Articles | Volume 22, issue 14
© Author(s) 2022. This work is distributed under
the Creative Commons Attribution 4.0 License.
the Creative Commons Attribution 4.0 License.
© Author(s) 2022. This work is distributed under
the Creative Commons Attribution 4.0 License.
the Creative Commons Attribution 4.0 License.
Measurement report: An exploratory study of fluorescence and cloud condensation nuclei activity of urban aerosols in San Juan, Puerto Rico
Droplet Measurement Technologies, LLC, Longmont, Colorado, USA
Department of Microbiology and Medical Zoology, School of Medicine, University of Puerto Rico – Medical Sciences Campus, San Juan, Puerto Rico, USA
Olga L. Mayol-Bracero
Department of Environmental Sciences, University of Puerto Rico – Río Piedras Campus, San Juan, Puerto Rico, USA
now at: Environment and Climate Sciences Department, Brookhaven National Laboratory, Upton, New York, USA
No articles found.
Mahen Konwar, Benjamin Werden, Edward C. Fortner, Sudarsan Bera, Mercy Varghese, Subharthi Chowdhuri, Kurt Hibert, Philip Croteau, John Jayne, Manjula Canagaratna, Neelam Malap, Sandeep Jayakumar, Shivsai A. Dixit, Palani Murugavel, Duncan Axisa, Darrel Baumgardner, Peter F. DeCarlo, Doug R. Worsnop, and Thara Prabhakaran
Atmos. Meas. Tech. Discuss.,
Revised manuscript under review for AMTShort summary
In a warm cloud seeding experiment hygroscopic particles are released to alter cloud processes to induce early raindrops. During Cloud Aerosol Interaction and Precipitation Enhancement Experiment, airborne mini-Aerosol Mass Spectrometers analyze the particles on which clouds form. The seeded clouds showed higher concentrations of Chlorine (Cl) and potassium (K), the oxidizing agents of flares. Small cloud droplet concentrations increased, and seeding particles were detected in deep cloud depths.
Graciela B. Raga, Darrel Baumgardner, Blanca Rios, Yanet Díaz-Esteban, Alejandro Jaramillo, Martin Gallagher, Bastien Sauvage, Pawel Wolff, and Gary Lloyd
Atmos. Chem. Phys., 22, 2269–2292,Short summary
The In-Service Aircraft for a Global Observing System (IAGOS) is a small fleet of commercial aircraft that carry a suite of meteorological, gas, aerosol, and cloud sensors and have been measuring worldwide for almost 9 years, since late 2011. Extreme ice events (EIEs) have been identified from the IAGOS cloud measurements and linked to surface emissions for biomass and fossil fuel consumption. The results reported here are highly relevant for climate change and flight operations forecasting.
Elvis Torres-Delgado, Darrel Baumgardner, and Olga L. Mayol-Bracero
Atmos. Chem. Phys., 21, 18011–18027,Short summary
African dust aerosols can travel thousands of kilometers and reach the Caribbean and other places, where they can serve as ice and cloud condensation nuclei and alter precipitation patterns. Cloud microphysical properties (droplet number and size) were measured in a Caribbean tropical montane cloud forest along with models and satellite products. The results of the study suggest that meteorology and air mass history are more important for cloud processes than aerosols transported from Africa.
Fernanda Córdoba, Carolina Ramírez-Romero, Diego Cabrera, Graciela B. Raga, Javier Miranda, Harry Alvarez-Ospina, Daniel Rosas, Bernardo Figueroa, Jong Sung Kim, Jacqueline Yakobi-Hancock, Talib Amador, Wilfrido Gutierrez, Manuel García, Allan K. Bertram, Darrel Baumgardner, and Luis A. Ladino
Atmos. Chem. Phys., 21, 4453–4470,Short summary
Most precipitation from deep clouds over the continents and in the intertropical convergence zone is strongly influenced by the presence of ice crystals whose formation requires the presence of aerosol particles. In the present study, the ability of three different aerosol types (i.e., marine aerosol, biomass burning, and African dust) to facilitate ice particle formation was assessed in the Yucatán Peninsula, Mexico.
Carolina Ramírez-Romero, Alejandro Jaramillo, María F. Córdoba, Graciela B. Raga, Javier Miranda, Harry Alvarez-Ospina, Daniel Rosas, Talib Amador, Jong Sung Kim, Jacqueline Yakobi-Hancock, Darrel Baumgardner, and Luis A. Ladino
Atmos. Chem. Phys., 21, 239–253,Short summary
Field measurements were conducted to confirm the arrival of African dust on the Yucatàn Peninsula. Aerosol particles were monitored at ground level by different online and off-line sensors. Several particulate matter peaks were observed with a relative increase in their levels of up to 500 % with respect to background conditions. Based on the chemical composition, back trajectories, vertical profiles, reanalysis, and satellite images, it was found that the peaks are linked to African dust.
Lester Alfonso, Graciela B. Raga, and Darrel Baumgardner
Atmos. Chem. Phys., 19, 14917–14932,Short summary
The aim of this paper is to find some observational evidence of gel formation in clouds, by analyzing the distribution of the largest droplet at an early stage of cloud formation, and to show that the mass of the gel (
lucky droplet) is a mixture of Gaussian and Gumbel distributions. The results obtained may help advance the understanding of precipitation formation and are a novel application of the theory of critical phenomena in cloud physics.
Viswanathan Bringi, Merhala Thurai, and Darrel Baumgardner
Atmos. Meas. Tech., 11, 1377–1384,Short summary
Raindrop fall velocities are important for rain rate estimation, soil erosion studies and in numerical modelling of rain formation in clouds. The assumption that the fall velocity is uniquely related to drop size is made inherently based on laboratory measurements under still air conditions from nearly 68 years ago. There have been very few measurements of drop fall speeds in natural rain under both still and turbulent wind conditions. We report on fall speed measurements in natural rain shafts.
Anja Costa, Jessica Meyer, Armin Afchine, Anna Luebke, Gebhard Günther, James R. Dorsey, Martin W. Gallagher, Andre Ehrlich, Manfred Wendisch, Darrel Baumgardner, Heike Wex, and Martina Krämer
Atmos. Chem. Phys., 17, 12219–12238,Short summary
The paper presents 38 h of in situ cloud spectrometer observations of microphysical cloud properties in the Arctic, midlatitudes and tropics. The clouds are classified via particle concentrations, size distributions, and – as a novelty – small particle aspherical fractions. Cloud-type profiles are given for different temperatures and locations. The results confine regions where different cloud transformation processes occurred and emphasise the importance of small particle shape detection.
Ulrich Schumann, Robert Baumann, Darrel Baumgardner, Sarah T. Bedka, David P. Duda, Volker Freudenthaler, Jean-Francois Gayet, Andrew J. Heymsfield, Patrick Minnis, Markus Quante, Ehrhard Raschke, Hans Schlager, Margarita Vázquez-Navarro, Christiane Voigt, and Zhien Wang
Atmos. Chem. Phys., 17, 403–438,Short summary
The initially linear clouds often seen behind aircraft are known as contrails. Contrails are prototype cirrus clouds forming under well-known conditions, but with less certain life cycle and climate effects. This paper collects contrail data from a large set of measurements and compares them among each other and with models. The observations show consistent contrail properties over a wide range of aircraft and atmosphere conditions. The dataset is available for further research.
Ana Graciela Ulke, Marcela M. Torres Brizuela, Graciela B. Raga, and Darrel Baumgardner
Nat. Hazards Earth Syst. Sci., 16, 2159–2175,Short summary
The eruption in June 2011 of the Puyehue-Cordón Caulle Volcanic Complex (Chile) impacted air traffic around the Southern Hemisphere for several months. The ash deposited in vast areas of the Patagonian steppe was subjected to the strong wind conditions prevalent during the austral winter and spring. An ash resuspension event impacted Buenos Aires and resulted in the closure of airports in the area on 16 October 2011. Measurements of aerosol properties clearly indicate the enhanced concentrations
Mark Hernandez, Anne E. Perring, Kevin McCabe, Greg Kok, Gary Granger, and Darrel Baumgardner
Atmos. Meas. Tech., 9, 3283–3292,Short summary
We have performed laboratory experiments examining a large set of known bacterial, fungal and pollen species using a Wideband Integrated Bioaerosol Sensor (WIBS). The instrumental response is shown to be sufficiently distinct for these classes of particles to distinguish between them, and this library will provide a framework for interpretation of UV-induced fluorescence measurements of atmospheric bioaerosol. Atmospheric implications and instrumental considerations are discussed.
Anna E. Luebke, Armin Afchine, Anja Costa, Jens-Uwe Grooß, Jessica Meyer, Christian Rolf, Nicole Spelten, Linnea M. Avallone, Darrel Baumgardner, and Martina Krämer
Atmos. Chem. Phys., 16, 5793–5809,Short summary
In this study, we present observational evidence to show that two distinct types of cirrus clouds exist – in situ origin and liquid origin cirrus. These two types differ by their formation mechanism and other properties. Airborne, in-cloud measurements of cloud ice water content (IWC), ice crystal concentration (Nice), and ice crystal size from the 2014 ML-CIRRUS campaign provide cloud samples that have been divided and analyzed according to their origin type.
María José Granados-Muñoz, Juan Antonio Bravo-Aranda, Darrel Baumgardner, Juan Luis Guerrero-Rascado, Daniel Pérez-Ramírez, Francisco Navas-Guzmán, Igor Veselovskii, Hassan Lyamani, Antonio Valenzuela, Francisco José Olmo, Gloria Titos, Javier Andrey, Anatoli Chaikovsky, Oleg Dubovik, Manuel Gil-Ojeda, and Lucas Alados-Arboledas
Atmos. Meas. Tech., 9, 1113–1133,Short summary
A Saharan dust event is studied in detail using ground-based remote sensing measurements from lidar technology, as well as sun- and star-photometers. The use of combined techniques allows for obtaining both profiles and column-integrated microphysical properties during night and daytime. Besides, for the first time a validation of the CAS-POL depolarization measurements and LIRIC profiles is performed, thanks to the availability of aircraft in situ measurements, obtaining reasonable agreement.
Martina Krämer, Christian Rolf, Anna Luebke, Armin Afchine, Nicole Spelten, Anja Costa, Jessica Meyer, Martin Zöger, Jessica Smith, Robert L. Herman, Bernhard Buchholz, Volker Ebert, Darrel Baumgardner, Stephan Borrmann, Marcus Klingebiel, and Linnea Avallone
Atmos. Chem. Phys., 16, 3463–3483,Short summary
A guide to cirrus clouds is compiled from extensive model simulations and aircraft observations. Two types of cirrus are found: rather thin in situ cirrus that form directly as ice and thicker liquid origin cirrus consisting of uplifted frozen liquid drops. Over Europe, thinner in situ and liquid origin cirrus occur often together with frontal systems, while over the US and the Tropics, thick liquid origin cirrus formed in large convective systems are detected more frequently.
A. Retama, D. Baumgardner, G. B. Raga, G. R. McMeeking, and J. W. Walker
Atmos. Chem. Phys., 15, 9693–9709,Short summary
Extended measurements of equivalent black carbon (eBC) derived from light absorption measurements have been made with a PAX over a 13 month period. The daily trends in eBC and other co-pollutants are evaluated with respect to season. The primary factors that led to large changes between the wet and dry seasons are the accelerated vertical mixing of boundary layer and free tropospheric air, by the formation of clouds and decreased actinic flux that reduces the production of ozone.
K. Beswick, D. Baumgardner, M. Gallagher, A. Volz-Thomas, P. Nedelec, K.-Y. Wang, and S. Lance
Atmos. Meas. Tech., 7, 1443–1457,
G. B. Raga, D. Baumgardner, A. G. Ulke, M. Torres Brizuela, and B. Kucienska
Nat. Hazards Earth Syst. Sci., 13, 2319–2330,
Related subject area
Subject: Aerosols | Research Activity: Laboratory Studies | Altitude Range: Troposphere | Science Focus: Physics (physical properties and processes)Analysis of insoluble particles in hailstones in ChinaInfluence of acidity on liquid–liquid phase transitions of mixed secondary organic aerosol (SOA) proxy–inorganic aerosol dropletsDeposition freezing, pore condensation freezing and adsorption: three processes, one description?Measurements and calculations of enhanced side- and back-scattering of visible radiation by black carbon aggregatesDirect observation for relative-humidity-dependent mixing states of submicron particles containing organic surfactants and inorganic saltsComplex refractive index and single scattering albedo of Icelandic dust in the shortwave part of the spectrumVolatility of aerosol particles from NO3 oxidation of various biogenic organic precursorsInsights into secondary organic aerosol formation from the day- and nighttime oxidation of PAHs and furans in an oxidation flow reactorIs transport of microplastics different from that of mineral dust? Results from idealized wind tunnel studiesSaturation vapor pressure characterization of selected low-volatility organic compounds using a residence time chamberJet aircraft lubrication oil droplets as contrail ice-forming particlesInfluence of the previous North Atlantic Oscillation (NAO) on the spring dust aerosols over North ChinaHUB: a method to model and extract the distribution of ice nucleation temperatures from drop-freezing experimentsSize-dependent hygroscopicity of levoglucosan and D-glucose aerosol nanoparticlesTechnical note: Sublimation of frozen CsCl solutions in an environmental scanning electron microscope (ESEM) – determining the number and size of salt particles relevant to sea salt aerosolsMicrophysics of liquid water in sub-10 nm ultrafine aerosol particlesComparing the ice nucleation properties of the kaolin minerals kaolinite and halloysitePhysicochemical properties of charcoal aerosols derived from biomass pyrolysis affect their ice-nucleating abilities at cirrus and mixed-phase cloud conditionsReconsideration of surface tension and phase state effects on cloud condensation nuclei activity based on the atomic force microscopy measurementHygroscopicity and CCN potential of DMS-derived aerosol particlesHybrid water adsorption and solubility partitioning for aerosol hygroscopicity and droplet growthExperimental development of a lake spray source function and its model implementation for Great Lakes surface emissionsThe effectiveness of the coagulation sink of 3–10 nm atmospheric particlesWhat caused the interdecadal shift in the El Niño–Southern Oscillation (ENSO) impact on dust mass concentration over northwestern South Asia?Viscosity and physical state of sucrose mixed with ammonium sulfate dropletsDistribution and stable carbon isotopic composition of dicarboxylic acids, ketocarboxylic acids and α-dicarbonyls in fresh and aged biomass burning aerosolsTime dependence of heterogeneous ice nucleation by ambient aerosols: laboratory observations and a formulation for modelsLaboratory studies of ice nucleation onto bare and internally mixed soot–sulfuric acid particlesEnhanced soot particle ice nucleation ability induced by aggregate compaction and densificationOpinion: Insights into updating Ambient Air Quality Directive 2008/50/ECOn the evolution of sub- and super-saturated water uptake of secondary organic aerosol in chamber experiments from mixed precursorsHygroscopicity of organic compounds as a function of organic functionality, water solubility, molecular weight, and oxidation levelParticle emissions from a modern heavy-duty diesel engine as ice nuclei in immersion freezing mode: a laboratory study on fossil and renewable fuelsComparison of saturation vapor pressures of α-pinene + O3 oxidation products derived from COSMO-RS computations and thermal desorption experimentsPhysical and chemical properties of black carbon and organic matter from different combustion and photochemical sources using aerodynamic aerosol classificationTechnical note: Pyrolysis principles explain time-resolved organic aerosol release from biomass burningThe effect of (NH4)2SO4 on the freezing properties of non-mineral dust ice-nucleating substances of atmospheric relevanceHeterogeneous ice nucleation ability of aerosol particles generated from Arctic sea surface microlayer and surface seawater samples at cirrus temperaturesAerosol formation and growth rates from chamber experiments using Kalman smoothingPhase state of secondary organic aerosol in chamber photo-oxidation of mixed precursorsIce nucleation on surrogates of boreal forest SOA particles: effect of water content and oxidative ageViscosity and phase state of aerosol particles consisting of sucrose mixed with inorganic saltsObservations on hygroscopic growth and phase transitions of mixed 1, 2, 6-hexanetriol ∕ (NH4)2SO4 particles: investigation of the liquid–liquid phase separation (LLPS) dynamic process and mechanism and secondary LLPS during the dehumidificationBoundary layer structure characteristics under objective classification of persistent pollution weather types in the Beijing areaProperties and emission factors of cloud condensation nuclei from biomass cookstoves – observations of a strong dependency on potassium content in the fuelMeasurement report: Effects of NOx and seed aerosol on highly oxygenated organic molecules (HOMs) from cyclohexene ozonolysisInteractions of organosulfates with water vapor under sub- and supersaturated conditionsLaboratory study of the collection efficiency of submicron aerosol particles by cloud droplets – Part I: Influence of relative humiditySize-resolved atmospheric ice-nucleating particles during East Asian dust eventsAqueous-phase behavior of glyoxal and methylglyoxal observed with carbon and oxygen K-edge X-ray absorption spectroscopy
Haifan Zhang, Xiangyu Lin, Qinghong Zhang, Kai Bi, Chan-Pang Ng, Yangze Ren, Huiwen Xue, Li Chen, and Zhuolin Chang
Atmos. Chem. Phys., 23, 13957–13971,Short summary
This work is the first study to simultaneously analyze the number concentrations and species of insoluble particles in hailstones. The size distribution of insoluble particles for each species vary greatly in different hailstorms but little in shells. Two classic size distribution modes of organics and dust were fitted for the description of insoluble particles in deep convection. Combining this study with future experiments will lead to refinement of weather and climate models.
Yueling Chen, Xiangyu Pei, Huichao Liu, Yikan Meng, Zhengning Xu, Fei Zhang, Chun Xiong, Thomas C. Preston, and Zhibin Wang
Atmos. Chem. Phys., 23, 10255–10265,Short summary
The impact of acidity on the phase transition behavior of levitated aerosol particles was examined. Our results revealed that lower acidity decreases the separation relative humidity of aerosol droplets mixed with ammonium sulfate and secondary organic aerosol proxy. Our research suggests that in real atmospheric conditions, with the high acidity found in many ambient aerosol particles, droplets encounter heightened impediments to phase separation and tend to display a homogeneous structure.
Mária Lbadaoui-Darvas, Ari Laaksonen, and Athanasios Nenes
Atmos. Chem. Phys., 23, 10057–10074,Short summary
Heterogeneous ice nucleation is the main ice formation mechanism in clouds. The mechanism of different freezing modes is to date unknown, which results in large model biases. Experiments do not allow for direct observation of ice nucleation at its native resolution. This work uses first principles molecular simulations to determine the mechanism of the least-understood ice nucleation mode and link it to adsorption through a novel modeling framework that unites ice and droplet formation.
Carynelisa Haspel, Cuiqi Zhang, Martin J. Wolf, Daniel J. Cziczo, and Maor Sela
Atmos. Chem. Phys., 23, 10091–10115,Short summary
Small particles, commonly termed aerosols, can be found throughout the atmosphere and come from both natural and anthropogenic sources. One important type of aerosol is black carbon (BC). In this study, we conducted laboratory measurements of light scattering by particles meant to mimic atmospheric BC and compared them to calculations of scattering. We find that it is likely that calculations underpredict the scattering by BC particles of certain polarizations of light in certain directions.
Chun Xiong, Binyu Kuang, Fei Zhang, Xiangyu Pei, Zhengning Xu, and Zhibin Wang
Atmos. Chem. Phys., 23, 8979–8991,Short summary
In hydration, an apparent water diffusion hindrance by an organic surfactant shell was confirmed, raising the inorganic deliquescence relative humidity (RH) to a nearly saturated condition. In dehydration, phase separations were observed for inorganic surfactant systems, showing a strong dependence on the organic molecular oxygen-to-carbon ratio. Our results could improve fundamental knowledge about aerosol mixing states and decrease uncertainty in model estimations of global radiative effects.
Clarissa Baldo, Paola Formenti, Claudia Di Biagio, Gongda Lu, Congbo Song, Mathieu Cazaunau, Edouard Pangui, Jean-Francois Doussin, Pavla Dagsson-Waldhauserova, Olafur Arnalds, David Beddows, A. Robert MacKenzie, and Zongbo Shi
Atmos. Chem. Phys., 23, 7975–8000,Short summary
This paper presents new shortwave spectral complex refractive index and single scattering albedo data for Icelandic dust. Our results show that the imaginary part of the complex refractive index of Icelandic dust is at the upper end of the range of low-latitude dust. Furthermore, we observed that Icelandic dust is more absorbing towards the near-infrared, which we attribute to its high magnetite content. These findings are important for modeling dust aerosol radiative effects in the Arctic.
Emelie L. Graham, Cheng Wu, David M. Bell, Amelie Bertrand, Sophie L. Haslett, Urs Baltensperger, Imad El Haddad, Radovan Krejci, Ilona Riipinen, and Claudia Mohr
Atmos. Chem. Phys., 23, 7347–7362,Short summary
The volatility of an aerosol particle is an important parameter for describing its atmospheric lifetime. We studied the volatility of secondary organic aerosols from nitrate-initiated oxidation of three biogenic precursors with experimental methods and model simulations. We saw higher volatility than for the corresponding ozone system, and our simulations produced variable results with different parameterizations which warrant a re-evaluation of the treatment of the nitrate functional group.
Abd El Rahman El Mais, Barbara D'Anna, Luka Drinovec, Andrew Lambe, Zhe Peng, Jean-Eudes Petit, Olivier Favez, Selim Ait-Aissa, and Alexandre Albinet
Polycyclic aromatic hydrocarbons (PAHS) and furans are key precursors of secondary organic aerosols (SOA) related to biomass burning emissions. We evaluated and compared the formation yields, physical and light absorption properties of laboratory-generated SOA from the oxidation of such compounds for both, daytime and nighttime reactivities. The results illustrate that PAHs are large SOA precursors and may contribute significantly to the biomass burning Brown Carbon (BrC) in the atmosphere.
Eike Maximilian Esders, Sebastian Sittl, Inka Krammel, Wolfgang Babel, Georg Papastavrou, and Christoph Karl Thomas
We asked, Is the transport of plastic dust via air different from mineral dust? We observed plastic and mineral particles in a wind tunnel and measured at what wind speeds the particles start to move. The results show that plastic and mineral particles smaller than 70 µm behave similarly. For bigger particles, plastic particles move more easily, as they weigh less. We conclude that it is no surprise, that like mineral dust, plastic dust is found all around the globe, transported via air.
Zijun Li, Noora Hyttinen, Miika Vainikka, Olli-Pekka Tikkasalo, Siegfried Schobesberger, and Taina Yli-Juuti
Atmos. Chem. Phys., 23, 6863–6877,Short summary
The saturation vapor pressure (psat) of low-volatility organic compounds (LVOCs) governs their partitioning between the gas and particle phases. To estimate the psat of selected LVOCs, we performed particle evaporation measurements in a residence time chamber at a temperature setting relevant to atmospheric aerosol formation and conducted state-of-the-art computational calculations. We found good agreement between the experimentally measured and model-estimated psat values for most LVOCs.
Joel Ponsonby, Leon King, Benjamin Murray, and Marc Stettler
Aerosol emissions from aircraft engines contribute to the formation of contrails, which have a climate impact as important as that of aviation’s CO2 emissions. For the first time, we experimentally investigate the freezing behaviour of water droplets formed on jet lubrication oil aerosol. We show that they can activate to form water droplets and discuss their potential impact on contrail formation. Our study has implications for contrails produce by future aircraft engine and fuel technologies.
Yan Li, Falei Xu, Juan Feng, Mengying Du, Wenjun Song, Chao Li, and Wenjing Zhao
Atmos. Chem. Phys., 23, 6021–6042,Short summary
There is a significantly negative relationship between boreal winter North Atlantic Oscillation (NAO) and dust aerosols (DAs) in the eastern part of China (30–40°N, 105–120°E), which is not a DA source area but is severely affected by the dust events (DEs). Under the effect of the NAO negative phase, main atmospheric circulation during the DEs is characterized by variation of the transient eddy flux. The work is of reference value to the prediction of DEs and the understanding of their causes.
Ingrid de Almeida Ribeiro, Konrad Meister, and Valeria Molinero
Atmos. Chem. Phys., 23, 5623–5639,Short summary
Ice formation is a key atmospheric process facilitated by a wide range of aerosols. We present a method to model and interpret ice nucleation experiments and extract the distribution of the potency of nucleation sites. We use the method to optimize the conditions of laboratory sampling and extract distributions of ice nucleation temperatures from bacteria, fungi, and pollen. These reveal unforeseen subpopulations of nuclei in these systems and how they respond to changes in their environment.
Ting Lei, Hang Su, Nan Ma, Ulrich Pöschl, Alfred Wiedensohler, and Yafang Cheng
Atmos. Chem. Phys., 23, 4763–4774,Short summary
We investigate the hygroscopic behavior of levoglucosan and D-glucose nanoparticles using a nano-HTDMA. There is a weak size dependence of the hygroscopic growth factor of levoglucosan and D-glucose with diameters down to 20 nm, while a strong size dependence of the hygroscopic growth factor of D-glucose has been clearly observed in the size range 6 to 20 nm. The use of the DKA method leads to good agreement with the hygroscopic growth factor of glucose nanoparticles with diameters down to 6 nm.
Lubica Vetráková, Vilém Neděla, Kamila Závacká, Xin Yang, and Dominik Heger
Atmos. Chem. Phys., 23, 4463–4488,Short summary
Salt aerosols are important to polar atmospheric chemistry and global climate. Therefore, we utilized a unique electron microscope to identify the most suitable conditions for formation of the small salt (CsCl) particles, proxies of the aerosols, from sublimating salty snow. Very low sublimation temperature and low salt concentration are needed for formation of such particles. These observations may help us to better understand polar spring ozone depletion and bromine explosion events.
Xiaohan Li and Ian C. Bourg
Atmos. Chem. Phys., 23, 2525–2556,Short summary
Aerosol particles with sizes smaller than 50 nm impact cloud formation and precipitation. Representation of this effect is hindered by limited understanding of the properties of liquid water in these particles. Our simulations of aerosol particles containing salt or organic compounds reveal that water enters a less cohesive phase at droplet sizes below 4 nm. This effect causes important deviations from theoretical predictions of aerosol properties, including phase state and hygroscopic growth.
Kristian Klumpp, Claudia Marcolli, Ana Alonso-Hellweg, Christopher H. Dreimol, and Thomas Peter
Atmos. Chem. Phys., 23, 1579–1598,Short summary
The prerequisites of a particle surface for efficient ice nucleation are still poorly understood. This study compares the ice nucleation activity of two chemically identical but morphologically different minerals (kaolinite and halloysite). We observe, on average, not only higher ice nucleation activities for halloysite than kaolinite but also higher diversity between individual samples. We identify the particle edges as being the most likely site for ice nucleation.
Fabian Mahrt, Carolin Rösch, Kunfeng Gao, Christopher H. Dreimol, Maria A. Zawadowicz, and Zamin A. Kanji
Atmos. Chem. Phys., 23, 1285–1308,Short summary
Major aerosol types emitted by biomass burning include soot, ash, and charcoal particles. Here, we investigated the ice nucleation activity of 400 nm size-selected particles of two different pyrolyis-derived charcoal types in the mixed phase and cirrus cloud regime. We find that ice nucleation is constrained to cirrus cloud conditions, takes place via pore condensation and freezing, and is largely governed by the particle porosity and mineral content.
Chun Xiong, Xueyan Chen, Xiaolei Ding, Binyu Kuang, Xiangyu Pei, Zhengning Xu, Shikuan Yang, Huan Hu, and Zhibin Wang
Atmos. Chem. Phys., 22, 16123–16135,Short summary
Water surface tension is applied widely in current aerosol–cloud models but could be inappropriate in the presence of atmospheric surfactants. With cloud condensation nuclei (CCN) activity and atomic force microscopy (AFM) measurement results of mixed inorganic salt and dicarboxylic acid particles, we concluded that surface tension reduction and phase state should be carefully considered in aerosol–cloud interactions. Our results could help to decease uncertainties in climate models.
Bernadette Rosati, Sini Isokääntä, Sigurd Christiansen, Mads Mørk Jensen, Shamjad P. Moosakutty, Robin Wollesen de Jonge, Andreas Massling, Marianne Glasius, Jonas Elm, Annele Virtanen, and Merete Bilde
Atmos. Chem. Phys., 22, 13449–13466,Short summary
Sulfate aerosols have a strong influence on climate. Due to the reduction in sulfur-based fossil fuels, natural sulfur emissions play an increasingly important role. Studies investigating the climate relevance of natural sulfur aerosols are scarce. We study the water uptake of such particles in the laboratory, demonstrating a high potential to take up water and form cloud droplets. During atmospheric transit, chemical processing affects the particles’ composition and thus their water uptake.
Kanishk Gohil, Chun-Ning Mao, Dewansh Rastogi, Chao Peng, Mingjin Tang, and Akua Asa-Awuku
Atmos. Chem. Phys., 22, 12769–12787,Short summary
The Hybrid Activity Model (HAM) is a promising new droplet growth model that can be potentially used for the analysis of any type of atmospheric compound. HAM may potentially improve the representation of hygroscopicity of organic aerosols in large-scale global climate models (GCMs), hence reducing the uncertainties in the climate forcing due to the aerosol indirect effect.
Charbel Harb and Hosein Foroutan
Atmos. Chem. Phys., 22, 11759–11779,Short summary
A model representation of lake spray aerosol (LSA) ejection from freshwater breaking waves is crucial for understanding their climatic and public health impacts. We develop an LSA emission parameterization and implement it in an atmospheric model to investigate Great Lakes surface emissions. We find that the same breaking wave is likely to produce fewer aerosols in freshwater than in saltwater and that Great Lakes emissions influence the regional aerosol burden and can reach the cloud layer.
Runlong Cai, Ella Häkkinen, Chao Yan, Jingkun Jiang, Markku Kulmala, and Juha Kangasluoma
Atmos. Chem. Phys., 22, 11529–11541,Short summary
The influences of new particle formation on the climate and air quality are governed by particle survival, which has been under debate due to uncertainties in the coagulation sink. Here we measure the coagulation coefficient of sub-10 nm particles and demonstrate that collisions between the freshly nucleated and background particles can effectively lead to coagulation. We further show that the effective coagulation sink is consistent with the new particle formation measured in urban Beijing.
Lamei Shi, Jiahua Zhang, Da Zhang, Jingwen Wang, Xianglei Meng, Yuqin Liu, and Fengmei Yao
Atmos. Chem. Phys., 22, 11255–11274,Short summary
Dust impacts climate and human life. Analyzing the interdecadal change in dust activity and its influence factors is crucial for disaster mitigation. Based on a linear regression method, this study revealed the interdecadal variability of relationships between ENSO and dust over northwestern South Asia from 1982 to 2014 and analyzed the effects of atmospheric factors on this interdecadal variability. The result sheds new light on numerical simulation involving the interdecadal variation of dust.
Rani Jeong, Joseph Lilek, Andreas Zuend, Rongshuang Xu, Man Nin Chan, Dohyun Kim, Hi Gyu Moon, and Mijung Song
Atmos. Chem. Phys., 22, 8805–8817,Short summary
In this study, the viscosities of particles of sucrose–H2O, AS–H2O, and sucrose–AS–H2O for OIRs of 4:1, 1:1, and 1:4 for decreasing RH, were quantified by poke-and-flow and bead-mobility techniques at 293 ± 1 K. Based on the viscosity results, the particles of binary and ternary systems ranged from liquid to semisolid, and even the solid state depending on the RH. Moreover, we compared the measured viscosities of ternary systems to the predicted viscosities with excellent agreement.
Minxia Shen, Kin Fai Ho, Wenting Dai, Suixin Liu, Ting Zhang, Qiyuan Wang, Jingjing Meng, Judith C. Chow, John G. Watson, Junji Cao, and Jianjun Li
Atmos. Chem. Phys., 22, 7489–7504,Short summary
Looking at characteristics and δ13C compositions of dicarboxylic acids and related compounds in BB aerosols, we used a combined combustion and aging system to generate fresh and aged aerosols from burning straw. The results showed the emission factors (EFaged) of total diacids of aging experiments were around an order of magnitude higher than EFfresh. This meant that dicarboxylic acids are involved with secondary photochemical processes in the atmosphere rather than primary emissions from BB.
Jonas K. F. Jakobsson, Deepak B. Waman, Vaughan T. J. Phillips, and Thomas Bjerring Kristensen
Atmos. Chem. Phys., 22, 6717–6748,Short summary
Long-lived cold-layer clouds at subzero temperatures are observed to be remarkably persistent in their generation of ice particles and snow precipitation. There is uncertainty about why this is so. This motivates the present lab study to observe the long-term ice-nucleating ability of aerosol samples from the real troposphere. Time dependence of their ice nucleation is observed to be weak in lab experiments exposing the samples to isothermal conditions for up to about 10 h.
Kunfeng Gao, Chong-Wen Zhou, Eszter J. Barthazy Meier, and Zamin A. Kanji
Atmos. Chem. Phys., 22, 5331–5364,Short summary
Incomplete combustion of fossil fuel produces carbonaceous particles called soot. These particles can affect cloud formation by acting as centres for droplet or ice formation. The atmospheric residence time of soot particles is of the order of days to weeks, which can result in them becoming coated by various trace species in the atmosphere such as acids. In this study, we quantify the cirrus cloud-forming ability of soot particles coated with the atmospherically ubiquitous sulfuric acid.
Kunfeng Gao, Franz Friebel, Chong-Wen Zhou, and Zamin A. Kanji
Atmos. Chem. Phys., 22, 4985–5016,Short summary
Soot particles impact cloud formation and radiative properties in the upper atmosphere where aircraft emit carbonaceous particles. We use cloud chambers to mimic the upper atmosphere temperature and humidity to test the influence of the morphology of the soot particles on ice cloud formation. For particles larger than 200 nm, the compacted (densified) samples have a higher affinity for ice crystal formation in the cirrus regime than the fluffy (un-compacted) soot particles of the same sample.
Joel Kuula, Hilkka Timonen, Jarkko V. Niemi, Hanna E. Manninen, Topi Rönkkö, Tareq Hussein, Pak Lun Fung, Sasu Tarkoma, Mikko Laakso, Erkka Saukko, Aino Ovaska, Markku Kulmala, Ari Karppinen, Lasse Johansson, and Tuukka Petäjä
Atmos. Chem. Phys., 22, 4801–4808,Short summary
Modern and up-to-date policies and air quality management strategies are instrumental in tackling global air pollution. As the European Union is preparing to revise Ambient Air Quality Directive 2008/50/EC, this paper initiates discussion on selected features of the directive that we believe would benefit from a reassessment. The scientific community has the most recent and deepest understanding of air pollution; thus, its contribution is essential.
Yu Wang, Aristeidis Voliotis, Dawei Hu, Yunqi Shao, Mao Du, Ying Chen, Judith Kleinheins, Claudia Marcolli, M. Rami Alfarra, and Gordon McFiggans
Atmos. Chem. Phys., 22, 4149–4166,Short summary
Aerosol water uptake plays a key role in atmospheric physicochemical processes. We designed chamber experiments on aerosol water uptake of secondary organic aerosol (SOA) from mixed biogenic and anthropogenic precursors with inorganic seed. Our results highlight this chemical composition influences the reconciliation of the sub- and super-saturated water uptake, providing laboratory evidence for understanding the chemical controls of water uptake of the multi-component aerosol.
Shuang Han, Juan Hong, Qingwei Luo, Hanbing Xu, Haobo Tan, Qiaoqiao Wang, Jiangchuan Tao, Yaqing Zhou, Long Peng, Yao He, Jingnan Shi, Nan Ma, Yafang Cheng, and Hang Su
Atmos. Chem. Phys., 22, 3985–4004,Short summary
We present the hygroscopicity of 23 organic species with different physicochemical properties using a hygroscopicity tandem differential mobility analyzer (HTDMA) and compare the results with previous studies. Based on the hygroscopicity parameter κ, the influence of different physicochemical properties that potentially drive hygroscopicity, such as the functionality, water solubility, molar volume, and O : C ratio of organics, are examined separately.
Kimmo Korhonen, Thomas Bjerring Kristensen, John Falk, Vilhelm B. Malmborg, Axel Eriksson, Louise Gren, Maja Novakovic, Sam Shamun, Panu Karjalainen, Lassi Markkula, Joakim Pagels, Birgitta Svenningsson, Martin Tunér, Mika Komppula, Ari Laaksonen, and Annele Virtanen
Atmos. Chem. Phys., 22, 1615–1631,Short summary
We investigated the ice-nucleating abilities of particulate emissions from a modern diesel engine using the portable ice-nuclei counter SPIN, a continuous-flow diffusion chamber instrument. Three different fuels were studied without blending, including fossil diesel and two renewable fuels, testing different emission aftertreatment systems and photochemical aging. We found that the diesel emissions were inefficient ice nuclei, and aging had no or little effect on their ice-nucleating abilities.
Noora Hyttinen, Iida Pullinen, Aki Nissinen, Siegfried Schobesberger, Annele Virtanen, and Taina Yli-Juuti
Atmos. Chem. Phys., 22, 1195–1208,Short summary
Accurate saturation vapor pressure estimates of atmospherically relevant organic compounds are critical for modeling secondary organic aerosol (SOA) formation. We investigated vapor pressures of highly oxygenated SOA constituents using state-of-the-art computational and experimental methods. We found a good agreement between low and extremely low vapor pressures estimated using the two methods, and the smallest molecules detected in our experiment were likely products of thermal decomposition.
Dawei Hu, M. Rami Alfarra, Kate Szpek, Justin M. Langridge, Michael I. Cotterell, Claire Belcher, Ian Rule, Zixia Liu, Chenjie Yu, Yunqi Shao, Aristeidis Voliotis, Mao Du, Brett Smith, Greg Smallwood, Prem Lobo, Dantong Liu, Jim M. Haywood, Hugh Coe, and James D. Allan
Atmos. Chem. Phys., 21, 16161–16182,Short summary
Here, we developed new techniques for investigating these properties in the laboratory and applied these to BC and BrC from different sources, including diesel exhaust, inverted propane flame and wood combustion. These have allowed us to quantify the changes in shape and chemical composition of different soots according to source and variables such as the moisture content of wood.
Mariam Fawaz, Anita Avery, Timothy B. Onasch, Leah R. Williams, and Tami C. Bond
Atmos. Chem. Phys., 21, 15605–15618,Short summary
Biomass burning is responsible for 90 % of the emissions of primary organic aerosols to the atmosphere. Emissions from biomass burning sources are considered chaotic. In this work, we developed a controlled experimental approach to understand the controlling factors in emission. Our results showed that emissions are repeatable and deterministic and that emissions from wood can be constrained.
Soleil E. Worthy, Anand Kumar, Yu Xi, Jingwei Yun, Jessie Chen, Cuishan Xu, Victoria E. Irish, Pierre Amato, and Allan K. Bertram
Atmos. Chem. Phys., 21, 14631–14648,Short summary
We studied the effect of (NH4)2SO4 on the immersion freezing of non-mineral dust ice-nucleating substances (INSs) and mineral dusts. (NH4)2SO4 had no effect on the median freezing temperature of 9 of the 10 tested non-mineral dust INSs, slightly decreased that of the other, and increased that of all the mineral dusts. The difference in the response of mineral dust and non-mineral dust INSs to (NH4)2SO4 suggests that they nucleate ice and/or interact with (NH4)2SO4 via different mechanisms.
Robert Wagner, Luisa Ickes, Allan K. Bertram, Nora Els, Elena Gorokhova, Ottmar Möhler, Benjamin J. Murray, Nsikanabasi Silas Umo, and Matthew E. Salter
Atmos. Chem. Phys., 21, 13903–13930,Short summary
Sea spray aerosol particles are a mixture of inorganic salts and organic matter from phytoplankton organisms. At low temperatures in the upper troposphere, both inorganic and organic constituents can induce the formation of ice crystals and thereby impact cloud properties and climate. In this study, we performed experiments in a cloud simulation chamber with particles produced from Arctic seawater samples to quantify the relative contribution of inorganic and organic species in ice formation.
Matthew Ozon, Dominik Stolzenburg, Lubna Dada, Aku Seppänen, and Kari E. J. Lehtinen
Atmos. Chem. Phys., 21, 12595–12611,Short summary
Measuring the rate at which aerosol particles are formed is of importance for understanding climate change. We present an analysis method based on Kalman smoothing, which retrieves new particle formation and growth rates from size-distribution measurements. We apply it to atmospheric simulation chamber experiments and show that it agrees well with traditional methods. In addition, it provides reliable uncertainty estimates, and we suggest instrument design optimisation for signal processing.
Yu Wang, Aristeidis Voliotis, Yunqi Shao, Taomou Zong, Xiangxinyue Meng, Mao Du, Dawei Hu, Ying Chen, Zhijun Wu, M. Rami Alfarra, and Gordon McFiggans
Atmos. Chem. Phys., 21, 11303–11316,Short summary
Aerosol phase behaviour plays a profound role in atmospheric physicochemical processes. We designed dedicated chamber experiments to study the phase state of secondary organic aerosol from biogenic and anthropogenic mixed precursors. Our results highlight the key role of the organic–inorganic ratio and relative humidity in phase state, but the sources and organic composition are less important. The result provides solid laboratory evidence for understanding aerosol phase in a complex atmosphere.
Ana A. Piedehierro, André Welti, Angela Buchholz, Kimmo Korhonen, Iida Pullinen, Ilkka Summanen, Annele Virtanen, and Ari Laaksonen
Atmos. Chem. Phys., 21, 11069–11078,Short summary
Ice crystals in cirrus clouds contain particles that start ice formation. We study whether particles forming above boreal forests can help in the making of cirrus clouds and if the water content in the particles affects this property. In the laboratory, we made boreal-forest-like particles and cooled and humidified them to measure whether an ice crystal develops. We found that only when dry can these particles form an ice crystal but no better than solution droplets.
Young-Chul Song, Joseph Lilek, Jae Bong Lee, Man Nin Chan, Zhijun Wu, Andreas Zuend, and Mijung Song
Atmos. Chem. Phys., 21, 10215–10228,Short summary
We report viscosity of binary mixtures of organic material / H2O and inorganic salts / H2O, as well as ternary mixtures of organic material / inorganic salts/ H2O, over the atmospheric relative humidity (RH) range. The viscosity measurements indicate that the studied mixed organic–inorganic particles range in phase state from liquid to semi-solid or even solid across the atmospheric RH range at a temperature of 293 K.
Shuaishuai Ma, Zhe Chen, Shufeng Pang, and Yunhong Zhang
Atmos. Chem. Phys., 21, 9705–9717,Short summary
LLPS, efflorescence and deliquescence of aerosol particles can be observed visually and determined quantitatively. Different LLPS mechanisms may dominate successively in mixed organic–inorganic particles. The formation of more concentrated inorganic inclusions may cause secondary LLPS. Furthermore, high inorganic factions may result in an inorganic salt crust enclosing the separated organic phases.
Zhaobin Sun, Xiujuan Zhao, Ziming Li, Guiqian Tang, and Shiguang Miao
Atmos. Chem. Phys., 21, 8863–8882,Short summary
Different weather types will shape significantly different structures of the pollution boundary layer. The findings of this study allow us to understand the inherent difference among heavy pollution boundary layers; in addition, they reveal the formation mechanism of haze pollution from an integrated synoptic-scale and boundary layer structure perspective.
Thomas Bjerring Kristensen, John Falk, Robert Lindgren, Christina Andersen, Vilhelm B. Malmborg, Axel C. Eriksson, Kimmo Korhonen, Ricardo Luis Carvalho, Christoffer Boman, Joakim Pagels, and Birgitta Svenningsson
Atmos. Chem. Phys., 21, 8023–8044,Short summary
Residential biomass combustion is a major anthropogenic source of aerosol particles on regional and global scales. Nevertheless, little is known about those aerosol particles' ability to act as cloud condensation nuclei (CCN) and thus influence cloud properties and climate. Our study shows a strong link between the potassium content in the fuel and emissions of CCN for different stove technologies. Previous studies may have underestimated the anthropogenic climate impact of these emissions.
Meri Räty, Otso Peräkylä, Matthieu Riva, Lauriane Quéléver, Olga Garmash, Matti Rissanen, and Mikael Ehn
Atmos. Chem. Phys., 21, 7357–7372,Short summary
Cyclohexene resembles certain relatively complex compounds in the atmosphere that through oxidation produce vapours that take part in aerosol formation. We studied the highly oxygenated organic molecules (HOMs) formed in cyclohexene ozonolysis, the relationship between their chemical composition and their tendency to condense onto seed aerosol, as well as the effect of NOx pollutants on their signals. Two existing models were also tested for their ability to predict the volatility of the HOMs.
Chao Peng, Patricia N. Razafindrambinina, Kotiba A. Malek, Lanxiadi Chen, Weigang Wang, Ru-Jin Huang, Yuqing Zhang, Xiang Ding, Maofa Ge, Xinming Wang, Akua A. Asa-Awuku, and Mingjin Tang
Atmos. Chem. Phys., 21, 7135–7148,Short summary
Organosulfates are important constituents in tropospheric aerosol particles, but their hygroscopic properties and cloud condensation nuclei activities are not well understood. In our work, three complementary techniques were employed to investigate the interactions of 11 organosulfates with water vapor under sub- and supersaturated conditions.
Alexis Dépée, Pascal Lemaitre, Thomas Gelain, Marie Monier, and Andrea Flossmann
Atmos. Chem. Phys., 21, 6945–6962,Short summary
Present article describe a new In-Cloud Aerosol Scavenging Experiment (In-CASE) that has been conceived to measure the collection efficiency of submicron aerosol particles by cloud droplets. The present article focuses on the influence of phoretic effects on the collection efficiency.
Jingchuan Chen, Zhijun Wu, Jie Chen, Naama Reicher, Xin Fang, Yinon Rudich, and Min Hu
Atmos. Chem. Phys., 21, 3491–3506,Short summary
Asian mineral dust is a crucial contributor to global ice-nucleating particles (INPs), while its size-resolved information on freezing activity is extremely rare. Here we conducted the first known INP measurements of size-resolved airborne East Asian dust particles. An explicit size dependence of both INP concentration and surface ice-active-site density was observed. The new parameterizations can be widely applied in models to better characterize and predict ice nucleation activities of dust.
Georgia Michailoudi, Jack J. Lin, Hayato Yuzawa, Masanari Nagasaka, Marko Huttula, Nobuhiro Kosugi, Theo Kurtén, Minna Patanen, and Nønne L. Prisle
Atmos. Chem. Phys., 21, 2881–2894,Short summary
This study provides insight into hydration of two significant atmospheric compounds, glyoxal and methylglyoxal. Using synchrotron radiation excited X-ray absorption spectroscopy, we confirm that glyoxal is fully hydrated in water, and for the first time, we experimentally detect enol structures in aqueous methylglyoxal. Our results support the contribution of these compounds to secondary organic aerosol formation, known to have a large uncertainty in atmospheric models and climate predictions.
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Baumgardner, D., Raga, G. B., and Muhlia, A.: Evidence for the formation of CCN by photochemical processes in Mexico City, Atmos. Environ., 38, 357–367, https://doi.org/10.1016/j.atmosenv.2003.10.008, 2004.
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Gabey, A. M., Gallagher, M. W., Whitehead, J., Dorsey, J. R., Kaye, P. H., and Stanley, W. R.: Measurements and comparison of primary biological aerosol above and below a tropical forest canopy using a dual channel fluorescence spectrometer, Atmos. Chem. Phys., 10, 4453–4466, https://doi.org/10.5194/acp-10-4453-2010, 2010.
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Gioda, A., Mayol-Bracero, O. L., Scatena, F. N., Weathers, K. C., Mateus, V. L., and McDowell, W. H.: Chemical constituents in clouds and rainwater in the Puerto Rican rainforest: Potential sources and seasonal drivers, Atmos. Environ., 68, 208–220, https://doi.org/10.1016/j.atmosenv.2012.11.017, 2013.
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Healy, D. A., Huffman, J. A., O'Connor, D. J., Pöhlker, C., Pöschl, U., and Sodeau, J. R.: Ambient measurements of biological aerosol particles near Killarney, Ireland: a comparison between real-time fluorescence and microscopy techniques, Atmos. Chem. Phys., 14, 8055–8069, https://doi.org/10.5194/acp-14-8055-2014, 2014.
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Here, the fluorescent characteristics and cloud-forming efficiency of aerosols at an urban site in Puerto Rico are discussed. The results from this pilot study highlight the capabilities of ultraviolet-induced fluorescence (UV-IF) measurements for characterizing the properties of fluorescing aerosol particles, as they relate to the daily evolution of primary biological aerosol particles. This work has established a database of measurements on which future, longer-term studies will be initiated.
Here, the fluorescent characteristics and cloud-forming efficiency of aerosols at an urban site...