Articles | Volume 16, issue 4
03 Mar 2016
Research article | 03 Mar 2016
Understanding cirrus ice crystal number variability for different heterogeneous ice nucleation spectra
Sylvia C. Sullivan et al.
No articles found.
Stylianos Kakavas, Spyros Pandis, and Athanasios Nenes
Atmos. Chem. Phys. Discuss.,
Preprint under review for ACPShort summary
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 year-long aerosol simulations over the continental US. We show that such organic water impacts can have an important impact on dry PM1 levels when RH levels and PM1 concentrations are high.
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. Discuss.,
Revised manuscript under review for ACPShort summary
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.
Emily D. Lenhardt, Lan Gao, Jens Redemann, Feng Xu, Sharon P. Burton, Brian Cairns, Ian Chang, Richard A. Ferrare, Chris A. Hostetler, Pablo E. Saide, Calvin Howes, Yohei Shinozuka, Snorre Stamnes, Mary Kacarab, Amie Dobracki, Jenny Wong, Steffen Freitag, and Athanasios Nenes
Atmos. Meas. Tech. Discuss.,
Preprint under review for AMTShort summary
Small atmospheric particles, such as smoke from wildfires or pollutants from human activities, impact cloud properties, and clouds have a strong influence on climate change. To better understand the distributions of these particles, we develop relationships to derive their concentrations from remote sensing measurements from an instrument called a lidar. Our method is reliable for smoke particles, and similar steps can be taken to develop similar relationships for other particle types.
Marios Chatziparaschos, Nikos Daskalakis, Stelios Myriokefalitakis, Nikos Kalivitis, Athanasios Nenes, Maria Gonçalves Ageitos, Montserrat Costa-Surós, Carlos Pérez García-Pando, Medea Zanoli, Mihalis Vrekoussis, and Maria Kanakidou
Atmos. Chem. Phys. Discuss.,
Revised manuscript accepted for ACPShort summary
Ice formation is enabled by Ice Nucleating Particles (INP) at higher temperatures than homogeneous formation and can profoundly affect the properties of clouds. Our global model results show that additionally to k-feldspar dust mineral that is globally the most important INP precursor, quartz, which is abundant in mineral dust, can be regionally significant, affecting different cloud level regimes (low-level clouds) than K-feldspar (mid-level clouds).
Caroline Dang, Michal Segal-Rozenhaimer, Haochi Che, Lu Zhang, Paola Formenti, Jonathan Taylor, Amie Dobracki, Sara Purdue, Pui-Shan Wong, Athanasios Nenes, Arthur Sedlacek III, Hugh Coe, Jens Redemann, Paquita Zuidema, Steven Howell, and James Haywood
Atmos. Chem. Phys., 22, 9389–9412,Short summary
Transmission electron microscopy was used to analyze aged African smoke particles and how the smoke interacts with the marine atmosphere. We found that the volatility of organic aerosol increases with biomass burning plume age, that black carbon is often mixed with potassium salts and that the marine atmosphere can incorporate Na and Cl into smoke particles. Marine salts are more processed when mixed with smoke plumes, and there are interesting Cl-rich yet Na-absent marine particles.
Lu Zhang, Michal Segal-Rozenhaimer, Haochi Che, Caroline Dang, Arthur J. Sedlacek III, Ernie R. Lewis, Amie Dobracki, Jenny P. S. Wong, Paola Formenti, Steven G. Howell, and Athanasios Nenes
Atmos. Chem. Phys., 22, 9199–9213,Short summary
Widespread biomass burning (BB) events occur annually in Africa and contribute ~ 1 / 3 of global BB emissions, which contain a large family of light-absorbing organics, known as brown carbon (BrC), whose absorption of incident radiation is difficult to estimate, leading to large uncertainties in the global radiative forcing estimation. This study quantifies the BrC absorption of aged BB particles and highlights the potential presence of absorbing iron oxides in this climatically important region.
Stelios Myriokefalitakis, Elisa Bergas-Massó, María Gonçalves-Ageitos, Carlos Pérez García-Pando, Twan van Noije, Philippe Le Sager, Akinori Ito, Eleni Athanasopoulou, Athanasios Nenes, Maria Kanakidou, Maarten C. Krol, and Evangelos Gerasopoulos
Geosci. Model Dev., 15, 3079–3120,Short summary
We here describe the implementation of atmospheric multiphase processes in the EC-Earth Earth system model. We provide global budgets of oxalate, sulfate, and iron-containing aerosols, along with an analysis of the links among atmospheric composition, aqueous-phase processes, and aerosol dissolution, supported by comparison to observations. This work is a first step towards an interactive calculation of the deposition of bioavailable atmospheric iron coupled to the model’s ocean component.
Ehud Strobach, Andrea Molod, Donifan Barahona, Atanas Trayanov, Dimitris Menemenlis, and Gael Forget
Geosci. Model Dev., 15, 2309–2324,Short summary
The Green's functions methodology offers a systematic, easy-to-implement, computationally cheap, scalable, and extendable method to tune uncertain parameters in models accounting for the dependent response of the model to a change in various parameters. Herein, we successfully show for the first time that long-term errors in earth system models can be considerably reduced using Green's functions methodology. The method can be easily applied to any model containing uncertain parameters.
Paraskevi Georgakaki, Georgia Sotiropoulou, Étienne Vignon, Anne-Claire Billault-Roux, Alexis Berne, and Athanasios Nenes
Atmos. Chem. Phys., 22, 1965–1988,Short summary
The modelling study focuses on the importance of ice multiplication processes in orographic mixed-phase clouds, which is one of the least understood cloud types in the climate system. We show that the consideration of ice seeding and secondary ice production through ice–ice collisional breakup is essential for correct predictions of precipitation in mountainous terrain, with important implications for radiation processes.
Irini Tsiodra, Georgios Grivas, Kalliopi Tavernaraki, Aikaterini Bougiatioti, Maria Apostolaki, Despina Paraskevopoulou, Alexandra Gogou, Constantine Parinos, Konstantina Oikonomou, Maria Tsagkaraki, Pavlos Zarmpas, Athanasios Nenes, and Nikolaos Mihalopoulos
Atmos. Chem. Phys., 21, 17865–17883,Short summary
We analyze observations from year-long measurements at Athens, Greece. Nighttime wintertime PAH levels are 4 times higher than daytime, and wintertime values are 15 times higher than summertime. Biomass burning aerosol during wintertime pollution events is responsible for these significant wintertime enhancements and accounts for 43 % of the population exposure to PAH carcinogenic risk. Biomass burning poses additional health risks beyond those associated with the high PM levels that develop.
Mária Lbadaoui-Darvas, Satoshi Takahama, and Athanasios Nenes
Atmos. Chem. Phys., 21, 17687–17714,Short summary
Aerosol–cloud interactions constitute the most uncertain contribution to climate change. The uptake kinetics of water by aerosol is a central process of cloud droplet formation, yet its molecular-scale mechanism is unknown. We use molecular simulations to study this process for phase-separated organic particles. Our results explain the increased cloud condensation activity of such particles and can be generalized over various compositions, thus possibly serving as a basis for future models.
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,Short summary
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.
Huisheng Bian, Eunjee Lee, Randal D. Koster, Donifan Barahona, Mian Chin, Peter R. Colarco, Anton Darmenov, Sarith Mahanama, Michael Manyin, Peter Norris, John Shilling, Hongbin Yu, and Fanwei Zeng
Atmos. Chem. Phys., 21, 14177–14197,Short summary
The study using the NASA Earth system model shows ~2.6 % increase in burning season gross primary production and ~1.5 % increase in annual net primary production across the Amazon Basin during 2010–2016 due to the change in surface downward direct and diffuse photosynthetically active radiation by biomass burning aerosols. Such an aerosol effect is strongly dependent on the presence of clouds. The cloud fraction at which aerosols switch from stimulating to inhibiting plant growth occurs at ~0.8.
Andreas Tilgner, Thomas Schaefer, Becky Alexander, Mary Barth, Jeffrey L. Collett Jr., Kathleen M. Fahey, Athanasios Nenes, Havala O. T. Pye, Hartmut Herrmann, and V. Faye McNeill
Atmos. Chem. Phys., 21, 13483–13536,Short summary
Feedbacks of acidity and atmospheric multiphase chemistry in deliquesced particles and clouds are crucial for the tropospheric composition, depositions, climate, and human health. This review synthesizes the current scientific knowledge on these feedbacks using both inorganic and organic aqueous-phase chemistry. Finally, this review outlines atmospheric implications and highlights the need for future investigations with respect to reducing emissions of key acid precursors in a changing world.
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,Short summary
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.
Georgia Sotiropoulou, Luisa Ickes, Athanasios Nenes, and Annica M. L. Ekman
Atmos. Chem. Phys., 21, 9741–9760,Short summary
Mixed-phase clouds are a large source of uncertainty in projections of the Arctic climate. This is partly due to the poor representation of the cloud ice formation processes. Implementing a parameterization for ice multiplication due to mechanical breakup upon collision of two ice particles in a high-resolution model improves cloud ice phase representation; however, cloud liquid remains overestimated.
Katherine H. Breen, Donifan Barahona, Tianle Yuan, Huisheng Bian, and Scott C. James
Atmos. Chem. Phys., 21, 7749–7771,Short summary
Increases in atmospheric aerosols affect the scattering and absorption of solar radiation by altering the macrophysical and microphysical processes of clouds. We analyzed aerosol–cloud interactions in response to degassing events from the Kilauea volcano in 2008 and 2018 by comparing satellite and simulated cloud properties. Results showed a threshold response to overcome meteorological effects that is largely controlled by aerosol concentration, composition, plume height, and ENSO state.
Athanasios Nenes, Spyros N. Pandis, Maria Kanakidou, Armistead G. Russell, Shaojie Song, Petros Vasilakos, and Rodney J. Weber
Atmos. Chem. Phys., 21, 6023–6033,Short summary
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.
Yilin Chen, Huizhong Shen, Jennifer Kaiser, Yongtao Hu, Shannon L. Capps, Shunliu Zhao, Amir Hakami, Jhih-Shyang Shih, Gertrude K. Pavur, Matthew D. Turner, Daven K. Henze, Jaroslav Resler, Athanasios Nenes, Sergey L. Napelenok, Jesse O. Bash, Kathleen M. Fahey, Gregory R. Carmichael, Tianfeng Chai, Lieven Clarisse, Pierre-François Coheur, Martin Van Damme, and Armistead G. Russell
Atmos. Chem. Phys., 21, 2067–2082,Short summary
Ammonia (NH3) emissions can exert adverse impacts on air quality and ecosystem well-being. NH3 emission inventories are viewed as highly uncertain. Here we optimize the NH3 emission estimates in the US using an air quality model and NH3 measurements from the IASI satellite instruments. The optimized NH3 emissions are much higher than the National Emissions Inventory estimates in April. The optimized NH3 emissions improved model performance when evaluated against independent observation.
Jens Redemann, Robert Wood, Paquita Zuidema, Sarah J. Doherty, Bernadette Luna, Samuel E. LeBlanc, Michael S. Diamond, Yohei Shinozuka, Ian Y. Chang, Rei Ueyama, Leonhard Pfister, Ju-Mee Ryoo, Amie N. Dobracki, Arlindo M. da Silva, Karla M. Longo, Meloë S. Kacenelenbogen, Connor J. Flynn, Kristina Pistone, Nichola M. Knox, Stuart J. Piketh, James M. Haywood, Paola Formenti, Marc Mallet, Philip Stier, Andrew S. Ackerman, Susanne E. Bauer, Ann M. Fridlind, Gregory R. Carmichael, Pablo E. Saide, Gonzalo A. Ferrada, Steven G. Howell, Steffen Freitag, Brian Cairns, Brent N. Holben, Kirk D. Knobelspiesse, Simone Tanelli, Tristan S. L'Ecuyer, Andrew M. Dzambo, Ousmane O. Sy, Greg M. McFarquhar, Michael R. Poellot, Siddhant Gupta, Joseph R. O'Brien, Athanasios Nenes, Mary Kacarab, Jenny P. S. Wong, Jennifer D. Small-Griswold, Kenneth L. Thornhill, David Noone, James R. Podolske, K. Sebastian Schmidt, Peter Pilewskie, Hong Chen, Sabrina P. Cochrane, Arthur J. Sedlacek, Timothy J. Lang, Eric Stith, Michal Segal-Rozenhaimer, Richard A. Ferrare, Sharon P. Burton, Chris A. Hostetler, David J. Diner, Felix C. Seidel, Steven E. Platnick, Jeffrey S. Myers, Kerry G. Meyer, Douglas A. Spangenberg, Hal Maring, and Lan Gao
Atmos. Chem. Phys., 21, 1507–1563,Short summary
Southern Africa produces significant biomass burning emissions whose impacts on regional and global climate are poorly understood. ORACLES (ObseRvations of Aerosols above CLouds and their intEractionS) is a 5-year NASA investigation designed to study the key processes that determine these climate impacts. The main purpose of this paper is to familiarize the broader scientific community with the ORACLES project, the dataset it produced, and the most important initial findings.
Stylianos Kakavas, David Patoulias, Maria Zakoura, Athanasios Nenes, and Spyros N. Pandis
Atmos. Chem. Phys., 21, 799–811,Short summary
The dependence of aerosol acidity on particle size, location, and altitude over Europe during a summertime period is investigated. Differences of up to 1–4 pH units are predicted between sub- and supermicron particles in northern and southern Europe. Particles of all sizes become increasingly acidic with altitude (0.5–2.5 pH units decrease over 2.5 km). The size-dependent pH differences carry important implications for pH-sensitive processes in the aerosol.
Georgia Sotiropoulou, Étienne Vignon, Gillian Young, Hugh Morrison, Sebastian J. O'Shea, Thomas Lachlan-Cope, Alexis Berne, and Athanasios Nenes
Atmos. Chem. Phys., 21, 755–771,Short summary
Summer clouds have a significant impact on the radiation budget of the Antarctic surface and thus on ice-shelf melting. However, these are poorly represented in climate models due to errors in their microphysical structure, including the number of ice crystals that they contain. We show that breakup from ice particle collisions can substantially magnify the ice crystal number concentration with significant implications for surface radiation. This process is currently missing in climate models.
Johannes Quaas, Antti Arola, Brian Cairns, Matthew Christensen, Hartwig Deneke, Annica M. L. Ekman, Graham Feingold, Ann Fridlind, Edward Gryspeerdt, Otto Hasekamp, Zhanqing Li, Antti Lipponen, Po-Lun Ma, Johannes Mülmenstädt, Athanasios Nenes, Joyce E. Penner, Daniel Rosenfeld, Roland Schrödner, Kenneth Sinclair, Odran Sourdeval, Philip Stier, Matthias Tesche, Bastiaan van Diedenhoven, and Manfred Wendisch
Atmos. Chem. Phys., 20, 15079–15099,Short summary
Anthropogenic pollution particles – aerosols – serve as cloud condensation nuclei and thus increase cloud droplet concentration and the clouds' reflection of sunlight (a cooling effect on climate). This Twomey effect is poorly constrained by models and requires satellite data for better quantification. The review summarizes the challenges in properly doing so and outlines avenues for progress towards a better use of aerosol retrievals and better retrievals of droplet concentrations.
Ari Laaksonen, Jussi Malila, and Athanasios Nenes
Atmos. Chem. Phys., 20, 13579–13589,Short summary
Aerosol particles containing black carbon are ubiquitous in the atmosphere and originate from combustion processes. We examine their capability to act as condensation centers for water vapor. We make use of published experimental data sets for different types of black carbon particles, ranging from very pure particles to particles that contain both black carbon and water soluble organic matter, and we show that a recently developed theory reproduces most of the experimental results.
Lanxiadi Chen, Chao Peng, Wenjun Gu, Hanjing Fu, Xing Jian, Huanhuan Zhang, Guohua Zhang, Jianxi Zhu, Xinming Wang, and Mingjin Tang
Atmos. Chem. Phys., 20, 13611–13626,Short summary
We investigated hygroscopic properties of a number of mineral dust particles in a quantitative manner, via measuring the sample mass at different relative humidities. The robust and comprehensive data obtained would significantly improve our knowledge of hygroscopicity of mineral dust and its impacts on atmospheric chemistry and climate.
Jie Gong, Xiping Zeng, Dong L. Wu, S. Joseph Munchak, Xiaowen Li, Stefan Kneifel, Davide Ori, Liang Liao, and Donifan Barahona
Atmos. Chem. Phys., 20, 12633–12653,Short summary
This work provides a novel way of using polarized passive microwave measurements to study the interlinked cloud–convection–precipitation processes. The magnitude of differences between polarized radiances is found linked to ice microphysics (shape, size, orientation and density), mesoscale dynamic and thermodynamic structures, and surface precipitation. We conclude that passive sensors with multiple polarized channel pairs may serve as cheaper and useful substitutes for spaceborne radar sensors.
Aikaterini Bougiatioti, Athanasios Nenes, Jack J. Lin, Charles A. Brock, Joost A. de Gouw, Jin Liao, Ann M. Middlebrook, and André Welti
Atmos. Chem. Phys., 20, 12163–12176,Short summary
The number concentration of droplets in clouds in the summertime in the southeastern United States is influenced by aerosol variations but limited by the strong competition for supersaturated water vapor. Concurrent variations in vertical velocity magnify the response of cloud droplet number to aerosol increases by up to a factor of 5. Omitting the covariance of vertical velocity with aerosol number may therefore bias estimates of the cloud albedo effect from aerosols.
Ifayoyinsola Ibikunle, Andreas Beyersdorf, Pedro Campuzano-Jost, Chelsea Corr, John D. Crounse, Jack Dibb, Glenn Diskin, Greg Huey, Jose-Luis Jimenez, Michelle J. Kim, Benjamin A. Nault, Eric Scheuer, Alex Teng, Paul O. Wennberg, Bruce Anderson, James Crawford, Rodney Weber, and Athanasios Nenes
Atmos. Chem. Phys. Discuss.,
Publication in ACP not foreseenShort summary
Analysis of observations over South Korea during the NASA/NIER KORUS-AQ field campaign show that aerosol is fairly acidic (mean pH 2.43 ± 0.68). Aerosol formation is always sensitive to HNO3 levels, especially in highly polluted regions, while it is only exclusively sensitive to NH3 in some rural/remote regions. Nitrate levels accumulate because dry deposition velocity is low. HNO3 reductions achieved by NOx controls can be the most effective PM reduction strategy for all conditions observed.
Shunliu Zhao, Matthew G. Russell, Amir Hakami, Shannon L. Capps, Matthew D. Turner, Daven K. Henze, Peter B. Percell, Jaroslav Resler, Huizhong Shen, Armistead G. Russell, Athanasios Nenes, Amanda J. Pappin, Sergey L. Napelenok, Jesse O. Bash, Kathleen M. Fahey, Gregory R. Carmichael, Charles O. Stanier, and Tianfeng Chai
Geosci. Model Dev., 13, 2925–2944,
Juan Manuel Rincón-Riveros, Maria Alejandra Rincón-Caro, Amy P. Sullivan, Juan Felipe Mendez-Espinosa, Luis Carlos Belalcazar, Miguel Quirama Aguilar, and Ricardo Morales Betancourt
Atmos. Chem. Phys., 20, 7459–7472,Short summary
Air pollution affects health for millions of people worldwide. This is particularly worrisome for citizens in emerging economies where air quality is often heavily deteriorated. We show how, every year, agricultural burns and forest fires in the grasslands of northern South America increase the concentration of harmful particles in the environment, further worsening air quality for nearly 60 million in this region, even when the fires occur hundreds of kilometers away from urban areas.
Havala O. T. Pye, Athanasios Nenes, Becky Alexander, Andrew P. Ault, Mary C. Barth, Simon L. Clegg, Jeffrey L. Collett Jr., Kathleen M. Fahey, Christopher J. Hennigan, Hartmut Herrmann, Maria Kanakidou, James T. Kelly, I-Ting Ku, V. Faye McNeill, Nicole Riemer, Thomas Schaefer, Guoliang Shi, Andreas Tilgner, John T. Walker, Tao Wang, Rodney Weber, Jia Xing, Rahul A. Zaveri, and Andreas Zuend
Atmos. Chem. Phys., 20, 4809–4888,Short summary
Acid rain is recognized for its impacts on human health and ecosystems, and programs to mitigate these effects have had implications for atmospheric acidity. Historical measurements indicate that cloud and fog droplet acidity has changed in recent decades in response to controls on emissions from human activity, while the limited trend data for suspended particles indicate acidity may be relatively constant. This review synthesizes knowledge on the acidity of atmospheric particles and clouds.
Athanasios Nenes, Spyros N. Pandis, Rodney J. Weber, and Armistead Russell
Atmos. Chem. Phys., 20, 3249–3258,Short summary
We show that aerosol acidity (pH) and liquid water content naturally emerge as previously ignored parameters that drive particulate matter formation in the atmosphere, and its sensitivity to emissions of ammonia and nitric acid. The simple framework presented is easily applied to ambient measurements or model output, and it provides the
chemical regimeof PM sensitivity to ammonia and nitric acid availability.
Mary Kacarab, K. Lee Thornhill, Amie Dobracki, Steven G. Howell, Joseph R. O'Brien, Steffen Freitag, Michael R. Poellot, Robert Wood, Paquita Zuidema, Jens Redemann, and Athanasios Nenes
Atmos. Chem. Phys., 20, 3029–3040,Short summary
We find that extensive biomass burning aerosol plumes from southern Africa can profoundly influence clouds in the southeastern Atlantic. Concurrent variations in vertical velocity, however, are found to magnify the relationship between boundary layer aerosol and the cloud droplet number. Neglecting these covariances may strongly bias the sign and magnitude of aerosol impacts on the cloud droplet number.
Arnaldo Negron, Natasha DeLeon-Rodriguez, Samantha M. Waters, Luke D. Ziemba, Bruce Anderson, Michael Bergin, Konstantinos T. Konstantinidis, and Athanasios Nenes
Atmos. Chem. Phys., 20, 1817–1838,Short summary
Airborne biological particles impact human health, cloud formation, and ecosystems, but few techniques are available to characterize their atmospheric abundance. Combining a newly developed high-volume sampling/flow cytometry technique together with an laser-induced fluorescence instrument, we detect a highly dynamic bioaerosol community over urban Atlanta, composed of pollen, fungi, and bacteria with low and high nucleic acid content.
Georgia Sotiropoulou, Sylvia Sullivan, Julien Savre, Gary Lloyd, Thomas Lachlan-Cope, Annica M. L. Ekman, and Athanasios Nenes
Atmos. Chem. Phys., 20, 1301–1316,Short summary
Arctic clouds constitute a large source of uncertainty in predictions of future climate. Observations indicate that the number concentration of cloud ice crystals exceeds the concentration of aerosols that can act as ice-nucleating particles (INPs). We show that ice multiplication due to mechanical break-up upon collisions between the few primary ice crystals (formed from INPs) can explain the discrepancy. Including a description of the process in climate models can improve cloud representation.
Michael A. Battaglia Jr., Rodney J. Weber, Athanasios Nenes, and Christopher J. Hennigan
Atmos. Chem. Phys., 19, 14607–14620,Short summary
The effects of water-soluble organic carbon (WSOC) on aerosol pH were characterized for aqueous-phase particles containing a mixture of inorganics and organics. The ISORROPIA-II and E-AIM models were used in conjunction with AIOMFAC to quantify the effect of organics on aerosol pH through (1) changes to the aerosol liquid water content and (2) changes to the hydrogen ion activity coefficient. The study included both organic acids and nonacids, at RH levels ranging from 70 to 90 %.
Eleni Marinou, Matthias Tesche, Athanasios Nenes, Albert Ansmann, Jann Schrod, Dimitra Mamali, Alexandra Tsekeri, Michael Pikridas, Holger Baars, Ronny Engelmann, Kalliopi-Artemis Voudouri, Stavros Solomos, Jean Sciare, Silke Groß, Florian Ewald, and Vassilis Amiridis
Atmos. Chem. Phys., 19, 11315–11342,Short summary
We assess the feasibility of ground-based and spaceborne lidars to retrieve profiles of cloud-relevant aerosol concentrations and ice-nucleating particles. The retrieved profiles are in good agreement with airborne in situ measurements. Our methodology will be applied to satellite observations in the future so as to provide a global 3D product of cloud-relevant properties.
George S. Fanourgakis, Maria Kanakidou, Athanasios Nenes, Susanne E. Bauer, Tommi Bergman, Ken S. Carslaw, Alf Grini, Douglas S. Hamilton, Jill S. Johnson, Vlassis A. Karydis, Alf Kirkevåg, John K. Kodros, Ulrike Lohmann, Gan Luo, Risto Makkonen, Hitoshi Matsui, David Neubauer, Jeffrey R. Pierce, Julia Schmale, Philip Stier, Kostas Tsigaridis, Twan van Noije, Hailong Wang, Duncan Watson-Parris, Daniel M. Westervelt, Yang Yang, Masaru Yoshioka, Nikos Daskalakis, Stefano Decesari, Martin Gysel-Beer, Nikos Kalivitis, Xiaohong Liu, Natalie M. Mahowald, Stelios Myriokefalitakis, Roland Schrödner, Maria Sfakianaki, Alexandra P. Tsimpidi, Mingxuan Wu, and Fangqun Yu
Atmos. Chem. Phys., 19, 8591–8617,Short summary
Effects of aerosols on clouds are important for climate studies but are among the largest uncertainties in climate projections. This study evaluates the skill of global models to simulate aerosol, cloud condensation nuclei (CCN) and cloud droplet number concentrations (CDNCs). Model results show reduced spread in CDNC compared to CCN due to the negative correlation between the sensitivities of CDNC to aerosol number concentration (air pollution) and updraft velocity (atmospheric dynamics).
Jenny P. S. Wong, Maria Tsagkaraki, Irini Tsiodra, Nikolaos Mihalopoulos, Kalliopi Violaki, Maria Kanakidou, Jean Sciare, Athanasios Nenes, and Rodney J. Weber
Atmos. Chem. Phys., 19, 7319–7334,Short summary
Biomass burning is a major source of light-absorbing organic species in atmospheric aerosols, and it can play an important role in climate and atmospheric chemistry. Through a combination of laboratory experiments and field observations, this work demonstrated that the light absorption properties of aged biomass burning organic aerosols are dominated by high-molecular-weight compounds. In addition, we found that total hydrated sugars may be a robust tracer for aged biomass burning aerosols.
Panayiotis Kalkavouras, Aikaterini Bougiatioti, Nikos Kalivitis, Iasonas Stavroulas, Maria Tombrou, Athanasios Nenes, and Nikolaos Mihalopoulos
Atmos. Chem. Phys., 19, 6185–6203,Short summary
We study how new particle formation (NPF) events affect clouds throughout the year at a ground site in the E Mediterranean. Using a new tools and evaluation metrics, NPF is found to affect only evening and nocturnal clouds by modestly increasing droplet number by 7 to 12 %. A conventional analysis based on CCN concentration at prescribed supersaturation levels or aerosol size can considerably bias the perceived influence of NPF events on regional clouds, the hydrological cycle, and climate.
Nønne L. Prisle, Jack J. Lin, Sara Purdue, Haisheng Lin, J. Carson Meredith, and Athanasios Nenes
Atmos. Chem. Phys., 19, 4741–4761,Short summary
We measure surface activity and cloud-forming potential of pollenkitt, an organic mixture coating pollen grains. Cloud droplet formation is affected through both surface tension and bulk depletion, with a consistent particle size-dependent signature. We observe nonideal solution effects in pollenkitt mixtures with ammonium sulfate salt. Our results suggest sensitivity of general water interactions, including cloud formation by pollen and their fragments, to both atmospheric humidity and aging.
Hongyu Guo, Athanasios Nenes, and Rodney J. Weber
Atmos. Chem. Phys., 18, 17307–17323,Short summary
Overprediction of fine-particle ammonium-sulfate molar ratios (R) by thermodynamic models is suggested as evidence for organic aerosol limiting the condensation of ammonia onto particles, with significant impacts on aerosol chemistry. We find that the effects of small amounts of salt and dust, combined with measurement artifacts, explain the discrepancy in R. These results are highly insensitive to mixing state. This means that aerosol predictions are much more robust than thought before.
Atmos. Chem. Phys., 18, 17119–17141,Short summary
This work develops a model for ice formation mediated by particles immersed within droplets. Ice nucleation is not only enhanced by the modification of the thermodynamic properties of the vicinal water but is also inhibited by decreased water mobility near the particle. The ice nucleation rate is thus determined by competing kinetic and thermodynamic factors during ice formation. A new regime where ice nucleation is mediated mainly by kinetics instead of thermodynamics is discovered.
Sylvia C. Sullivan, Christian Barthlott, Jonathan Crosier, Ilya Zhukov, Athanasios Nenes, and Corinna Hoose
Atmos. Chem. Phys., 18, 16461–16480,Short summary
Ice crystal formation in clouds can occur via thermodynamic nucleation, but also via mechanical collisions between pre-existing crystals or co-existing droplets. When descriptions of this mechanical ice generation are implemented into the COSMO weather model, we find that the contributions to crystal number from thermodynamic and mechanical processes are of the same order. Mechanical ice generation also intensifies differences in precipitation intensity between dynamic and quiescent regions.
Stelios Myriokefalitakis, Akinori Ito, Maria Kanakidou, Athanasios Nenes, Maarten C. Krol, Natalie M. Mahowald, Rachel A. Scanza, Douglas S. Hamilton, Matthew S. Johnson, Nicholas Meskhidze, Jasper F. Kok, Cecile Guieu, Alex R. Baker, Timothy D. Jickells, Manmohan M. Sarin, Srinivas Bikkina, Rachel Shelley, Andrew Bowie, Morgane M. G. Perron, and Robert A. Duce
Biogeosciences, 15, 6659–6684,Short summary
The first atmospheric iron (Fe) deposition model intercomparison is presented in this study, as a result of the deliberations of the United Nations Joint Group of Experts on the Scientific Aspects of Marine Environmental Protection (GESAMP; http://www.gesamp.org/) Working Group 38. We conclude that model diversity over remote oceans reflects uncertainty in the Fe content parameterizations of dust aerosols, combustion aerosol emissions and the size distribution of transported aerosol Fe.
Sara Bacer, Sylvia C. Sullivan, Vlassis A. Karydis, Donifan Barahona, Martina Krämer, Athanasios Nenes, Holger Tost, Alexandra P. Tsimpidi, Jos Lelieveld, and Andrea Pozzer
Geosci. Model Dev., 11, 4021–4041,Short summary
The complexity of ice nucleation mechanisms and aerosol--ice interactions makes their representation still challenging in atmospheric models. We have implemented a comprehensive ice crystal formation parameterization in the global chemistry-climate model EMAC to improve the representation of ice crystal number concentrations. The newly implemented parameterization takes into account processes which were previously neglected by the standard version of the model.
Petros Vasilakos, Armistead Russell, Rodney Weber, and Athanasios Nenes
Atmos. Chem. Phys., 18, 12765–12775,Short summary
In this work, we investigated the role of emission reductions on aerosol acidity and particulate nitrate. We found that models exhibit positive biases in pH predictions, attributed to very high levels of crustal elements (Mg, Ca, K) in model simulations, which in turn led to an increasing aerosol pH trend over the past decade and allowed nitrate to become an important component of aerosol, which is inconsistent with the measurements, highlighting the importance of accurate pH prediction.
Hongyu Guo, Rene Otjes, Patrick Schlag, Astrid Kiendler-Scharr, Athanasios Nenes, and Rodney J. Weber
Atmos. Chem. Phys., 18, 12241–12256,Short summary
Reduction in ammonia has been proposed as a way to lower fine particle mass and improve air quality, but gas-phase ammonia is linked to agricultural productivity. We assess the feasibility of ammonia control at a variety of locations through an aerosol thermodynamic analysis. We show that aerosol response to ammonia control is highly nonlinear and only becomes effective when ambient particle pH drops below approximately 3. Particle pH is a relevant aerosol air quality parameter.
Theodora Nah, Hongyu Guo, Amy P. Sullivan, Yunle Chen, David J. Tanner, Athanasios Nenes, Armistead Russell, Nga Lee Ng, L. Gregory Huey, and Rodney J. Weber
Atmos. Chem. Phys., 18, 11471–11491,Short summary
We present measurements from a field study conducted in an agriculturally intensive region in the southeastern US during the fall of 2016 to investigate how NH3 affects particle acidity and SOA formation via gas–particle partitioning of semi-volatile organic acids. For this study, higher NH3 concentrations relative to what has been measured in the region in previous studies had minor effects on PM1 organic acids and their influence on the overall organic aerosol and PM1 mass concentrations.
Evangelia Kostenidou, Eleni Karnezi, James R. Hite Jr., Aikaterini Bougiatioti, Kate Cerully, Lu Xu, Nga L. Ng, Athanasios Nenes, and Spyros N. Pandis
Atmos. Chem. Phys., 18, 5799–5819,Short summary
The volatility distribution of organic aerosol (OA) and its sources during the Southern Oxidant and Aerosol Study (SOAS) was estimated. The volatility distribution of all components covered a wide range including both semi-volatile and low-volatility components. The oxygen content of the factors can be combined with their estimated volatility and hygroscopicity to provide a better view of their physical properties.
Julia Schmale, Silvia Henning, Stefano Decesari, Bas Henzing, Helmi Keskinen, Karine Sellegri, Jurgita Ovadnevaite, Mira L. Pöhlker, Joel Brito, Aikaterini Bougiatioti, Adam Kristensson, Nikos Kalivitis, Iasonas Stavroulas, Samara Carbone, Anne Jefferson, Minsu Park, Patrick Schlag, Yoko Iwamoto, Pasi Aalto, Mikko Äijälä, Nicolas Bukowiecki, Mikael Ehn, Göran Frank, Roman Fröhlich, Arnoud Frumau, Erik Herrmann, Hartmut Herrmann, Rupert Holzinger, Gerard Kos, Markku Kulmala, Nikolaos Mihalopoulos, Athanasios Nenes, Colin O'Dowd, Tuukka Petäjä, David Picard, Christopher Pöhlker, Ulrich Pöschl, Laurent Poulain, André Stephan Henry Prévôt, Erik Swietlicki, Meinrat O. Andreae, Paulo Artaxo, Alfred Wiedensohler, John Ogren, Atsushi Matsuki, Seong Soo Yum, Frank Stratmann, Urs Baltensperger, and Martin Gysel
Atmos. Chem. Phys., 18, 2853–2881,Short summary
Collocated long-term observations of cloud condensation nuclei (CCN) number concentrations, particle number size distributions and chemical composition from 12 sites are synthesized. Observations cover coastal environments, the Arctic, the Mediterranean, the boreal and rain forest, high alpine and continental background sites, and Monsoon-influenced areas. We interpret regional and seasonal variability. CCN concentrations are predicted with the κ–Köhler model and compared to the measurements.
Sylvia C. Sullivan, Corinna Hoose, Alexei Kiselev, Thomas Leisner, and Athanasios Nenes
Atmos. Chem. Phys., 18, 1593–1610,Short summary
Ice multiplication (IM) processes can have a profound impact on cloud and precipitation development but are poorly understood. Here we study whether a lower limit of ice nuclei exists to initiate IM. The lower limit is found to be extremely low (0.01 per liter or less). A counterintuitive but profound conclusion thus emerges: IM requires cloud formation around a thermodynamic
sweet spotand is sensitive to fluctuations in cloud condensation nuclei concentration alone.
Khairunnisa Yahya, Timothy Glotfelty, Kai Wang, Yang Zhang, and Athanasios Nenes
Geosci. Model Dev., 10, 2333–2363,
Petros Vasilakos, Yong-Ηa Kim, Jeffrey R. Pierce, Sotira Yiacoumi, Costas Tsouris, and Athanasios Nenes
Geosci. Model Dev. Discuss.,
Revised manuscript not acceptedShort summary
Radioactive charging can significantly impact the way radioactive aerosols behave, and as a result their lifetime, but such effects are neglected in predictive model studies of radioactive plumes. We extend a well-established model that simulates the evolution of atmospheric particulate matter to account for radioactive charging effects in an accurate and computationally efficient way. It is shown that radioactivity can strongly impact the deposition patterns of aerosol.
Hongyu Guo, Jiumeng Liu, Karl D. Froyd, James M. Roberts, Patrick R. Veres, Patrick L. Hayes, Jose L. Jimenez, Athanasios Nenes, and Rodney J. Weber
Atmos. Chem. Phys., 17, 5703–5719,Short summary
Fine particle pH is linked to many environmental impacts by affecting particle concentration and composition. Predicted Pasadena, CA (CalNex campaign), PM1 pH is 1.9 and PM2.5 pH 2.7, the latter higher due to sea salts. The model predicted gas–particle partitionings of HNO3–NO3−, NH3–NH4+, and HCl–Cl− are in good agreement, verifying the model predictions. A summary of contrasting locations in the US and eastern Mediterranean shows fine particles are generally highly acidic, with pH below 3.
Vlassis A. Karydis, Alexandra P. Tsimpidi, Sara Bacer, Andrea Pozzer, Athanasios Nenes, and Jos Lelieveld
Atmos. Chem. Phys., 17, 5601–5621,Short summary
The importance of mineral dust for cloud droplet formation is studied by considering the adsorption activation of insoluble dust particles and the thermodynamic interactions between mineral cations and inorganic anions. This study demonstrates that a comprehensive treatment of the CCN activity of mineral dust and its chemical and thermodynamic interactions with inorganic species by chemistry climate models is important to realistically account for aerosol–chemistry–cloud–climate interaction.
Alexandra Tsekeri, Vassilis Amiridis, Franco Marenco, Athanasios Nenes, Eleni Marinou, Stavros Solomos, Phil Rosenberg, Jamie Trembath, Graeme J. Nott, James Allan, Michael Le Breton, Asan Bacak, Hugh Coe, Carl Percival, and Nikolaos Mihalopoulos
Atmos. Meas. Tech., 10, 83–107,Short summary
The In situ/Remote sensing aerosol Retrieval Algorithm (IRRA) provides vertical profiles of aerosol optical, microphysical and hygroscopic properties from airborne in situ and remote sensing measurements. The algorithm is highly advantageous for aerosol characterization in humid conditions, employing the ISORROPIA II model for acquiring the particle hygroscopic growth. IRRA can find valuable applications in aerosol–cloud interaction schemes and in validation of active space-borne sensors.
Havala O. T. Pye, Benjamin N. Murphy, Lu Xu, Nga L. Ng, Annmarie G. Carlton, Hongyu Guo, Rodney Weber, Petros Vasilakos, K. Wyat Appel, Sri Hapsari Budisulistiorini, Jason D. Surratt, Athanasios Nenes, Weiwei Hu, Jose L. Jimenez, Gabriel Isaacman-VanWertz, Pawel K. Misztal, and Allen H. Goldstein
Atmos. Chem. Phys., 17, 343–369,Short summary
We use a chemical transport model to examine how organic compounds in the atmosphere interact with water present in particles. Organic compounds themselves lead to water uptake, and organic compounds interact with water associated with inorganic compounds in the rural southeast atmosphere. Including interactions of organic compounds with water requires a treatment of nonideality to more accurately represent aerosol observations during the Southern Oxidant and Aerosol Study (SOAS) 2013.
Panayiotis Kalkavouras, Elissavet Bossioli, Spiros Bezantakos, Aikaterini Bougiatioti, Nikos Kalivitis, Iasonas Stavroulas, Giorgos Kouvarakis, Anna P. Protonotariou, Aggeliki Dandou, George Biskos, Nikolaos Mihalopoulos, Athanasios Nenes, and Maria Tombrou
Atmos. Chem. Phys., 17, 175–192,Short summary
Concentrations of chemically and size-resolved submicron aerosol particles along with concentrations of gases and meteorological variables were measured at Santorini and Finokalia (central and southern Aegean Sea) during the Etesians. Particle nucleation bursts were recorded. The NPF can double CCN number (at 0.1 % supersaturation), but the resulting strong competition for water vapor in cloudy updrafts decreases maximum supersaturation by 14 % and augments the potential droplet number by 12 %.
Stelios Myriokefalitakis, Athanasios Nenes, Alex R. Baker, Nikolaos Mihalopoulos, and Maria Kanakidou
Biogeosciences, 13, 6519–6543,Short summary
The global atmospheric cycle of P is simulated accounting for natural and anthropogenic sources, acid dissolution of dust aerosol and changes in atmospheric acidity. Simulations show that P-containing dust dissolution flux may have increased in the last 150 years but is expected to decrease in the future, and biological particles are important carriers of bioavailable P to the ocean. These insights to the P cycle have important implications for marine ecosystem responses to climate change.
Carsten Warneke, Michael Trainer, Joost A. de Gouw, David D. Parrish, David W. Fahey, A. R. Ravishankara, Ann M. Middlebrook, Charles A. Brock, James M. Roberts, Steven S. Brown, Jonathan A. Neuman, Brian M. Lerner, Daniel Lack, Daniel Law, Gerhard Hübler, Iliana Pollack, Steven Sjostedt, Thomas B. Ryerson, Jessica B. Gilman, Jin Liao, John Holloway, Jeff Peischl, John B. Nowak, Kenneth C. Aikin, Kyung-Eun Min, Rebecca A. Washenfelder, Martin G. Graus, Mathew Richardson, Milos Z. Markovic, Nick L. Wagner, André Welti, Patrick R. Veres, Peter Edwards, Joshua P. Schwarz, Timothy Gordon, William P. Dube, Stuart A. McKeen, Jerome Brioude, Ravan Ahmadov, Aikaterini Bougiatioti, Jack J. Lin, Athanasios Nenes, Glenn M. Wolfe, Thomas F. Hanisco, Ben H. Lee, Felipe D. Lopez-Hilfiker, Joel A. Thornton, Frank N. Keutsch, Jennifer Kaiser, Jingqiu Mao, and Courtney D. Hatch
Atmos. Meas. Tech., 9, 3063–3093,Short summary
In this paper we describe the experimental approach, the science goals and early results of the NOAA SENEX campaign, which was focused on studying the interactions between biogenic and anthropogenic emissions to form secondary pollutants. During SENEX, the NOAA WP-3D aircraft conducted 20 research flights between 27 May and 10 July 2013 based out of Smyrna, TN. The SENEX flights included day- and nighttime flights in the Southeast as well as flights over areas with intense shale gas extraction.
Aikaterini Bougiatioti, Spiros Bezantakos, Iasonas Stavroulas, Nikos Kalivitis, Panagiotis Kokkalis, George Biskos, Nikolaos Mihalopoulos, Alexandros Papayannis, and Athanasios Nenes
Atmos. Chem. Phys., 16, 7389–7409,Short summary
BBOA from long-range transport exhibits increased CCN concentrations for particles larger than 100 nm. At the same time the hygroscopicity parameter decreased for all particle sizes, as sub-100 nm particles appear to be richer in less hygroscopic organic material, while larger particles become less hygroscopic due to condensation of less hygroscopic gaseous compounds. Finally, atmospheric processing of freshly emitted BBOA to more oxidized organic aerosol can result in a 2-fold increase of κ.
Swen Metzger, Benedikt Steil, Mohamed Abdelkader, Klaus Klingmüller, Li Xu, Joyce E. Penner, Christos Fountoukis, Athanasios Nenes, and Jos Lelieveld
Atmos. Chem. Phys., 16, 7213–7237,Short summary
We introduce an unique single parameter framework to efficiently parameterize the aerosol water uptake for mixtures of semi-volatile and non-volatile compounds, being entirely based on the single solute specific coefficient introduced in Metzger et al. (2012).
Aikaterini Bougiatioti, Panayiota Nikolaou, Iasonas Stavroulas, Giorgos Kouvarakis, Rodney Weber, Athanasios Nenes, Maria Kanakidou, and Nikolaos Mihalopoulos
Atmos. Chem. Phys., 16, 4579–4591,Short summary
Atmospheric aerosols and relevant parameters were measured in the eastern Mediterranean during summer and fall 2012. Submicron aerosol water can contribute up to 33 % of total mass, and 27.5 % of this can be associated with organics. Using these data, the pH of the submicron aerosols was calculated to be highly acidic, varying from 0.5 to 2.8 and independently of air masses origin. Such pH values could increase nutrient availability and thus sea water productivity of the Mediterranean Sea.
Christopher R. Hoyle, Clare S. Webster, Harald E. Rieder, Athanasios Nenes, Emanuel Hammer, Erik Herrmann, Martin Gysel, Nicolas Bukowiecki, Ernest Weingartner, Martin Steinbacher, and Urs Baltensperger
Atmos. Chem. Phys., 16, 4043–4061,Short summary
A simple statistical model to predict the number of aerosols which activate to form cloud droplets in warm clouds has been established, based on regression analysis of data from the high-altitude site Jungfraujoch. It is found that cloud droplet formation at the Jungfraujoch is predominantly controlled by the number concentration of aerosol particles. A statistical model based on only the number of particles larger than 80nm can explain 79 % of the observed variance in droplet numbers.
Yong-ha Kim, Sotira Yiacoumi, Athanasios Nenes, and Costas Tsouris
Atmos. Chem. Phys., 16, 3449–3462,Short summary
Three microphysical approaches are proposed to incorporate mutual effects of particle charging and coagulation in predictions of transient charge and size distributions of atmospheric particles, including radioactive aerosols. The three approaches have different levels of complexities and are applicable to various laboratory and field atmospheric studies. Also, these approaches can be easily incorporated into aerosol transport models at different scales to account for particle charging effects.
L. M. Zamora, R. A. Kahn, M. J. Cubison, G. S. Diskin, J. L. Jimenez, Y. Kondo, G. M. McFarquhar, A. Nenes, K. L. Thornhill, A. Wisthaler, A. Zelenyuk, and L. D. Ziemba
Atmos. Chem. Phys., 16, 715–738,Short summary
Based on extensive aircraft campaigns, we quantify how biomass burning smoke affects subarctic and Arctic liquid cloud microphysical properties. Enhanced cloud albedo may decrease short-wave radiative flux by between 2 and 4 Wm2 or more in some subarctic conditions. Smoke halved average cloud droplet diameter. In one case study, it also appeared to limit droplet formation. Numerous Arctic background Aitken particles can also interact with combustion particles, perhaps affecting their properties.
Atmos. Chem. Phys., 15, 13819–13831,Short summary
This paper describes the process of the transfer of water molecules between liquid and the ice during the early stages of ice formation. Using concepts of nonreversible thermodynamics, it is shown that the activation energy can be defined in terms of the bulk self-diffusivity of water and the probability of interface transfer. The application of this model to classical nucleation theory shows good agreement of measured nucleation rates with experimental results for temperatures as low as 190K.
M. Paramonov, V.-M. Kerminen, M. Gysel, P. P. Aalto, M. O. Andreae, E. Asmi, U. Baltensperger, A. Bougiatioti, D. Brus, G. P. Frank, N. Good, S. S. Gunthe, L. Hao, M. Irwin, A. Jaatinen, Z. Jurányi, S. M. King, A. Kortelainen, A. Kristensson, H. Lihavainen, M. Kulmala, U. Lohmann, S. T. Martin, G. McFiggans, N. Mihalopoulos, A. Nenes, C. D. O'Dowd, J. Ovadnevaite, T. Petäjä, U. Pöschl, G. C. Roberts, D. Rose, B. Svenningsson, E. Swietlicki, E. Weingartner, J. Whitehead, A. Wiedensohler, C. Wittbom, and B. Sierau
Atmos. Chem. Phys., 15, 12211–12229,Short summary
The research paper presents the first comprehensive overview of field measurements with the CCN Counter performed at a large number of locations around the world within the EUCAARI framework. The paper sheds light on the CCN number concentrations and activated fractions around the world and their dependence on the water vapour supersaturation ratio, the dependence of aerosol hygroscopicity on particle size, and seasonal and diurnal variation of CCN activation and hygroscopic properties.
N. Kalivitis, V.-M. Kerminen, G. Kouvarakis, I. Stavroulas, A. Bougiatioti, A. Nenes, H. E. Manninen, T. Petäjä, M. Kulmala, and N. Mihalopoulos
Atmos. Chem. Phys., 15, 9203–9215,Short summary
Cloud condensation nuclei (CCN) production associated with atmospheric new particle formation (NPF) is presented, and this is the first direct evidence of CCN production resulting from NPF in the eastern Mediterranean atmosphere. We show that condensation of both gaseous sulfuric acid and organic compounds from multiple sources leads to the rapid growth of nucleated particles. Sub-100nm particles were found to be substantially less hygroscopic than larger particles during the active NPF period.
S. H. Budisulistiorini, X. Li, S. T. Bairai, J. Renfro, Y. Liu, Y. J. Liu, K. A. McKinney, S. T. Martin, V. F. McNeill, H. O. T. Pye, A. Nenes, M. E. Neff, E. A. Stone, S. Mueller, C. Knote, S. L. Shaw, Z. Zhang, A. Gold, and J. D. Surratt
Atmos. Chem. Phys., 15, 8871–8888,Short summary
Isoprene epoxydiols (IEPOX) are major gas-phase products from the atmospheric oxidation of isoprene that yield secondary organic aerosol (SOA) by reactive uptake onto acidic sulfate aerosol. We report a substantial contribution of IEPOX-derived SOA to the total fine aerosol collected during summer. IEPOX-derived SOA measured by online and offline mass spectrometry techniques is correlated with acidic sulfate aerosol, demonstrating the critical role of anthropogenic emissions in its formation.
K. M. Cerully, A. Bougiatioti, J. R. Hite Jr., H. Guo, L. Xu, N. L. Ng, R. Weber, and A. Nenes
Atmos. Chem. Phys., 15, 8679–8694,Short summary
The hygroscopicity of SE US aerosol is mostly water-soluble, with a hygroscopicity that is insensitive to partial volatilization in a thermodenuder. The most and least oxidized components of the aerosol are the most hygroscopic of organic constituents. No clear relationship was found between organic aerosol hygroscopicity and oxygen-to-carbon ratio. The aerosol factors covary in a way that induces the observed diurnal invariance in total organic hygroscopicity.
L. Hildebrandt Ruiz, A. L. Paciga, K. M. Cerully, A. Nenes, N. M. Donahue, and S. N. Pandis
Atmos. Chem. Phys., 15, 8301–8313,Short summary
Secondary organic aerosol (SOA) is transformed after its initial formation. We explored the effects of this chemical aging on the composition, mass yield, volatility, and hygroscopicity of SOA formed from the photo-oxidation of small aromatic volatile organic compounds. Higher exposure to the hydroxyl radical resulted in different SOA composition, average carbon oxidation state, and mass yield. The vapor pressure of SOA formed under different conditions varied by as much as a factor of 30.
Y. Shinozuka, A. D. Clarke, A. Nenes, A. Jefferson, R. Wood, C. S. McNaughton, J. Ström, P. Tunved, J. Redemann, K. L. Thornhill, R. H. Moore, T. L. Lathem, J. J. Lin, and Y. J. Yoon
Atmos. Chem. Phys., 15, 7585–7604,
S. Myriokefalitakis, N. Daskalakis, N. Mihalopoulos, A. R. Baker, A. Nenes, and M. Kanakidou
Biogeosciences, 12, 3973–3992,Short summary
The global atmospheric cycle of Fe is simulated accounting for natural and combustion sources, proton- and organic ligand-promoted Fe dissolution from dust aerosol and changes in anthropogenic emissions, and thus in atmospheric acidity. Simulations show that Fe dissolution may have increased in the last 150 years and is expected to decrease due to air pollution regulations. Reductions in dissolved-Fe deposition can further limit the primary productivity over high-nutrient-low-chlorophyll water.
H. Guo, L. Xu, A. Bougiatioti, K. M. Cerully, S. L. Capps, J. R. Hite Jr., A. G. Carlton, S.-H. Lee, M. H. Bergin, N. L. Ng, A. Nenes, and R. J. Weber
Atmos. Chem. Phys., 15, 5211–5228,Short summary
Particle pH can affect many aerosol processes, including gas-particle partitioning, SOA formation, and mobilization of toxic redox metals. pH is challenging to directly measure and often improperly characterized by proxies like ion balances or molar ratios of measured aerosol ionic species. We present a detailed analysis predicting pH with a thermodynamic model, verify the prediction, and test pH sensitivity to model inputs based on data from the SOAS field campaign.
C. J. Hennigan, J. Izumi, A. P. Sullivan, R. J. Weber, and A. Nenes
Atmos. Chem. Phys., 15, 2775–2790,Short summary
We show that the ion balance and molar ratio methods are unsuitable for use as aerosol pH proxies. Our recommendation is that 1) thermodynamic equilibrium models constrained by both gas and aerosol inputs run in the forward (open) mode, and 2) the phase partitioning of ammonia provides the best predictions of aerosol pH. Given the significance of acidity for numerous chemical processes in the atmosphere, the implications of this study are important and far reaching.
Y. You, V. P. Kanawade, J. A. de Gouw, A. B. Guenther, S. Madronich, M. R. Sierra-Hernández, M. Lawler, J. N. Smith, S. Takahama, G. Ruggeri, A. Koss, K. Olson, K. Baumann, R. J. Weber, A. Nenes, H. Guo, E. S. Edgerton, L. Porcelli, W. H. Brune, A. H. Goldstein, and S.-H. Lee
Atmos. Chem. Phys., 14, 12181–12194,Short summary
Amiens play important roles in atmospheric secondary aerosol formation and human health, but the fast response measurements of amines are lacking. Here we show measurements in a southeastern US forest and a moderately polluted midwestern site. Our results show that gas to particle conversion is an important process that controls ambient amine concentrations and that biomass burning is an important source of amines.
R. Morales Betancourt and A. Nenes
Geosci. Model Dev., 7, 2345–2357,
D. Barahona, A. Molod, J. Bacmeister, A. Nenes, A. Gettelman, H. Morrison, V. Phillips, and A. Eichmann
Geosci. Model Dev., 7, 1733–1766,
Atmos. Chem. Phys., 14, 7665–7680,
B. Gantt, J. He, X. Zhang, Y. Zhang, and A. Nenes
Atmos. Chem. Phys., 14, 7485–7497,
G. Drozd, J. Woo, S. A. K. Häkkinen, A. Nenes, and V. F. McNeill
Atmos. Chem. Phys., 14, 5205–5215,
S. Romakkaniemi, A. Jaatinen, A. Laaksonen, A. Nenes, and T. Raatikainen
Atmos. Meas. Tech., 7, 1377–1384,
A. Bougiatioti, I. Stavroulas, E. Kostenidou, P. Zarmpas, C. Theodosi, G. Kouvarakis, F. Canonaco, A. S. H. Prévôt, A. Nenes, S. N. Pandis, and N. Mihalopoulos
Atmos. Chem. Phys., 14, 4793–4807,
R. Morales Betancourt and A. Nenes
Atmos. Chem. Phys., 14, 4809–4826,
M. Trail, A. P. Tsimpidi, P. Liu, K. Tsigaridis, Y. Hu, A. Nenes, and A. G. Russell
Geosci. Model Dev., 6, 1429–1445,
S. Lance, T. Raatikainen, T. B. Onasch, D. R. Worsnop, X.-Y. Yu, M. L. Alexander, M. R. Stolzenburg, P. H. McMurry, J. N. Smith, and A. Nenes
Atmos. Chem. Phys., 13, 5049–5062,
R. H. Moore, V. A. Karydis, S. L. Capps, T. L. Lathem, and A. Nenes
Atmos. Chem. Phys., 13, 4235–4251,
T. L. Lathem, A. J. Beyersdorf, K. L. Thornhill, E. L. Winstead, M. J. Cubison, A. Hecobian, J. L. Jimenez, R. J. Weber, B. E. Anderson, and A. Nenes
Atmos. Chem. Phys., 13, 2735–2756,
M. Frosch, M. Bilde, A. Nenes, A. P. Praplan, Z. Jurányi, J. Dommen, M. Gysel, E. Weingartner, and U. Baltensperger
Atmos. Chem. Phys., 13, 2283–2297,
Y. C. Sud, D. Lee, L. Oreopoulos, D. Barahona, A. Nenes, and M. J. Suarez
Geosci. Model Dev., 6, 57–79,
Related subject area
Subject: Aerosols | Research Activity: Atmospheric Modelling | Altitude Range: Troposphere | Science Focus: Physics (physical properties and processes)Meteorological export and deposition fluxes of black carbon on glaciers of the central Chilean AndesFuture changes in atmospheric rivers over East Asia under stratospheric aerosol interventionModeling the influence of chain length on secondary organic aerosol (SOA) formation via multiphase reactions of alkanesHow aerosol size matters in aerosol optical depth (AOD) assimilation and the optimization using the Ångström exponentMicrophysical, macrophysical, and radiative responses of subtropical marine clouds to aerosol injectionsHemispheric-wide climate response to regional COVID-19-related aerosol emission reductions: the prominent role of atmospheric circulation adjustmentsImpacts of an aerosol layer on a midlatitude continental system of cumulus clouds: how do these impacts depend on the vertical location of the aerosol layer?Impact of phase state and non-ideal mixing on equilibration timescales of secondary organic aerosol partitioningA global climatology of ice-nucleating particles under cirrus conditions derived from model simulations with MADE3 in EMACEnviro-HIRLAM model estimates of elevated black carbon pollution over Ukraine resulted from forest firesWhere does the dust deposited over the Sierra Nevada snow come from?Instant and delayed effects of March biomass burning aerosols over the Indochina PeninsulaAerosol–cloud interaction in the atmospheric chemistry model GRAPES_Meso5.1/CUACE and its impacts on mesoscale numerical weather prediction under haze pollution conditions in Jing–Jin–Ji in ChinaSurvival probabilities of atmospheric particles: comparison based on theory, cluster population simulations, and observations in BeijingThe simulation of mineral dust in the United Kingdom Earth System Model UKESM1Dust pollution in China affected by different spatial and temporal types of El NiñoAn improved representation of aerosol mixing state for air quality–weather interactionsCirculation-regulated impacts of aerosol pollution on urban heat island in BeijingSize-resolved dust direct radiative effect efficiency derived from satellite observationsModeling coarse and giant desert dust particlesFire–climate interactions through the aerosol radiative effect in a global chemistry–climate–vegetation modelContributions of meteorology and anthropogenic emissions to the trends in winter PM2.5 in eastern China 2013–2018Impacts of condensable particulate matter on atmospheric organic aerosols and fine particulate matter (PM2.5) in ChinaMapping the dependence of black carbon radiative forcing on emission region and seasonRegional PM2.5 pollution confined by atmospheric internal boundaries in the North China Plain: boundary layer structures and numerical simulationToward targeted observations of the meteorological initial state for improving the PM2.5 forecast of a heavy haze event that occurred in the Beijing–Tianjin–Hebei regionBelow-cloud scavenging of aerosol by rain: a review of numerical modelling approaches and sensitivity simulations with mineral dust in the Met Office's Unified ModelAggravated Air Pollution and Health Burden due to Traffic Congestion in Urban ChinaPredicting gridded winter PM2.5 concentration in the east of ChinaSatellite-based evaluation of AeroCom model bias in biomass burning regionsImpacts of marine organic emissions on low-level stratiform clouds – a large eddy simulator studyAviation contrail climate effects in the North Atlantic from 2016 to 2021Source attribution of cloud condensation nuclei and their impact on stratocumulus clouds and radiation in the south-eastern AtlanticRole of K-feldspar and quartz in global ice nucleation by mineral dust in mixed-phase cloudsSimulating wildfire emissions and plume rise using geostationary satellite fire radiative power measurements: a case study of the 2019 Williams Flats fireAtomistic and coarse-grained simulations reveal increased ice nucleation activity on silver iodide surfaces in slit and wedge geometriesSecondary aerosol formation in marine Arctic environments: a model measurement comparison at Ny-ÅlesundEffective radiative forcing of anthropogenic aerosols in E3SM version 1: historical changes, causality, decomposition, and parameterization sensitivitiesExamination of aerosol impacts on convective clouds and precipitation in two metropolitan areas in East Asia; how varying depths of convective clouds between the areas diversify those aerosol effects?Influence of emission size distribution and nucleation on number concentrations over Greater ParisImpact of stratospheric aerosol intervention geoengineering on surface air temperature in China: a surface energy budget perspectiveRegional impacts of black carbon morphologies on shortwave aerosol–radiation interactions: a comparative study between the US and ChinaTropospheric warming over the northern Indian Ocean caused by South Asian anthropogenic aerosols: possible impact on the upper troposphere and lower stratosphereIntraseasonal variation of the northeast Asian anomalous anticyclone and its impacts on PM2.5 pollution in the North China Plain in early winterInverse modeling of the 2021 spring super dust storms in East AsiaProjected increases in wildfires may challenge regulatory curtailment of PM2.5 over the eastern US by 2050Causal influences of El Niño–Southern Oscillation on global dust activitiesFormation, radiative forcing, and climatic effects of severe regional hazeAdvances in air quality research – current and emerging challengesLarge-eddy-simulation study on turbulent particle deposition and its dependence on atmospheric-boundary-layer stability
Rémy Lapere, Nicolás Huneeus, Sylvain Mailler, Laurent Menut, and Florian Couvidat
Atmos. Chem. Phys., 23, 1749–1768,Short summary
Glaciers in the Andes of central Chile are shrinking rapidly in response to global warming. This melting is accelerated by the deposition of opaque particles onto snow and ice. In this work, model simulations quantify typical deposition rates of soot on glaciers in summer and winter months and show that the contribution of emissions from Santiago is not as high as anticipated. Additionally, the combination of regional- and local-scale meteorology explains the seasonality in deposition.
Ju Liang and Jim Haywood
Atmos. Chem. Phys., 23, 1687–1703,Short summary
The recent record-breaking flood events in China during the summer of 2021 highlight the importance of mitigating the risks from future changes in high-impact weather systems under global warming. Based on a state-of-the-art Earth system model, we demonstrate a pilot study on the responses of atmospheric rivers and extreme precipitation over East Asia to anthropogenically induced climate warming and an unconventional mitigation strategy – stratospheric aerosol injection.
Azad Madhu, Myoseon Jang, and David Deacon
Atmos. Chem. Phys., 23, 1661–1675,Short summary
SOA formation is simulated using the UNIPAR model for series of linear alkanes. The inclusion of autoxidation reactions within the explicit gas mechanisms of C9–C12 was found to significantly improve predictions. Available product distributions were extrapolated with an incremental volatility coefficient (IVC) to predict SOA formation of alkanes without explicit mechanisms. These product distributions were used to simulate SOA formation from C13 and C15 and had good agreement with chamber data.
Jianbing Jin, Bas Henzing, and Arjo Segers
Atmos. Chem. Phys., 23, 1641–1660,Short summary
Aerosol models and satellite retrieval algorithms rely on different aerosol size assumptions. In practice, differences between simulations and observations do not always reflect the difference in aerosol amount. To avoid inconsistencies, we designed a hybrid assimilation approach. Different from a standard aerosol optical depth (AOD) assimilation that directly assimilates AODs, the hybrid one estimates aerosol size parameters by assimilating Ängström observations before assimilating the AODs.
Je-Yun Chun, Robert Wood, Peter Blossey, and Sarah J. Doherty
Atmos. Chem. Phys., 23, 1345–1368,Short summary
We investigate the impact of injected aerosol on subtropical low marine clouds under a variety of meteorological conditions using high-resolution model simulations. This study illustrates processes perturbed by aerosol injections and their impact on cloud properties (e.g., cloud number concentration, thickness, and cover). We show that those responses are highly sensitive to background meteorological conditions, such as precipitation, and background cloud properties.
Nora L. S. Fahrenbach and Massimo A. Bollasina
Atmos. Chem. Phys., 23, 877–894,Short summary
We studied the monthly-scale climate response to COVID-19 aerosol emission reductions during January–May 2020 using climate models. Our results show global temperature and rainfall anomalies driven by circulation changes. The climate patterns reverse polarity from JF to MAM due to a shift in the main SO2 reduction region from China to India. This real-life example of rapid climate adjustments to abrupt, regional aerosol emission reduction has large implications for future climate projections.
Seoung Soo Lee, Junshik Um, Won Jun Choi, Kyung-Ja Ha, Chang Hoon Jung, Jianping Guo, and Youtong Zheng
Atmos. Chem. Phys., 23, 273–286,Short summary
This paper elaborates on process-level mechanisms regarding how the interception of radiation by aerosols interacts with the surface heat fluxes and atmospheric instability in warm cumulus clouds. This paper elucidates how these mechanisms vary with the location or altitude of an aerosol layer. This elucidation indicates that the location of aerosol layers should be taken into account for parameterizations of aerosol–cloud interactions.
Meredith Schervish and Manabu Shiraiwa
Atmos. Chem. Phys., 23, 221–233,Short summary
Secondary organic aerosols (SOAs) can exhibit complex non-ideal behavior and adopt an amorphous semisolid state. We simulate condensation of semi-volatile compounds into a phase-separated particle to investigate the effect of non-ideality and particle phase state on the equilibration timescale of SOA partitioning. Our results provide useful insights into the interpretation of experimental observations and the description and treatment of SOA in aerosol models.
Christof G. Beer, Johannes Hendricks, and Mattia Righi
Atmos. Chem. Phys., 22, 15887–15907,Short summary
Ice-nucleating particles (INPs) have important influences on cirrus clouds and the climate system; however, their global atmospheric distribution in the cirrus regime is still very uncertain. We present a global climatology of INPs under cirrus conditions derived from model simulations, considering the mineral dust, soot, crystalline ammonium sulfate, and glassy organics INP types. The comparison of respective INP concentrations indicates the large importance of ammonium sulfate particles.
Mykhailo Savenets, Larysa Pysarenko, Svitlana Krakovska, Alexander Mahura, and Tuukka Petäjä
Atmos. Chem. Phys., 22, 15777–15791,Short summary
The paper explores the spatio-temporal variability of black carbon during a wildfire in August 2010, with a focus on Ukraine. As a research tool, the seamless Enviro-HIRLAM modelling system is used for investigating the atmospheric transport of aerosol particles emitted by wildfires from remote and local sources. The results of this study improve our understanding of the physical and chemical processes and the interactions of aerosols in the atmosphere.
Huilin Huang, Yun Qian, Ye Liu, Cenlin He, Jianyu Zheng, Zhibo Zhang, and Antonis Gkikas
Atmos. Chem. Phys., 22, 15469–15488,Short summary
Using a clustering method developed in the field of artificial neural networks, we identify four typical dust transport patterns across the Sierra Nevada, associated with the mesoscale and regional-scale wind circulations. Our results highlight the connection between dust transport and dominant weather patterns, which can be used to understand dust transport in a changing climate.
Anbao Zhu, Haiming Xu, Jiechun Deng, Jing Ma, and Shaofeng Hua
Atmos. Chem. Phys., 22, 15425–15447,Short summary
This study demonstrates the instant and delayed effects of biomass burning (BB) aerosols on precipitation over the Indochina Peninsula (ICP). The convection suppression due to the BB aerosol-induced stabilized atmosphere dominates over the favorable water-vapor condition induced by large-scale circulation responses, leading to an overall reduced precipitation in March, while the delayed effect promotes precipitation from early April to mid April due to the anomalous atmospheric circulations.
Wenjie Zhang, Hong Wang, Xiaoye Zhang, Liping Huang, Yue Peng, Zhaodong Liu, Xiao Zhang, and Huizheng Che
Atmos. Chem. Phys., 22, 15207–15221,Short summary
Aerosol–cloud interaction (ACI) is first implemented in the atmospheric chemistry system GRAPES_Meso5.1/CUACE. ACI can improve the simulated cloud, temperature, and precipitation under haze pollution conditions in Jing-Jin-Ji in China. This paper demonstrates the critical role of ACI in current numerical weather prediction over the severely polluted region.
Santeri Tuovinen, Runlong Cai, Veli-Matti Kerminen, Jingkun Jiang, Chao Yan, Markku Kulmala, and Jenni Kontkanen
Atmos. Chem. Phys., 22, 15071–15091,Short summary
We compare observed survival probabilities of atmospheric particles from Beijing, China, with survival probabilities based on analytical formulae and model simulations. We find observed survival probabilities under polluted conditions at smaller sizes to be higher, while at larger sizes they are lower than or similar to theoretical survival probabilities. Uncertainties in condensation sink and growth rate are unlikely to explain higher-than-predicted survival probabilities at smaller sizes.
Stephanie Woodward, Alistair A. Sellar, Yongming Tang, Marc Stringer, Andrew Yool, Eddy Robertson, and Andy Wiltshire
Atmos. Chem. Phys., 22, 14503–14528,Short summary
We describe the dust scheme in the UKESM1 Earth system model and show generally good agreement with observations. Comparing with the closely related HadGEM3-GC3.1 model, we show that dust differences are not only due to inter-model differences but also to the dust size distribution. Under climate change, HadGEM3-GC3.1 dust hardly changes, but UKESM1 dust decreases because that model includes the vegetation response which, in our models, has a bigger impact on dust than climate change itself.
Yang Yang, Liangying Zeng, Hailong Wang, Pinya Wang, and Hong Liao
Atmos. Chem. Phys., 22, 14489–14502,Short summary
Using an aerosol–climate model, dust pollution in China affected by different spatial and temporal types of El Niño are examined. Both eastern and central Pacific El Niño and short-duration El Niño increase winter dust concentrations over northern China, while long-duration El Niño decreases concentrations. Only long-duration El Niño events can significantly affect dust over China in the following spring. This study has profound implications for air pollution control and dust storm prediction.
Robin Stevens, Andrei Ryjkov, Mahtab Majdzadeh, and Ashu Dastoor
Atmos. Chem. Phys., 22, 13527–13549,Short summary
Absorbing particles like black carbon can be coated with other matter. How much radiation these particles absorb depends on the coating thickness. The removal of these particles by clouds and rain depends on the coating composition. These effects are important for both climate and air quality. We implement a more detailed representation of these particles in an air quality model which accounts for both coating thickness and composition. We find a significant effect on particle concentrations.
Fan Wang, Gregory R. Carmichael, Jing Wang, Bin Chen, Bo Huang, Yuguo Li, Yuanjian Yang, and Meng Gao
Atmos. Chem. Phys., 22, 13341–13353,Short summary
Unprecedented urbanization in China has led to serious urban heat island (UHI) issues, exerting intense heat stress on urban residents. We find diverse influences of aerosol pollution on urban heat island intensity (UHII) under different circulations. Our results also highlight the role of black carbon in aggravating UHI, especially during nighttime. It could thus be targeted for cooperative management of heat islands and aerosol pollution.
Qianqian Song, Zhibo Zhang, Hongbin Yu, Jasper F. Kok, Claudia Di Biagio, Samuel Albani, Jianyu Zheng, and Jiachen Ding
Atmos. Chem. Phys., 22, 13115–13135,Short summary
This study developed a dataset that enables us to efficiently calculate dust direct radiative effect (DRE, i.e., cooling or warming our planet) for any given dust size distribution in addition to three sets of dust mineral components and two dust shapes. We demonstrate and validate the method of using this dataset to calculate dust DRE. Moreover, using this dataset we found that dust mineral composition is a more important factor in determining dust DRE than dust size and shape.
Eleni Drakaki, Vassilis Amiridis, Alexandra Tsekeri, Antonis Gkikas, Emmanouil Proestakis, Sotirios Mallios, Stavros Solomos, Christos Spyrou, Eleni Marinou, Claire L. Ryder, Demetri Bouris, and Petros Katsafados
Atmos. Chem. Phys., 22, 12727–12748,Short summary
State-of-the-art atmospheric dust models have limitations in accounting for a realistic dust size distribution (emission, transport). We modify the parameterization of the mineral dust cycle by including particles with diameter >20 μm, as indicated by observations over deserts. Moreover, we investigate the effects of reduced settling velocities of dust particles. Model results are evaluated using airborne and spaceborne dust measurements above Cabo Verde.
Chenguang Tian, Xu Yue, Jun Zhu, Hong Liao, Yang Yang, Yadong Lei, Xinyi Zhou, Hao Zhou, Yimian Ma, and Yang Cao
Atmos. Chem. Phys., 22, 12353–12366,Short summary
We quantify the impacts of fire aerosols on climate through direct, indirect, and albedo effects. In atmosphere-only simulations, we find global fire aerosols cause surface cooling and rainfall inhibition over many land regions. These fast atmospheric perturbations further lead to a reduction in regional leaf area index and lightning activities. By considering the feedback of fire aerosols on humidity, lightning, and leaf area index, we predict a slight reduction in fire emissions.
Yanxing Wu, Run Liu, Yanzi Li, Junjie Dong, Zhijiong Huang, Junyu Zheng, and Shaw Chen Liu
Atmos. Chem. Phys., 22, 11945–11955,Short summary
Multiple linear regression (MLR) analyses often interpret the correlation coefficient (r2) as the contribution of an independent variable to the dependent variable. Since a good correlation does not imply a causal relationship, we propose that r2 should be interpreted as the maximum possible contribution. Moreover, MLR results are sensitive to the length of time analyzed; long-term analysis gives a more accurate assessment because of its additional constraints.
Mengying Li, Shaocai Yu, Xue Chen, Zhen Li, Yibo Zhang, Zhe Song, Weiping Liu, Pengfei Li, Xiaoye Zhang, Meigen Zhang, Yele Sun, Zirui Liu, Caiping Sun, Jingkun Jiang, Shuxiao Wang, Benjamin N. Murphy, Kiran Alapaty, Rohit Mathur, Daniel Rosenfeld, and John H. Seinfeld
Atmos. Chem. Phys., 22, 11845–11866,Short summary
This study constructed an emission inventory of condensable particulate matter (CPM) in China with a focus on organic aerosols (OAs), based on collected CPM emission information. The results show that OA emissions are enhanced twofold for the years 2014 and 2017 after the inclusion of CPM in the new inventory. Sensitivity cases demonstrated the significant contributions of CPM emissions from stationary combustion and mobile sources to primary, secondary, and total OA concentrations.
Petri Räisänen, Joonas Merikanto, Risto Makkonen, Mikko Savolahti, Alf Kirkevåg, Maria Sand, Øyvind Seland, and Antti-Ilari Partanen
Atmos. Chem. Phys., 22, 11579–11602,Short summary
A climate model is used to evaluate how the radiative forcing (RF) associated with black carbon (BC) emissions depends on the latitude, longitude, and seasonality of emissions. It is found that both the direct RF (BC absorption of solar radiation in air) and snow RF (BC absorption in snow/ice) depend strongly on the emission region and season. The results suggest that, for a given mass of BC emitted, climatic impacts are likely to be largest for high-latitude emissions due to the large snow RF.
Xipeng Jin, Xuhui Cai, Mingyuan Yu, Yu Song, Xuesong Wang, Hongsheng Zhang, and Tong Zhu
Atmos. Chem. Phys., 22, 11409–11427,Short summary
Meteorological discontinuities in the vertical direction define the lowest atmosphere as the boundary layer, while in the horizontal direction it identifies the contrast zone as the internal boundary. Both of them determine the polluted air mass dimension over the North China Plain. This study reveals the boundary layer structures under three categories of internal boundaries, modified by thermal, dynamical, and blending effects. It provides a new insight to understand regional pollution.
Lichao Yang, Wansuo Duan, Zifa Wang, and Wenyi Yang
Atmos. Chem. Phys., 22, 11429–11453,Short summary
The initial meteorological state has a great impact on PM2.5 forecasts. Assimilating additional observations is an effective way to improve the accuracy of the initial meteorological state. Here we used an advanced optimization approach to identify where we should preferentially place the meteorological observations associated with PM2.5 forecasts in the Beijing–Tianjin–Hebei region of China. We provide evidence that the target observation strategy is effective for improving PM2.5 forecasts.
Anthony C. Jones, Adrian Hill, John Hemmings, Pascal Lemaitre, Arnaud Quérel, Claire L. Ryder, and Stephanie Woodward
Atmos. Chem. Phys., 22, 11381–11407,Short summary
As raindrops fall to the ground, they capture aerosol (i.e. below-cloud scavenging or BCS). Many different BCS schemes are available to climate models, and it is unclear what the impact of selecting one scheme over another is. Here, various BCS models are outlined and then applied to mineral dust in climate model simulations. We find that dust concentrations are highly sensitive to the BCS scheme, with dust atmospheric lifetimes ranging from 5 to 44 d.
Peng Wang, Ruhan Zhang, Shida Sun, Meng Gao, Bo Zheng, Dan Zhang, Yangli Zhang, Gregory R. Carmichael, and Hongliang Zhang
Atmos. Chem. Phys. Discuss.,
Revised manuscript accepted for ACPShort summary
In China, vehicles have jumped significantly in the recent decade. This caused severe traffic congestion and aggravated air pollution. In this study, we developed a new temporal-allocation approach to quantify the impacts of traffic congestion. We found that traffic congestion worsens air quality and health burden across China, especially in the urban clusters. More effective and comprehensive vehicle emission control policies should be implemented to improve air quality in China.
Zhicong Yin, Mingkeng Duan, Yuyan Li, Tianbao Xu, and Huijun Wang
Atmos. Chem. Phys., 22, 11173–11185,Short summary
The PM2.5 concentration has been greatly reduced in recent years in China and has entered a crucial stage that required fine seasonal prediction. However, there is still no study aimed at predicting gridded PM2.5 concentration. A model for seasonal prediction of gridded winter PM2.5 concentration in the east of China was developed by analyzing the contributions of emissions and climate variability, which could provide scientific support for air pollution control at the regional and city levels.
Qirui Zhong, Nick Schutgens, Guido van der Werf, Twan van Noije, Kostas Tsigaridis, Susanne E. Bauer, Tero Mielonen, Alf Kirkevåg, Øyvind Seland, Harri Kokkola, Ramiro Checa-Garcia, David Neubauer, Zak Kipling, Hitoshi Matsui, Paul Ginoux, Toshihiko Takemura, Philippe Le Sager, Samuel Rémy, Huisheng Bian, Mian Chin, Kai Zhang, Jialei Zhu, Svetlana G. Tsyro, Gabriele Curci, Anna Protonotariou, Ben Johnson, Joyce E. Penner, Nicolas Bellouin, Ragnhild B. Skeie, and Gunnar Myhre
Atmos. Chem. Phys., 22, 11009–11032,Short summary
Aerosol optical depth (AOD) errors for biomass burning aerosol (BBA) are evaluated in 18 global models against satellite datasets. Notwithstanding biases in satellite products, they allow model evaluations. We observe large and diverse model biases due to errors in BBA. Further interpretations of AOD diversities suggest large biases exist in key processes for BBA which require better constraining. These results can contribute to further model improvement and development.
Marje Prank, Juha Tonttila, Jaakko Ahola, Harri Kokkola, Thomas Kühn, Sami Romakkaniemi, and Tomi Raatikainen
Atmos. Chem. Phys., 22, 10971–10992,Short summary
Aerosols and clouds persist as the dominant sources of uncertainty in climate projections. In this modelling study, we investigate the role of marine aerosols in influencing the lifetime of low-level clouds. Our high resolution simulations show that sea spray can both extend and shorten the lifetime of the cloud layer depending on the model setup. The impact of the primary marine organics is relatively limited while secondary aerosol from monoterpenes can have larger impact.
Roger Teoh, Ulrich Schumann, Edward Gryspeerdt, Marc Shapiro, Jarlath Molloy, George Koudis, Christiane Voigt, and Marc E. J. Stettler
Atmos. Chem. Phys., 22, 10919–10935,Short summary
Aircraft condensation trails (contrails) contribute to over half of the climate forcing attributable to aviation. This study uses historical air traffic and weather data to simulate contrails in the North Atlantic over 5 years, from 2016 to 2021. We found large intra- and inter-year variability in contrail radiative forcing and observed a 66 % reduction due to COVID-19. Most warming contrails predominantly result from night-time flights in winter.
Haochi Che, Philip Stier, Duncan Watson-Parris, Hamish Gordon, and Lucia Deaconu
Atmos. Chem. Phys., 22, 10789–10807,Short summary
Extensive stratocumulus clouds over the south-eastern Atlantic (SEA) can lead to a cooling effect on the climate. A key pathway by which aerosols affect cloud properties is by acting as cloud condensation nuclei (CCN). Here, we investigated the source attribution of CCN in the SEA as well as the cloud responses. Our results show that aerosol nucleation contributes most to CCN in the marine boundary layer. In terms of emissions, anthropogenic sources contribute most to the CCN and cloud droplets.
Marios Chatziparaschos, Nikos Daskalakis, Stelios Myriokefalitakis, Nikos Kalivitis, Athanasios Nenes, Maria Gonçalves Ageitos, Montserrat Costa-Surós, Carlos Pérez García-Pando, Medea Zanoli, Mihalis Vrekoussis, and Maria Kanakidou
Atmos. Chem. Phys. Discuss.,
Revised manuscript accepted for ACPShort summary
Ice formation is enabled by Ice Nucleating Particles (INP) at higher temperatures than homogeneous formation and can profoundly affect the properties of clouds. Our global model results show that additionally to k-feldspar dust mineral that is globally the most important INP precursor, quartz, which is abundant in mineral dust, can be regionally significant, affecting different cloud level regimes (low-level clouds) than K-feldspar (mid-level clouds).
Aditya Kumar, R. Bradley Pierce, Ravan Ahmadov, Gabriel Pereira, Saulo Freitas, Georg Grell, Chris Schmidt, Allen Lenzen, Joshua P. Schwarz, Anne E. Perring, Joseph M. Katich, John Hair, Jose L. Jimenez, Pedro Campuzano-Jost, and Hongyu Guo
Atmos. Chem. Phys., 22, 10195–10219,Short summary
We use the WRF-Chem model with new implementations of GOES-16 wildfire emissions and plume rise based on fire radiative power (FRP) to interpret aerosol observations during the 2019 NASA–NOAA FIREX-AQ field campaign and perform model evaluations. The model shows significant improvements in simulating the variety of aerosol loading environments sampled during FIREX-AQ. Our results also highlight the importance of accurate wildfire diurnal cycle and aerosol chemical mechanisms in models.
Golnaz Roudsari, Olli H. Pakarinen, Bernhard Reischl, and Hanna Vehkamäki
Atmos. Chem. Phys., 22, 10099–10114,Short summary
We use atomistic simulations to study heterogeneous ice nucleation on silver iodide surfaces in slit and wedge geometries at low supercooling which serve as a model of irregularities on real atmospheric aerosol particle surfaces. The revealed microscopic ice nucleation mechanisms in confined geometries strongly support the experimental evidence for the importance of surface features such as cracks or pits functioning as active sites for ice nucleation in the atmosphere.
Carlton Xavier, Metin Baykara, Robin Wollesen de Jonge, Barbara Altstädter, Petri Clusius, Ville Vakkari, Roseline Thakur, Lisa Beck, Silvia Becagli, Mirko Severi, Rita Traversi, Radovan Krejci, Peter Tunved, Mauro Mazzola, Birgit Wehner, Mikko Sipilä, Markku Kulmala, Michael Boy, and Pontus Roldin
Atmos. Chem. Phys., 22, 10023–10043,Short summary
The focus of this work is to study and improve our understanding of processes involved in the formation and growth of new particles in a remote Arctic marine environment. We run the 1D model ADCHEM along air mass trajectories arriving at Ny-Ålesund in May 2018. The model finds that ion-mediated H2SO4–NH3 nucleation can explain the observed new particle formation at Ny-Ålesund. The growth of particles is driven via H2SO4 condensation and formation of methane sulfonic acid in the aqueous phase.
Kai Zhang, Wentao Zhang, Hui Wan, Philip J. Rasch, Steven J. Ghan, Richard C. Easter, Xiangjun Shi, Yong Wang, Hailong Wang, Po-Lun Ma, Shixuan Zhang, Jian Sun, Susannah M. Burrows, Manish Shrivastava, Balwinder Singh, Yun Qian, Xiaohong Liu, Jean-Christophe Golaz, Qi Tang, Xue Zheng, Shaocheng Xie, Wuyin Lin, Yan Feng, Minghuai Wang, Jin-Ho Yoon, and L. Ruby Leung
Atmos. Chem. Phys., 22, 9129–9160,Short summary
Here we analyze the effective aerosol forcing simulated by E3SM version 1 using both century-long free-running and short nudged simulations. The aerosol forcing in E3SMv1 is relatively large compared to other models, mainly due to the large indirect aerosol effect. Aerosol-induced changes in liquid and ice cloud properties in E3SMv1 have a strong correlation. The aerosol forcing estimates in E3SMv1 are sensitive to the parameterization changes in both liquid and ice cloud processes.
Seoung Soo Lee, Jinho Choi, Goun Kim, Kyung-Ja Ha, Kyong-Hwan Seo, Chang Hoon Jung, Junshik Um, Youtong Zheng, Jianping Guo, Sang-Keun Song, Yun Gon Lee, and Nobuyuki Utsumi
Atmos. Chem. Phys., 22, 9059–9081,Short summary
This study investigates how aerosols affect clouds and precipitation and how the aerosol effects vary with varying types of clouds that are characterized by cloud depth in two metropolitan areas in East Asia. As cloud depth increases, the enhancement of precipitation amount transitions to no changes in precipitation amount with increasing aerosol concentrations. This indicates that cloud depth needs to be considered for a comprehensive understanding of aerosol-cloud interactions.
Karine Sartelet, Youngseob Kim, Florian Couvidat, Maik Merkel, Tuukka Petäjä, Jean Sciare, and Alfred Wiedensohler
Atmos. Chem. Phys., 22, 8579–8596,Short summary
A methodology is defined to estimate number emissions from an inventory providing mass emissions. Number concentrations are simulated over Greater Paris using different nucleation parameterisations (binary, ternary involving sulfuric acid and ammonia, and heteromolecular involving sulfuric acid and extremely low-volatility organics, ELVOCs). The comparisons show that ternary nucleation may not be a dominant process for new particle formation in cities, but they stress the role of ELVOCs.
Zhaochen Liu, Xianmei Lang, and Dabang Jiang
Atmos. Chem. Phys., 22, 7667–7680,Short summary
Stratospheric aerosol intervention geoengineering is considered a potential means to counteract global warming. Here the impact of stratospheric aerosol intervention geoengineering on surface air temperature over China and related physical processes are investigated. Results show that the increased stratospheric aerosols cause surface cooling over China. The temperature responses vary with models, regions, and seasons and are largely related to net surface shortwave radiation changes.
Jie Luo, Zhengqiang Li, Chenchong Zhang, Qixing Zhang, Yongming Zhang, Ying Zhang, Gabriele Curci, and Rajan K. Chakrabarty
Atmos. Chem. Phys., 22, 7647–7666,Short summary
The fractal black carbon was applied to re-evaluate the regional impacts of morphologies on aerosol–radiation interactions (ARIs), and the effects were compared between the US and China. The regional-mean clear-sky ARI is significantly affected by the BC morphology, and relative differences of 17.1 % and 38.7 % between the fractal model with a Df of 1.8 and the spherical model were observed in eastern China and the northwest US, respectively.
Suvarna Fadnavis, Prashant Chavan, Akash Joshi, Sunil M. Sonbawne, Asutosh Acharya, Panuganti C. S. Devara, Alexandru Rap, Felix Ploeger, and Rolf Müller
Atmos. Chem. Phys., 22, 7179–7191,Short summary
We show that large amounts of anthropogenic aerosols are transported from South Asia to the northern Indian Ocean. These aerosols are then lifted into the UTLS by the ascending branch of the Hadley circulation. They are further transported to the Southern Hemisphere and downward via westerly ducts over the tropical Atlantic and Pacific. These aerosols increase tropospheric heating, resulting in an increase in water vapor, which is then transported to the UTLS.
Xiadong An, Wen Chen, Peng Hu, Shangfeng Chen, and Lifang Sheng
Atmos. Chem. Phys., 22, 6507–6521,Short summary
The intraseasonal NAAA usually establishes quickly on day −3 with a life span of 8 days. Further results revealed that the probability of regional PM2.5 pollution related to the NAAA for at least 2 days in the NCP is 80% in NDJ period 2000–2021. Particularly, air quality in the NCP tends to deteriorate on day 2 prior to the peak day of the NAAA and reaches a peak on day −1 with a life cycle of 4 days. The corresponding meteorological conditions support these conclusions.
Jianbing Jin, Mijie Pang, Arjo Segers, Wei Han, Li Fang, Baojie Li, Haochuan Feng, Hai Xiang Lin, and Hong Liao
Atmos. Chem. Phys., 22, 6393–6410,Short summary
Super dust storms reappeared in East Asia last spring after being absent for one and a half decades. Accurate simulation of such super sandstorms is valuable, but challenging due to imperfect emissions. In this study, the emissions of these dust storms are estimated by assimilating multiple observations. The results reveal that emissions originated from both China and Mongolia. However, for northern China, long-distance transport from Mongolia contributes much more dust than Chinese deserts.
Chandan Sarangi, Yun Qian, Ruby Leung, Yang Zhang, Yufei Zou, and Yuhang Wang
Atmos. Chem. Phys. Discuss.,
Revised manuscript accepted for ACPShort summary
We show that for air quality, the densely-populated eastern US may see even larger impacts of wildfires due to long-distance smoke transport and associated positive climatic impacts, partially compensating the improvements from regulations in anthropogenic emissions. This study highlights the tension between natural and anthropogenic contributions and the non-local nature of air pollution that complicate regulatory strategies for improving future regional air quality for human health.
Thanh Le and Deg-Hyo Bae
Atmos. Chem. Phys., 22, 5253–5263,Short summary
Here we assess the response of dust activities to El Niño–Southern Oscillation (ENSO) over the 1850–2014 period using climate model outputs. Our results show that ENSO is an important driver of dust deposition and dust transportation with high consensus across models. However, the results indicate that ENSO is unlikely to show causal impacts on dust emissions of major dust sources. This study allows us to obtain further understanding of the linkages between ENSO and dust cycle at a global scale.
Yun Lin, Yuan Wang, Bowen Pan, Jiaxi Hu, Song Guo, Misti Levy Zamora, Pengfei Tian, Qiong Su, Yuemeng Ji, Jiayun Zhao, Mario Gomez-Hernandez, Min Hu, and Renyi Zhang
Atmos. Chem. Phys., 22, 4951–4967,Short summary
Severe regional haze events, which are characterized by exceedingly high levels of fine particulate matter (PM), occur frequently in many developing countries (such as China and India), with profound implications for human health, weather, and climate. Our work establishes a synthetic view for the dominant regional features during severe haze events, unraveling rapid in situ PM production and inefficient transport, both of which are amplified by atmospheric stagnation.
Ranjeet S. Sokhi, Nicolas Moussiopoulos, Alexander Baklanov, John Bartzis, Isabelle Coll, Sandro Finardi, Rainer Friedrich, Camilla Geels, Tiia Grönholm, Tomas Halenka, Matthias Ketzel, Androniki Maragkidou, Volker Matthias, Jana Moldanova, Leonidas Ntziachristos, Klaus Schäfer, Peter Suppan, George Tsegas, Greg Carmichael, Vicente Franco, Steve Hanna, Jukka-Pekka Jalkanen, Guus J. M. Velders, and Jaakko Kukkonen
Atmos. Chem. Phys., 22, 4615–4703,Short summary
This review of air quality research focuses on developments over the past decade. The article considers current and future challenges that are important from air quality research and policy perspectives and highlights emerging prominent gaps of knowledge. The review also examines how air pollution management needs to adapt to new challenges and makes recommendations to guide the direction for future air quality research within the wider community and to provide support for policy.
Xin Yin, Cong Jiang, Yaping Shao, Ning Huang, and Jie Zhang
Atmos. Chem. Phys., 22, 4509–4522,Short summary
Through a series of numerical experiments using the large-eddy-simulation model, we have developed an improved particle deposition scheme that takes into account transient wind shear fluctuations. Statistical analysis of the simulation results shows that the shear stress can be well approximated by a Weibull distribution and that the new scheme provides more accurate predictions than the conventional scheme, particularly under weak wind conditions and strong convective atmospheric conditions.
Barahona, D.: On the ice nucleation spectrum, Atmos. Chem. Phys., 12, 3733–3752, https://doi.org/10.5194/acp-12-3733-2012, 2012.
Barahona, D. and Nenes, A.: Parameterization of cirrus cloud formation in large-scale models: Homogeneous nucleation, J. Geophys. Res., 113, D11211, https://doi.org/10.1029/2007JD009355, 2008.
Barahona, D. and Nenes, A.: Parameterizing the competition between homogeneous and heterogeneous freezing in cirrus cloud formation – monodisperse ice nuclei, Atmos. Chem. Phys., 9, 369–381, https://doi.org/10.5194/acp-9-369-2009, 2009a.
Barahona, D. and Nenes, A.: Parameterizing the competition between homogeneous and heterogeneous freezing in ice cloud formation – polydisperse ice nuclei, Atmos. Chem. Phys., 9, 5933–5948, https://doi.org/10.5194/acp-9-5933-2009, 2009b.
Barahona, D. and Nenes, A.: Dynamical states of low temperature cirrus, Atmos. Chem. Phys., 11, 3757–3771, https://doi.org/10.5194/acp-11-3757-2011, 2011.
Barahona, D., Rodriguez, J., and Nenes, A.: Sensitivity of the global distribution of cirrus ice crystal concentration to heterogeneous freezing, J. Geoph. Res., 115, D23213, https://doi.org/10.1029/2010JD014273, 2010.
Barahona, D., Molod, A., Bacmeister, J., Nenes, A., Gettelman, A., Morrison, H., Phillips, V., and Eichmann, A.: Development of two-moment cloud microphysics for liquid and ice within the NASA Goddard Earth Observing System Model (GEOS-5), Geosci. Model Dev., 7, 1733–1766, https://doi.org/10.5194/gmd-7-1733-2014, 2014.
Boucher, O., Randall, D., Artaxo, P., Bretherton, C., Feingold, G., Forster, P., Kerminen, V.-M., Kondo, Y., Liao, H., Lohmann, U., Rasch, P., Sathessh, S., Sherwood, S., Stevens, B., and Zhang, X.: Clouds and Aerosols, in: Climate Change 2013: The Physical Science Basis. Contribution of Working Group I to the Fifth Assessment Report of the Intergovernmental Panel on Climate Change, Cambridge University Press, 2013.
Brewer, J.: Evidence for a world circulation provided by the measurements of helium and water vapour distribution in the stratosphere, Q. J. Roy. Meteor. Soc., 75, 351–363, https://doi.org/10.1002/qj.49707532603, 1949.
Broadley, S. L., Murray, B. J., Herbert, R. J., Atkinson, J. D., Dobbie, S., Malkin, T. L., Condliffe, E., and Neve, L.: Immersion mode heterogeneous ice nucleation by an illite rich powder representative of atmospheric mineral dust, Atmos. Chem. Phys., 12, 287–307, https://doi.org/10.5194/acp-12-287-2012, 2012.
Capps, S. L., Henze, D. K., Hakami, A., Russell, A. G., and Nenes, A.: ANISORROPIA: the adjoint of the aerosol thermodynamic model ISORROPIA, Atmos. Chem. Phys., 12, 527–543, https://doi.org/10.5194/acp-12-527-2012, 2012.
Chen, J.-P., Hazra, A., and Levin, Z.: Parameterizing ice nucleation rates using contact angle and activation energy derived from laboratory data, Atmos. Chem. Phys., 8, 7431–7449, https://doi.org/10.5194/acp-8-7431-2008, 2008.
Chen, T., Rossow, W. B., and Zhang, Y.: Radiative effects of cloud-type variations, J. Climate, 13, 264–286, https://doi.org/10.1175/1520-0442(2000)013<0264:REOCTV>2.0.CO;2, 2000.
Connolly, P. J., Möhler, O., Field, P. R., Saathoff, H., Burgess, R., Choularton, T., and Gallagher, M.: Studies of heterogeneous freezing by three different desert dust samples, Atmos. Chem. Phys., 9, 2805–2824, https://doi.org/10.5194/acp-9-2805-2009, 2009.
Cox, S. J., Kathmann, S. M., Slater, B., and Michaelides, A.: Molecular simulations of heterogeneous ice nucleation. I. Controlling ice nucleation through surface hydrophilicity, J. Chem. Phys., 142, 184704, https://doi.org/10.1063/1.4919714, 2015.
Crawford, I., Möhler, O., Schnaiter, M., Saathoff, H., Liu, D., McMeeking, G., Linke, C., Flynn, M., Bower, K. N., Connolly, P. J., Gallagher, M. W., and Coe, H.: Studies of propane flame soot acting as heterogeneous ice nuclei in conjunction with single particle soot photometer measurements, Atmos. Chem. Phys., 11, 9549–9561, https://doi.org/10.5194/acp-11-9549-2011, 2011.
Curry, J. A. and Khvorostyanov, V. I.: Assessment of some parameterizations of heterogeneous ice nucleation in cloud and climate models, Atmos. Chem. Phys., 12, 1151–1172, https://doi.org/10.5194/acp-12-1151-2012, 2012.
Cziczo, D., Froyd, K., Hoose, C., Jensen, E., Diao, M., Zondlo, M., Smith, J., Twohy, C., and Murphy, D.: Clarifying the dominant sources and mechanisms of cirrus cloud formation, Science, 340, 1320–1324, https://doi.org/10.1126/science.1234145, 2013.
d'Almeida, G.: On the variability of desert aerosol radiative characteristics, J. Geophys. Res., 92, 3017–3026, https://doi.org/10.1029/JD092iD03p03017, 1987.
DeMott, P. J., Rogers, D. C., Kreidenweis, S. M., Chen, Y., Twohy, C. H., Baumgardner, D., Heymsfield A. J., and Chan, K. R.: The role of heterogeneous freezing nucleation in upper tropospheric clouds: Inferences from SUCCESS, Geophys. Res. Lett., 25, 1387–1390, 1998.
DeMott, P., Chen, Y., Kreidenweis, S., Rogers, D., and Sherman, D.: Ice formation by black carbon particles, Geophys. Res. Lett., 26, 2429–2432, https://doi.org/10.1029/1999GL900580, 1999.
DeMott, P. J., Prenni, A. J., Liu, X., Kreidenweis, S. M., Petters, M. D., Twohy, C. H., Richardson, M. S., Eidhammer, T., and Rogers, D. C.: Predicting global atmospheric ice nuclei distributions and their impacts on climate, P. Natl. Acad. Sci., 107, 11217–11222, https://doi.org/10.1073/pnas.0910818107, 2010.
Dentener, F., Kinne, S., Bond, T., Boucher, O., Cofala, J., Generoso, S., Ginoux, P., Gong, S., Hoelzemann, J. J., Ito, A., Marelli, L., Penner, J. E., Putaud, J.-P., Textor, C., Schulz, M., van der Werf, G. R., and Wilson, J.: Emissions of primary aerosol and precursor gases in the years 2000 and 1750 prescribed data-sets for AeroCom, Atmos. Chem. Phys., 6, 4321–4344, https://doi.org/10.5194/acp-6-4321-2006, 2006.
Errico, R. M.: What is an adjoint model?, B. Am. Meterol. Soc., 78, 2577–2591, https://doi.org/10.1175/1520-0477(1997)<2577:WIAAM>2.0.CO;2, 1997.
Field, P. R., Möhler, O., Connolly, P., Krämer, M., Cotton, R., Heymsfield, A. J., Saathoff, H., and Schnaiter, M.: Some ice nucleation characteristics of Asian and Saharan desert dust, Atmos. Chem. Phys., 6, 2991–3006, https://doi.org/10.5194/acp-6-2991-2006, 2006.
Giering, R. and Kaminski, T.: Recipes for Adjoint Code Construction, ACM Trans. Mathematical Software, 24, 437–474, https://doi.org/10.1145/293686.293695, 1998.
Guo, H., Liu, Y., Daum, P., Senum, G., and Tao, W.-K.: Characteristics of vertical velocity in marine stratocumulus: comparison of large eddy simulations with observations, Environ. Res. Lett., 3, 045020, https://doi.org/10.1088/1748-9326/3/4/045020, 2008.
Hakami, A., Henze, D., Seinfeld, J., Singh, K., Sandu, A., Kim, S., Byun, D., and Li, Q.: The Adjoint of CMAQ, Environ. Sci. Technol., 41, 7807–7817, https://doi.org/10.1021/es070944p, 2007.
Hascoët, L. and Pascual, V.: TAPENADE 2.1 user's guide, INRIA Technical Report RT-0300, p. 78, 2004.
Hiranuma, N., Hoffmann, N., Kiselev, A., Dreyer, A., Zhang, K., Kulkarni, G., Koop, T., and Möhler, O.: Influence of surface morphology on the immersion mode ice nucleation efficiency of hematite particles, Atmos. Chem. Phys., 14, 2315–2324, https://doi.org/10.5194/acp-14-2315-2014, 2014..
Hoose, C. and Möhler, O.: Heterogeneous ice nucleation on atmospheric aerosols: a review of results from laboratory experiments, Atmos. Chem. Phys., 12, 9817–9854, https://doi.org/10.5194/acp-12-9817-2012, 2012.
Jensen, E. J., Kinne, S., and Toon, O. B.: Tropical cirrus cloud radiative forcing – sensitivity studies, Geophys. Res. Lett., 21, 2023–2026, https://doi.org/10.1029/94GL01358, 1994.
Jensen, E. J., Pfister, L., Bui, T.-P., Lawson, P., and Baumgardner, D.: Ice nucleation and cloud microphysical properties in tropical tropopause layer cirrus, Atmos. Chem. Phys., 10, 1369–1384, https://doi.org/10.5194/acp-10-1369-2010, 2010.
Jensen, E. J., Lawson, R. P., Bergman, J. W., Pfister, L., Bui, T. P., and Schmitt, C. G.: Physical processes controlling ice concentrations in synoptically forced, midlatitude cirrus, J. Geophys. Res., 118, 5348–5360, https://doi.org/10.1002/jgrd.50421, 2013.
Kalesse, H. and Kollias, P.: Climatology of high cloud dynamics using profiling ARM Doppler Radar observations, J. Climate, 26, 6340–6359, https://doi.org/10.1175/JCLI-D-12-00695.1, 2013.
Karcher, B. and Lohmann, U.: A Parameterization of cirrus cloud formation: Homogeneous freezing including effects of aerosol size, J. Geophys. Res., 107, 4698, https://doi.org/10.1029/2001JD001429, 2002.
Karydis, V. A., Capps, S. L., Russell, A. G., and Nenes, A.: Adjoint sensitivity of global cloud droplet number to aerosol and dynamical parameters, Atmos. Chem. Phys., 12, 9041–9055, https://doi.org/10.5194/acp-12-9041-2012, 2012.
Köhler, K. A., DeMott, P. J., Kreidenweis, S. M., Popovicheva, O. B., Petters, M. D., Carrico, C. M., Kireeva, E. D., Khokhlova, T. D., and Shonija, N. K.: Cloud condensation nuclei and ice nucleation activity of hydrophobic and hydrophilic soot particles, Phys. Chem. Chem. Phys., 11, 7906–7920, https://doi.org/10.1039/B905334B, 2009.
Koop, T., Luo, B., Tsias, A., and Peter, T.: Water activity as the determinant for homogeneous ice nucleation in aqueous solutions, Nature, 406, 611–614, https://doi.org/10.1038/35020537, 2000.
Krämer, M., Schiller, C., Afchine, A., Bauer, R., Gensch, I., Mangold, A., Schlicht, S., Spelten, N., Sitnikov, N., Borrmann, S., de Reus, M., and Spichtinger, P.: Ice supersaturations and cirrus cloud crystal numbers, Atmos. Chem. Phys., 9, 3505–3522, https://doi.org/10.5194/acp-9-3505-2009, 2009.
Kulkarni, G., Fan, J., Comstock, J. M., Liu, X., and Ovchinnikov, M.: Laboratory measurements and model sensitivity studies of dust deposition ice nucleation, Atmos. Chem. Phys., 12, 7295–7308, https://doi.org/10.5194/acp-12-7295-2012, 2012.
Lamarque, J.-F., Bond, T. C., Eyring, V., Granier, C., Heil, A., Klimont, Z., Lee, D., Liousse, C., Mieville, A., Owen, B., Schultz, M. G., Shindell, D., Smith, S. J., Stehfest, E., Van Aardenne, J., Cooper, O. R., Kainuma, M., Mahowald, N., McConnell, J. R., Naik, V., Riahi, K., and van Vuuren, D. P.: Historical (1850–2000) gridded anthropogenic and biomass burning emissions of reactive gases and aerosols: methodology and application, Atmos. Chem. Phys., 10, 7017–7039, https://doi.org/10.5194/acp-10-7017-2010, 2010.
Lin, R.-F., Starr, D. O., Reichardt, J., and DeMott, P. J.: Nucleation in synoptically forced cirrostratus, J. Geophys. Res., 110, D08208, https://doi.org/10.1029/2004JD005362, 2005.
Liu, X. and Penner, J.: Ice nucleation parameterization for global models, Met. Zeit., 14, 499–514, https://doi.org/10.1127/0941-2948/2005/0059, 2005.
Liu, X., Easter, R. C., Ghan, S. J., Zaveri, R., Rasch, P., Shi, X., Lamarque, J.-F., Gettelman, A., Morrison, H., Vitt, F., Conley, A., Park, S., Neale, R., Hannay, C., Ekman, A. M. L., Hess, P., Mahowald, N., Collins, W., Iacono, M. J., Bretherton, C. S., Flanner, M. G., and Mitchell, D.: Toward a minimal representation of aerosols in climate models: description and evaluation in the Community Atmosphere Model CAM5, Geosci. Model Dev., 5, 709-739, https://doi.org/10.5194/gmd-5-709-2012, 2012a.
Liu, X., Shi, X., Zhang, K., Jensen, E. J., Gettelman, A., Barahona, D., Nenes, A., and Lawson, P.: Sensitivity studies of dust ice nuclei effect on cirrus clouds with the Community Atmosphere Model CAM5, Atmos. Chem. Phys., 12, 12061–12079, https://doi.org/10.5194/acp-12-12061-2012, 2012b.
Lupi, L., Hudait, A., and Molinero, V.: Heterogeneous Nucleation of Ice on Carbon Surfaces, J. Am. Chem. Soc., 136, 3156–3164, https://doi.org/10.1021/ja411507a, 2014.
Marcolli, C., Gedamke, S., Peter, T., and Zobrist, B.: Efficiency of immersion mode ice nucleation on surrogates of mineral dust, Atmos. Chem. Phys., 7, 5081–5091, https://doi.org/10.5194/acp-7-5081-2007, 2007.
Meyers, M., DeMott, P., and Cotton, R.: New primary ice-nucleation parameterization in an explicit cloud model, J. Appl. Meteorol., 31, 708–721, https://doi.org/10.1175/1520-0450(1992)031<0708:NPINPI>2.0.CO;2, 1992.
Möhler, O., Field, P. R., Connolly, P., Benz, S., Saathoff, H., Schnaiter, M., Wagner, R., Cotton, R., Krämer, M., Mangold, A., and Heymsfield, A. J.: Efficiency of the deposition mode ice nucleation on mineral dust particles, Atmos. Chem. Phys., 6, 3007–3021, https://doi.org/10.5194/acp-6-3007-2006, 2006.
Morales, R. and Nenes, A.: Characteristic updrafts for computing distribution-averaged cloud droplet number and stratocumulus cloud properties, J. Geophys. Res., 115, D18220, https://doi.org/10.1029/2009JD013233, 2010.
Morales Betancourt, R. and Nenes, A.: Understanding the contributions of aerosol properties and parameterization discrepancies to droplet number variability in a global climate model, Atmos. Chem. Phys., 14, 4809–4826, https://doi.org/10.5194/acp-14-4809-2014, 2014.
Morales Betancourt, R., Lee, D., Oreopoulos, L., Sud, Y. C., Barahona, D., and Nenes, A.: Sensitivity of cirrus and mixed-phase clouds to the ice nuclei spectra in McRAS-AC: single column model simulations, Atmos. Chem. Phys., 12, 10679–10692, https://doi.org/10.5194/acp-12-10679-2012, 2012.
Muhlbauer, A., Kalesse, H., and Kollias, P.: Vertical velocities and turbulence in midlatitude anvil cirrus: A comparison between in situ aircraft measurements and ground-based Doppler cloud radar retrievals, Geophys. Res. Lett., 41, 7814–7821, https://doi.org/10.1002/2014GL062279, 2014.
Muhlbauer, A., Ackerman, T. P., Lawson, R. P., Xie, S., and Zhang, Y.: Evaluation of cloud-resolving model simulations of midlatitude cirrus with ARM and A-train observations, J. Geophys. Res., 120, 6597–6618, https://doi.org/10.1002/2014JD022570, 2015.
Murray, B. J., Wilson, T. W., Dobbie, S., Cui, Z., Al-Jumur S. M. R. K., Möhler, O., Schnaiter M., Wagner R., Benz S., Niemand, M., Saathoff, H., Ebert, V., Wagner, S., and Kärcher, B.: Heterogeneous nucleation of ice particles on glassy aerosol under cirrus conditions, Nat. Geosci., 3, 233–237, 2010.
Murray, B., O'Sullivan, D., Atkinson, J., and Webb, M.: Ice nucleation by particles immersed in supercooled cloud droplets, Chem. Soc. Rev., 41, 6519–6554, https://doi.org/10.1039/c2cs35200a, 2012.
Niedermeier, D., Hartmann, S., Shaw, R. A., Covert, D., Mentel, T. F., Schneider, J., Poulain, L., Reitz, P., Spindler, C., Clauss, T., Kiselev, A., Hallbauer, E., Wex, H., Mildenberger, K., and Stratmann, F.: Heterogeneous freezing of droplets with immersed mineral dust particles – measurements and parameterization, Atmos. Chem. Phys., 10, 3601–3614, https://doi.org/10.5194/acp-10-3601-2010, 2010.
Niemand, M., Möhler, O., Vogel, B., Vogel, H., and Hoose, C.: A particle-surface-area-based parameterization of immersion freezing on desert dust particles, J. Atmos. Sci., 69, 3077–3092, https://doi.org/10.1175/JAS-D-11-0249.1, 2012.
Phillips, V., DeMott, P., and Andronache, C.: An empirical parameterization of heterogeneous ice nucleation for multiple chemical species of aerosol, J. Atmos. Sci., 65, 2757–2783, https://doi.org/10.1175/2007JAS2546.1, 2008.
Phillips, V., DeMott, P., Andronache, C., Pratt, K., Prather, K., Subramanian, R., and Twohy, C.: Improvements to an empirical parameterization of heterogeneous ice nucleation and its comparison with observations, J. Atmos. Sci., 70, 378–409, https://doi.org/10.1175/JAS-D-12-080.1, 2013.
Popovicheva, O., Persiantseva, N., Shonija, N., DeMott, P., Koehler, K., Petters, M., Kreidenweis, S., Tishkova, V., Demirdjian, B., and Suzanne, J.: Water interaction with hydrophobic and hydrophilic soot particles, Phys. Chem. Chem. Phys., 10, 2332–2344, https://doi.org/10.1039/b718944n, 2007.
Prenni, A., Harrington, J., Tjernström, M., DeMott, P., Avramov, A., Long, C., Kreidenweis, S., Olsson, P., and Verlinde, J.: Can Ice-Nucleating Aerosols Affect Arctic Seasonal Climate?, B. Am. Meteorol. Soc., 88, 541–550, https://doi.org/10.1175/BAMS-88-4-541, 2007.
Pruppacher, H. and Klett, J.: Microphysics of clouds and precipitation, 2nd Edn., Kluwer Academic Publishers, Boston, MA, 1997.
Reinhardt, A. and Doye, J. P. K.: Effects of surface interactions on heterogeneous ice nucleation for a monatomic water model, J. Chem. Phys., 141, 084501, https://doi.org/10.1063/1.4892804, 2014.
Ren, C. and MacKenzie, A.: Cirrus parameterization and the role of ice nuclei, Q. J. Roy. Meteor. Soc., 131, 1585–1605, https://doi.org/10.1256/qj.04.126, 2005.
Savre, J., Ekman, A., Svensson, G., and Tjernström, M.: Parameterizing ice nucleation ability of mineral dust particles in the deposition mode: numerical investigations using large eddy simulation, AIP Proceedings, 1527, 922, https://doi.org/10.1063/1.4803422, 2013.
Sheyko, B., Sullivan, S. C., Morales-Betancourt, R., Capps, S., Barahona, D., Shi, X., Liu, X., and Nenes, A.: Quantifying sensitivities of ice crystal number and sources of ice crystal number variability in CAM 5.1 using the adjoint of a physically based cirrus formation parameterization, J. Geophys. Res., 120, 2834–2854, https://doi.org/10.1002/2014JD022457, 2015.
Shi, X., Liu, X., and Zhang, K.: Effects of pre-existing ice crystals on cirrus clouds and comparison between different ice nucleation parameterizations with the Community Atmosphere Model (CAM5), Atmos. Chem. Phys., 15, 1503–1520, https://doi.org/10.5194/acp-15-1503-2015, 2015.
Skrotzki, J., Connolly, P., Schnaiter, M., Saathoff, H., Möhler, O., Wagner, R., Niemand, M., Ebert, V., and Leisner, T.: The accommodation coefficient of water molecules on ice – cirrus cloud studies at the AIDA simulation chamber, Atmos. Chem. Phys., 13, 4451–4466, https://doi.org/10.5194/acp-13-4451-2013, 2013.
Spichtinger, P. and Gierens, K. M.: Modelling of cirrus clouds – Part 1b: Structuring cirrus clouds by dynamics, Atmos. Chem. Phys., 9, 707–719, https://doi.org/10.5194/acp-9-707-2009, 2009.
Spichtinger, P. and Krämer, M.: Tropical tropopause ice clouds: a dynamic approach to the mystery of low crystal numbers, Atmos. Chem. Phys., 13, 9801–9818, https://doi.org/10.5194/acp-13-9801-2013, 2013.
Steinke, I., Hoose, C., Möhler, O., Connolly, P., and Leisner, T.: A new temperature- and humidity-dependent surface site density approach for deposition ice nucleation, Atmos. Chem. Phys., 15, 3703–3717, https://doi.org/10.5194/acp-15-3703-2015, 2015.
Vali, G.: Interpretation of freezing nucleation experiments: singular and stochastic; sites and surfaces, Atmos. Chem. Phys., 14, 5271–5294, https://doi.org/10.5194/acp-14-5271-2014, 2014.
Wang, Y., Liu, X., Hoose, C., and Wang, B.: Different contact angle distributions for heterogeneous ice nucleation in the Community Atmospheric Model version 5, Atmos. Chem. Phys., 14, 10411–10430, https://doi.org/10.5194/acp-14-10411-2014, 2014.
Whitby, K.: The physical characteristics of sulfur aerosols, Atmos. Environ., 41, 25–49, https://doi.org/10.1016/0004-6981(78)90196-8, 2007.
Xie, S., Liu, X., Zhao, C., and Zhang, Y.: Sensitivity of CAM5-simulated Arctic clouds and radiation to nucleation parameterization, J. Climate, 26, 5981–5999, https://doi.org/10.1175/JCLI-D-12-00517.1, 2013.
Zhang, K., Liu, X., Wang, M., Comstock, J. M., Mitchell, D. L., Mishra, S., and Mace, G. G.: Evaluating and constraining ice cloud parameterizations in CAM5 using aircraft measurements from the SPARTICUS campaign, Atmos. Chem. Phys., 13, 4963–4982, https://doi.org/10.5194/acp-13-4963-2013, 2013.
Zuberi, B., Bertram, A., Cassa, C., Molina, L., and Molina, M.: Heterogeneous nucleation of ice in ammonium sulfate-water particles with mineral dust immersions, Geophys. Res. Lett., 29, 142.1–142.4, https://doi.org/10.1029/2001GL014289, 2002.
We use the adjoint model of a cirrus parameterization to quantify sources of crystal variability for various ice-nucleating spectra and output from CAM5. The sensitivities can be directly linked to nucleation regime and efficiency of various INP. The lab-based spectrum calculates much higher INP efficiencies than field-based ones, owing to aerosol surface properties. The sensitivity to temperature tends to be low, due to the compensating effects of temperature on INP spectrum parameters.
We use the adjoint model of a cirrus parameterization to quantify sources of crystal variability...