and high latitudes.
Karam Mansour, Stefano Decesari, Darius Ceburnis, Jurgita Ovadnevaite, Lynn M. Russell, Marco Paglione, Laurent Poulain, Shan Huang, Colin O'Dowd, and Matteo Rinaldi
Earth Syst. Sci. Data, 16, 2717–2740, https://doi.org/10.5194/essd-16-2717-2024, https://doi.org/10.5194/essd-16-2717-2024, 2024
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We propose and evaluate machine learning predictive algorithms to model freshly formed biogenic methanesulfonic acid and sulfate concentrations. The long-term constructed dataset covers the North Atlantic at an unprecedented resolution. The improved parameterization of biogenic sulfur aerosols at regional scales is essential for determining their radiative forcing, which could help further understand marine-aerosol–cloud interactions and reduce uncertainties in climate models
Manuel Santos Gutiérrez, Mickaël David Chekroun, and Ilan Koren
EGUsphere, https://doi.org/https://doi.org/10.48550/arXiv.2405.11545, https://doi.org/https://doi.org/10.48550/arXiv.2405.11545, 2024
Preprint withdrawn
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Natalie Brett, Kathy S. Law, Steve R. Arnold, Javier G. Fochesatto, Jean-Christophe Raut, Tatsuo Onishi, Robert Gilliam, Kathleen Fahey, Deanna Huff, George Pouliot, Brice Barret, Elsa Dieudonne, Roman Pohorsky, Julia Schmale, Andrea Baccarini, Slimane Bekki, Gianluca Pappaccogli, Federico Scoto, Stefano Decesari, Antonio Donateo, Meeta Cesler-Maloney, William Simpson, Patrice Medina, Barbara D'Anna, Brice Temime-Roussel, Joel Savarino, Sarah Albertin, Jingqiu Mao, Becky Alexander, Allison Moon, Peter F. DeCarlo, Vanessa Selimovic, Robert Yokelson, and Ellis S. Robinson
EGUsphere, https://doi.org/10.5194/egusphere-2024-1450, https://doi.org/10.5194/egusphere-2024-1450, 2024
This preprint is open for discussion and under review for Atmospheric Chemistry and Physics (ACP).
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Processes influencing dispersion of local anthropogenic emissions in Arctic wintertime are investigated with dispersion model simulations. Modelled power plant plume rise that considers surface and elevated temperature inversions improves results compared to observations. Modelled near-surface concentrations are improved by representation of vertical mixing and emission estimates. Large increases in diesel vehicle emissions at temperatures reaching -35 °C are required to reproduce observed NOx.
Marco Paglione, David C. S. Beddows, Anna Jones, Thomas Lachlan-Cope, Matteo Rinaldi, Stefano Decesari, Francesco Manarini, Mara Russo, Karam Mansour, Roy M. Harrison, Andrea Mazzanti, Emilio Tagliavini, and Manuel Dall'Osto
Atmos. Chem. Phys., 24, 6305–6322, https://doi.org/10.5194/acp-24-6305-2024, https://doi.org/10.5194/acp-24-6305-2024, 2024
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Applying factor analysis techniques to H-NMR spectra, we present the organic aerosol (OA) source apportionment of PM1 samples collected in parallel at two Antarctic stations, namely Signy and Halley, allowing investigation of aerosol–climate interactions in an unperturbed atmosphere. Our results show remarkable differences between pelagic (open-ocean) and sympagic (sea-ice-influenced) air masses and indicate that various sources and processes are controlling Antarctic aerosols.
Ulrike Proske, Sylvaine Ferrachat, and Ulrike Lohmann
Atmos. Chem. Phys., 24, 5907–5933, https://doi.org/10.5194/acp-24-5907-2024, https://doi.org/10.5194/acp-24-5907-2024, 2024
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Climate models include treatment of aerosol particles because these influence clouds and radiation. Over time their representation has grown increasingly detailed. This complexity may hinder our understanding of model behaviour. Thus here we simplify the aerosol representation of our climate model by prescribing mean concentrations, which saves run time and helps to discover unexpected model behaviour. We conclude that simplifications provide a new perspective for model study and development.
Antonio Donateo, Daniela Famulari, Donato Giovannelli, Arturo Mariani, Mauro Mazzola, Stefano Decesari, and Gianluca Pappaccogli
EGUsphere, https://doi.org/10.5194/egusphere-2024-1440, https://doi.org/10.5194/egusphere-2024-1440, 2024
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This study focuses on direct measurements of CO2 and CH4 turbulent eddy covariance fluxes in tundra ecosystems in the Svalbard Islands over a two-year period. Our results reveal dynamic interactions between climatic conditions and ecosystem activities such as photosynthesis and microbial activity. The observed net summertime methane uptake is correlated with the activation and aeration of soil microorganisms. High temperature anomalies increase CO2 and CH4 emissions.
Erin N. Raif, Sarah L. Barr, Mark D. Tarn, James B. McQuaid, Martin I. Daily, Steven J. Abel, Paul A. Barrett, Keith N. Bower, Paul R. Field, Kenneth S. Carslaw, and Benjamin J. Murray
EGUsphere, https://doi.org/10.5194/egusphere-2024-1502, https://doi.org/10.5194/egusphere-2024-1502, 2024
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Ice-nucleating particles (INPs) allow ice to form in clouds at temperatures warmer than -35°C. We measured INP concentrations over the Norwegian and Barents seas in weather events where cold air is ejected from the Arctic. These concentrations were among the highest measured in the Arctic and it is likely that the INPs were transported to the Arctic from distant regions. These results show it is important to consider hemispheric-scale INP processes to understand INP concentrations in the Arctic.
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.
Andreas Aktypis, Dontavious Sippial, Christina Vasilakopoulou, Angeliki Matrali, Christos Kaltsonoudis, Andrea Simonati, Marco Paglione, Matteo Rinaldi, Stefano Decesari, and Spyros Pandis
EGUsphere, https://doi.org/10.5194/egusphere-2024-1317, https://doi.org/10.5194/egusphere-2024-1317, 2024
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A dual chamber system was deployed in two different environments (Po Valley, Italy and Pertouli forest, Greece) to study the potential of ambient air directly injected into the chambers, to form secondary aerosol. In the Po Valley, the system reacts rapidly forming large amounts of SOA, while in Pertouli the corresponding SOA formation chemistry appears to have been practically terminated before the beginning of most experiments, so there is little additional SOA formation potential left.
Zane Dedekind, Ulrike Proske, Sylvaine Ferrachat, Ulrike Lohmann, and David Neubauer
Atmos. Chem. Phys., 24, 5389–5404, https://doi.org/10.5194/acp-24-5389-2024, https://doi.org/10.5194/acp-24-5389-2024, 2024
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Ice particles precipitating into lower clouds from an upper cloud, the seeder–feeder process, can enhance precipitation. A numerical modeling study conducted in the Swiss Alps found that 48 % of observed clouds were overlapping, with the seeder–feeder process occurring in 10 % of these clouds. Inhibiting the seeder–feeder process reduced the surface precipitation and ice particle growth rates, which were further reduced when additional ice multiplication processes were included in the model.
Tiantian Wang, Jun Zhang, Houssni Lamkaddam, Kun Li, Ka Yuen Cheung, Lisa Kattner, Erlend Gammelsæter, Michael Bauer, Zachary C. J. Decker, Deepika Bhattu, Rujin Huang, Rob L. Modini, Jay G. Slowik, Imad El Haddad, Andre S. H. Prevot, and David M. Bell
EGUsphere, https://doi.org/10.5194/egusphere-2024-1161, https://doi.org/10.5194/egusphere-2024-1161, 2024
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Our study analyzes real-time emissions of primary organic gases from solid fuel combustion, including residential and open burning. Using Vocus-PTR-TOF, we tested various fuels, finding higher emissions from wood burning. Statistical tests identified unique characteristic compounds. IVOCs are key precursors to SOA formation, particularly in open burning. Our insights benefit air quality, climate, and health, advancing atmospheric chemistry and aiding accurate emission assessments.
Edward C. Chan, Ilona J. Jäkel, Basit Khan, Martijn Schaap, Timothy M. Butler, Renate Forkel, and Sabine Banzhaf
Geosci. Model Dev. Discuss., https://doi.org/10.5194/gmd-2024-61, https://doi.org/10.5194/gmd-2024-61, 2024
Revised manuscript under review for GMD
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An enhanced emission module has been developed for the PALM model system, allowing greater levels of flexibility and performance in modelling emission sources across different sectors. A model for parametrized domestic emissions has also been included, for which an idealized model run is conducted for PM10. The results show that, in addition to individual sources and diurnal variations in energy consumption, vertical transport and urban topology play a role in the PM concentration distribution.
Audrey Fortems-Cheiney, Gregoire Broquet, Elise Potier, Robin Plauchu, Antoine Berchet, Isabelle Pison, Hugo Denier van der Gon, and Stijn Dellaert
Atmos. Chem. Phys., 24, 4635–4649, https://doi.org/10.5194/acp-24-4635-2024, https://doi.org/10.5194/acp-24-4635-2024, 2024
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We have estimated the carbon monixide (CO) European emissions from satellite observations of the MOPITT instrument at the relatively high resolution of 0.5° for a period of over 10 years from 2011 to 2021. The analysis of the inversion results reveals the challenges associated with the inversion of CO emissions at the regional scale over Europe.
Ville-Veikko Paunu, Niko Karvosenoja, David Segersson, Susana López-Aparicio, Ole-Kenneth Nielsen, Marlene Schmidt Plejdrup, Throstur Thorsteinsson, Dam Thanh Vo, Jeroen Kuenen, Hugo Denier van der Gon, Jukka-Pekka Jalkanen, Jørgen Brandt, and Camilla Geels
Earth Syst. Sci. Data, 16, 1453–1474, https://doi.org/10.5194/essd-16-1453-2024, https://doi.org/10.5194/essd-16-1453-2024, 2024
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Air pollution is an important cause of adverse health effects, even in Nordic countries. To assess their health impacts, emission inventories with high spatial resolution are needed. We studied how national data and methods for the spatial distribution of the emissions compare to a European level inventory. For road transport the methods are well established, but for machinery and off-road emissions the current recommendations for the spatial distribution of these emissions should be improved.
Jing Cai, Juha Sulo, Yifang Gu, Sebastian Holm, Runlong Cai, Steven Thomas, Almuth Neuberger, Fredrik Mattsson, Marco Paglione, Stefano Decesari, Matteo Rinaldi, Rujing Yin, Diego Aliaga, Wei Huang, Yuanyuan Li, Yvette Gramlich, Giancarlo Ciarelli, Lauriane Quéléver, Nina Sarnela, Katrianne Lehtipalo, Nora Zannoni, Cheng Wu, Wei Nie, Juha Kangasluoma, Claudia Mohr, Markku Kulmala, Qiaozhi Zha, Dominik Stolzenburg, and Federico Bianchi
Atmos. Chem. Phys., 24, 2423–2441, https://doi.org/10.5194/acp-24-2423-2024, https://doi.org/10.5194/acp-24-2423-2024, 2024
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By combining field measurements, simulations and recent chamber experiments, we investigate new particle formation (NPF) and growth in the Po Valley, where both haze and frequent NPF occur. Our results show that sulfuric acid, ammonia and amines are the dominant NPF precursors there. A high NPF rate and a lower condensation sink lead to a greater survival probability for newly formed particles, highlighting the importance of gas-to-particle conversion for aerosol concentrations.
Weijun Quan, Zhenfa Wang, Lin Qiao, Xiangdong Zheng, Junli Jin, Yinruo Li, Xiaomei Yin, Zhiqiang Ma, and Martin Wild
Earth Syst. Sci. Data, 16, 961–983, https://doi.org/10.5194/essd-16-961-2024, https://doi.org/10.5194/essd-16-961-2024, 2024
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Radiation components play important roles in various fields such as the Earth’s surface radiation budget, ecosystem productivity, and human health. In this study, a dataset consisting of quality-assured daily data of nine radiation components is presented based on the in situ measurements at the Shangdianzi regional GAW station in China during 2013–2022. The dataset can be applied in the validation of satellite products and numerical models and investigation of atmospheric radiation.
Xinyue Shao, Minghuai Wang, Xinyi Dong, Yaman Liu, Wenxiang Shen, Stephen Arnold, Leighton Regayre, Meinrat Andreae, Mira Pöhlker, Duseong Jo, Man Yue, and Ken Carslaw
EGUsphere, https://doi.org/10.5194/egusphere-2024-401, https://doi.org/10.5194/egusphere-2024-401, 2024
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Highly oxygenated organic molecules (HOMs) play an important role in atmospheric new particle formation (NPF). By explicitly coupling the chemical mechanism of HOMs and a comprehensive nucleation scheme in a global climate model. The updated model shows better agreement with measurements of nucleation rate, growth rate, NPF event frequency. Our results reveal that HOMs-driven NPF leads to a considerable increase in particle and cloud condensation nuclei burden globally.
Alexandros Milousis, Alexandra P. Tsimpidi, Holger Tost, Spyros N. Pandis, Athanasios Nenes, Astrid Kiendler-Scharr, and Vlassis A. Karydis
Geosci. Model Dev., 17, 1111–1131, https://doi.org/10.5194/gmd-17-1111-2024, https://doi.org/10.5194/gmd-17-1111-2024, 2024
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This study aims to evaluate the newly developed ISORROPIA-lite aerosol thermodynamic module within the EMAC model and explore discrepancies in global atmospheric simulations of aerosol composition and acidity by utilizing different aerosol phase states. Even though local differences were found in regions where the RH ranged from 20 % to 60 %, on a global scale the results are similar. Therefore, ISORROPIA-lite can be a reliable and computationally effective alternative to ISORROPIA II in EMAC.
Anna J. Miller, Fabiola Ramelli, Christopher Fuchs, Nadja Omanovic, Robert Spirig, Huiying Zhang, Ulrike Lohmann, Zamin A. Kanji, and Jan Henneberger
Atmos. Meas. Tech., 17, 601–625, https://doi.org/10.5194/amt-17-601-2024, https://doi.org/10.5194/amt-17-601-2024, 2024
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We present a method for aerosol and cloud research using two uncrewed aerial vehicles (UAVs). The UAVs have a propeller heating mechanism that allows flights in icing conditions, which has so far been a limitation for cloud research with UAVs. One UAV burns seeding flares, producing a plume of particles that causes ice formation in supercooled clouds. The second UAV measures aerosol size distributions and is used for measuring the seeding plume or for characterizing the boundary layer.
Ruben Urraca, Greet Janssens-Maenhout, Nicolás Álamos, Lucas Berna-Peña, Monica Crippa, Sabine Darras, Stijn Dellaert, Hugo Denier van der Gon, Mark Dowell, Nadine Gobron, Claire Granier, Giacomo Grassi, Marc Guevara, Diego Guizzardi, Kevin Gurney, Nicolás Huneeus, Sekou Keita, Jeroen Kuenen, Ana Lopez-Noreña, Enrique Puliafito, Geoffrey Roest, Simone Rossi, Antonin Soulie, and Antoon Visschedijk
Earth Syst. Sci. Data, 16, 501–523, https://doi.org/10.5194/essd-16-501-2024, https://doi.org/10.5194/essd-16-501-2024, 2024
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CoCO2-MOSAIC 1.0 is a global mosaic of regional bottom-up inventories providing gridded (0.1×0.1) monthly emissions of anthropogenic CO2. Regional inventories include country-specific information and finer spatial resolution than global inventories. CoCO2-MOSAIC provides harmonized access to these datasets and can be considered as a regionally accepted reference to assess the quality of global inventories, as done in the current paper.
Stella E. I. Manavi and Spyros N. Pandis
Atmos. Chem. Phys., 24, 891–909, https://doi.org/10.5194/acp-24-891-2024, https://doi.org/10.5194/acp-24-891-2024, 2024
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Organic vapors of intermediate volatility have often been neglected as sources of atmospheric organic aerosol. In this work we use a new approach for their simulation and quantify the contribution of these compounds emitted by transportation sources (gasoline and diesel vehicles) to particulate matter over Europe. The estimated secondary organic aerosol levels are on average 60 % higher than predicted by previous approaches. However, these estimates are probably lower limits.
Marc Guevara, Santiago Enciso, Carles Tena, Oriol Jorba, Stijn Dellaert, Hugo Denier van der Gon, and Carlos Pérez García-Pando
Earth Syst. Sci. Data, 16, 337–373, https://doi.org/10.5194/essd-16-337-2024, https://doi.org/10.5194/essd-16-337-2024, 2024
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A global dataset of emissions from thermal power plants was created for the year 2018. The resulting catalogue reports annual emissions of CO2 and co-emitted species (NOx, CO, SO2 and CH4) for more than 16000 individual facilities at their exact geographical locations. Information on the temporal and vertical distributions of the emissions is also provided at the facility level. The dataset is intended to support current and future satellite emission monitoring and inverse modelling efforts.
Andreas Aktypis, Christos Kaltsonoudis, David Patoulias, Panayiotis Kalkavouras, Angeliki Matrali, Christina N. Vasilakopoulou, Evangelia Kostenidou, Kalliopi Florou, Nikos Kalivitis, Aikaterini Bougiatioti, Konstantinos Eleftheriadis, Stergios Vratolis, Maria I. Gini, Athanasios Kouras, Constantini Samara, Mihalis Lazaridis, Sofia-Eirini Chatoutsidou, Nikolaos Mihalopoulos, and Spyros N. Pandis
Atmos. Chem. Phys., 24, 65–84, https://doi.org/10.5194/acp-24-65-2024, https://doi.org/10.5194/acp-24-65-2024, 2024
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Extensive continuous particle number size distribution measurements took place during two summers (2020 and 2021) at 11 sites in Greece for the investigation of the frequency and the spatial extent of new particle formation. The frequency during summer varied from close to zero in southwestern Greece to more than 60 % in the northern, central, and eastern regions. The spatial variability can be explained by the proximity of the sites to coal-fired power plants and agricultural areas.
Stefania Gilardoni, Dominic Heslin-Rees, Mauro Mazzola, Vito Vitale, Michael Sprenger, and Radovan Krejci
Atmos. Chem. Phys., 23, 15589–15607, https://doi.org/10.5194/acp-23-15589-2023, https://doi.org/10.5194/acp-23-15589-2023, 2023
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Models still fail in reproducing black carbon (BC) temporal variability in the Arctic. Analysis of equivalent BC concentrations in the European Arctic shows that BC seasonal variability is modulated by the efficiency of removal by precipitation during transport towards high latitudes. Short-term variability is controlled by synoptic-scale circulation patterns. The advection of warm air from lower latitudes is an effective pollution transport pathway during summer.
Rolf Müller, Ulrich Pöschl, Thomas Koop, Thomas Peter, and Ken Carslaw
Atmos. Chem. Phys., 23, 15445–15453, https://doi.org/10.5194/acp-23-15445-2023, https://doi.org/10.5194/acp-23-15445-2023, 2023
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Paul J. Crutzen was a pioneer in atmospheric sciences and a kind-hearted, humorous person with empathy for the private lives of his colleagues and students. He made fundamental scientific contributions to a wide range of scientific topics in all parts of the atmosphere. Paul was among the founders of the journal Atmospheric Chemistry and Physics. His work will continue to be a guide for generations of scientists and environmental policymakers to come.
Hamza Ahsan, Hailong Wang, Jingbo Wu, Mingxuan Wu, Steven J. Smith, Susanne Bauer, Harrison Suchyta, Dirk Olivié, Gunnar Myhre, Hitoshi Matsui, Huisheng Bian, Jean-François Lamarque, Ken Carslaw, Larry Horowitz, Leighton Regayre, Mian Chin, Michael Schulz, Ragnhild Bieltvedt Skeie, Toshihiko Takemura, and Vaishali Naik
Atmos. Chem. Phys., 23, 14779–14799, https://doi.org/10.5194/acp-23-14779-2023, https://doi.org/10.5194/acp-23-14779-2023, 2023
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We examine the impact of the assumed effective height of SO2 injection, SO2 and BC emission seasonality, and the assumed fraction of SO2 emissions injected as SO4 on climate and chemistry model results. We find that the SO2 injection height has a large impact on surface SO2 concentrations and, in some models, radiative flux. These assumptions are a
hiddensource of inter-model variability and may be leading to bias in some climate model results.
Jun Zhang, Kun Li, Tiantian Wang, Erlend Gammelsæter, Rico K. Y. Cheung, Mihnea Surdu, Sophie Bogler, Deepika Bhattu, Dongyu S. Wang, Tianqu Cui, Lu Qi, Houssni Lamkaddam, Imad El Haddad, Jay G. Slowik, Andre S. H. Prevot, and David M. Bell
Atmos. Chem. Phys., 23, 14561–14576, https://doi.org/10.5194/acp-23-14561-2023, https://doi.org/10.5194/acp-23-14561-2023, 2023
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We conducted burning experiments to simulate various types of solid fuel combustion, including residential burning, wildfires, agricultural burning, cow dung, and plastic bag burning. The chemical composition of the particles was characterized using mass spectrometers, and new potential markers for different fuels were identified using statistical analysis. This work improves our understanding of emissions from solid fuel burning and offers support for refined source apportionment.
Hossein Maazallahi, Antonio Delre, Charlotte Scheutz, Anders M. Fredenslund, Stefan Schwietzke, Hugo Denier van der Gon, and Thomas Röckmann
Atmos. Meas. Tech., 16, 5051–5073, https://doi.org/10.5194/amt-16-5051-2023, https://doi.org/10.5194/amt-16-5051-2023, 2023
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Measurement methods are increasingly deployed to verify reported methane emissions of gas leaks. This study describes unique advantages and limitations of three methods. Two methods are rapidly deployed, but uncertainties and biases exist for some leak locations. In contrast, the suction method could accurately determine leak rates in principle. However, this method, which provides data for the German emission inventory, creates an overall low bias in our study due to non-random site selection.
Stylianos Kakavas, Spyros N. Pandis, and Athanasios Nenes
Atmos. Chem. Phys., 23, 13555–13564, https://doi.org/10.5194/acp-23-13555-2023, https://doi.org/10.5194/acp-23-13555-2023, 2023
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Water uptake from organic species in aerosol can affect the partitioning of semi-volatile inorganic compounds but are not considered in global and chemical transport models. We address this with a version of the PM-CAMx model that considers such organic water effects and use it to carry out 1-year aerosol simulations over the continental US. We show that such organic water impacts can increase dry PM1 levels by up to 2 μg m-3 when RH levels and PM1 concentrations are high.
Boyang Jiao, Yucheng Su, Qingxiang Li, Veronica Manara, and Martin Wild
Earth Syst. Sci. Data, 15, 4519–4535, https://doi.org/10.5194/essd-15-4519-2023, https://doi.org/10.5194/essd-15-4519-2023, 2023
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This paper develops an observational integrated and homogenized global-terrestrial (except for Antarctica) SSRIH station. This is interpolated into a 5° × 5° SSRIH grid and reconstructed into a long-term (1955–2018) global land (except for Antarctica) 5° × 2.5° SSR anomaly dataset (SSRIH20CR) by an improved partial convolutional neural network deep-learning method. SSRIH20CR yields trends of −1.276 W m−2 per decade over the dimming period and 0.697 W m−2 per decade over the brightening period.
Matthew J. McGrath, Ana Maria Roxana Petrescu, Philippe Peylin, Robbie M. Andrew, Bradley Matthews, Frank Dentener, Juraj Balkovič, Vladislav Bastrikov, Meike Becker, Gregoire Broquet, Philippe Ciais, Audrey Fortems-Cheiney, Raphael Ganzenmüller, Giacomo Grassi, Ian Harris, Matthew Jones, Jürgen Knauer, Matthias Kuhnert, Guillaume Monteil, Saqr Munassar, Paul I. Palmer, Glen P. Peters, Chunjing Qiu, Mart-Jan Schelhaas, Oksana Tarasova, Matteo Vizzarri, Karina Winkler, Gianpaolo Balsamo, Antoine Berchet, Peter Briggs, Patrick Brockmann, Frédéric Chevallier, Giulia Conchedda, Monica Crippa, Stijn N. C. Dellaert, Hugo A. C. Denier van der Gon, Sara Filipek, Pierre Friedlingstein, Richard Fuchs, Michael Gauss, Christoph Gerbig, Diego Guizzardi, Dirk Günther, Richard A. Houghton, Greet Janssens-Maenhout, Ronny Lauerwald, Bas Lerink, Ingrid T. Luijkx, Géraud Moulas, Marilena Muntean, Gert-Jan Nabuurs, Aurélie Paquirissamy, Lucia Perugini, Wouter Peters, Roberto Pilli, Julia Pongratz, Pierre Regnier, Marko Scholze, Yusuf Serengil, Pete Smith, Efisio Solazzo, Rona L. Thompson, Francesco N. Tubiello, Timo Vesala, and Sophia Walther
Earth Syst. Sci. Data, 15, 4295–4370, https://doi.org/10.5194/essd-15-4295-2023, https://doi.org/10.5194/essd-15-4295-2023, 2023
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Accurate estimation of fluxes of carbon dioxide from the land surface is essential for understanding future impacts of greenhouse gas emissions on the climate system. A wide variety of methods currently exist to estimate these sources and sinks. We are continuing work to develop annual comparisons of these diverse methods in order to clarify what they all actually calculate and to resolve apparent disagreement, in addition to highlighting opportunities for increased understanding.
Guangyu Li, Elise K. Wilbourn, Zezhen Cheng, Jörg Wieder, Allison Fagerson, Jan Henneberger, Ghislain Motos, Rita Traversi, Sarah D. Brooks, Mauro Mazzola, Swarup China, Athanasios Nenes, Ulrike Lohmann, Naruki Hiranuma, and Zamin A. Kanji
Atmos. Chem. Phys., 23, 10489–10516, https://doi.org/10.5194/acp-23-10489-2023, https://doi.org/10.5194/acp-23-10489-2023, 2023
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In this work, we present results from an Arctic field campaign (NASCENT) in Ny-Ålesund, Svalbard, on the abundance, variability, physicochemical properties, and potential sources of ice-nucleating particles (INPs) relevant for mixed-phase cloud formation. This work improves the data coverage of Arctic INPs and aerosol properties, allowing for the validation of models predicting cloud microphysical and radiative properties of mixed-phase clouds in the rapidly warming Arctic.
Foteini Stavropoulou, Katarina Vinković, Bert Kers, Marcel de Vries, Steven van Heuven, Piotr Korbeń, Martina Schmidt, Julia Wietzel, Pawel Jagoda, Jaroslav M. Necki, Jakub Bartyzel, Hossein Maazallahi, Malika Menoud, Carina van der Veen, Sylvia Walter, Béla Tuzson, Jonas Ravelid, Randulph Paulo Morales, Lukas Emmenegger, Dominik Brunner, Michael Steiner, Arjan Hensen, Ilona Velzeboer, Pim van den Bulk, Hugo Denier van der Gon, Antonio Delre, Maklawe Essonanawe Edjabou, Charlotte Scheutz, Marius Corbu, Sebastian Iancu, Denisa Moaca, Alin Scarlat, Alexandru Tudor, Ioana Vizireanu, Andreea Calcan, Magdalena Ardelean, Sorin Ghemulet, Alexandru Pana, Aurel Constantinescu, Lucian Cusa, Alexandru Nica, Calin Baciu, Cristian Pop, Andrei Radovici, Alexandru Mereuta, Horatiu Stefanie, Alexandru Dandocsi, Bas Hermans, Stefan Schwietzke, Daniel Zavala-Araiza, Huilin Chen, and Thomas Röckmann
Atmos. Chem. Phys., 23, 10399–10412, https://doi.org/10.5194/acp-23-10399-2023, https://doi.org/10.5194/acp-23-10399-2023, 2023
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In this study, we quantify CH4 emissions from onshore oil production sites in Romania at source and facility level using a combination of ground- and drone-based measurement techniques. We show that the total CH4 emissions in our studied areas are much higher than the emissions reported to UNFCCC, and up to three-quarters of the detected emissions are related to operational venting. Our results suggest that oil and gas production infrastructure in Romania holds a massive mitigation potential.
Jean-Philippe Putaud, Enrico Pisoni, Alexander Mangold, Christoph Hueglin, Jean Sciare, Michael Pikridas, Chrysanthos Savvides, Jakub Ondracek, Saliou Mbengue, Alfred Wiedensohler, Kay Weinhold, Maik Merkel, Laurent Poulain, Dominik van Pinxteren, Hartmut Herrmann, Andreas Massling, Claus Nordstroem, Andrés Alastuey, Cristina Reche, Noemí Pérez, Sonia Castillo, Mar Sorribas, Jose Antonio Adame, Tuukka Petaja, Katrianne Lehtipalo, Jarkko Niemi, Véronique Riffault, Joel F. de Brito, Augustin Colette, Olivier Favez, Jean-Eudes Petit, Valérie Gros, Maria I. Gini, Stergios Vratolis, Konstantinos Eleftheriadis, Evangelia Diapouli, Hugo Denier van der Gon, Karl Espen Yttri, and Wenche Aas
Atmos. Chem. Phys., 23, 10145–10161, https://doi.org/10.5194/acp-23-10145-2023, https://doi.org/10.5194/acp-23-10145-2023, 2023
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Many European people are still exposed to levels of air pollution that can affect their health. COVID-19 lockdowns in 2020 were used to assess the impact of the reduction in human mobility on air pollution across Europe by comparing measurement data with values that would be expected if no lockdown had occurred. We show that lockdown measures did not lead to consistent decreases in the concentrations of fine particulate matter suspended in the air, and we investigate why.
Bernhard M. Enz, Jan P. Engelmann, and Ulrike Lohmann
Geosci. Model Dev., 16, 5093–5112, https://doi.org/10.5194/gmd-16-5093-2023, https://doi.org/10.5194/gmd-16-5093-2023, 2023
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An algorithm to track tropical cyclones in model simulation data has been developed. The algorithm uses many combinations of varying parameter thresholds to detect weaker phases of tropical cyclones while still being resilient to false positives. It is shown that the algorithm performs well and adequately represents the tropical cyclone activity of the underlying simulation data. The impact of false positives on overall tropical cyclone activity is shown to be insignificant.
Yong Zhang, Jie Tian, Qiyuan Wang, Lu Qi, Manousos Ioannis Manousakas, Yuemei Han, Weikang Ran, Yele Sun, Huikun Liu, Renjian Zhang, Yunfei Wu, Tianqu Cui, Kaspar Rudolf Daellenbach, Jay Gates Slowik, André S. H. Prévôt, and Junji Cao
Atmos. Chem. Phys., 23, 9455–9471, https://doi.org/10.5194/acp-23-9455-2023, https://doi.org/10.5194/acp-23-9455-2023, 2023
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PM2.5 pollution still frequently occurs in northern China during winter, and it is necessary to figure out the causes of air pollution based on intensive real-time measurement. The findings elaborate the chemical characteristics and source contributions of PM2.5 in three pilot cities, reveal potential formation mechanisms of secondary aerosols, and highlight the importance of controlling biomass burning and inhibiting generation of secondary aerosol for air quality improvement.
Gijs Leguijt, Joannes D. Maasakkers, Hugo A. C. Denier van der Gon, Arjo J. Segers, Tobias Borsdorff, and Ilse Aben
Atmos. Chem. Phys., 23, 8899–8919, https://doi.org/10.5194/acp-23-8899-2023, https://doi.org/10.5194/acp-23-8899-2023, 2023
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We present a fast method to evaluate carbon monoxide emissions from cities in Africa. Carbon monoxide is important for climate change in an indirect way, as it is linked to ozone, methane, and carbon dioxide. Our measurements are made with a satellite that sees the entire globe every single day. This means that we can check from space whether the current knowledge of emission rates is up to date. We make the comparison and show that the emission rates in northern Africa are underestimated.
Sophie L. Haslett, David M. Bell, Varun Kumar, Jay G. Slowik, Dongyu S. Wang, Suneeti Mishra, Neeraj Rastogi, Atinderpal Singh, Dilip Ganguly, Joel Thornton, Feixue Zheng, Yuanyuan Li, Wei Nie, Yongchun Liu, Wei Ma, Chao Yan, Markku Kulmala, Kaspar R. Daellenbach, David Hadden, Urs Baltensperger, Andre S. H. Prevot, Sachchida N. Tripathi, and Claudia Mohr
Atmos. Chem. Phys., 23, 9023–9036, https://doi.org/10.5194/acp-23-9023-2023, https://doi.org/10.5194/acp-23-9023-2023, 2023
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In Delhi, some aspects of daytime and nighttime atmospheric chemistry are inverted, and parodoxically, vehicle emissions may be limiting other forms of particle production. This is because the nighttime emissions of nitrogen oxide (NO) by traffic and biomass burning prevent some chemical processes that would otherwise create even more particles and worsen the urban haze.
Jinghui Lian, Thomas Lauvaux, Hervé Utard, François-Marie Bréon, Grégoire Broquet, Michel Ramonet, Olivier Laurent, Ivonne Albarus, Mali Chariot, Simone Kotthaus, Martial Haeffelin, Olivier Sanchez, Olivier Perrussel, Hugo Anne Denier van der Gon, Stijn Nicolaas Camiel Dellaert, and Philippe Ciais
Atmos. Chem. Phys., 23, 8823–8835, https://doi.org/10.5194/acp-23-8823-2023, https://doi.org/10.5194/acp-23-8823-2023, 2023
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This study quantifies urban CO2 emissions via an atmospheric inversion for the Paris metropolitan area over a 6-year period from 2016 to 2021. Results show a long-term decreasing trend of about 2 % ± 0.6 % per year in the annual CO2 emissions over Paris. We conclude that our current capacity can deliver near-real-time CO2 emission estimates at the city scale in under a month, and the results agree within 10 % with independent estimates from multiple city-scale inventories.
Leighton A. Regayre, Lucia Deaconu, Daniel P. Grosvenor, David M. H. Sexton, Christopher Symonds, Tom Langton, Duncan Watson-Paris, Jane P. Mulcahy, Kirsty J. Pringle, Mark Richardson, Jill S. Johnson, John W. Rostron, Hamish Gordon, Grenville Lister, Philip Stier, and Ken S. Carslaw
Atmos. Chem. Phys., 23, 8749–8768, https://doi.org/10.5194/acp-23-8749-2023, https://doi.org/10.5194/acp-23-8749-2023, 2023
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Aerosol forcing of Earth’s energy balance has persisted as a major cause of uncertainty in climate simulations over generations of climate model development. We show that structural deficiencies in a climate model are exposed by comprehensively exploring parametric uncertainty and that these deficiencies limit how much the model uncertainty can be reduced through observational constraint. This provides a future pathway towards building models with greater physical realism and lower uncertainty.
Marc Guevara, Hervé Petetin, Oriol Jorba, Hugo Denier van der Gon, Jeroen Kuenen, Ingrid Super, Claire Granier, Thierno Doumbia, Philippe Ciais, Zhu Liu, Robin D. Lamboll, Sabine Schindlbacher, Bradley Matthews, and Carlos Pérez García-Pando
Atmos. Chem. Phys., 23, 8081–8101, https://doi.org/10.5194/acp-23-8081-2023, https://doi.org/10.5194/acp-23-8081-2023, 2023
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This study provides an intercomparison of European 2020 emission changes derived from official inventories, which are reported by countries under the framework of several international conventions and directives, and non-official near-real-time estimates, the use of which has significantly grown since the COVID-19 outbreak. The results of the work are used to produce recommendations on how best to approach and make use of near-real-time emissions for modelling and monitoring applications.
Imad El Haddad, Kaspar Daellenbach, Robin Modini, Jay Slowik, Abhishek Upadhyay, David Bell, Danielle Vienneau, Kees De Hoogh, and Andre S. H. Prevot
EGUsphere, https://doi.org/10.5194/egusphere-2023-1472, https://doi.org/10.5194/egusphere-2023-1472, 2023
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This opinion paper explores how advances in aerosol science inform our understanding of the health impacts of outdoor particulate pollution. We advocate for a shift in the way we target PM pollution, focusing the most harmful anthropogenic emissions, while exempting uncontrollable or non-detrimental components. We highlight key observations and modelling developments needed to achieve this shift.
Colin Tully, David Neubauer, Diego Villanueva, and Ulrike Lohmann
Atmos. Chem. Phys., 23, 7673–7698, https://doi.org/10.5194/acp-23-7673-2023, https://doi.org/10.5194/acp-23-7673-2023, 2023
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This study details the first attempt with a GCM to simulate a fully prognostic aerosol species specifically for cirrus climate intervention. The new approach is in line with the real-world delivery mechanism via aircraft. However, to achieve an appreciable signal from seeding, smaller particles were needed, and their mass emissions needed to be scaled by at least a factor of 100. These biases contributed to either overseeding or small and insignificant effects in response to seeding cirrus.
Amir Yazdani, Satoshi Takahama, John K. Kodros, Marco Paglione, Mauro Masiol, Stefania Squizzato, Kalliopi Florou, Christos Kaltsonoudis, Spiro D. Jorga, Spyros N. Pandis, and Athanasios Nenes
Atmos. Chem. Phys., 23, 7461–7477, https://doi.org/10.5194/acp-23-7461-2023, https://doi.org/10.5194/acp-23-7461-2023, 2023
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Organic aerosols directly emitted from wood and pellet stove combustion are found to chemically transform (approximately 15 %–35 % by mass) under daytime aging conditions simulated in an environmental chamber. A new marker for lignin-like compounds is found to degrade at a different rate than previously identified biomass burning markers and can potentially provide indication of aging time in ambient samples.
Antonio Donateo, Gianluca Pappaccogli, Daniela Famulari, Mauro Mazzola, Federico Scoto, and Stefano Decesari
Atmos. Chem. Phys., 23, 7425–7445, https://doi.org/10.5194/acp-23-7425-2023, https://doi.org/10.5194/acp-23-7425-2023, 2023
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This work aims to measure the turbulent fluxes and the dry deposition velocity for size-segregated particles (from ultrafine to quasi-coarse range) at an Arctic site (Svalbard). Aiming to characterize the effect of surface properties on dry deposition, continuous observations were performed from the coldest months (on snow surface) to the snow melting period and throughout the summer (snow-free surface). A data fit of the deposition velocity as a function of particle diameters will be provided.
Emelie L. Graham, Cheng Wu, David M. Bell, Amelie Bertrand, Sophie L. Haslett, Urs Baltensperger, Imad El Haddad, Radovan Krejci, Ilona Riipinen, and Claudia Mohr
Atmos. Chem. Phys., 23, 7347–7362, https://doi.org/10.5194/acp-23-7347-2023, https://doi.org/10.5194/acp-23-7347-2023, 2023
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The volatility of an aerosol particle is an important parameter for describing its atmospheric lifetime. We studied the volatility of secondary organic aerosols from nitrate-initiated oxidation of three biogenic precursors with experimental methods and model simulations. We saw higher volatility than for the corresponding ozone system, and our simulations produced variable results with different parameterizations which warrant a re-evaluation of the treatment of the nitrate functional group.
Petro Uruci, Dontavious Sippial, Anthoula Drosatou, and Spyros N. Pandis
Atmos. Meas. Tech., 16, 3155–3172, https://doi.org/10.5194/amt-16-3155-2023, https://doi.org/10.5194/amt-16-3155-2023, 2023
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In this work we develop an algorithm for the synthesis of the measurements performed in atmospheric simulation chambers regarding the formation of secondary organic aerosol (SOA). Novel features of the algorithm are its ability to use measurements of SOA yields, thermodenuders, and isothermal dilution; its estimation of parameters that can be used directly in atmospheric chemical transport models; and finally its estimates of the uncertainty in SOA formation yields.
Andreas Forstmaier, Jia Chen, Florian Dietrich, Juan Bettinelli, Hossein Maazallahi, Carsten Schneider, Dominik Winkler, Xinxu Zhao, Taylor Jones, Carina van der Veen, Norman Wildmann, Moritz Makowski, Aydin Uzun, Friedrich Klappenbach, Hugo Denier van der Gon, Stefan Schwietzke, and Thomas Röckmann
Atmos. Chem. Phys., 23, 6897–6922, https://doi.org/10.5194/acp-23-6897-2023, https://doi.org/10.5194/acp-23-6897-2023, 2023
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Large cities emit greenhouse gases which contribute to global warming. In this study, we measured the release of one important green house gas, methane, in Hamburg. Multiple sources that contribute to methane emissions were located and quantified. Methane sources were found to be mainly caused by human activity (e.g., by release from oil and gas refineries). Moreover, potential natural sources have been located, such as the Elbe River and lakes.
Daniel P. Grosvenor and Kenneth S. Carslaw
Atmos. Chem. Phys., 23, 6743–6773, https://doi.org/10.5194/acp-23-6743-2023, https://doi.org/10.5194/acp-23-6743-2023, 2023
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We determine what causes long-term trends in short-wave (SW) radiative fluxes in two climate models. A positive trend occurs between 1850 and 1970 (increasing SW reflection) and a negative trend between 1970 and 2014; the pre-1970 positive trend is mainly driven by an increase in cloud droplet number concentrations due to increases in aerosol, and the 1970–2014 trend is driven by a decrease in cloud fraction, which we attribute to changes in clouds caused by greenhouse gas-induced warming.
Lucía Caudillo, Mihnea Surdu, Brandon Lopez, Mingyi Wang, Markus Thoma, Steffen Bräkling, Angela Buchholz, Mario Simon, Andrea C. Wagner, Tatjana Müller, Manuel Granzin, Martin Heinritzi, Antonio Amorim, David M. Bell, Zoé Brasseur, Lubna Dada, Jonathan Duplissy, Henning Finkenzeller, Xu-Cheng He, Houssni Lamkaddam, Naser G. A. Mahfouz, Vladimir Makhmutov, Hanna E. Manninen, Guillaume Marie, Ruby Marten, Roy L. Mauldin, Bernhard Mentler, Antti Onnela, Tuukka Petäjä, Joschka Pfeifer, Maxim Philippov, Ana A. Piedehierro, Birte Rörup, Wiebke Scholz, Jiali Shen, Dominik Stolzenburg, Christian Tauber, Ping Tian, António Tomé, Nsikanabasi Silas Umo, Dongyu S. Wang, Yonghong Wang, Stefan K. Weber, André Welti, Marcel Zauner-Wieczorek, Urs Baltensperger, Richard C. Flagan, Armin Hansel, Jasper Kirkby, Markku Kulmala, Katrianne Lehtipalo, Douglas R. Worsnop, Imad El Haddad, Neil M. Donahue, Alexander L. Vogel, Andreas Kürten, and Joachim Curtius
Atmos. Chem. Phys., 23, 6613–6631, https://doi.org/10.5194/acp-23-6613-2023, https://doi.org/10.5194/acp-23-6613-2023, 2023
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In this study, we present an intercomparison of four different techniques for measuring the chemical composition of nanoparticles. The intercomparison was performed based on the observed chemical composition, calculated volatility, and analysis of the thermograms. We found that the methods generally agree on the most important compounds that are found in the nanoparticles. However, they do see different parts of the organic spectrum. We suggest potential explanations for these differences.
Huan Liu, Ilan Koren, Orit Altaratz, and Mickaël D. Chekroun
Atmos. Chem. Phys., 23, 6559–6569, https://doi.org/10.5194/acp-23-6559-2023, https://doi.org/10.5194/acp-23-6559-2023, 2023
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Clouds' responses to global warming contribute the largest uncertainty in climate prediction. Here, we analyze 42 years of global cloud cover in reanalysis data and show a decreasing trend over most continents and an increasing trend over the tropical and subtropical oceans. A reduction in near-surface relative humidity can explain the decreasing trend in cloud cover over land. Our results suggest potential stress on the terrestrial water cycle, associated with global warming.
Christina N. Vasilakopoulou, Kalliopi Florou, Christos Kaltsonoudis, Iasonas Stavroulas, Nikolaos Mihalopoulos, and Spyros N. Pandis
Atmos. Meas. Tech., 16, 2837–2850, https://doi.org/10.5194/amt-16-2837-2023, https://doi.org/10.5194/amt-16-2837-2023, 2023
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The offline aerosol mass spectrometry technique is a useful tool for the source apportionment of organic aerosol in areas and periods during which an aerosol mass spectrometer is not available. In this work, an improved offline technique was developed and evaluated in an effort to capture most of the partially soluble and insoluble organic aerosol material, reducing the uncertainty of the corresponding source apportionment significantly.
Colin Tully, David Neubauer, and Ulrike Lohmann
Geosci. Model Dev., 16, 2957–2973, https://doi.org/10.5194/gmd-16-2957-2023, https://doi.org/10.5194/gmd-16-2957-2023, 2023
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A new method to simulate deterministic ice nucleation processes based on the differential activated fraction was evaluated against a cumulative approach. Box model simulations of heterogeneous-only ice nucleation within cirrus suggest that the latter approach likely underpredicts the ice crystal number concentration. Longer simulations with a GCM show that choosing between these two approaches impacts ice nucleation competition within cirrus but leads to small and insignificant climate effects.
Ernesto Reyes-Villegas, Douglas Lowe, Jill S. Johnson, Kenneth S. Carslaw, Eoghan Darbyshire, Michael Flynn, James D. Allan, Hugh Coe, Ying Chen, Oliver Wild, Scott Archer-Nicholls, Alex Archibald, Siddhartha Singh, Manish Shrivastava, Rahul A. Zaveri, Vikas Singh, Gufran Beig, Ranjeet Sokhi, and Gordon McFiggans
Atmos. Chem. Phys., 23, 5763–5782, https://doi.org/10.5194/acp-23-5763-2023, https://doi.org/10.5194/acp-23-5763-2023, 2023
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Organic aerosols (OAs), their sources and their processes remain poorly understood. The volatility basis set (VBS) approach, implemented in air quality models such as WRF-Chem, can be a useful tool to describe primary OA (POA) production and aging. However, the main disadvantage is its complexity. We used a Gaussian process simulator to reproduce model results and to estimate the sources of model uncertainty. We do this by comparing the outputs with OA observations made at Delhi, India, in 2018.
Xuemei Wang, Hamish Gordon, Daniel P. Grosvenor, Meinrat O. Andreae, and Ken S. Carslaw
Atmos. Chem. Phys., 23, 4431–4461, https://doi.org/10.5194/acp-23-4431-2023, https://doi.org/10.5194/acp-23-4431-2023, 2023
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New particle formation in the upper troposphere is important for the global boundary layer aerosol population, and they can be transported downward in Amazonia. We use a global and a regional model to quantify the number of aerosols that are formed at high altitude and transported downward in a 1000 km region. We find that the majority of the aerosols are from outside the region. This suggests that the 1000 km region is unlikely to be a
closed loopfor aerosol formation, transport and growth.
Ruth Price, Andrea Baccarini, Julia Schmale, Paul Zieger, Ian M. Brooks, Paul Field, and Ken S. Carslaw
Atmos. Chem. Phys., 23, 2927–2961, https://doi.org/10.5194/acp-23-2927-2023, https://doi.org/10.5194/acp-23-2927-2023, 2023
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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.
Zane Dedekind, Jacopo Grazioli, Philip H. Austin, and Ulrike Lohmann
Atmos. Chem. Phys., 23, 2345–2364, https://doi.org/10.5194/acp-23-2345-2023, https://doi.org/10.5194/acp-23-2345-2023, 2023
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Simulations allowing ice particles to collide with one another producing more ice particles represented surface observations of ice particles accurately. An increase in ice particles formed through collisions was related to sharp changes in the wind direction and speed with height. Changes in wind speed and direction can therefore cause more enhanced collisions between ice particles and alter how fast and how much precipitation forms. Simulations were conducted with the atmospheric model COSMO.
Samuel J. Cliff, Will Drysdale, James D. Lee, Carole Helfter, Eiko Nemitz, Stefan Metzger, and Janet F. Barlow
Atmos. Chem. Phys., 23, 2315–2330, https://doi.org/10.5194/acp-23-2315-2023, https://doi.org/10.5194/acp-23-2315-2023, 2023
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Emissions of nitrogen oxides (NOx) to the atmosphere are an ongoing air quality issue. This study directly measures emissions of NOx and carbon dioxide from a tall tower in central London during the coronavirus pandemic. It was found that transport NOx emissions had reduced by >73 % since 2017 as a result of air quality policy and reduced congestion during coronavirus restrictions. During this period, central London was thought to be dominated by point-source heat and power generation emissions.
Spiro D. Jorga, Kalliopi Florou, David Patoulias, and Spyros N. Pandis
Atmos. Chem. Phys., 23, 85–97, https://doi.org/10.5194/acp-23-85-2023, https://doi.org/10.5194/acp-23-85-2023, 2023
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We take advantage of this unexpected low, new particle formation frequency in Greece and use a dual atmospheric simulation chamber system with starting point ambient air in an effort to gain insight about the chemical species that is limiting nucleation in this area. A potential nucleation precursor, ammonia, was added in one of the chambers while the other one was used as a reference. The addition of ammonia assisted new particle formation in almost 50 % of the experiments conducted.
Pooja V. Pawar, Sachin D. Ghude, Gaurav Govardhan, Prodip Acharja, Rachana Kulkarni, Rajesh Kumar, Baerbel Sinha, Vinayak Sinha, Chinmay Jena, Preeti Gunwani, Tapan Kumar Adhya, Eiko Nemitz, and Mark A. Sutton
Atmos. Chem. Phys., 23, 41–59, https://doi.org/10.5194/acp-23-41-2023, https://doi.org/10.5194/acp-23-41-2023, 2023
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In this study, for the first time in South Asia we compare simulated ammonia, ammonium, and total ammonia using the WRF-Chem model and MARGA measurements during winter in the Indo-Gangetic Plain region. Since observations show HCl promotes the fraction of high chlorides in Delhi, we added HCl / Cl emissions to the model. We conducted three sensitivity experiments with changes in HCl emissions, and improvements are reported in accurately simulating ammonia, ammonium, and total ammonia.
Daniel J. Bryant, Beth S. Nelson, Stefan J. Swift, Sri Hapsari Budisulistiorini, Will S. Drysdale, Adam R. Vaughan, Mike J. Newland, James R. Hopkins, James M. Cash, Ben Langford, Eiko Nemitz, W. Joe F. Acton, C. Nicholas Hewitt, Tuhin Mandal, Bhola R. Gurjar, Shivani, Ranu Gadi, James D. Lee, Andrew R. Rickard, and Jacqueline F. Hamilton
Atmos. Chem. Phys., 23, 61–83, https://doi.org/10.5194/acp-23-61-2023, https://doi.org/10.5194/acp-23-61-2023, 2023
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This paper investigates the sources of isoprene and monoterpene compounds and their particulate-phase oxidation products in Delhi, India. This was done to improve our understanding of the sources, concentrations, and fate of volatile emissions in megacities. By studying the chemical composition of offline filter samples, we report that a significant share of the oxidised organic aerosol in Delhi is from isoprene and monoterpenes. This has implications for human health and policy development.
Lukas Eickhoff, Maddalena Bayer-Giraldi, Naama Reicher, Yinon Rudich, and Thomas Koop
Biogeosciences, 20, 1–14, https://doi.org/10.5194/bg-20-1-2023, https://doi.org/10.5194/bg-20-1-2023, 2023
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The formation of ice is an important process in Earth’s atmosphere, biosphere, and cryosphere, in particular in polar regions. Our research focuses on the influence of the sea ice diatom Fragilariopsis cylindrus and of molecules produced by it upon heterogenous ice nucleation. For that purpose, we studied the freezing of tiny droplets containing the diatoms in a microfluidic device. Together with previous studies, our results suggest a common freezing behaviour of various sea ice diatoms.
Elisa T. Sena, Ilan Koren, Orit Altaratz, and Alexander B. Kostinski
Atmos. Chem. Phys., 22, 16111–16122, https://doi.org/10.5194/acp-22-16111-2022, https://doi.org/10.5194/acp-22-16111-2022, 2022
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We used record-breaking statistics together with spatial information to create record-breaking SST maps. The maps reveal warming patterns in the overwhelming majority of the ocean and coherent islands of cooling, where low records occur more frequently than high ones. Some of these cooling spots are well known; however, a surprising elliptical area in the Southern Ocean is observed as well. Similar analyses can be performed on other key climatological variables to explore their trend patterns.
Srijana Lama, Sander Houweling, K. Folkert Boersma, Ilse Aben, Hugo A. C. Denier van der Gon, and Maarten C. Krol
Atmos. Chem. Phys., 22, 16053–16071, https://doi.org/10.5194/acp-22-16053-2022, https://doi.org/10.5194/acp-22-16053-2022, 2022
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Hydroxyl radical (OH) is the important chemical species that determines the lifetime of some greenhouse gases and trace gases. OH plays a vital role in air pollution chemistry. OH has a short lifetime and is extremely difficult to measure directly. OH concentrations derived from the chemistry transport model (CTM) have uncertainties of >50 %. Therefore, in this study, OH is derived indirectly using satellite date in urban plumes.
Yandong Tong, Lu Qi, Giulia Stefenelli, Dongyu Simon Wang, Francesco Canonaco, Urs Baltensperger, André Stephan Henry Prévôt, and Jay Gates Slowik
Atmos. Meas. Tech., 15, 7265–7291, https://doi.org/10.5194/amt-15-7265-2022, https://doi.org/10.5194/amt-15-7265-2022, 2022
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We present a method for positive matrix factorisation (PMF) analysis on a single dataset that includes measurements from both EESI-TOF and AMS in Zurich, Switzerland. For the first time, we resolved and quantified secondary organic aerosol (SOA) sources. Meanwhile, we also determined the retrieved EESI-TOF factor-dependent sensitivities. This method provides a framework for exploiting semi-quantitative, high-resolution instrumentation for quantitative source apportionment.
Qiuyan Wang, Hua Zhang, Su Yang, Qi Chen, Xixun Zhou, Bing Xie, Yuying Wang, Guangyu Shi, and Martin Wild
Atmos. Chem. Phys., 22, 15867–15886, https://doi.org/10.5194/acp-22-15867-2022, https://doi.org/10.5194/acp-22-15867-2022, 2022
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The present-day land energy balance over East Asia is estimated for the first time. Results indicate that high aerosol loadings, clouds, and the Tibet Plateau (TP) over East Asia play vital roles in the shortwave budgets, while the TP is responsible for the longwave budgets during this regional energy budget assessment. This study provides a perspective to understand fully how the potential factors influence the diversifying regional energy budget assessments.
Brian T. Dinkelacker, Pablo Garcia Rivera, Ioannis Kioutsioukis, Peter J. Adams, and Spyros N. Pandis
Geosci. Model Dev., 15, 8899–8912, https://doi.org/10.5194/gmd-15-8899-2022, https://doi.org/10.5194/gmd-15-8899-2022, 2022
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The performance of a chemical transport model in reproducing PM2.5 concentrations and composition was evaluated at the finest scale using measurements from regulatory sites as well as a network of low-cost monitors. Total PM2.5 mass is reproduced well by the model during the winter when compared to regulatory measurements, but in the summer PM2.5 is underpredicted, mainly due to difficulties in reproducing regional secondary organic aerosol levels.
Julie Thérèse Pasquier, Jan Henneberger, Fabiola Ramelli, Annika Lauber, Robert Oscar David, Jörg Wieder, Tim Carlsen, Rosa Gierens, Marion Maturilli, and Ulrike Lohmann
Atmos. Chem. Phys., 22, 15579–15601, https://doi.org/10.5194/acp-22-15579-2022, https://doi.org/10.5194/acp-22-15579-2022, 2022
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It is important to understand how ice crystals and cloud droplets form in clouds, as their concentrations and sizes determine the exact radiative properties of the clouds. Normally, ice crystals form from aerosols, but we found evidence for the formation of additional ice crystals from the original ones over a large temperature range within Arctic clouds. In particular, additional ice crystals were formed during collisions of several ice crystals or during the freezing of large cloud droplets.
Leighton A. Regayre, Lucia Deaconu, Daniel P. Grosvenor, David Sexton, Christopher C. Symonds, Tom Langton, Duncan Watson-Paris, Jane P. Mulcahy, Kirsty J. Pringle, Mark Richardson, Jill S. Johnson, John Rostron, Hamish Gordon, Grenville Lister, Philip Stier, and Ken S. Carslaw
EGUsphere, https://doi.org/10.5194/egusphere-2022-1330, https://doi.org/10.5194/egusphere-2022-1330, 2022
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We show that potential structural deficiencies in a climate model can be exposed by comprehensively exploring its parametric uncertainty, and that these deficiencies limit how much the model uncertainty can be reduced through observational constraint. Combined consideration of parametric and structural uncertainties provides a future pathway towards building models that have greater physical realism and lower uncertainty.
Pascal Wintjen, Frederik Schrader, Martijn Schaap, Burkhard Beudert, Richard Kranenburg, and Christian Brümmer
Biogeosciences, 19, 5287–5311, https://doi.org/10.5194/bg-19-5287-2022, https://doi.org/10.5194/bg-19-5287-2022, 2022
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For the first time, we compared four methods for estimating the annual dry deposition of total reactive nitrogen into a low-polluted forest ecosystem. In our analysis, we used 2.5 years of flux measurements, an in situ modeling approach, a large-scale chemical transport model (CTM), and canopy budget models. Annual nitrogen dry deposition budgets ranged between 4.3 and 6.7 kg N ha−1 a−1, depending on the applied method.
Marsailidh M. Twigg, Augustinus J. C. Berkhout, Nicholas Cowan, Sabine Crunaire, Enrico Dammers, Volker Ebert, Vincent Gaudion, Marty Haaima, Christoph Häni, Lewis John, Matthew R. Jones, Bjorn Kamps, John Kentisbeer, Thomas Kupper, Sarah R. Leeson, Daiana Leuenberger, Nils O. B. Lüttschwager, Ulla Makkonen, Nicholas A. Martin, David Missler, Duncan Mounsor, Albrecht Neftel, Chad Nelson, Eiko Nemitz, Rutger Oudwater, Celine Pascale, Jean-Eudes Petit, Andrea Pogany, Nathalie Redon, Jörg Sintermann, Amy Stephens, Mark A. Sutton, Yuk S. Tang, Rens Zijlmans, Christine F. Braban, and Bernhard Niederhauser
Atmos. Meas. Tech., 15, 6755–6787, https://doi.org/10.5194/amt-15-6755-2022, https://doi.org/10.5194/amt-15-6755-2022, 2022
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Ammonia (NH3) gas in the atmosphere impacts the environment, human health, and, indirectly, climate. Historic NH3 monitoring was labour intensive, and the instruments were complicated. Over the last decade, there has been a rapid technology development, including “plug-and-play” instruments. This study is an extensive field comparison of the currently available technologies and provides evidence that for routine monitoring, standard operating protocols are required for datasets to be comparable.
Caroline C. Womack, Steven S. Brown, Steven J. Ciciora, Ru-Shan Gao, Richard J. McLaughlin, Michael A. Robinson, Yinon Rudich, and Rebecca A. Washenfelder
Atmos. Meas. Tech., 15, 6643–6652, https://doi.org/10.5194/amt-15-6643-2022, https://doi.org/10.5194/amt-15-6643-2022, 2022
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We present a new miniature instrument to measure nitrogen dioxide (NO2) using cavity-enhanced spectroscopy. NO2 contributes to the formation of pollutants such as ozone and particulate matter, and its concentration can vary widely near sources. We developed this lightweight (3.05 kg) low-power (<35 W) instrument to measure NO2 on uncrewed aircraft vehicles (UAVs) and demonstrate that it has the accuracy and precision needed for atmospheric field measurements.
Christina Vasilakopoulou, Iasonas Stavroulas, Nikolaos Mihalopoulos, and Spyros N. Pandis
Atmos. Meas. Tech., 15, 6419–6431, https://doi.org/10.5194/amt-15-6419-2022, https://doi.org/10.5194/amt-15-6419-2022, 2022
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Offline aerosol mass spectrometer (AMS) measurements can provide valuable information about ambient organic aerosols when online AMS measurements are not available. In this study, we examine whether and how the low time resolution (usually 24 h) of the offline technique affects source apportionment results. We concluded that use of the daily averages resulted in estimated average contributions that were within 8 % of the total OA compared with the high-resolution analysis.
Stella E. I. Manavi and Spyros N. Pandis
Geosci. Model Dev., 15, 7731–7749, https://doi.org/10.5194/gmd-15-7731-2022, https://doi.org/10.5194/gmd-15-7731-2022, 2022
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The paper describes the first step towards the development of a simulation framework for the chemistry and secondary organic aerosol production of intermediate-volatility organic compounds (IVOCs). These compounds can be a significant source of organic particulate matter. Our approach treats IVOCs as lumped compounds that retain their chemical characteristics. Estimated IVOC emissions from road transport were a factor of 8 higher than emissions used in previous applications.
Aristeidis Voliotis, Mao Du, Yu Wang, Yunqi Shao, Thomas J. Bannan, Michael Flynn, Spyros N. Pandis, Carl J. Percival, M. Rami Alfarra, and Gordon McFiggans
Atmos. Chem. Phys., 22, 13677–13693, https://doi.org/10.5194/acp-22-13677-2022, https://doi.org/10.5194/acp-22-13677-2022, 2022
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The addition of a low-yield precursor to the reactive mixture of aVOC and bVOC can increase or decrease the SOA volatility that is system-dependent. Therefore, the SOA volatility of the mixtures cannot always be predicted based on the additivity. In complex mixtures the formation of lower-volatility products likely outweighs the formation of products with higher volatility. The unique products of each mixture contribute significantly to the signal, suggesting interactions can be important.
David M. Bell, Cheng Wu, Amelie Bertrand, Emelie Graham, Janne Schoonbaert, Stamatios Giannoukos, Urs Baltensperger, Andre S. H. Prevot, Ilona Riipinen, Imad El Haddad, and Claudia Mohr
Atmos. Chem. Phys., 22, 13167–13182, https://doi.org/10.5194/acp-22-13167-2022, https://doi.org/10.5194/acp-22-13167-2022, 2022
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A series of studies designed to investigate the evolution of organic aerosol were performed in an atmospheric simulation chamber, using a common oxidant found at night (NO3). The chemical composition steadily changed from its initial composition via different chemical reactions that were taking place inside of the aerosol particle. These results show that the composition of organic aerosol steadily changes during its lifetime in the atmosphere.
Ville Leinonen, Harri Kokkola, Taina Yli-Juuti, Tero Mielonen, Thomas Kühn, Tuomo Nieminen, Simo Heikkinen, Tuuli Miinalainen, Tommi Bergman, Ken Carslaw, Stefano Decesari, Markus Fiebig, Tareq Hussein, Niku Kivekäs, Radovan Krejci, Markku Kulmala, Ari Leskinen, Andreas Massling, Nikos Mihalopoulos, Jane P. Mulcahy, Steffen M. Noe, Twan van Noije, Fiona M. O'Connor, Colin O'Dowd, Dirk Olivie, Jakob B. Pernov, Tuukka Petäjä, Øyvind Seland, Michael Schulz, Catherine E. Scott, Henrik Skov, Erik Swietlicki, Thomas Tuch, Alfred Wiedensohler, Annele Virtanen, and Santtu Mikkonen
Atmos. Chem. Phys., 22, 12873–12905, https://doi.org/10.5194/acp-22-12873-2022, https://doi.org/10.5194/acp-22-12873-2022, 2022
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We provide the first extensive comparison of detailed aerosol size distribution trends between in situ observations from Europe and five different earth system models. We investigated aerosol modes (nucleation, Aitken, and accumulation) separately and were able to show the differences between measured and modeled trends and especially their seasonal patterns. The differences in model results are likely due to complex effects of several processes instead of certain specific model features.
Marta Via, Gang Chen, Francesco Canonaco, Kaspar R. Daellenbach, Benjamin Chazeau, Hasna Chebaicheb, Jianhui Jiang, Hannes Keernik, Chunshui Lin, Nicolas Marchand, Cristina Marin, Colin O'Dowd, Jurgita Ovadnevaite, Jean-Eudes Petit, Michael Pikridas, Véronique Riffault, Jean Sciare, Jay G. Slowik, Leïla Simon, Jeni Vasilescu, Yunjiang Zhang, Olivier Favez, André S. H. Prévôt, Andrés Alastuey, and María Cruz Minguillón
Atmos. Meas. Tech., 15, 5479–5495, https://doi.org/10.5194/amt-15-5479-2022, https://doi.org/10.5194/amt-15-5479-2022, 2022
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This work presents the differences resulting from two techniques (rolling and seasonal) of the positive matrix factorisation model that can be run for organic aerosol source apportionment. The current state of the art suggests that the rolling technique is more accurate, but no proof of its effectiveness has been provided yet. This paper tackles this issue in the context of a synthetic dataset and a multi-site real-world comparison.
Johannes Quaas, Hailing Jia, Chris Smith, Anna Lea Albright, Wenche Aas, Nicolas Bellouin, Olivier Boucher, Marie Doutriaux-Boucher, Piers M. Forster, Daniel Grosvenor, Stuart Jenkins, Zbigniew Klimont, Norman G. Loeb, Xiaoyan Ma, Vaishali Naik, Fabien Paulot, Philip Stier, Martin Wild, Gunnar Myhre, and Michael Schulz
Atmos. Chem. Phys., 22, 12221–12239, https://doi.org/10.5194/acp-22-12221-2022, https://doi.org/10.5194/acp-22-12221-2022, 2022
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Pollution particles cool climate and offset part of the global warming. However, they are washed out by rain and thus their effect responds quickly to changes in emissions. We show multiple datasets to demonstrate that aerosol emissions and their concentrations declined in many regions influenced by human emissions, as did the effects on clouds. Consequently, the cooling impact on the Earth energy budget became smaller. This change in trend implies a relative warming.
Florin N. Isenrich, Nadia Shardt, Michael Rösch, Julia Nette, Stavros Stavrakis, Claudia Marcolli, Zamin A. Kanji, Andrew J. deMello, and Ulrike Lohmann
Atmos. Meas. Tech., 15, 5367–5381, https://doi.org/10.5194/amt-15-5367-2022, https://doi.org/10.5194/amt-15-5367-2022, 2022
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Ice nucleation in the atmosphere influences cloud properties and lifetimes. Microfluidic instruments have recently been used to investigate ice nucleation, but these instruments are typically made out of a polymer that contributes to droplet instability over extended timescales and relatively high temperature uncertainty. To address these drawbacks, we develop and validate a new microfluidic instrument that uses fluoropolymer tubing to extend droplet stability and improve temperature accuracy.
Brian T. Dinkelacker, Pablo Garcia Rivera, Ksakousti Skyllakou, Peter J. Adams, and Spyros N. Pandis
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2022-648, https://doi.org/10.5194/acp-2022-648, 2022
Revised manuscript not accepted
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A number of factors have influenced the biogenic secondary organic aerosol (SOA) levels in the southeastern US from 2001 to 2010. The increases in temperature have led to an increase of the emissions of biogenic volatile organic compounds by trees and a corresponding increase of the SOA. However, this increase has been balanced by the reductions in the anthropogenic emissions of organic gases and particulate matter as well as of the oxides of nitrogen keeping the biogenic SOA roughly constant.
Colin Tully, David Neubauer, Nadja Omanovic, and Ulrike Lohmann
Atmos. Chem. Phys., 22, 11455–11484, https://doi.org/10.5194/acp-22-11455-2022, https://doi.org/10.5194/acp-22-11455-2022, 2022
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The proposed geoengineering method, cirrus cloud thinning, was evaluated using a more physically based microphysics scheme coupled to a more realistic approach for calculating ice cloud fractions in the ECHAM-HAM GCM. Sensitivity tests reveal that using the new ice cloud fraction approach and increasing the critical ice saturation ratio for ice nucleation on seeding particles reduces warming from overseeding. However, this geoengineering method is unlikely to be feasible on a global scale.
Amy H. Peace, Ben B. B. Booth, Leighton A. Regayre, Ken S. Carslaw, David M. H. Sexton, Céline J. W. Bonfils, and John W. Rostron
Earth Syst. Dynam., 13, 1215–1232, https://doi.org/10.5194/esd-13-1215-2022, https://doi.org/10.5194/esd-13-1215-2022, 2022
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Anthropogenic aerosol emissions have been linked to driving climate responses such as shifts in the location of tropical rainfall. However, the interaction of aerosols with climate remains one of the most uncertain aspects of climate modelling and limits our ability to predict future climate change. We use an ensemble of climate model simulations to investigate what impact the large uncertainty in how aerosols interact with climate has on predicting future tropical rainfall shifts.
Jörg Wieder, Nikola Ihn, Claudia Mignani, Moritz Haarig, Johannes Bühl, Patric Seifert, Ronny Engelmann, Fabiola Ramelli, Zamin A. Kanji, Ulrike Lohmann, and Jan Henneberger
Atmos. Chem. Phys., 22, 9767–9797, https://doi.org/10.5194/acp-22-9767-2022, https://doi.org/10.5194/acp-22-9767-2022, 2022
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Ice formation and its evolution in mixed-phase clouds are still uncertain. We evaluate the lidar retrieval of ice-nucleating particle concentration in dust-dominated and continental air masses over the Swiss Alps with in situ observations. A calibration factor to improve the retrieval from continental air masses is proposed. Ice multiplication factors are obtained with a new method utilizing remote sensing. Our results indicate that secondary ice production occurs at temperatures down to −30 °C.
Alexander D. Harrison, Daniel O'Sullivan, Michael P. Adams, Grace C. E. Porter, Edmund Blades, Cherise Brathwaite, Rebecca Chewitt-Lucas, Cassandra Gaston, Rachel Hawker, Ovid O. Krüger, Leslie Neve, Mira L. Pöhlker, Christopher Pöhlker, Ulrich Pöschl, Alberto Sanchez-Marroquin, Andrea Sealy, Peter Sealy, Mark D. Tarn, Shanice Whitehall, James B. McQuaid, Kenneth S. Carslaw, Joseph M. Prospero, and Benjamin J. Murray
Atmos. Chem. Phys., 22, 9663–9680, https://doi.org/10.5194/acp-22-9663-2022, https://doi.org/10.5194/acp-22-9663-2022, 2022
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The formation of ice in clouds fundamentally alters cloud properties; hence it is important we understand the special aerosol particles that can nucleate ice when immersed in supercooled cloud droplets. In this paper we show that African desert dust that has travelled across the Atlantic to the Caribbean nucleates ice much less well than we might have expected.
Will S. Drysdale, Adam R. Vaughan, Freya A. Squires, Sam J. Cliff, Stefan Metzger, David Durden, Natchaya Pingintha-Durden, Carole Helfter, Eiko Nemitz, C. Sue B. Grimmond, Janet Barlow, Sean Beevers, Gregor Stewart, David Dajnak, Ruth M. Purvis, and James D. Lee
Atmos. Chem. Phys., 22, 9413–9433, https://doi.org/10.5194/acp-22-9413-2022, https://doi.org/10.5194/acp-22-9413-2022, 2022
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Measurements of NOx emissions are important for a good understanding of air quality. While there are many direct measurements of NOx concentration, there are very few measurements of its emission. Measurements of emissions provide constraints on emissions inventories and air quality models. This article presents measurements of NOx emission from the BT Tower in central London in 2017 and compares them with inventories, finding that they underestimate by a factor of ∼1.48.
Chuan Ping Lee, Mihnea Surdu, David M. Bell, Josef Dommen, Mao Xiao, Xueqin Zhou, Andrea Baccarini, Stamatios Giannoukos, Günther Wehrle, Pascal André Schneider, Andre S. H. Prevot, Jay G. Slowik, Houssni Lamkaddam, Dongyu Wang, Urs Baltensperger, and Imad El Haddad
Atmos. Meas. Tech., 15, 3747–3760, https://doi.org/10.5194/amt-15-3747-2022, https://doi.org/10.5194/amt-15-3747-2022, 2022
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Real-time detection of both the gas and particle phase is needed to elucidate the sources and chemical reaction pathways of organic vapors and particulate matter. The Dual-EESI was developed to measure gas- and particle-phase species to provide new insights into aerosol sources or formation mechanisms. After characterizing the relative gas and particle response factors of EESI via organic aerosol uptake experiments, the Dual-EESI is more sensitive toward gas-phase analyes.
Varun Kumar, Stamatios Giannoukos, Sophie L. Haslett, Yandong Tong, Atinderpal Singh, Amelie Bertrand, Chuan Ping Lee, Dongyu S. Wang, Deepika Bhattu, Giulia Stefenelli, Jay S. Dave, Joseph V. Puthussery, Lu Qi, Pawan Vats, Pragati Rai, Roberto Casotto, Rangu Satish, Suneeti Mishra, Veronika Pospisilova, Claudia Mohr, David M. Bell, Dilip Ganguly, Vishal Verma, Neeraj Rastogi, Urs Baltensperger, Sachchida N. Tripathi, André S. H. Prévôt, and Jay G. Slowik
Atmos. Chem. Phys., 22, 7739–7761, https://doi.org/10.5194/acp-22-7739-2022, https://doi.org/10.5194/acp-22-7739-2022, 2022
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Here we present source apportionment results from the first field deployment in Delhi of an extractive electrospray ionization time-of-flight mass spectrometer (EESI-TOF). The EESI-TOF is a recently developed instrument capable of providing uniquely detailed online chemical characterization of organic aerosol (OA), in particular the secondary OA (SOA) fraction. Here, we are able to apportion not only primary OA but also SOA to specific sources, which is performed for the first time in Delhi.
Marc Guevara, Hervé Petetin, Oriol Jorba, Hugo Denier van der Gon, Jeroen Kuenen, Ingrid Super, Jukka-Pekka Jalkanen, Elisa Majamäki, Lasse Johansson, Vincent-Henri Peuch, and Carlos Pérez García-Pando
Earth Syst. Sci. Data, 14, 2521–2552, https://doi.org/10.5194/essd-14-2521-2022, https://doi.org/10.5194/essd-14-2521-2022, 2022
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To control the spread of the COVID-19 disease, European governments implemented mobility restriction measures that resulted in an unprecedented drop in anthropogenic emissions. This work presents a dataset of emission adjustment factors that allows quantifying changes in 2020 European primary emissions per country and pollutant sector at the daily scale. The resulting dataset can be used as input in modelling studies aiming at quantifying the impact of COVID-19 on air quality levels.
Ulrike Proske, Sylvaine Ferrachat, David Neubauer, Martin Staab, and Ulrike Lohmann
Atmos. Chem. Phys., 22, 4737–4762, https://doi.org/10.5194/acp-22-4737-2022, https://doi.org/10.5194/acp-22-4737-2022, 2022
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Cloud microphysical processes shape cloud properties and are therefore important to represent in climate models. Their parameterization has grown more complex, making the model results more difficult to interpret. Using sensitivity analysis we test how the global aerosol–climate model ECHAM-HAM reacts to changes to these parameterizations. The model is sensitive to the parameterization of ice crystal autoconversion but not to, e.g., self-collection, suggesting that it may be simplified.
Jörg Wieder, Claudia Mignani, Mario Schär, Lucie Roth, Michael Sprenger, Jan Henneberger, Ulrike Lohmann, Cyril Brunner, and Zamin A. Kanji
Atmos. Chem. Phys., 22, 3111–3130, https://doi.org/10.5194/acp-22-3111-2022, https://doi.org/10.5194/acp-22-3111-2022, 2022
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We investigate the variation in ice-nucleating particles (INPs) relevant for primary ice formation in mixed-phased clouds over the Alps based on simultaneous in situ observations at a mountaintop and a nearby high valley (1060 m height difference). In most cases, advection from the surrounding lower regions was responsible for changes in INP concentration, causing a diurnal cycle at the mountaintop. Our study underlines the importance of the planetary boundary layer as an INP reserve.
Julia Schmale, Sangeeta Sharma, Stefano Decesari, Jakob Pernov, Andreas Massling, Hans-Christen Hansson, Knut von Salzen, Henrik Skov, Elisabeth Andrews, Patricia K. Quinn, Lucia M. Upchurch, Konstantinos Eleftheriadis, Rita Traversi, Stefania Gilardoni, Mauro Mazzola, James Laing, and Philip Hopke
Atmos. Chem. Phys., 22, 3067–3096, https://doi.org/10.5194/acp-22-3067-2022, https://doi.org/10.5194/acp-22-3067-2022, 2022
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Long-term data sets of Arctic aerosol properties from 10 stations across the Arctic provide evidence that anthropogenic influence on the Arctic atmospheric chemical composition has declined in winter, a season which is typically dominated by mid-latitude emissions. The number of significant trends in summer is smaller than in winter, and overall the pattern is ambiguous with some significant positive and negative trends. This reflects the mixed influence of natural and anthropogenic emissions.
Christian Brümmer, Jeremy J. Rüffer, Jean-Pierre Delorme, Pascal Wintjen, Frederik Schrader, Burkhard Beudert, Martijn Schaap, and Christof Ammann
Earth Syst. Sci. Data, 14, 743–761, https://doi.org/10.5194/essd-14-743-2022, https://doi.org/10.5194/essd-14-743-2022, 2022
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Field campaigns were carried out to investigate the biosphere–atmosphere exchange of selected reactive nitrogen compounds over different land surfaces using two different analytical devices for ammonia and total reactive nitrogen. The datasets improve our understanding of the temporal variability of surface–atmosphere exchange in different ecosystems, thereby providing validation opportunities for inferential models simulating the exchange of reactive nitrogen.
Pablo Garcia Rivera, Brian T. Dinkelacker, Ioannis Kioutsioukis, Peter J. Adams, and Spyros N. Pandis
Atmos. Chem. Phys., 22, 2011–2027, https://doi.org/10.5194/acp-22-2011-2022, https://doi.org/10.5194/acp-22-2011-2022, 2022
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The contribution of various pollution sources to the variability of fine PM in an urban area was examined using as an example the city of Pittsburgh. Biomass burning aerosol shows the largest variability during the winter with local maxima within the city and in the suburbs. During both periods the largest contributing source to the average PM2.5 is particles from outside the modeling domain. The average population-weighted PM2.5 concentration does not change significantly with resolution.
Jeroen Kuenen, Stijn Dellaert, Antoon Visschedijk, Jukka-Pekka Jalkanen, Ingrid Super, and Hugo Denier van der Gon
Earth Syst. Sci. Data, 14, 491–515, https://doi.org/10.5194/essd-14-491-2022, https://doi.org/10.5194/essd-14-491-2022, 2022
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This paper presents an 18-year time series for anthropogenic emissions for the main air pollutants in Europe, distinguishing 15 main source categories. It provides a complete overview of emissions to air and is designed to support air quality modelling. The data build where possible on official country total emissions used in the policy processes, but where necessary alternative data were used. The emission data are spatially distributed at high resolution (~ 6 km x 6 km) in a consistent way.
Zhi-Hui Zhang, Elena Hartner, Battist Utinger, Benjamin Gfeller, Andreas Paul, Martin Sklorz, Hendryk Czech, Bin Xia Yang, Xin Yi Su, Gert Jakobi, Jürgen Orasche, Jürgen Schnelle-Kreis, Seongho Jeong, Thomas Gröger, Michal Pardo, Thorsten Hohaus, Thomas Adam, Astrid Kiendler-Scharr, Yinon Rudich, Ralf Zimmermann, and Markus Kalberer
Atmos. Chem. Phys., 22, 1793–1809, https://doi.org/10.5194/acp-22-1793-2022, https://doi.org/10.5194/acp-22-1793-2022, 2022
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Using a novel setup, we comprehensively characterized the formation of particle-bound reactive oxygen species (ROS) in anthropogenic and biogenic secondary organic aerosols (SOAs). We found that more than 90 % of all ROS components in both SOA types have a short lifetime. Our results also show that photochemical aging promotes particle-bound ROS production and enhances the oxidative potential of the aerosols. We found consistent results between chemical-based and biological-based ROS analyses.
David Patoulias and Spyros N. Pandis
Atmos. Chem. Phys., 22, 1689–1706, https://doi.org/10.5194/acp-22-1689-2022, https://doi.org/10.5194/acp-22-1689-2022, 2022
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Our simulations indicate that the recently identified production and subsequent condensation effect of extremely low-volatility organic compounds have a smaller-than-expected effect on the total concentration of atmospheric particles. On the other hand, the oxidation of intermediate-volatility organic compounds leads to decreases in the ultrafine-particle concentrations. These results improve our understanding of the links between secondary organic aerosol formation and ultrafine particles.
Nicolás Álamos, Nicolás Huneeus, Mariel Opazo, Mauricio Osses, Sebastián Puja, Nicolás Pantoja, Hugo Denier van der Gon, Alejandra Schueftan, René Reyes, and Rubén Calvo
Earth Syst. Sci. Data, 14, 361–379, https://doi.org/10.5194/essd-14-361-2022, https://doi.org/10.5194/essd-14-361-2022, 2022
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This study presents the first high-resolution national inventory of anthropogenic emissions for Chile (Inventario Nacional de Emisiones Antropogénicas, INEMA). Emissions for vehicular, industrial, energy, mining and residential sectors are estimated for the period 2015–2017 and spatially distributed onto a high-resolution grid (1 × 1 km). This inventory will support policies seeking to mitigate climate change and improve air quality by providing qualified scientific spatial emission information.
Pascal Wintjen, Frederik Schrader, Martijn Schaap, Burkhard Beudert, and Christian Brümmer
Biogeosciences, 19, 389–413, https://doi.org/10.5194/bg-19-389-2022, https://doi.org/10.5194/bg-19-389-2022, 2022
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Fluxes of total reactive nitrogen (∑Nr) over a low polluted forest were analyzed with regard to their temporal dynamics. Mostly deposition was observed with median fluxes ranging from −15 to −5 ng N m−2 s−1, corresponding to a range of deposition velocities from 0.2 to 0.5 cm s−1. While seasonally changing contributions of NH3 and NOx to the ∑Nr signal were found, we estimate an annual total N deposition (dry+wet) of 12.2 and 10.9 kg N ha−1 a−1 in the 2 years of observation.
Peifeng Su, Jorma Joutsensaari, Lubna Dada, Martha Arbayani Zaidan, Tuomo Nieminen, Xinyang Li, Yusheng Wu, Stefano Decesari, Sasu Tarkoma, Tuukka Petäjä, Markku Kulmala, and Petri Pellikka
Atmos. Chem. Phys., 22, 1293–1309, https://doi.org/10.5194/acp-22-1293-2022, https://doi.org/10.5194/acp-22-1293-2022, 2022
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We regarded the banana shapes in the surface plots as a special kind of object (similar to cats) and applied an instance segmentation technique to automatically identify the new particle formation (NPF) events (especially the strongest ones), in addition to their growth rates, start times, and end times. The automatic method generalized well on datasets collected in different sites, which is useful for long-term data series analysis and obtaining statistical properties of NPF events.
Miska Olin, David Patoulias, Heino Kuuluvainen, Jarkko V. Niemi, Topi Rönkkö, Spyros N. Pandis, Ilona Riipinen, and Miikka Dal Maso
Atmos. Chem. Phys., 22, 1131–1148, https://doi.org/10.5194/acp-22-1131-2022, https://doi.org/10.5194/acp-22-1131-2022, 2022
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An emission factor particle size distribution was determined from the measurements at an urban traffic site. It was used in updating a pre-existing emission inventory, and regional modeling was performed after the update. Emission inventories typically underestimate nanoparticle emissions due to challenges in determining them with high certainty. This update reveals that the simulated aerosol levels have previously been underestimated especially for urban areas and for sub-50 nm particles.
Shelley van der Graaf, Enrico Dammers, Arjo Segers, Richard Kranenburg, Martijn Schaap, Mark W. Shephard, and Jan Willem Erisman
Atmos. Chem. Phys., 22, 951–972, https://doi.org/10.5194/acp-22-951-2022, https://doi.org/10.5194/acp-22-951-2022, 2022
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CrIS NH3 satellite observations are assimilated into the LOTOS-EUROS model using two different methods. In the first method the data are used to fit spatially varying NH3 emission time factors. In the second method a local ensemble transform Kalman filter is used. Compared to in situ observations, combining both methods led to the most significant improvements in the modeled concentrations and deposition, illustrating the usefulness of CrIS NH3 to improve the spatiotemporal distribution of NH3.
Dalrin Ampritta Amaladhasan, Claudia Heyn, Christopher R. Hoyle, Imad El Haddad, Miriam Elser, Simone M. Pieber, Jay G. Slowik, Antonio Amorim, Jonathan Duplissy, Sebastian Ehrhart, Vladimir Makhmutov, Ugo Molteni, Matti Rissanen, Yuri Stozhkov, Robert Wagner, Armin Hansel, Jasper Kirkby, Neil M. Donahue, Rainer Volkamer, Urs Baltensperger, Martin Gysel-Beer, and Andreas Zuend
Atmos. Chem. Phys., 22, 215–244, https://doi.org/10.5194/acp-22-215-2022, https://doi.org/10.5194/acp-22-215-2022, 2022
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We use a combination of models for gas-phase chemical reactions and equilibrium gas–particle partitioning of isoprene-derived secondary organic aerosols (SOAs) informed by dark ozonolysis experiments conducted in the CLOUD chamber. Our predictions cover high to low relative humidities (RHs) and quantify how SOA mass yields are enhanced at high RH as well as the impact of inorganic seeds of distinct hygroscopicities and acidities on the coupled partitioning of water and semi-volatile organics.
Rachel E. Hawker, Annette K. Miltenberger, Jill S. Johnson, Jonathan M. Wilkinson, Adrian A. Hill, Ben J. Shipway, Paul R. Field, Benjamin J. Murray, and Ken S. Carslaw
Atmos. Chem. Phys., 21, 17315–17343, https://doi.org/10.5194/acp-21-17315-2021, https://doi.org/10.5194/acp-21-17315-2021, 2021
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We find that ice-nucleating particles (INPs), aerosols that can initiate the freezing of cloud droplets, cause substantial changes to the properties of radiatively important convectively generated anvil cirrus. The number concentration of INPs had a large effect on ice crystal number concentration while the INP temperature dependence controlled ice crystal size and cloud fraction. The results indicate information on INP number and source is necessary for the representation of cloud glaciation.
Clémence Rose, Martine Collaud Coen, Elisabeth Andrews, Yong Lin, Isaline Bossert, Cathrine Lund Myhre, Thomas Tuch, Alfred Wiedensohler, Markus Fiebig, Pasi Aalto, Andrés Alastuey, Elisabeth Alonso-Blanco, Marcos Andrade, Begoña Artíñano, Todor Arsov, Urs Baltensperger, Susanne Bastian, Olaf Bath, Johan Paul Beukes, Benjamin T. Brem, Nicolas Bukowiecki, Juan Andrés Casquero-Vera, Sébastien Conil, Konstantinos Eleftheriadis, Olivier Favez, Harald Flentje, Maria I. Gini, Francisco Javier Gómez-Moreno, Martin Gysel-Beer, Anna Gannet Hallar, Ivo Kalapov, Nikos Kalivitis, Anne Kasper-Giebl, Melita Keywood, Jeong Eun Kim, Sang-Woo Kim, Adam Kristensson, Markku Kulmala, Heikki Lihavainen, Neng-Huei Lin, Hassan Lyamani, Angela Marinoni, Sebastiao Martins Dos Santos, Olga L. Mayol-Bracero, Frank Meinhardt, Maik Merkel, Jean-Marc Metzger, Nikolaos Mihalopoulos, Jakub Ondracek, Marco Pandolfi, Noemi Pérez, Tuukka Petäjä, Jean-Eudes Petit, David Picard, Jean-Marc Pichon, Veronique Pont, Jean-Philippe Putaud, Fabienne Reisen, Karine Sellegri, Sangeeta Sharma, Gerhard Schauer, Patrick Sheridan, James Patrick Sherman, Andreas Schwerin, Ralf Sohmer, Mar Sorribas, Junying Sun, Pierre Tulet, Ville Vakkari, Pieter Gideon van Zyl, Fernando Velarde, Paolo Villani, Stergios Vratolis, Zdenek Wagner, Sheng-Hsiang Wang, Kay Weinhold, Rolf Weller, Margarita Yela, Vladimir Zdimal, and Paolo Laj
Atmos. Chem. Phys., 21, 17185–17223, https://doi.org/10.5194/acp-21-17185-2021, https://doi.org/10.5194/acp-21-17185-2021, 2021
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Aerosol particles are a complex component of the atmospheric system the effects of which are among the most uncertain in climate change projections. Using data collected at 62 stations, this study provides the most up-to-date picture of the spatial distribution of particle number concentration and size distribution worldwide, with the aim of contributing to better representation of aerosols and their interactions with clouds in models and, therefore, better evaluation of their impact on climate.
Ksakousti Skyllakou, Pablo Garcia Rivera, Brian Dinkelacker, Eleni Karnezi, Ioannis Kioutsioukis, Carlos Hernandez, Peter J. Adams, and Spyros N. Pandis
Atmos. Chem. Phys., 21, 17115–17132, https://doi.org/10.5194/acp-21-17115-2021, https://doi.org/10.5194/acp-21-17115-2021, 2021
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Significant reductions in pollutant emissions took place in the US from 1990 to 2010. The reductions in sulfur dioxide emissions from electric-generating units have dominated the reductions in fine particle mass. The reductions in transportation emissions have led to a 30 % reduction of elemental concentrations and of organic particulate matter by a factor of 3. On the other hand, changes in biomass burning and biogenic secondary organic aerosol have been modest.
Lucía Caudillo, Birte Rörup, Martin Heinritzi, Guillaume Marie, Mario Simon, Andrea C. Wagner, Tatjana Müller, Manuel Granzin, Antonio Amorim, Farnoush Ataei, Rima Baalbaki, Barbara Bertozzi, Zoé Brasseur, Randall Chiu, Biwu Chu, Lubna Dada, Jonathan Duplissy, Henning Finkenzeller, Loïc Gonzalez Carracedo, Xu-Cheng He, Victoria Hofbauer, Weimeng Kong, Houssni Lamkaddam, Chuan P. Lee, Brandon Lopez, Naser G. A. Mahfouz, Vladimir Makhmutov, Hanna E. Manninen, Ruby Marten, Dario Massabò, Roy L. Mauldin, Bernhard Mentler, Ugo Molteni, Antti Onnela, Joschka Pfeifer, Maxim Philippov, Ana A. Piedehierro, Meredith Schervish, Wiebke Scholz, Benjamin Schulze, Jiali Shen, Dominik Stolzenburg, Yuri Stozhkov, Mihnea Surdu, Christian Tauber, Yee Jun Tham, Ping Tian, António Tomé, Steffen Vogt, Mingyi Wang, Dongyu S. Wang, Stefan K. Weber, André Welti, Wang Yonghong, Wu Yusheng, Marcel Zauner-Wieczorek, Urs Baltensperger, Imad El Haddad, Richard C. Flagan, Armin Hansel, Kristina Höhler, Jasper Kirkby, Markku Kulmala, Katrianne Lehtipalo, Ottmar Möhler, Harald Saathoff, Rainer Volkamer, Paul M. Winkler, Neil M. Donahue, Andreas Kürten, and Joachim Curtius
Atmos. Chem. Phys., 21, 17099–17114, https://doi.org/10.5194/acp-21-17099-2021, https://doi.org/10.5194/acp-21-17099-2021, 2021
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We performed experiments in the CLOUD chamber at CERN at low temperatures to simulate new particle formation in the upper free troposphere (at −30 ºC and −50 ºC). We measured the particle and gas phase and found that most of the compounds present in the gas phase are detected as well in the particle phase. The major compounds in the particles are C8–10 and C18–20. Specifically, we showed that C5 and C15 compounds are detected in a mixed system with isoprene and α-pinene at −30 ºC, 20 % RH.
Margarita Choulga, Greet Janssens-Maenhout, Ingrid Super, Efisio Solazzo, Anna Agusti-Panareda, Gianpaolo Balsamo, Nicolas Bousserez, Monica Crippa, Hugo Denier van der Gon, Richard Engelen, Diego Guizzardi, Jeroen Kuenen, Joe McNorton, Gabriel Oreggioni, and Antoon Visschedijk
Earth Syst. Sci. Data, 13, 5311–5335, https://doi.org/10.5194/essd-13-5311-2021, https://doi.org/10.5194/essd-13-5311-2021, 2021
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People worry that growing man-made carbon dioxide (CO2) concentrations lead to climate change. Global models, use of observations, and datasets can help us better understand behaviour of CO2. Here a tool to compute uncertainty in man-made CO2 sources per country per year and month is presented. An example of all sources separated into seven groups (intensive and average energy, industry, humans, ground and air transport, others) is presented. Results will be used to predict CO2 concentrations.
Xinyuan Hou, Martin Wild, Doris Folini, Stelios Kazadzis, and Jan Wohland
Earth Syst. Dynam., 12, 1099–1113, https://doi.org/10.5194/esd-12-1099-2021, https://doi.org/10.5194/esd-12-1099-2021, 2021
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Solar photovoltaics (PV) matters for the carbon neutrality goal. We use climate scenarios to quantify climate risk for PV in Europe and find higher PV potential. The seasonal cycle of PV generation changes in most places. We find an increase in the spatial correlations of daily PV production, implying that PV power balancing through redistribution will be more difficult in the future. Thus, changes in the spatiotemporal structure of PV generation should be included in power system design.
Mark F. Lunt, Alistair J. Manning, Grant Allen, Tim Arnold, Stéphane J.-B. Bauguitte, Hartmut Boesch, Anita L. Ganesan, Aoife Grant, Carole Helfter, Eiko Nemitz, Simon J. O'Doherty, Paul I. Palmer, Joseph R. Pitt, Chris Rennick, Daniel Say, Kieran M. Stanley, Ann R. Stavert, Dickon Young, and Matt Rigby
Atmos. Chem. Phys., 21, 16257–16276, https://doi.org/10.5194/acp-21-16257-2021, https://doi.org/10.5194/acp-21-16257-2021, 2021
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We present an evaluation of the UK's methane emissions between 2013 and 2020 using a network of tall tower measurement sites. We find emissions that are consistent in both magnitude and trend with the UK's reported emissions, with a declining trend driven by a decrease in emissions from England. The impact of various components of the modelling set-up on these findings are explored through a number of sensitivity studies.
Eshkol Eytan, Ilan Koren, Orit Altaratz, Mark Pinsky, and Alexander Khain
Atmos. Chem. Phys., 21, 16203–16217, https://doi.org/10.5194/acp-21-16203-2021, https://doi.org/10.5194/acp-21-16203-2021, 2021
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Describing cloud mixing processes is among the most challenging fronts in cloud physics. Therefore, the adiabatic fraction (AF) that serves as a mixing measure is a valuable metric. We use high-resolution (10 m) simulations of single clouds with a passive tracer to test the skill of different methods used to derive AF. We highlight a method that is insensitive to the available cloud samples and allows considering microphysical effects on AF estimations in different environmental conditions.
Dongyu S. Wang, Chuan Ping Lee, Jordan E. Krechmer, Francesca Majluf, Yandong Tong, Manjula R. Canagaratna, Julia Schmale, André S. H. Prévôt, Urs Baltensperger, Josef Dommen, Imad El Haddad, Jay G. Slowik, and David M. Bell
Atmos. Meas. Tech., 14, 6955–6972, https://doi.org/10.5194/amt-14-6955-2021, https://doi.org/10.5194/amt-14-6955-2021, 2021
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To understand the sources and fate of particulate matter in the atmosphere, the ability to quantitatively describe its chemical composition is essential. In this work, we developed a calibration method for a state-of-the-art measurement technique without the need for chemical standards. Statistical analyses identified the driving factors behind instrument sensitivity variability towards individual components of particulate matter.
Spiro D. Jorga, Kalliopi Florou, Christos Kaltsonoudis, John K. Kodros, Christina Vasilakopoulou, Manuela Cirtog, Axel Fouqueau, Bénédicte Picquet-Varrault, Athanasios Nenes, and Spyros N. Pandis
Atmos. Chem. Phys., 21, 15337–15349, https://doi.org/10.5194/acp-21-15337-2021, https://doi.org/10.5194/acp-21-15337-2021, 2021
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We test the hypothesis that significant secondary organic aerosol production can take place even during winter nights through the oxidation of the emitted organic vapors by the nitrate radicals produced during the reaction of ozone and nitrogen oxides. Our experiments, using as a starting point the ambient air of an urban area with high biomass burning activity, demonstrate that, even with sunlight, there is 20 %–70 % additional organic aerosol formed in a few hours.
Heather Guy, Ian M. Brooks, Ken S. Carslaw, Benjamin J. Murray, Von P. Walden, Matthew D. Shupe, Claire Pettersen, David D. Turner, Christopher J. Cox, William D. Neff, Ralf Bennartz, and Ryan R. Neely III
Atmos. Chem. Phys., 21, 15351–15374, https://doi.org/10.5194/acp-21-15351-2021, https://doi.org/10.5194/acp-21-15351-2021, 2021
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We present the first full year of surface aerosol number concentration measurements from the central Greenland Ice Sheet. Aerosol concentrations here have a distinct seasonal cycle from those at lower-altitude Arctic sites, which is driven by large-scale atmospheric circulation. Our results can be used to help understand the role aerosols might play in Greenland surface melt through the modification of cloud properties. This is crucial in a rapidly changing region where observations are sparse.
Zane Dedekind, Annika Lauber, Sylvaine Ferrachat, and Ulrike Lohmann
Atmos. Chem. Phys., 21, 15115–15134, https://doi.org/10.5194/acp-21-15115-2021, https://doi.org/10.5194/acp-21-15115-2021, 2021
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The RACLETS campaign combined cloud and snow research to improve the understanding of precipitation formation in clouds. A numerical weather prediction model, COSMO, was used to assess the importance of ice crystal enhancement by ice–ice collisions for cloud properties. We found that the number of ice crystals increased by 1 to 3 orders of magnitude when ice–ice collisions were permitted to occur, reducing localized regions of high precipitation and, thereby, improving the model performance.
Gang Chen, Yulia Sosedova, Francesco Canonaco, Roman Fröhlich, Anna Tobler, Athanasia Vlachou, Kaspar R. Daellenbach, Carlo Bozzetti, Christoph Hueglin, Peter Graf, Urs Baltensperger, Jay G. Slowik, Imad El Haddad, and André S. H. Prévôt
Atmos. Chem. Phys., 21, 15081–15101, https://doi.org/10.5194/acp-21-15081-2021, https://doi.org/10.5194/acp-21-15081-2021, 2021
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A novel, advanced source apportionment technique was applied to a dataset measured in Magadino. Rolling positive matrix factorisation (PMF) allows for retrieving more realistic, time-dependent, and detailed information on organic aerosol sources. The strength of the rolling PMF mechanism is highlighted by comparing it with results derived from conventional seasonal PMF. Overall, this comprehensive interpretation of aerosol chemical speciation monitor data could be a role model for similar work.
Quanfu He, Zheng Fang, Ofir Shoshanim, Steven S. Brown, and Yinon Rudich
Atmos. Chem. Phys., 21, 14927–14940, https://doi.org/10.5194/acp-21-14927-2021, https://doi.org/10.5194/acp-21-14927-2021, 2021
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Rayleigh scattering and absorption cross sections for CO2, N2O, SF6, O2, and CH4 were measured between 307 and 725 nm. New dispersion relations for N2O, SF6, and CH4 in the UV–vis range were derived. This study provides refractive index dispersion relations, scattering, and absorption cross sections which are highly needed for accurate instrument calibration and for improved accuracy of Rayleigh scattering parameterizations for major greenhouse gases in Earth's atmosphere.
Anna K. Tobler, Alicja Skiba, Francesco Canonaco, Griša Močnik, Pragati Rai, Gang Chen, Jakub Bartyzel, Miroslaw Zimnoch, Katarzyna Styszko, Jaroslaw Nęcki, Markus Furger, Kazimierz Różański, Urs Baltensperger, Jay G. Slowik, and Andre S. H. Prevot
Atmos. Chem. Phys., 21, 14893–14906, https://doi.org/10.5194/acp-21-14893-2021, https://doi.org/10.5194/acp-21-14893-2021, 2021
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Kraków is among the cities with the highest particulate matter levels within Europe. We conducted long-term and highly time-resolved measurements of the chemical composition of submicron particlulate matter (PM1). Combined with advanced source apportionment techniques, which allow for time-dependent factor profiles, our results elucidate that traffic and residential heating (biomass burning and coal combustion) as well as oxygenated organic aerosol are the key PM sources in Kraków.
Cheng Wu, David M. Bell, Emelie L. Graham, Sophie Haslett, Ilona Riipinen, Urs Baltensperger, Amelie Bertrand, Stamatios Giannoukos, Janne Schoonbaert, Imad El Haddad, Andre S. H. Prevot, Wei Huang, and Claudia Mohr
Atmos. Chem. Phys., 21, 14907–14925, https://doi.org/10.5194/acp-21-14907-2021, https://doi.org/10.5194/acp-21-14907-2021, 2021
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Night-time reactions of biogenic volatile organic compounds and nitrate radicals can lead to the formation of secondary organic aerosol (BSOANO3). Here, we study the impacts of light exposure on the BSOANO3 from three biogenic precursors. Our results suggest that photolysis causes photodegradation of a substantial fraction of BSOANO3, changes the chemical composition and bulk volatility, and might be a potentially important loss pathway of BSOANO3 during the night-to-day transition.
Mehliyar Sadiq, Paul I. Palmer, Mark F. Lunt, Liang Feng, Ingrid Super, Stijn N. C. Dellaert, and Hugo A. C. Denier van der Gon
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2021-816, https://doi.org/10.5194/acp-2021-816, 2021
Publication in ACP not foreseen
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We make use of high-resolution emission inventory of CO2 and co-emitted tracers, satellite measurements, together with nested atmospheric transport model simulation, to investigate how reactive trace gases such as nitrogen dioxide and carbon monoxide can be used as proxies to determine the combustion contribution to atmospheric CO2 over Europe. We find stronger correlation in ratios of nitrogen dioxide and carbon dioxide between emission and satellite observed and modelled column concentration.
Mao Xiao, Christopher R. Hoyle, Lubna Dada, Dominik Stolzenburg, Andreas Kürten, Mingyi Wang, Houssni Lamkaddam, Olga Garmash, Bernhard Mentler, Ugo Molteni, Andrea Baccarini, Mario Simon, Xu-Cheng He, Katrianne Lehtipalo, Lauri R. Ahonen, Rima Baalbaki, Paulus S. Bauer, Lisa Beck, David Bell, Federico Bianchi, Sophia Brilke, Dexian Chen, Randall Chiu, António Dias, Jonathan Duplissy, Henning Finkenzeller, Hamish Gordon, Victoria Hofbauer, Changhyuk Kim, Theodore K. Koenig, Janne Lampilahti, Chuan Ping Lee, Zijun Li, Huajun Mai, Vladimir Makhmutov, Hanna E. Manninen, Ruby Marten, Serge Mathot, Roy L. Mauldin, Wei Nie, Antti Onnela, Eva Partoll, Tuukka Petäjä, Joschka Pfeifer, Veronika Pospisilova, Lauriane L. J. Quéléver, Matti Rissanen, Siegfried Schobesberger, Simone Schuchmann, Yuri Stozhkov, Christian Tauber, Yee Jun Tham, António Tomé, Miguel Vazquez-Pufleau, Andrea C. Wagner, Robert Wagner, Yonghong Wang, Lena Weitz, Daniela Wimmer, Yusheng Wu, Chao Yan, Penglin Ye, Qing Ye, Qiaozhi Zha, Xueqin Zhou, Antonio Amorim, Ken Carslaw, Joachim Curtius, Armin Hansel, Rainer Volkamer, Paul M. Winkler, Richard C. Flagan, Markku Kulmala, Douglas R. Worsnop, Jasper Kirkby, Neil M. Donahue, Urs Baltensperger, Imad El Haddad, and Josef Dommen
Atmos. Chem. Phys., 21, 14275–14291, https://doi.org/10.5194/acp-21-14275-2021, https://doi.org/10.5194/acp-21-14275-2021, 2021
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Experiments at CLOUD show that in polluted environments new particle formation (NPF) is largely driven by the formation of sulfuric acid–base clusters, stabilized by amines, high ammonia concentrations or lower temperatures. While oxidation products of aromatics can nucleate, they play a minor role in urban NPF. Our experiments span 4 orders of magnitude variation of observed NPF rates in ambient conditions. We provide a framework based on NPF and growth rates to interpret ambient observations.
Aristeidis Voliotis, Yu Wang, Yunqi Shao, Mao Du, Thomas J. Bannan, Carl J. Percival, Spyros N. Pandis, M. Rami Alfarra, and Gordon McFiggans
Atmos. Chem. Phys., 21, 14251–14273, https://doi.org/10.5194/acp-21-14251-2021, https://doi.org/10.5194/acp-21-14251-2021, 2021
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Secondary organic aerosol (SOA) formation from mixtures of volatile precursors can be affected by the molecular interactions of the products. Composition and volatility measurements of SOA formed from mixtures of anthropogenic and biogenic precursors reveal processes that can increase or decrease the SOA volatility. The unique products of the mixture were more oxygenated and less volatile than those from either precursor. Analytical context is provided to explore the SOA volatility in mixtures.
Beth S. Nelson, Gareth J. Stewart, Will S. Drysdale, Mike J. Newland, Adam R. Vaughan, Rachel E. Dunmore, Pete M. Edwards, Alastair C. Lewis, Jacqueline F. Hamilton, W. Joe Acton, C. Nicholas Hewitt, Leigh R. Crilley, Mohammed S. Alam, Ülkü A. Şahin, David C. S. Beddows, William J. Bloss, Eloise Slater, Lisa K. Whalley, Dwayne E. Heard, James M. Cash, Ben Langford, Eiko Nemitz, Roberto Sommariva, Sam Cox, Shivani, Ranu Gadi, Bhola R. Gurjar, James R. Hopkins, Andrew R. Rickard, and James D. Lee
Atmos. Chem. Phys., 21, 13609–13630, https://doi.org/10.5194/acp-21-13609-2021, https://doi.org/10.5194/acp-21-13609-2021, 2021
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Ozone production at an urban site in Delhi is sensitive to volatile organic compound (VOC) concentrations, particularly those of the aromatic, monoterpene, and alkene VOC classes. The change in ozone production by varying atmospheric pollutants according to their sources, as defined in an emissions inventory, is investigated. The study suggests that reducing road transport emissions alone does not reduce reactive VOCs in the atmosphere enough to perturb an increase in ozone production.
Paolo Pelucchi, David Neubauer, and Ulrike Lohmann
Geosci. Model Dev., 14, 5413–5434, https://doi.org/10.5194/gmd-14-5413-2021, https://doi.org/10.5194/gmd-14-5413-2021, 2021
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Stratocumulus are thin clouds whose cloud cover is underestimated in climate models partly due to overly low vertical resolution. We develop a scheme that locally refines the vertical grid based on a physical constraint for the cloud top. Global simulations show that the scheme, implemented only in the radiation routine, can increase stratocumulus cloud cover. However, this effect is poorly propagated to the simulated cloud cover. The scheme's limitations and possible ways forward are discussed.
Gloria Titos, María A. Burgos, Paul Zieger, Lucas Alados-Arboledas, Urs Baltensperger, Anne Jefferson, James Sherman, Ernest Weingartner, Bas Henzing, Krista Luoma, Colin O'Dowd, Alfred Wiedensohler, and Elisabeth Andrews
Atmos. Chem. Phys., 21, 13031–13050, https://doi.org/10.5194/acp-21-13031-2021, https://doi.org/10.5194/acp-21-13031-2021, 2021
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This paper investigates the impact of water uptake on aerosol optical properties, in particular the aerosol light-scattering coefficient. Although in situ measurements are performed at low relative humidity (typically at
RH < 40 %), to address the climatic impact of aerosol particles it is necessary to take into account the effect that water uptake may have on the aerosol optical properties.
Chuan Ping Lee, Mihnea Surdu, David M. Bell, Houssni Lamkaddam, Mingyi Wang, Farnoush Ataei, Victoria Hofbauer, Brandon Lopez, Neil M. Donahue, Josef Dommen, Andre S. H. Prevot, Jay G. Slowik, Dongyu Wang, Urs Baltensperger, and Imad El Haddad
Atmos. Meas. Tech., 14, 5913–5923, https://doi.org/10.5194/amt-14-5913-2021, https://doi.org/10.5194/amt-14-5913-2021, 2021
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Extractive electrospray ionization mass spectrometry (EESI-MS) has been deployed for high throughput online detection of particles with minimal fragmentation. Our study elucidates the extraction mechanism between the particles and electrospray (ES) droplets of different properties. The results show that the extraction rate is likely affected by the coagulation rate between the particles and ES droplets. Once coagulated, the particles undergo complete extraction within the ES droplet.
Vaios Moschos, Martin Gysel-Beer, Robin L. Modini, Joel C. Corbin, Dario Massabò, Camilla Costa, Silvia G. Danelli, Athanasia Vlachou, Kaspar R. Daellenbach, Sönke Szidat, Paolo Prati, André S. H. Prévôt, Urs Baltensperger, and Imad El Haddad
Atmos. Chem. Phys., 21, 12809–12833, https://doi.org/10.5194/acp-21-12809-2021, https://doi.org/10.5194/acp-21-12809-2021, 2021
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This study provides a holistic approach to studying the spectrally resolved light absorption by atmospheric brown carbon (BrC) and black carbon using long time series of daily samples from filter-based measurements. The obtained results provide (1) a better understanding of the aerosol absorption profile and its dependence on BrC and on lensing from less absorbing coatings and (2) an estimation of the most important absorbers at typical European locations.
Janne Lampilahti, Hanna E. Manninen, Tuomo Nieminen, Sander Mirme, Mikael Ehn, Iida Pullinen, Katri Leino, Siegfried Schobesberger, Juha Kangasluoma, Jenni Kontkanen, Emma Järvinen, Riikka Väänänen, Taina Yli-Juuti, Radovan Krejci, Katrianne Lehtipalo, Janne Levula, Aadu Mirme, Stefano Decesari, Ralf Tillmann, Douglas R. Worsnop, Franz Rohrer, Astrid Kiendler-Scharr, Tuukka Petäjä, Veli-Matti Kerminen, Thomas F. Mentel, and Markku Kulmala
Atmos. Chem. Phys., 21, 12649–12663, https://doi.org/10.5194/acp-21-12649-2021, https://doi.org/10.5194/acp-21-12649-2021, 2021
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We studied aerosol particle formation and growth in different parts of the planetary boundary layer at two different locations (Po Valley, Italy, and Hyytiälä, Finland). The observations consist of airborne measurements on board an instrumented Zeppelin and a small airplane combined with comprehensive ground-based measurements.
Tom Dror, Mickaël D. Chekroun, Orit Altaratz, and Ilan Koren
Atmos. Chem. Phys., 21, 12261–12272, https://doi.org/10.5194/acp-21-12261-2021, https://doi.org/10.5194/acp-21-12261-2021, 2021
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A part of continental shallow convective cumulus (Cu) was shown to share properties such as organization and formation over vegetated areas, thus named green Cu. Mechanisms behind the formed patterns are not understood. We use different metrics and an empirical orthogonal function (EOF) to decompose the dataset and quantify organization factors (cloud streets and gravity waves). We show that clouds form a highly organized grid structure over hundreds of kilometers at the field lifetime.
Ernesto Reyes-Villegas, Upasana Panda, Eoghan Darbyshire, James M. Cash, Rutambhara Joshi, Ben Langford, Chiara F. Di Marco, Neil J. Mullinger, Mohammed S. Alam, Leigh R. Crilley, Daniel J. Rooney, W. Joe F. Acton, Will Drysdale, Eiko Nemitz, Michael Flynn, Aristeidis Voliotis, Gordon McFiggans, Hugh Coe, James Lee, C. Nicholas Hewitt, Mathew R. Heal, Sachin S. Gunthe, Tuhin K. Mandal, Bhola R. Gurjar, Shivani, Ranu Gadi, Siddhartha Singh, Vijay Soni, and James D. Allan
Atmos. Chem. Phys., 21, 11655–11667, https://doi.org/10.5194/acp-21-11655-2021, https://doi.org/10.5194/acp-21-11655-2021, 2021
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This paper shows the first multisite online measurements of PM1 in Delhi, India, with measurements over different seasons in Old Delhi and New Delhi in 2018. Organic aerosol (OA) source apportionment was performed using positive matrix factorisation (PMF). Traffic was the main primary aerosol source for both OAs and black carbon, seen with PMF and Aethalometer model analysis, indicating that control of primary traffic exhaust emissions would make a significant reduction to Delhi air pollution.
Kyle B. Delwiche, Sara Helen Knox, Avni Malhotra, Etienne Fluet-Chouinard, Gavin McNicol, Sarah Feron, Zutao Ouyang, Dario Papale, Carlo Trotta, Eleonora Canfora, You-Wei Cheah, Danielle Christianson, Ma. Carmelita R. Alberto, Pavel Alekseychik, Mika Aurela, Dennis Baldocchi, Sheel Bansal, David P. Billesbach, Gil Bohrer, Rosvel Bracho, Nina Buchmann, David I. Campbell, Gerardo Celis, Jiquan Chen, Weinan Chen, Housen Chu, Higo J. Dalmagro, Sigrid Dengel, Ankur R. Desai, Matteo Detto, Han Dolman, Elke Eichelmann, Eugenie Euskirchen, Daniela Famulari, Kathrin Fuchs, Mathias Goeckede, Sébastien Gogo, Mangaliso J. Gondwe, Jordan P. Goodrich, Pia Gottschalk, Scott L. Graham, Martin Heimann, Manuel Helbig, Carole Helfter, Kyle S. Hemes, Takashi Hirano, David Hollinger, Lukas Hörtnagl, Hiroki Iwata, Adrien Jacotot, Gerald Jurasinski, Minseok Kang, Kuno Kasak, John King, Janina Klatt, Franziska Koebsch, Ken W. Krauss, Derrick Y. F. Lai, Annalea Lohila, Ivan Mammarella, Luca Belelli Marchesini, Giovanni Manca, Jaclyn Hatala Matthes, Trofim Maximov, Lutz Merbold, Bhaskar Mitra, Timothy H. Morin, Eiko Nemitz, Mats B. Nilsson, Shuli Niu, Walter C. Oechel, Patricia Y. Oikawa, Keisuke Ono, Matthias Peichl, Olli Peltola, Michele L. Reba, Andrew D. Richardson, William Riley, Benjamin R. K. Runkle, Youngryel Ryu, Torsten Sachs, Ayaka Sakabe, Camilo Rey Sanchez, Edward A. Schuur, Karina V. R. Schäfer, Oliver Sonnentag, Jed P. Sparks, Ellen Stuart-Haëntjens, Cove Sturtevant, Ryan C. Sullivan, Daphne J. Szutu, Jonathan E. Thom, Margaret S. Torn, Eeva-Stiina Tuittila, Jessica Turner, Masahito Ueyama, Alex C. Valach, Rodrigo Vargas, Andrej Varlagin, Alma Vazquez-Lule, Joseph G. Verfaillie, Timo Vesala, George L. Vourlitis, Eric J. Ward, Christian Wille, Georg Wohlfahrt, Guan Xhuan Wong, Zhen Zhang, Donatella Zona, Lisamarie Windham-Myers, Benjamin Poulter, and Robert B. Jackson
Earth Syst. Sci. Data, 13, 3607–3689, https://doi.org/10.5194/essd-13-3607-2021, https://doi.org/10.5194/essd-13-3607-2021, 2021
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Methane is an important greenhouse gas, yet we lack knowledge about its global emissions and drivers. We present FLUXNET-CH4, a new global collection of methane measurements and a critical resource for the research community. We use FLUXNET-CH4 data to quantify the seasonality of methane emissions from freshwater wetlands, finding that methane seasonality varies strongly with latitude. Our new database and analysis will improve wetland model accuracy and inform greenhouse gas budgets.
Toprak Aslan, Olli Peltola, Andreas Ibrom, Eiko Nemitz, Üllar Rannik, and Ivan Mammarella
Atmos. Meas. Tech., 14, 5089–5106, https://doi.org/10.5194/amt-14-5089-2021, https://doi.org/10.5194/amt-14-5089-2021, 2021
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Vertical turbulent fluxes of gases measured by the eddy covariance (EC) technique are subject to high-frequency losses. There are different methods used to describe this low-pass filtering effect and to correct the measured fluxes. In this study, we analysed the systematic uncertainty related to this correction for various attenuation and signal-to-noise ratios. A new and robust transfer function method is finally proposed.
Olli Peltola, Toprak Aslan, Andreas Ibrom, Eiko Nemitz, Üllar Rannik, and Ivan Mammarella
Atmos. Meas. Tech., 14, 5071–5088, https://doi.org/10.5194/amt-14-5071-2021, https://doi.org/10.5194/amt-14-5071-2021, 2021
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Gas fluxes measured by the eddy covariance (EC) technique are subject to filtering due to non-ideal instrumentation. For linear first-order systems this filtering causes also a time lag between vertical wind speed and gas signal which is additional to the gas travel time in the sampling line. The effect of this additional time lag on EC fluxes is ignored in current EC data processing routines. Here we show that this oversight biases EC fluxes and hence propose an approach to rectify this bias.
Congbo Song, Manuel Dall'Osto, Angelo Lupi, Mauro Mazzola, Rita Traversi, Silvia Becagli, Stefania Gilardoni, Stergios Vratolis, Karl Espen Yttri, David C. S. Beddows, Julia Schmale, James Brean, Agung Ghani Kramawijaya, Roy M. Harrison, and Zongbo Shi
Atmos. Chem. Phys., 21, 11317–11335, https://doi.org/10.5194/acp-21-11317-2021, https://doi.org/10.5194/acp-21-11317-2021, 2021
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We present a cluster analysis of relatively long-term (2015–2019) aerosol aerodynamic volume size distributions up to 20 μm in the Arctic for the first time. The study found that anthropogenic and natural aerosols comprised 27 % and 73 % of the occurrence of the coarse-mode aerosols, respectively. Our study shows that about two-thirds of the coarse-mode aerosols are related to two sea-spray-related aerosol clusters, indicating that sea spray aerosol may more complex in the Arctic environment.
Paraskevi Georgakaki, Aikaterini Bougiatioti, Jörg Wieder, Claudia Mignani, Fabiola Ramelli, Zamin A. Kanji, Jan Henneberger, Maxime Hervo, Alexis Berne, Ulrike Lohmann, and Athanasios Nenes
Atmos. Chem. Phys., 21, 10993–11012, https://doi.org/10.5194/acp-21-10993-2021, https://doi.org/10.5194/acp-21-10993-2021, 2021
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Aerosol and cloud observations coupled with a droplet activation parameterization was used to investigate the aerosol–cloud droplet link in alpine mixed-phase clouds. Predicted droplet number, Nd, agrees with observations and never exceeds a characteristic “limiting droplet number”, Ndlim, which depends solely on σw. Nd becomes velocity limited when it is within 50 % of Ndlim. Identifying when dynamical changes control Nd variability is central for understanding aerosol–cloud interactions.
Ramiro Checa-Garcia, Yves Balkanski, Samuel Albani, Tommi Bergman, Ken Carslaw, Anne Cozic, Chris Dearden, Beatrice Marticorena, Martine Michou, Twan van Noije, Pierre Nabat, Fiona M. O'Connor, Dirk Olivié, Joseph M. Prospero, Philippe Le Sager, Michael Schulz, and Catherine Scott
Atmos. Chem. Phys., 21, 10295–10335, https://doi.org/10.5194/acp-21-10295-2021, https://doi.org/10.5194/acp-21-10295-2021, 2021
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Thousands of tons of dust are emitted into the atmosphere every year, producing important impacts on the Earth system. However, current global climate models are not yet able to reproduce dust emissions, transport and depositions with the desirable accuracy. Our study analyses five different Earth system models to report aspects to be improved to reproduce better available observations, increase the consistency between models and therefore decrease the current uncertainties.
James M. Cash, Ben Langford, Chiara Di Marco, Neil J. Mullinger, James Allan, Ernesto Reyes-Villegas, Ruthambara Joshi, Mathew R. Heal, W. Joe F. Acton, C. Nicholas Hewitt, Pawel K. Misztal, Will Drysdale, Tuhin K. Mandal, Shivani, Ranu Gadi, Bhola Ram Gurjar, and Eiko Nemitz
Atmos. Chem. Phys., 21, 10133–10158, https://doi.org/10.5194/acp-21-10133-2021, https://doi.org/10.5194/acp-21-10133-2021, 2021
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We present the first real-time composition of submicron particulate matter (PM1) in Old Delhi using high-resolution aerosol mass spectrometry. Seasonal analysis shows peak concentrations occur during the post-monsoon, and novel-tracers reveal the largest sources are a combination of local open and regional crop residue burning. Strong links between increased chloride aerosol concentrations and burning sources of PM1 suggest burning sources are responsible for the post-monsoon chloride peak.
Yandong Tong, Veronika Pospisilova, Lu Qi, Jing Duan, Yifang Gu, Varun Kumar, Pragati Rai, Giulia Stefenelli, Liwei Wang, Ying Wang, Haobin Zhong, Urs Baltensperger, Junji Cao, Ru-Jin Huang, André S. H. Prévôt, and Jay G. Slowik
Atmos. Chem. Phys., 21, 9859–9886, https://doi.org/10.5194/acp-21-9859-2021, https://doi.org/10.5194/acp-21-9859-2021, 2021
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We investigate SOA sources and formation processes by a field deployment of the EESI-TOF-MS and L-TOF AMS in Beijing in late autumn and early winter. Our study shows that the sources and processes giving rise to haze events in Beijing are variable and seasonally dependent: (1) in the heating season, SOA formation is driven by oxidation of aromatics from solid fuel combustion; and (2) under high-NOx and RH conditions, aqueous-phase chemistry can be a major contributor to SOA formation.
Ana Maria Roxana Petrescu, Matthew J. McGrath, Robbie M. Andrew, Philippe Peylin, Glen P. Peters, Philippe Ciais, Gregoire Broquet, Francesco N. Tubiello, Christoph Gerbig, Julia Pongratz, Greet Janssens-Maenhout, Giacomo Grassi, Gert-Jan Nabuurs, Pierre Regnier, Ronny Lauerwald, Matthias Kuhnert, Juraj Balkovič, Mart-Jan Schelhaas, Hugo A. C. Denier van der
Gon, Efisio Solazzo, Chunjing Qiu, Roberto Pilli, Igor B. Konovalov, Richard A. Houghton, Dirk Günther, Lucia Perugini, Monica Crippa, Raphael Ganzenmüller, Ingrid T. Luijkx, Pete Smith, Saqr Munassar, Rona L. Thompson, Giulia Conchedda, Guillaume Monteil, Marko Scholze, Ute Karstens, Patrick Brockmann, and Albertus Johannes Dolman
Earth Syst. Sci. Data, 13, 2363–2406, https://doi.org/10.5194/essd-13-2363-2021, https://doi.org/10.5194/essd-13-2363-2021, 2021
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This study is topical and provides a state-of-the-art scientific overview of data availability from bottom-up and top-down CO2 fossil emissions and CO2 land fluxes in the EU27+UK. The data integrate recent emission inventories with ecosystem data, land carbon models and regional/global inversions for the European domain, aiming at reconciling CO2 estimates with official country-level UNFCCC national GHG inventories in support to policy and facilitating real-time verification procedures.
Robbie Ramsay, Chiara F. Di Marco, Mathew R. Heal, Matthias Sörgel, Paulo Artaxo, Meinrat O. Andreae, and Eiko Nemitz
Biogeosciences, 18, 2809–2825, https://doi.org/10.5194/bg-18-2809-2021, https://doi.org/10.5194/bg-18-2809-2021, 2021
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The exchange of the gas ammonia between the atmosphere and the surface is an important biogeochemical process, but little is known of this exchange for certain ecosystems, such as the Amazon rainforest. This study took measurements of ammonia exchange over an Amazon rainforest site and subsequently modelled the observed deposition and emission patterns. We observed emissions of ammonia from the rainforest, which can be simulated accurately by using a canopy resistance modelling approach.
Fabiola Ramelli, Jan Henneberger, Robert O. David, Johannes Bühl, Martin Radenz, Patric Seifert, Jörg Wieder, Annika Lauber, Julie T. Pasquier, Ronny Engelmann, Claudia Mignani, Maxime Hervo, and Ulrike Lohmann
Atmos. Chem. Phys., 21, 6681–6706, https://doi.org/10.5194/acp-21-6681-2021, https://doi.org/10.5194/acp-21-6681-2021, 2021
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Orographic mixed-phase clouds are an important source of precipitation, but the ice formation processes within them remain uncertain. Here we investigate the origin of ice crystals in a mixed-phase cloud in the Swiss Alps using aerosol and cloud data from in situ and remote sensing observations. We found that ice formation primarily occurs in cloud top generating cells. Our results indicate that secondary ice processes are active in the feeder region, which can enhance orographic precipitation.
Marcia Akemi Yamasoe, Nilton Manuel Évora Rosário, Samantha Novaes Santos Martins Almeida, and Martin Wild
Atmos. Chem. Phys., 21, 6593–6603, https://doi.org/10.5194/acp-21-6593-2021, https://doi.org/10.5194/acp-21-6593-2021, 2021
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Spatio-temporal disparity to assess global dimming and brightening phenomena has been a critical topic. For instance, few studies addressed surface solar irradiation (SSR) long-term trend in South America. In this study, SSR, sunshine duration (SD) and the diurnal temperature range (DTR) are analysed for São Paulo, Brazil. We found a dimming phase, identified by SSR, SD and DTR, extending till 1983. Then, while SSR is still declining, consistent with cloud increasing, SD and DTR are increasing.
Athanasios Nenes, Spyros N. Pandis, Maria Kanakidou, Armistead G. Russell, Shaojie Song, Petros Vasilakos, and Rodney J. Weber
Atmos. Chem. Phys., 21, 6023–6033, https://doi.org/10.5194/acp-21-6023-2021, https://doi.org/10.5194/acp-21-6023-2021, 2021
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Ecosystems and air quality are affected by the dry deposition of inorganic reactive nitrogen (Nr, the sum of ammonium and nitrate). Its large variability is driven by the large difference in deposition velocity of N when in the gas or particle phase. Here we show that aerosol liquid water and acidity, by affecting gas–particle partitioning, modulate the dry deposition velocity of NH3, HNO3, and Nr worldwide. These effects explain the rapid accumulation of nitrate aerosol during haze events.
Georgia N. Theodoritsi, Giancarlo Ciarelli, and Spyros N. Pandis
Geosci. Model Dev., 14, 2041–2055, https://doi.org/10.5194/gmd-14-2041-2021, https://doi.org/10.5194/gmd-14-2041-2021, 2021
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Two schemes based on the volatility basis set were used for the simulation of biomass burning organic aerosol (bbOA) in the continental US. The first is the default scheme of the PMCAMx-SR model, and the second is a recently developed scheme based on laboratory experiments. The alternative bbOA scheme predicts much higher concentrations. The default scheme performed better during summer and fall, while the alternative scheme was a little better during spring.
Rachel E. Hawker, Annette K. Miltenberger, Jonathan M. Wilkinson, Adrian A. Hill, Ben J. Shipway, Zhiqiang Cui, Richard J. Cotton, Ken S. Carslaw, Paul R. Field, and Benjamin J. Murray
Atmos. Chem. Phys., 21, 5439–5461, https://doi.org/10.5194/acp-21-5439-2021, https://doi.org/10.5194/acp-21-5439-2021, 2021
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The impact of aerosols on clouds is a large source of uncertainty for future climate projections. Our results show that the radiative properties of a complex convective cloud field in the Saharan outflow region are sensitive to the temperature dependence of ice-nucleating particle concentrations. This means that differences in the aerosol source or composition, for the same aerosol size distribution, can cause differences in the outgoing radiation from regions dominated by tropical convection.
Weiqi Xu, Chun Chen, Yanmei Qiu, Ying Li, Zhiqiang Zhang, Eleni Karnezi, Spyros N. Pandis, Conghui Xie, Zhijie Li, Jiaxing Sun, Nan Ma, Wanyun Xu, Pingqing Fu, Zifa Wang, Jiang Zhu, Douglas R. Worsnop, Nga Lee Ng, and Yele Sun
Atmos. Chem. Phys., 21, 5463–5476, https://doi.org/10.5194/acp-21-5463-2021, https://doi.org/10.5194/acp-21-5463-2021, 2021
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Here aerosol volatility and viscosity at a rural site (Gucheng) and an urban site (Beijing) in the North China Plain (NCP) were investigated in summer and winter. Our results showed that organic aerosol (OA) in winter in the NCP is more volatile than that in summer due to enhanced primary emissions from coal combustion and biomass burning. We also found that OA existed mainly as a solid in winter in Beijing but as semisolids in Beijing in summer and Gucheng in winter.
Fabiola Ramelli, Jan Henneberger, Robert O. David, Annika Lauber, Julie T. Pasquier, Jörg Wieder, Johannes Bühl, Patric Seifert, Ronny Engelmann, Maxime Hervo, and Ulrike Lohmann
Atmos. Chem. Phys., 21, 5151–5172, https://doi.org/10.5194/acp-21-5151-2021, https://doi.org/10.5194/acp-21-5151-2021, 2021
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Interactions between dynamics, microphysics and orography can enhance precipitation. Yet the exact role of these interactions is still uncertain. Here we investigate the role of low-level blocking and turbulence for precipitation by combining remote sensing and in situ observations. The observations show that blocked flow can induce the formation of feeder clouds and that turbulence can enhance hydrometeor growth, demonstrating the importance of local flow effects for orographic precipitation.
Ulrike Proske, Verena Bessenbacher, Zane Dedekind, Ulrike Lohmann, and David Neubauer
Atmos. Chem. Phys., 21, 5195–5216, https://doi.org/10.5194/acp-21-5195-2021, https://doi.org/10.5194/acp-21-5195-2021, 2021
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Ice crystals falling out of one cloud can initiate freezing in a second cloud below. We estimate the occurrence frequency of this natural cloud seeding over Switzerland from satellite data and sublimation calculations. We find that such situations with an ice cloud above another cloud are frequent and that the falling crystals survive the fall between two clouds in a significant number of cases, suggesting that natural cloud seeding is an important phenomenon over Switzerland.
Ananth Ranjithkumar, Hamish Gordon, Christina Williamson, Andrew Rollins, Kirsty Pringle, Agnieszka Kupc, Nathan Luke Abraham, Charles Brock, and Ken Carslaw
Atmos. Chem. Phys., 21, 4979–5014, https://doi.org/10.5194/acp-21-4979-2021, https://doi.org/10.5194/acp-21-4979-2021, 2021
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The effect aerosols have on climate can be better understood by studying their vertical and spatial distribution throughout the atmosphere. We use observation data from the ATom campaign and evaluate the vertical profile of aerosol number concentration, sulfur dioxide and condensation sink using the UKESM (UK Earth System Model). We identify uncertainties in key atmospheric processes that help improve their theoretical representation in global climate models.
Jianhui Jiang, Imad El Haddad, Sebnem Aksoyoglu, Giulia Stefenelli, Amelie Bertrand, Nicolas Marchand, Francesco Canonaco, Jean-Eudes Petit, Olivier Favez, Stefania Gilardoni, Urs Baltensperger, and André S. H. Prévôt
Geosci. Model Dev., 14, 1681–1697, https://doi.org/10.5194/gmd-14-1681-2021, https://doi.org/10.5194/gmd-14-1681-2021, 2021
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We developed a box model with a volatility basis set to simulate organic aerosol (OA) from biomass burning and optimized the vapor-wall-loss-corrected OA yields with a genetic algorithm. The optimized parameterizations were then implemented in the air quality model CAMx v6.5. Comparisons with ambient measurements indicate that the vapor-wall-loss-corrected parameterization effectively improves the model performance in predicting OA, which reduced the mean fractional bias from −72.9 % to −1.6 %.
Annika Lauber, Jan Henneberger, Claudia Mignani, Fabiola Ramelli, Julie T. Pasquier, Jörg Wieder, Maxime Hervo, and Ulrike Lohmann
Atmos. Chem. Phys., 21, 3855–3870, https://doi.org/10.5194/acp-21-3855-2021, https://doi.org/10.5194/acp-21-3855-2021, 2021
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An accurate prediction of the ice crystal number concentration (ICNC) is important to determine the radiation budget, lifetime, and precipitation formation of clouds. Even though secondary-ice processes can increase the ICNC by several orders of magnitude, they are poorly constrained and lack a well-founded quantification. During measurements on a mountain slope, a high ICNC of small ice crystals was observed just below 0 °C, attributed to a secondary-ice process and parametrized in this study.