The balance between the amounts of ice and supercooled water in clouds over the world's oceans strongly influences how much these clouds can dampen or amplify global warming. Aerosol particles which catalyse ice formation can dramatically reduce the amount of supercooled water in clouds; hence we argue that we need a concerted effort to improve our understanding of these ice-nucleating particles if we are to improve our predictions of climate change.
We address the phenomenon of ice enhancement in the vicinity of warm hydrometeors using highly accurate flow simulation techniques. It is found that the transiently supersaturated zones induced by the hydrometeor's wake are by far larger than what has been previously estimated. The ice enhancement is quantified on the micro- and macroscale, and its relevance is discussed. The results provided may contribute to a (currently unavailable) parametrization of the phenomenon.
The year 2019 was particularly rich for the stratospheric aerosol layer due to two volcanic eruptions (at Raikoke and Ulawun) and wildfire events. With satellite observations and models, we describe the exceptionally complex situation following the Raikoke eruption. The respective plume overwhelmed the Northern Hemisphere stratosphere in terms of aerosol load and resulted in the highest climate impact throughout the past decade.
Jann Schrod, Erik S. Thomson, Daniel Weber, Jens Kossmann, Christopher Pöhlker, Jorge Saturno, Florian Ditas, Paulo Artaxo, Valérie Clouard, Jean-Marie Saurel, Martin Ebert, Joachim Curtius, and Heinz G. Bingemer
Long-term ice-nucleating particle (INP) data are presented from four semi-pristine sites located in the Amazon, the Caribbean, Germany and the Arctic. Average INP concentrations did not differ by orders of magnitude between the sites. For all sites short-term variability dominated the time series, which lacked clear trends and seasonalities. Common drivers to explain the INP levels and their variations could not be identified, illustrating the complex nature of heterogeneous ice nucleation.
Solar geoengineering has been introduced to mitigate human-caused global warming by reflecting sunlight back into space. This research investigates the impact of solar geoengineering on the tropical Pacific climate. We find that solar geoengineering can compensate some of the greenhouse-induced changes in the tropical Pacific but not all. In particular, solar geoengineering will result in significant changes in rainfall, sea surface temperatures, and increased frequency of extreme ENSO events.
Measurements of the multi-wavelength Raman polarization lidar PollyXT have been combined with measurements of pollen type and concentration using a traditional pollen sampler at a rural forest site in Kuopio, Finland. The depolarization ratio was enhanced when there were pollen grains in the atmosphere, illustrating the potential of lidar to track pollen grains in the atmosphere. The depolarization ratio of pure pollen particles was assessed for birch and pine pollen using a novel algorithm.
A novel lidar method to study cloud microphysical properties (of liquid water clouds) and to study aerosol–cloud interaction (ACI) is developed and presented in this paper. In Part 1, the theoretical framework including an error analysis is given together with an overview of the aerosol information that the same lidar system can obtain. The ACI concept based on aerosol and cloud information is also explained. Applications of the proposed approach to lidar measurements are presented in Part 2.
Ozone depletion over Antarctica was shown to influence the tropospheric jet in the Southern Hemisphere. We investigate the atmospheric response to ozone depletion comparing climate model ensembles with interactive and prescribed ozone fields. We show that allowing feedbacks between ozone chemistry and model physics as well as including asymmetries in ozone leads to a strengthened ozone depletion signature in the stratosphere but does not significantly affect the tropospheric jet position.
A long historical emission inventory of major air pollutants in Asia during 1950–2015 was developed as Regional Emission inventory in ASia version 3 (REASv3). Trends of emissions and changes in source contributions in countries and regions in Asia during these 6 decades were analyzed. REASv3 provides monthly gridded data with 0.25° by 0.25° resolution for major source categories as well as table of emissions by countries and sub-regions for major sectors and fuel types.
Huihui Wu, Jonathan W. Taylor, Kate Szpek, Justin M. Langridge, Paul I. Williams, Michael Flynn, James D. Allan, Steven J. Abel, Joseph Pitt, Michael I. Cotterell, Cathryn Fox, Nicholas W. Davies, Jim Haywood, and Hugh Coe
Airborne measurements of highly aged biomass burning aerosols (BBAs) over the remote southeast Atlantic provide unique aerosol parameters for climate models. Our observations demonstrate the persistence of strongly absorbing BBAs across wide regions of the South Atlantic. We also found significant vertical variation in the single-scattering albedo of these BBAs, as a function of relative chemical composition and size. Aerosol properties in the marine BL are suggested to be separated from the FT.
Martina Krämer, Christian Rolf, Nicole Spelten, Armin Afchine, David Fahey, Eric Jensen, Sergey Khaykin, Thomas Kuhn, Paul Lawson, Alexey Lykov, Laura L. Pan, Martin Riese, Andrew Rollins, Fred Stroh, Troy Thornberry, Veronika Wolf, Sarah Woods, Peter Spichtinger, Johannes Quaas, and Odran Sourdeval
To improve the representations of cirrus clouds in climate predictions, extended knowledge of their properties and geographical distribution is required. This study presents extensive airborne in situ and satellite remote sensing climatologies of cirrus and humidity, which serve as a guide to cirrus clouds. Further, exemplary radiative characteristics of cirrus types and also in situ observations of tropical tropopause layer cirrus and humidity in the Asian monsoon anticyclone are shown.
Atmospheric particles are important in relation to human health and the global climate. As the global temperature changes, so may the atmospheric chemistry controlling the formation of particles from reactions of naturally emitted volatile organic compounds (VOCs). In the current work, we show how temperatures influence the formation and chemical composition of atmospheric particles from α-pinene: a biogenic VOC largely emitted in high-latitude environments such as the boreal forests.
Condensational growth of Aitken-mode particles is a major source of cloud condensation nuclei in the remote marine boundary layer. It has been long thought that over remote oceans, condensation growth is dominated by sulfate that derives from ocean-emitted dimethyl sulfide. In this study, we present the first long-term observational evidence that, contrary to conventional thinking, organics play an even more important role than sulfate in particle growth over remote oceans throughout the year.
Cloud water pH affects atmospheric chemistry, and acid rain damages ecosystems. We use model simulations along with observations to present a global view of cloud water and precipitation pH. Sulfuric acid, nitric acid, and ammonia control the pH in the northern midlatitudes, but carboxylic acids and dust cations are important in the tropics and subtropics. The acid inputs to many nitrogen-saturated ecosystems are high enough to cause acidification, with ammonium as the main acidifying species.
We investigate the effects of future land use and land cover change (LULCC) on surface ozone air quality worldwide and find that LULCC can significantly influence ozone in North America and Europe via modifying surface energy balance, boundary-layer meteorology, and regional circulation. The strength of such “biogeophysical effects” of LULCC is strongly dependent on forest type and generally greater than the “biogeochemical effects” via changing deposition and emission fluxes alone.
Jonathan W. Taylor, Huihui Wu, Kate Szpek, Keith Bower, Ian Crawford, Michael J. Flynn, Paul I. Williams, James Dorsey, Justin M. Langridge, Michael I. Cotterell, Cathryn Fox, Nicholas W. Davies, Jim M. Haywood, and Hugh Coe
Every year, huge plumes of smoke hundreds of miles wide travel over the south Atlantic Ocean from fires in central and southern Africa. These plumes absorb the sun’s energy and warm the climate. We used airborne optical instrumentation to determine how absorbing the smoke was as well as the relative importance of black and brown carbon. We also tested different ways of simulating these properties that could be used in a climate model.
W. Richard Leaitch, John K. Kodros, Megan D. Willis, Sarah Hanna, Hannes Schulz, Elisabeth Andrews, Heiko Bozem, Julia Burkart, Peter Hoor, Felicia Kolonjari, John A. Ogren, Sangeeta Sharma, Meng Si, Knut von Salzen, Allan K. Bertram, Andreas Herber, Jonathan P. D. Abbatt, and Jeffrey R. Pierce
Black carbon is a factor in the warming of the Arctic atmosphere due to its ability to absorb light, but the uncertainty is high and few observations have been made in the high Arctic above 80° N. We combine airborne and ground-based observations in the springtime Arctic, at and above 80° N, with simulations from a global model to show that light absorption by black carbon may be much larger than modelled. However, the uncertainty remains high.
We compared the volatility distributions of secondary organic aerosol (SOA) constituents estimated from isothermal evaporation experiments from either particle size change data, by process modelling and global optimization, or from mass spectrometer data with positive matrix factorization analysis. Our results show that, despite the two very different estimation methods, the volatility distributions are comparable if uncertainties are taken into account.
Rapid urbanization has increased the consumption of fossil fuel, contributing the degradation of urban air quality. Burning efficiency is a major factor determining the impact of fuel burning on the environment. We quantify the burning efficiency of fossil fuel use over six megacities using satellite remote sensing data. City governance can use these results to understand air pollution scenarios and to formulate effective air pollution control strategies.
The amount of energy reflected back into space because of man-made particles is highly uncertain. Processes related to naturally occurring particles cause most of the uncertainty, but these processes are poorly constrained by present-day measurements. We show that measurements over the Southern Ocean, far from pollution sources, efficiently reduce climate model uncertainties. Our results pave the way to designing experiments and measurement campaigns that reduce this uncertainty even further.
Water vapour has a complex spectrum and absorbs from the microwave to the near-UV where it dissociates. There is limited knowledge of the absorption features in the near-UV, and there is a large disagreement for the available models and experiments. We created a new ab initio model that is in good agreement with observation at 363 nm. At lower wavelengths, our calculations suggest that the latest experiments overestimate absorption. This has implications for trace gas retrievals in the near-UV.
Cirrus clouds appearing in the upper troposphere and lower stratosphere have important impacts on the radiation budget and climate change. We revisited global stratospheric cirrus clouds with CALIPSO and for the first time with MIPAS satellite observations. Stratospheric cirrus clouds related to deep convection are frequently detected in the tropics. At middle latitudes, MIPAS detects more than twice as many stratospheric cirrus clouds due to higher detection sensitivity.
Recent lower stratospheric ozone decreases remain unexplained. We show that chemistry–climate models are not generally able to reproduce mid-latitude ozone and water vapour changes. Our analysis of observations provides evidence that climate change may be responsible for the ozone trends. While model projections suggest that extratropical ozone should recover by 2100, our study raises questions about their efficacy in simulating lower stratospheric changes in this region.
Christopher J. Smith, Ryan J. Kramer, Gunnar Myhre, Kari Alterskjær, William Collins, Adriana Sima, Olivier Boucher, Jean-Louis Dufresne, Pierre Nabat, Martine Michou, Seiji Yukimoto, Jason Cole, David Paynter, Hideo Shiogama, Fiona M. O'Connor, Eddy Robertson, Andy Wiltshire, Timothy Andrews, Cécile Hannay, Ron Miller, Larissa Nazarenko, Alf Kirkevåg, Dirk Olivié, Stephanie Fiedler, Anna Lewinschal, Chloe Mackallah, Martin Dix, Robert Pincus, and Piers M. Forster
The spread in effective radiative forcing for both CO2 and aerosols is narrower in the latest CMIP6 (Coupled Model Intercomparison Project) generation than in CMIP5. For the case of CO2 it is likely that model radiation parameterisations have improved. Tropospheric and stratospheric radiative adjustments to the forcing behave differently for different forcing agents, and there is still significant diversity in how clouds respond to forcings, particularly for total anthropogenic forcing.
Mario Simon, Lubna Dada, Martin Heinritzi, Wiebke Scholz, Dominik Stolzenburg, Lukas Fischer, Andrea C. Wagner, Andreas Kürten, Birte Rörup, Xu-Cheng He, João Almeida, Rima Baalbaki, Andrea Baccarini, Paulus S. Bauer, Lisa Beck, Anton Bergen, Federico Bianchi, Steffen Bräkling, Sophia Brilke, Lucia Caudillo, Dexian Chen, Biwu Chu, António Dias, Danielle C. Draper, Jonathan Duplissy, Imad El-Haddad, Henning Finkenzeller, Carla Frege, Loic Gonzalez-Carracedo, Hamish Gordon, Manuel Granzin, Jani Hakala, Victoria Hofbauer, Christopher R. Hoyle, Changhyuk Kim, Weimeng Kong, Houssni Lamkaddam, Chuan P. Lee, Katrianne Lehtipalo, Markus Leiminger, Huajun Mai, Hanna E. Manninen, Guillaume Marie, Ruby Marten, Bernhard Mentler, Ugo Molteni, Leonid Nichman, Wei Nie, Andrea Ojdanic, Antti Onnela, Eva Partoll, Tuukka Petäjä, Joschka Pfeifer, Maxim Philippov, Lauriane L. J. Quéléver, Ananth Ranjithkumar, Matti P. Rissanen, Simon Schallhart, Siegfried Schobesberger, Simone Schuchmann, Jiali Shen, Mikko Sipilä, Gerhard Steiner, Yuri Stozhkov, Christian Tauber, Yee J. Tham, António R. Tomé, Miguel Vazquez-Pufleau, Alexander L. Vogel, Robert Wagner, Mingyi Wang, Dongyu S. Wang, Yonghong Wang, Stefan K. Weber, Yusheng Wu, Mao Xiao, Chao Yan, Penglin Ye, Qing Ye, Marcel Zauner-Wieczorek, Xueqin Zhou, Urs Baltensperger, Josef Dommen, Richard C. Flagan, Armin Hansel, Markku Kulmala, Rainer Volkamer, Paul M. Winkler, Douglas R. Worsnop, Neil M. Donahue, Jasper Kirkby, and Joachim Curtius
Highly oxygenated organic compounds (HOMs) have been identified as key vapors involved in atmospheric new-particle formation (NPF). The molecular distribution, HOM yield, and NPF from α-pinene oxidation experiments were measured at the CLOUD chamber over a wide tropospheric-temperature range. This study shows on a molecular scale that despite the sharp reduction in HOM yield at lower temperatures, the reduced volatility counteracts this effect and leads to an overall increase in the NPF rate.
The switch from the use of coal to natural gas or oil for energy generation potentially reduces the impact on global warming due to lower CO2 emissions with the same energy content. However, this climate benefit is offset by fugitive methane emissions during the production and distribution process. We quantify emission and leakage rates relative to production for several large production regions based on satellite observations to evaluate the climate footprint of the gas and oil industry.
Martine Collaud Coen, Elisabeth Andrews, Andrés Alastuey, Todor Petkov Arsov, John Backman, Benjamin T. Brem, Nicolas Bukowiecki, Cédric Couret, Konstantinos Eleftheriadis, Harald Flentje, Markus Fiebig, Martin Gysel-Beer, Jenny L. Hand, András Hoffer, Rakesh Hooda, Christoph Hueglin, Warren Joubert, Melita Keywood, Jeong Eun Kim, Sang-Woo Kim, Casper Labuschagne, Neng-Huei Lin, Yong Lin, Cathrine Lund Myhre, Krista Luoma, Hassan Lyamani, Angela Marinoni, Olga L. Mayol-Bracero, Nikos Mihalopoulos, Marco Pandolfi, Natalia Prats, Anthony J. Prenni, Jean-Philippe Putaud, Ludwig Ries, Fabienne Reisen, Karine Sellegri, Sangeeta Sharma, Patrick Sheridan, James Patrick Sherman, Junying Sun, Gloria Titos, Elvis Torres, Thomas Tuch, Rolf Weller, Alfred Wiedensohler, Paul Zieger, and Paolo Laj
Long-term trends of aerosol radiative properties (52 stations) prove that aerosol load has significantly decreased over the last 20 years. Scattering trends are negative in Europe (EU) and North America (NA), not ss in Asia, and show a mix of positive and negative trends at polar stations. Absorption has mainly negative trends. The single scattering albedo has positive trends in Asia and eastern EU and negative in western EU and NA, leading to a global positive median trend of 0.02 % per year.
Excessive atmospheric reactive nitrogen (Nr) deposition can cause a series of negative effects. Thus, it is necessary to accurately estimate Nr deposition to evaluate its impact on the ecosystems and environment. Scientists attempted to estimate surface Nr concentration and deposition using satellite retrievals. We give a thorough review of recent advances in estimating surface Nr concentration and deposition using satellite retrievals of NO2 and NH3 and summarize the existing challenges.
Kevin Ohneiser, Albert Ansmann, Holger Baars, Patric Seifert, Boris Barja, Cristofer Jimenez, Martin Radenz, Audrey Teisseire, Athina Floutsi, Moritz Haarig, Andreas Foth, Alexandra Chudnovsky, Ronny Engelmann, Félix Zamorano, Johannes Bühl, and Ulla Wandinger
Unique lidar observations of a strong perturbation in stratospheric aerosol conditions in the Southern Hemisphere caused by the extreme Australian bushfires in 2019–2020 are presented. One of the main goals of this article is to provide the CALIPSO and Aeolus spaceborne lidar science teams with basic input parameters (lidar ratios, depolarization ratios) for a trustworthy documentation of this record-breaking event.
Francesca Gallo, Janek Uin, Stephen Springston, Jian Wang, Guangjie Zheng, Chongai Kuang, Robert Wood, Eduardo B. Azevedo, Allison McComiskey, Fan Mei, Adam Theisen, Jenni Kyrouac, and Allison C. Aiken
Continuous high-time-resolution ambient data can include periods when aerosol properties do not represent regional aerosol processes due to high-concentration local events. We develop a novel aerosol mask at the U.S. Department of Energy’s Atmospheric Radiation Measurement (ARM) facility in the eastern North Atlantic (ENA). We use two ground sites to validate the mask, include a comparison with aircraft overflights, and provide guidance to increase data quality at ENA and other locations.
Dominik Stolzenburg, Mario Simon, Ananth Ranjithkumar, Andreas Kürten, Katrianne Lehtipalo, Hamish Gordon, Sebastian Ehrhart, Henning Finkenzeller, Lukas Pichelstorfer, Tuomo Nieminen, Xu-Cheng He, Sophia Brilke, Mao Xiao, António Amorim, Rima Baalbaki, Andrea Baccarini, Lisa Beck, Steffen Bräkling, Lucía Caudillo Murillo, Dexian Chen, Biwu Chu, Lubna Dada, António Dias, Josef Dommen, Jonathan Duplissy, Imad El Haddad, Lukas Fischer, Loic Gonzalez Carracedo, Martin Heinritzi, Changhyuk Kim, Theodore K. Koenig, Weimeng Kong, Houssni Lamkaddam, Chuan Ping Lee, Markus Leiminger, Zijun Li, Vladimir Makhmutov, Hanna E. Manninen, Guillaume Marie, Ruby Marten, Tatjana Müller, Wei Nie, Eva Partoll, Tuukka Petäjä, Joschka Pfeifer, Maxim Philippov, Matti P. Rissanen, Birte Rörup, Siegfried Schobesberger, Simone Schuchmann, Jiali Shen, Mikko Sipilä, Gerhard Steiner, Yuri Stozhkov, Christian Tauber, Yee Jun Tham, António Tomé, Miguel Vazquez-Pufleau, Andrea C. Wagner, Mingyi Wang, Yonghong Wang, Stefan K. Weber, Daniela Wimmer, Peter J. Wlasits, Yusheng Wu, Qing Ye, Marcel Zauner-Wieczorek, Urs Baltensperger, Kenneth S. Carslaw, Joachim Curtius, Neil M. Donahue, Richard C. Flagan, Armin Hansel, Markku Kulmala, Jos Lelieveld, Rainer Volkamer, Jasper Kirkby, and Paul M. Winkler
Sulfuric acid is a major atmospheric vapour for aerosol formation. If new particles grow fast enough, they can act as cloud droplet seeds or affect air quality. In a controlled laboratory set-up, we demonstrate that van der Waals forces enhance growth from sulfuric acid. We disentangle the effects of ammonia, ions and particle hydration, presenting a complete picture of sulfuric acid growth from molecular clusters onwards. In a climate model, we show its influence on the global aerosol budget.
The Montreal Protocol was agreed in 1987 to limit and then stop the production of man-made CFCs, which destroy stratospheric ozone. As a result, the atmospheric abundances of CFCs are now declining in the atmosphere. However, the atmospheric abundance of CFC-11 is not declining as expected under complete compliance with the Montreal Protocol. Using the UM-UKCA chemistry–climate model, we explore the impact of future unregulated production of CFC-11 on ozone recovery.
Camille Mouchel-Vallon, Julia Lee-Taylor, Alma Hodzic, Paulo Artaxo, Bernard Aumont, Marie Camredon, David Gurarie, Jose-Luis Jimenez, Donald H. Lenschow, Scot T. Martin, Janaina Nascimento, John J. Orlando, Brett B. Palm, John E. Shilling, Manish Shrivastava, and Sasha Madronich
The GoAmazon 2014/5 field campaign took place near the city of Manaus, Brazil, isolated in the Amazon rainforest, to study the impacts of urban pollution on natural air masses. We simulated this campaign with an extremely detailed organic chemistry model to understand how the city would affect the growth and composition of natural aerosol particles. Discrepancies between the model and the measurements indicate that the chemistry of naturally emitted organic compounds is still poorly understood.
Future trends in air pollution and greenhouse gas emissions in China are of great concern to the community. Here we developed a sophisticated dynamic projection model to understand 2015–2050 emission pathways under a range of socio-economic, climate policy, and pollution control scenarios. By coupling strong low-carbon transitions and clean air policy, emissions of major air pollutants in China will be reduced by 58–87 % during 2015–2050. This work can support future co-governance policy design.
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
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.
This report describes a simple, safe and effective method to prepare nitrate esters of terpenes (carene, limonene, perillic alcohol, beta-pinene and alpha-pinene) which are key oxidation products in the atmosphere. These compounds are implicated in the formation of secondary organic aerosols. A compilation of the relevant spectroscopic data has been presented. The availability of these compounds and their characterization data will enable further study of the structure–reactivity relationships.
Given their critical impact on radiative forcing, sulfate aerosols have been extensively studied using their isotope signatures (δ34S, ∆33S, ∆36S, δ18O, and ∆17O). A striking observation is that ∆33S > 0 ‰, implying a missing reservoir in the sulfur cycle. Here, we measured ∆33S < 0 ‰ in black crust sulfates (i.e., formed on carbonate walls) that must therefore result from distinct chemical pathway(s) compared to sulfate aerosols, and they may well represent this complementary reservoir.
Thin (~ 100 m) supercooled liquid water (SLW, water staying in liquid phase below 0 °C) clouds have been detected, analysed, and modelled over the Dome C (Concordia, Antarctica) station during the austral summer 2018–2019 using observations and meteorological analyses. The SLW clouds were observed at the top of the planetary boundary layer and the SLW content was always strongly underestimated by the model indicating an incorrect simulation of the surface energy budget of the Antarctic Plateau.
Clara Orbe, David A. Plummer, Darryn W. Waugh, Huang Yang, Patrick Jöckel, Douglas E. Kinnison, Beatrice Josse, Virginie Marecal, Makoto Deushi, Nathan Luke Abraham, Alexander T. Archibald, Martyn P. Chipperfield, Sandip Dhomse, Wuhu Feng, and Slimane Bekki
Atmospheric composition is strongly influenced by global-scale winds that are not always properly simulated in computer models. A common approach to correct for this bias is to relax or nudge to the observed winds. Here we systematically evaluate how well this technique performs across a large suite of chemistry–climate models in terms of its ability to reproduce key aspects of both the tropospheric and stratospheric circulations.
We demonstrate for the first time that large festivals can be significant methane sources, though they are not included in emission inventories. We combined in situ measurements with a Gaussian plume model to determine the Oktoberfest emissions and show that they are not due solely to human biogenic emissions, but are instead primarily fossil fuel related. Our study provides the foundation to develop reduction policies for such events and new pathways to mitigate fossil fuel methane emissions.
Cloud water content and the number of droplets inside clouds covary with boundary layer depth. This covariation may amplify the change in water content due to a change in droplet number inferred from long-term observations. Taking this into account shows that the change in water content for increased droplet number in observations and high-resolution simulations agrees in shallow boundary layers. Meanwhile, deep boundary layers are under-sampled in process-scale simulations and observations.
The Nimbus 7 limb infrared monitor of the stratosphere (LIMS) instrument operated from October 25, 1978, through May 28, 1979. This note focuses on the lower stratosphere of the southern hemisphere, subpolar regions in relation to the position of the polar vortex. Both LIMS ozone and nitric acid show reductions within the edge of the polar vortex at 46 hPa near 60° S from late October through mid-November 1978, indicating that there was a chemical loss of Antarctic ozone some weeks earlier.
Methanethiol (MeSH) is a reduced sulfur gas originating from phytoplankton, with a global ocean source of ~ 17 % of dimethyl sulfide (DMS). It has been little studied and is rarely observed over the ocean. In this work, MeSH was measured at much higher levels than previously observed (3–36 % of parallel DMS mixing ratios). MeSH could be a significant source of atmospheric sulfur over productive regions of the ocean, but its distribution, and its atmospheric impact, requires more investigation.
Using observations from instruments deployed to a small island in the southeast Atlantic, we study days when the atmospheric concentrations of particles near the surface are exceptionally low. Interestingly, these ultra-clean boundary layers occur in the same months as the smokiest boundary layers associated with biomass burning in Africa. We find evidence that enhancements in drizzle scavenging, on top of a seasonal maximum in cloudiness and precipitation, likely drive these conditions.
This study attempts identification of mechanisms of secondary ice production (SIP) based on the observation of small faceted ice crystals. It was found that in both mesoscale convective systems and frontal clouds, SIP was observed right above the melting layer and extended to the higher altitudes with colder temperatures. A principal conclusion of this work is that the freezing drop shattering mechanism is plausibly accounting for the measured ice concentrations in the observed condition.
The amount of the micronutrient selenium in food largely depends on the amount and form of selenium in soil. The atmosphere acts as a source of selenium to soils through deposition, yet little information is available about atmospheric selenium cycling. Therefore, we built the first global atmospheric selenium model. Through sensitivity and uncertainty analysis we determine that selenium can be transported thousands of kilometers and that measurements of selenium emissions should be prioritized.
Concurrent measurements of the altitude profiles of the concentration of cloud condensation nuclei (CCNs), as a function of supersaturation (ranging from 0.2 % to 1.0 %), and aerosol optical properties were carried out aboard an instrumented aircraft across the Indo-Gangetic Plain (IGP) just prior to the onset of the 2016 Indian summer monsoon (ISM). A high CCN concentration is observed up to 2.5 km across the IGP, indicating the significant possibility of aerosol indirect effects.
Albert Ansmann, Rodanthi-Elisavet Mamouri, Johannes Bühl, Patric Seifert, Ronny Engelmann, Julian Hofer, Argyro Nisantzi, James D. Atkinson, Zamin A. Kanji, Berko Sierau, Mihalis Vrekoussis, and Jean Sciare
For the first time, a closure study of the relationship between the ice-nucleating particle concentration (INPC) and ice crystal number concentration (ICNC) in altocumulus and cirrus layers, solely based on ground-based active remote sensing, is presented. The closure studies were conducted in Cyprus. A focus was on altocumulus and cirrus layers which developed in pronounced Saharan dust layers. The closure studies show that heterogeneous ice nucleation can play a dominant role in ice formation.
Using data from the GOSAT satellite between 2010 and 2016 and a Bayesian inversion approach, we estimate monthly emissions of methane from tropical Africa. We find an increase in methane emissions during this period, driven in part by rising emissions from South Sudan. Using ancillary data we attribute this short-term emissions rise to an increase in the extent of the Sudd wetlands driven by increased outflow from the East African lakes.
In this study we explore 17 years of aerosol number size distribution data (10–390 nm) observed at Aspvreten (58.8° N, 17.4° E, 25 m a.s.l.). The station, located in northern Europe, is representative of rural background conditions. The study focused on identifying trends in aerosol number size distribution properties. The study shows that total number has decreased by 30 % and aerosol submicron mass by 50 % on average. Observed trends vary strongly with both season and particle size.
Boundary layer (BL) semi-direct effects in the remote SE Atlantic are investigated using LASIC field measurements and satellite retrievals. Low-cloud cover and cloud liquid water path decrease with increasing smoke loadings in the BL. Daily-mean surface-based mixed layer is warmer by 0.5 K, moisture accumulates near the surface throughout the night, and the BL deepens by 200 m, with LWPs and cloud top heights increasing, in the sunlit morning hours, as part of the smoke-altered BL diurnal cycle.
This study, benefiting especially from recently developed mass spectrometry observations of aerosols, highlights unknown properties of volcanic sulfates in the troposphere. It shows their specific chemical fingerprint, distinct from those of freshly emitted industrial sulfates and background aerosols. We also demonstrate the large-scale persistence of the volcanic sulfate pollution over weeks. Hence, these results cast light on the impact of tropospheric eruptions on air quality and climate.
This study addresses the relative impact of orography, soil moisture, and aerosols on precipitation over Germany in different weather regimes. We find that the impact of these perturbations is higher for weak than for strong large-scale forcing. Furthermore, aerosols and soil moisture are both of similar importance for precipitation forecasting, which indicates that their inclusion in operational ensemble forecasting should be assessed in the future.
The formation mechanism of a severe haze episode that occurred over North China in December 2015, the aerosol radiative impacts on the haze event and the influence mechanism were examined. The PM2.5 increase during the aerosol accumulation stage was mainly attributed to strong production by the aerosol chemistry process and weak removal by advection and vertical mixing. Restrained vertical mixing was the main reason for near-surface PM2.5 increase when aerosol radiative feedback was considered.
The quantification of anthropogenic emissions with current CO2 satellite sensors is difficult, but NO2 is co-emitted, making it a suitable tracer of recently emitted CO2. We analyze enhancements of CO2 and NO2 observed by OCO-2 and S5P and estimate the CO2 plume cross-sectional fluxes that we compare with emission databases. Our results demonstrate the usefulness of simultaneous satellite observations of CO2 and NO2 as envisaged for the European Copernicus anthropogenic CO2 monitoring mission
We investigate the transport pathways of water vapour from the upper troposphere in the Asian monsoon region to the stratosphere. In the employed chemistry-transport model we use a tagging method, such that the impact of different source regions on the stratospheric water vapour budget can be quantified. A key finding is that the Asian monsoon (compared to other source regions) is very efficient in transporting air masses and water vapour to the tropical and extratropical stratosphere.
Predictions of global warming require predictions of how much CO2 will be taken up by the oceans, how much by land plants, and how much will stay in the atmosphere. Measurements of atmospheric oxygen (O2) help with these predictions if we also know the ratio of O2 release to CO2 uptake in land plants. We have measured this ratio in a midlatitude forest and find a lower value than the one in wide use. If truly applicable, our results call for a modest adjustment in the global carbon budget.
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
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).
Biomass burning is one of the largest sources of atmospheric pollutants worldwide. This paper presents an up-to-date compilation of emission factors for over 120 trace gas and aerosol species from the different forms of open vegetation fires and domestic biofuel use, based on an analysis of over 370 published studies. Using these emission factors and current global burning activity data, the annual emissions of important species released by the various types of biomass burning are estimated.
Aerosol acidity plays a key role in secondary aerosol formation. To provide a more comprehensive reference for aerosol pH and a basis for controlling secondary aerosol generation, this study used the latest data covering four seasons and different particle sizes to obtain the characteristics of aerosol pH and explore the main factors affecting aerosol pH and gas–particle partitioning in the Beijing area.
Joannes D. Maasakkers, Daniel J. Jacob, Melissa P. Sulprizio, Tia R. Scarpelli, Hannah Nesser, Jian-Xiong Sheng, Yuzhong Zhang, Monica Hersher, A. Anthony Bloom, Kevin W. Bowman, John R. Worden, Greet Janssens-Maenhout, and Robert J. Parker
We use 2010–2015 satellite observations of atmospheric methane to improve estimates of methane emissions and their trends, as well as the concentration and trend of tropospheric OH (hydroxyl radical, methane's main sink). We find overestimates of Chinese coal and Middle East oil/gas emissions in the prior estimate. The 2010–2015 growth in methane is attributed to an increase in emissions from India, China, and areas with large tropical wetlands. The contribution from OH is small in comparison.
We measured hydroxyl radical (•OH), singlet oxygen (1O2*), and organic triplets (3C*) in illuminated aqueous particle extracts. After measuring the impact of dilution on oxidant concentrations, we extrapolated our results to predict them in ambient particles – 1O2* and 3C* concentrations appear to be greatly enhanced, while •OH appears largely unchanged. Two of these oxidants (1O2*, 3C*) are not yet included in atmospheric models, and our results make it possible to include them in the future.
This study provides compelling new evidence that the surface winter warming observed over the Northern Hemisphere continents following the 1991 eruption of Mt. Pinatubo was, very likely, completely unrelated to the eruption. This result has implications for earlier eruptions, as the evidence presented here demonstrates that the surface signal of even the very largest known eruptions may be swamped by the internal variability at high latitudes.
Aerosols are released by natural and human activities. When aerosols encounter clouds they interact in what is known as the indirect effect. Brighter clouds are expected due to the microphysical response; however, certain environments can trigger a modified response. Limits on the stability, humidity, and cloud thickness are applied regionally to investigate local cloud responses to aerosol, resulting in a range of indirect effects that would result in significant cooling or slight warming.
Sulfate is a key species contributing to particle formation and growth during wintertime Chinese haze events. This study combines observations and modeling of oxygen isotope signatures in sulfate aerosol to investigate its formation mechanisms, with a focus on heterogeneous production on aerosol surface via H2O2, O3, and NO2 and trace metal catalyzed oxidation. Contributions from different formation pathways are presented.
James Brooks, James D. Allan, Paul I. Williams, Dantong Liu, Cathryn Fox, Jim Haywood, Justin M. Langridge, Ellie J. Highwood, Sobhan K. Kompalli, Debbie O'Sullivan, Suresh S. Babu, Sreedharan K. Satheesh, Andrew G. Turner, and Hugh Coe
Our study, for the first time, presents measurements of aerosol chemical composition and physical characteristics across northern India in the pre-monsoon and monsoon seasons of 2016 using the FAAM BAe-146 UK research aircraft. Across northern India, an elevated aerosol layer dominated by sulfate aerosol exists that diminishes with monsoon arrival. The Indo-Gangetic Plain (IGP) boundary layer is dominated by organics, whereas outside the IGP sulfate dominates with increased scattering aerosol.
In this paper we present a new description of statistical probability density functions (pdfs) of polar mesospheric clouds (PMC). We derive a new class of pdfs that describes successfully the probability statistic of ALOMAR lidar observations of different ice parameters. As a main advantage the new method allows us to connect different observational PMC distributions of lidar and satellite data, and also to compare with distributions from ice model studies.
As frozen soil, called permafrost, increasingly thaws over the years, scientists have put much effort into understanding how this may increase carbon emissions, which would exacerbate climate change. Our work supports the emerging view that these efforts should also include nitrous oxide (N2O), a more potent greenhouse gas. Using a low-flying aircraft to study thousands of acres of Alaskan permafrost, we observed average N2O emissions higher than typically assumed for regions such as this.
Jerry R. Ziemke, Luke D. Oman, Sarah A. Strode, Anne R. Douglass, Mark A. Olsen, Richard D. McPeters, Pawan K. Bhartia, Lucien Froidevaux, Gordon J. Labow, Jacquie C. Witte, Anne M. Thompson, David P. Haffner, Natalya A. Kramarova, Stacey M. Frith, Liang-Kang Huang, Glen R. Jaross, Colin J. Seftor, Mathew T. Deland, and Steven L. Taylor
Both a 38-year merged satellite record of tropospheric ozone from TOMS/OMI/MLS/OMPS and a MERRA-2 GMI model simulation show large increases of 6–7 Dobson units from the Near East to India–East Asia and eastward over the Pacific. These increases in tropospheric ozone are attributed to increases in pollution over the region over the last several decades. Secondary 38-year increases of 4–5 Dobson units with both GMI model and satellite measurements occur over central African–tropical Atlantic.
Chloromethane is the most important natural carrier of chlorine to the stratosphere. From a newly determined carbon isotope effect of −11.2 ‰ for the tropospheric loss of CH3Cl we derive a tropical rainforest CH3Cl source of 670 ± 200 Gg a−1, 60 % smaller than previous estimates. A revision of previous bottom-up estimates using above-ground biomass instead of rainforest area strongly supports this lower estimate. Our results suggest a large unknown tropical value of 1530 ± 200 Gg a−1.
The ability of positive matrix factorization (PMF) factor analysis to identify and quantify the organic aerosol (OA) sources accurately is tested in this modeling study. The estimated uncertainty of the contribution of fresh biomass burning is less than 30 % and of the other primary sources is less than 40 %, when these sources contribute more than 20 % to the OA. Τhe first oxygenated OA factor includes mainly highly aged OA, while the second oxygenated OA factor contains fresher secondary OA.
Katherine B. Benedict, Yong Zhou, Barkley C. Sive, Anthony J. Prenni, Kristi A. Gebhart, Emily V. Fischer, Ashley Evanoski-Cole, Amy P. Sullivan, Sara Callahan, Bret A. Schichtel, Huiting Mao, Ying Zhou, and Jeffrey L. Collett Jr.
Rocky Mountain National Park experiences high ozone concentrations that can exceed the National Ambient Air Quality Standard. As part of the FRAPPÉ field campaign, a suite of volatile organic compounds were measured to characterize the sources of ozone precursors that contribute to high ozone in the park. These measurements indicate emissions from the Front Range in Colorado tied to oil and gas operations, urban areas, and the stratosphere contribute to episodes of elevated ozone.
This paper assesses the structural changes in the shallow and transition branches of the BDC induced by El Nino using the Lagrangian model simulations driven by ERAi and JRA-55 combined with MLS observations. We found a clear evidence of a weakening of the transition branch due to an upward shift in the dissipation height of the planetary and gravity waves and a strengthening of the shallow branch due to enhanced GW breaking in the tropics–subtropics and PW breaking at high latitudes.
Volcanic sulfur can have climatic impacts for the planet via sulfate aerosol formation, leading also to pollution events. We provide model constraints on tropospheric volcanic sulfate formation, with implications for its lifetime and impacts on regional air quality. Oxygen isotope investigations from our model suggest that in the poor tropospheric plumes of halogens, the O2/TMI sulfur oxidation pathway might significantly control sulfate production. The produced sulfate has no isotopic anomaly.
Michael Weger, Bernd Heinold, Christa Engler, Ulrich Schumann, Axel Seifert, Romy Fößig, Christiane Voigt, Holger Baars, Ulrich Blahak, Stephan Borrmann, Corinna Hoose, Stefan Kaufmann, Martina Krämer, Patric Seifert, Fabian Senf, Johannes Schneider, and Ina Tegen
The impact of desert dust on cloud formation is investigated for a major Saharan dust event over Europe by interactive regional dust modeling. Dust particles are very efficient ice-nucleating particles promoting the formation of ice crystals in clouds. The simulations show that the observed extensive cirrus development was likely related to the above-average dust load. The interactive dust–cloud feedback in the model significantly improves the agreement with aircraft and satellite observations.
Spatial structures of wave disturbances in the upper atmosphere were investigated with space-borne imaging from the International Space Station. The wave disturbance occurred around an altitude of 100 km, and is called a mesospheric bore. The large-scale structure of mesospheric bores has not been fully captured by previous ground-based imagers, but the space-borne imaging captured a bore with a wide field of view, and showed that bores can have a large undulating wave front as long as 2000 km.
Using light diffraction it is possible to detect microscopic features within ice particles that have not yet been fully characterized. Here, this technique was applied in airborne measurements, where it was found that majority of atmospheric ice particles have features that significantly change the way ice particles interact with solar light. The microscopic features make ice-containing clouds more reflective than previously thought, which could have consequences for predicting our climate.
Wolfgang Woiwode, Andreas Dörnbrack, Martina Bramberger, Felix Friedl-Vallon, Florian Haenel, Michael Höpfner, Sören Johansson, Erik Kretschmer, Isabell Krisch, Thomas Latzko, Hermann Oelhaf, Johannes Orphal, Peter Preusse, Björn-Martin Sinnhuber, and Jörn Ungermann
GLORIA observations during two crossings of the polar front jet stream resolve the fine mesoscale structure of a tropopause fold in high detail. Tracer–tracer correlations of H2O and O3 are presented as a function of potential temperature and reveal an active mixing region. Our study confirms conceptual models of tropopause folds, validates the high quality of ECMWF IFS forecasts, and suggests that mountain waves are capable of modulating exchange processes in the vicinity of tropopause folds.
The number concentration of ice crystals (Ni) is a key cloud property that remains very uncertain due to difficulties in determining it using satellites. This lack of global observational constraints limits our ability to constrain this property in models responsible for predicting future climate. This pair of papers fills this gap by showing and analyzing the first rigorously evaluated global climatology of Ni, leading to new information shedding light on the processes that control high clouds.
To tackle the problem of severe air pollution, China has implemented active clean air policies in recent years. We quantified China’s anthropogenic emissions during 2010–2017 and identified the major driving forces of these trends by using a combination of bottom-up emission inventory and index decomposition analysis (IDA) approaches. The major air pollutants have reduced their emissions by 17–62 % during 2010–2017. The IDA results suggest that emission control measures are the main drivers.
Reanalyses (RAs) are models which assimilate observations and are widely used as proxies for the true atmospheric state. Here, we resample six leading RAs using the weighting functions of four high-res satellite instruments, allowing a like-for-like comparison. We find that the RAs generally reproduce the satellite data well, except at high altitudes and in the tropics. However, we also find that the RAs more tightly correlate with each other than with observations, even those they assimilate.
Emissions of carbon tetrafluoride CF4, NF3 and CHF3 in east Asia have been calculated using atmospheric measurements and an atmospheric transport model. We calculate emissions of CF4 to be quite constant between the years 2008 and 2015 for both China and South Korea, with 2015 emissions calculated at 4.33 ± 2.65 Gg yr-1 and 0.36 ± 0.11 Gg yr-1, respectively. Emission estimates of NF3 from South Korea could be made with relatively small uncertainty at 0.6 ± 0.07 Gg yr-1 in 2015.
Ben Kravitz, Philip J. Rasch, Hailong Wang, Alan Robock, Corey Gabriel, Olivier Boucher, Jason N. S. Cole, Jim Haywood, Duoying Ji, Andy Jones, Andrew Lenton, John C. Moore, Helene Muri, Ulrike Niemeier, Steven Phipps, Hauke Schmidt, Shingo Watanabe, Shuting Yang, and Jin-Ho Yoon
Marine cloud brightening has been proposed as a means of geoengineering/climate intervention, or deliberately altering the climate system to offset anthropogenic climate change. In idealized simulations that highlight contrasts between land and ocean, we find that the globe warms, including the ocean due to transport of heat from land. This study reinforces that no net energy input into the Earth system does not mean that temperature will necessarily remain unchanged.
This study extends our previous investigation in dust–radiation interactions to investigate SRF and its feedbacks on the regional climate and the dust cycle over east Asia by use of the CAM4-BAM. Our results show that SRF increases the east Asian dust emissions significantly by 13.7 % in the spring, in contrast to −7.6 % of decreased dust emissions by DRF. Hence, a significant feature of SRF on the Tibetan Plateau can create a positive feedback loop to enhance the dust cycle over east Asia.
Small particles in Earth's atmosphere (also referred to as atmospheric aerosols) emitted by human activities impact Earth's climate in complex ways and play an important role in Earth's water cycle. We use a climate modeling approach and find that aerosols from the United States and Europe can have substantial effects on rainfall in far-away regions such as Africa's Sahel or the Mediterranean. Air pollution controls in these regions may help reduce the likelihood and severity of Sahel drought.
Extremely large light extinction coefficients of 500 Mm-1, about 20 times higher than after the Pinatubo volcanic eruptions in 1991, were observed by EARLINET lidars in the stratosphere over central Europe from 21 to 22 August, 2017. This paper provides an overview based on ground-based (lidar, AERONET) and satellite (MODIS, OMI) remote sensing.
This paper presents the first direct atmospheric observations of the formation and evolution of tar balls (TBs) in forest fires collected during the Department of Energy’s Biomass Burning Observation Project (BBOP). We quantify, for the first time, the TB mass fraction in the BB plumes and show that this mass fraction increases from less than 1 % to 50 % within the first couple of hours of plume aging. Using Mie theory we find that TBs are consistent with being weak light absorbers.
Ciao-Kai Liang, J. Jason West, Raquel A. Silva, Huisheng Bian, Mian Chin, Yanko Davila, Frank J. Dentener, Louisa Emmons, Johannes Flemming, Gerd Folberth, Daven Henze, Ulas Im, Jan Eiof Jonson, Terry J. Keating, Tom Kucsera, Allen Lenzen, Meiyun Lin, Marianne Tronstad Lund, Xiaohua Pan, Rokjin J. Park, R. Bradley Pierce, Takashi Sekiya, Kengo Sudo, and Toshihiko Takemura
Emissions from one continent affect air quality and health elsewhere. Here we quantify the effects of intercontinental PM2.5 and ozone transport on human health using a new multi-model ensemble, evaluating the health effects of emissions from six world regions and three emission source sectors. Emissions from one region have significant health impacts outside of that source region; similarly, foreign emissions contribute significantly to air-pollution-related deaths in several world regions.
Saharan dust wet deposited in Granada (Spain) on 21–23 February 2017 during the most extreme red rain event of the last decades led to the deposition of ~ 140 000 T of dust just in the city of Granada, dwarfing any other standard Saharan dust events taking place in the area. The multianalytical study of Saharan dust disclosed potential source areas and the mineralogy and composition of the size fractions of desert dust as well as its potential biogeochemical, radiative, and health effects.
Aurélien Chauvigné, Olivier Jourdan, Alfons Schwarzenboeck, Christophe Gourbeyre, Jean François Gayet, Christiane Voigt, Hans Schlager, Stefan Kaufmann, Stephan Borrmann, Sergej Molleker, Andreas Minikin, Tina Jurkat, and Ulrich Schumann
This paper demonstrates a new form of statistical analysis of contrail to cirrus evolution. The authors show well-separated analyses of the different stages of the contrail's evolution, which allows us to study their optical, microphysical, and chemical properties. These results could be used to develop representative parameterizations of the scattering and geometrical properties of the ice crystals’ shapes and sizes, observed in the visible wavelength range.
This paper tackles a major issue for air quality over East Asia: ozone pollution produced over a major source, like the North China Plain, and the contribution of ozone produced while being transported across the continent and the surrounding seas. The main originality of the paper lays in the fact that this photochemical production of ozone is observationally quantified with new multispectral satellite observations offering unique skills to observe the ozone pollution plumes near the surface.
From 3 years of observations from the CATS lidar on the International Space Station we document the daily cycle of the vertical distribution of clouds.
This is the first time this is documented over several continents and oceans using finely resolved measurements on a near-global scale from a single instrument.
We show that other instruments observing clouds from space, like CALIPSO, document extremes of the daily cycle over ocean and closer to the average over land.
Kanako Sekimoto, Abigail R. Koss, Jessica B. Gilman, Vanessa Selimovic, Matthew M. Coggon, Kyle J. Zarzana, Bin Yuan, Brian M. Lerner, Steven S. Brown, Carsten Warneke, Robert J. Yokelson, James M. Roberts, and Joost de Gouw
We found that on average 85 % of the VOC emissions from biomass burning across various fuels representative of the western US (including various coniferous and chaparral fuels) can be explained using only two emission profiles: (i) a high-temperature pyrolysis profile and (ii) a low-temperature pyrolysis profile. The high-temperature profile is quantitatively similar between different fuel types (r2 > 0.84), and likewise for the low-temperature profile.
Sandip S. Dhomse, Douglas Kinnison, Martyn P. Chipperfield, Ross J. Salawitch, Irene Cionni, Michaela I. Hegglin, N. Luke Abraham, Hideharu Akiyoshi, Alex T. Archibald, Ewa M. Bednarz, Slimane Bekki, Peter Braesicke, Neal Butchart, Martin Dameris, Makoto Deushi, Stacey Frith, Steven C. Hardiman, Birgit Hassler, Larry W. Horowitz, Rong-Ming Hu, Patrick Jöckel, Beatrice Josse, Oliver Kirner, Stefanie Kremser, Ulrike Langematz, Jared Lewis, Marion Marchand, Meiyun Lin, Eva Mancini, Virginie Marécal, Martine Michou, Olaf Morgenstern, Fiona M. O'Connor, Luke Oman, Giovanni Pitari, David A. Plummer, John A. Pyle, Laura E. Revell, Eugene Rozanov, Robyn Schofield, Andrea Stenke, Kane Stone, Kengo Sudo, Simone Tilmes, Daniele Visioni, Yousuke Yamashita, and Guang Zeng
We analyse simulations from the Chemistry-Climate Model Initiative (CCMI) to estimate the return dates of the stratospheric ozone layer from depletion by anthropogenic chlorine and bromine. The simulations from 20 models project that global column ozone will return to 1980 values in 2047 (uncertainty range 2042–2052). Return dates in other regions vary depending on factors related to climate change and importance of chlorine and bromine. Column ozone in the tropics may continue to decline.
A major phenomenon in the stratosphere is the Quasi Biennial Oscillation (QBO). Although a feature of the equatorial stratosphere, its influence extends to surface weather at both equatorial and mid latitudes. Improved knowledge of mechanisms of influence should help to improve weather forecasts. In this paper, QBO impacts at the surface are characterized and dominant mechanisms explored. Three pathways are identified, referred to as the tropical, subtropical and polar routes.
2017 marks the 30th anniversary of the Montreal Protocol, which was implemented to protect the stratospheric ozone layer from the harmful effects of synthetic ozone depleting substances. Since the late 1990s atmospheric concentrations of these species have begun to decline, and as a result ozone concentrations are expected to increase. In this study we use an ensemble of chemistry–climate simulations to investigate recent ozone trends and search for early signs of ozone recovery.
A numerical model also used for operational weather forecast was applied to investigate the impact of contrails and contrail cirrus on the radiative fluxes at the earth's surface. Accounting for contrails produced by aircraft enables the model to simulate high clouds that are otherwise missing. In a case study, we find that the effect of these extra clouds is to reduce the incoming shortwave radiation at the surface as well as the production of photovoltaic power by up to 10 %.
David S. McLagan, Carl P. J. Mitchell, Alexandra Steffen, Hayley Hung, Cecilia Shin, Geoff W. Stupple, Mark L. Olson, Winston T. Luke, Paul Kelley, Dean Howard, Grant C. Edwards, Peter F. Nelson, Hang Xiao, Guey-Rong Sheu, Annekatrin Dreyer, Haiyong Huang, Batual Abdul Hussain, Ying D. Lei, Ilana Tavshunsky, and Frank Wania
A new passive air sampler for gaseous mercury was tested at 20 sites on four continents. These sites have in common that they use the state-of-the-art active air sampling technique for gaseous mercury on a continuous basis and therefore allow for an evaluation and calibration of the passive sampler. The sampler proved to work exceptionally well, with a precision and accuracy on par with the active
instrument and better than what has previously been achieved with passive samplers.
Synergistic effects between SOA formation and SO2 oxidation through Criegee chemistry and reactive uptake by organic peroxides were observed. The relative importance of these two pathways (Criegee vs. peroxide) varies with relative humidity. The latter SO2 loss mechanism to organic peroxides in SOA has not previously been identified. Our results suggest a new pathway of atmospheric SO2 oxidation, which may contribute to the missing mechanisms of high-sulfate production in the polluted areas.
Detecting trends in short data sets of stratospheric molecules is difficult because of variability due to dynamical fluctuations. We suggest that one way around this difficulty is using the measurements of one molecule to remove dynamical variability from the measurements of another molecule. We illustrate this using Aura MLS measurements of N2O to help us sort out issues in the determination of trends in HCl. This shows that HCl is decreasing throughout the middle stratosphere as expected.
Following decades of successful regulatory policies focused on combustion-related sources (e.g. motor vehicles), emissions from non-combustion sources have become increasingly important for urban air quality. Using multiple approaches, we demonstrate that emissions from consumer, commercial, and industrial products and materials have become prominent contributors to the formation of photochemical smog (i.e. secondary organic particulate matter and ozone) and its associated health effects.
Emma Leedham Elvidge, Harald Bönisch, Carl A. M. Brenninkmeijer, Andreas Engel, Paul J. Fraser, Eileen Gallacher, Ray Langenfelds, Jens Mühle, David E. Oram, Eric A. Ray, Anna R. Ridley, Thomas Röckmann, William T. Sturges, Ray F. Weiss, and Johannes C. Laube
Chemical species measured in stratospheric air can be used as proxies for stratospheric circulation changes which cannot be measured directly. A range of tracers is important to understand changing stratospheric dynamics. We demonstrate the suitability of PFCs and HFCs as tracers and support recent work that reduces the current stratospheric lifetime of SF6. Updates to policy-relevant parameters (e.g. stratospheric lifetime) linked to this change are provided for O3-depleting substances.
Stelios Kazadzis, Natalia Kouremeti, Henri Diémoz, Julian Gröbner, Bruce W. Forgan, Monica Campanelli, Victor Estellés, Kathleen Lantz, Joseph Michalsky, Thomas Carlund, Emilio Cuevas, Carlos Toledano, Ralf Becker, Stephan Nyeki, Panagiotis G. Kosmopoulos, Viktar Tatsiankou, Laurent Vuilleumier, Frederick M. Denn, Nozomu Ohkawara, Osamu Ijima, Philippe Goloub, Panagiotis I. Raptis, Michael Milner, Klaus Behrens, Africa Barreto, Giovanni Martucci, Emiel Hall, James Wendell, Bryan E. Fabbri, and Christoph Wehrli
Aerosol optical depth measured from ground-based sun photometers is the most important parameter for studying the changes in the Earth's radiation balance due to aerosols. Representatives for various sun photometer types belonging to individual institutions or international aerosol networks gather every 5 years, for 3 weeks, in Davos, Switzerland, in order to compare their aeorosol optical depth retrievals. This work presents the results of the latest (fourth) filter radiometer intercomparison.
This paper revisits the chemistry leading to strong ozone depletion in the Antarctic. We focus on the heart of the ozone layer in the lowermost stratosphere in the core of the vortex. We argue that chemical cycles (referred to as HCl null cycles) that have hitherto been largely neglected counteract the deactivation of chlorine and are therefore key to ozone depletion in the core of the Antarctic vortex. The key process to full activation of chlorine is the photolysis of formaldehyde.
The National Observatory of Athens has been collecting solar radiation, sunshine duration, and cloud and visibility data/observations since the beginning of the 20th century. In this work we present surface solar radiation data since 1953 and reconstructed data since 1900. We have attempted to show and discuss the long-term changes in solar surface radiation over Athens, Greece, using these unique datasets.
This paper commemorates the 30-year anniversary of the initial signing of the Montreal Protocol (MP) on substances that deplete the ozone layer. The MP is so far successful in reducing ozone-depleting substances, and total ozone decline was successfully stopped by the late 1990s. Total ozone levels have been mostly stable since then. In some regions, barely significant upward trends are observed that suggest an emergence into the expected ozone recovery phase.
William T. Ball, Justin Alsing, Daniel J. Mortlock, Johannes Staehelin, Joanna D. Haigh, Thomas Peter, Fiona Tummon, Rene Stübi, Andrea Stenke, John Anderson, Adam Bourassa, Sean M. Davis, Doug Degenstein, Stacey Frith, Lucien Froidevaux, Chris Roth, Viktoria Sofieva, Ray Wang, Jeannette Wild, Pengfei Yu, Jerald R. Ziemke, and Eugene V. Rozanov
Using a robust analysis, with artefact-corrected ozone data, we confirm upper stratospheric ozone is recovering following the Montreal Protocol, but that lower stratospheric ozone (50° S–50° N) has continued to decrease since 1998, and the ozone layer as a whole (60° S–60° N) may be lower today than in 1998. No change in total column ozone may be due to increasing tropospheric ozone. State-of-the-art models do not reproduce lower stratospheric ozone decreases.
Meinrat O. Andreae, Armin Afchine, Rachel Albrecht, Bruna Amorim Holanda, Paulo Artaxo, Henrique M. J. Barbosa, Stephan Borrmann, Micael A. Cecchini, Anja Costa, Maximilian Dollner, Daniel Fütterer, Emma Järvinen, Tina Jurkat, Thomas Klimach, Tobias Konemann, Christoph Knote, Martina Krämer, Trismono Krisna, Luiz A. T. Machado, Stephan Mertes, Andreas Minikin, Christopher Pöhlker, Mira L. Pöhlker, Ulrich Pöschl, Daniel Rosenfeld, Daniel Sauer, Hans Schlager, Martin Schnaiter, Johannes Schneider, Christiane Schulz, Antonio Spanu, Vinicius B. Sperling, Christiane Voigt, Adrian Walser, Jian Wang, Bernadett Weinzierl, Manfred Wendisch, and Helmut Ziereis
We made airborne measurements of aerosol particle concentrations and properties over the Amazon Basin. We found extremely high concentrations of very small particles in the region between 8 and 14 km altitude all across the basin, which had been recently formed by gas-to-particle conversion at these altitudes. This makes the upper troposphere a very important source region of atmospheric particles with significant implications for the Earth's climate system.
Camilla W. Stjern, Helene Muri, Lars Ahlm, Olivier Boucher, Jason N. S. Cole, Duoying Ji, Andy Jones, Jim Haywood, Ben Kravitz, Andrew Lenton, John C. Moore, Ulrike Niemeier, Steven J. Phipps, Hauke Schmidt, Shingo Watanabe, and Jón Egill Kristjánsson
Marine cloud brightening (MCB) has been proposed to help limit global warming. We present here the first multi-model assessment of idealized MCB simulations from the Geoengineering Model Intercomparison Project. While all models predict a global cooling as intended, there is considerable spread between the models both in terms of radiative forcing and the climate response, largely linked to the substantial differences in the models' representation of clouds.
Gravity waves (GWs) as well as solar tides are a key driving mechanism for the circulation in the Earth's atmosphere. The temporal variation of these waves is studied using a record long 10-day continuous Rayleigh–Mie–Raman lidar sounding at midlatitudes. This data set shows a large variability of these waves on timescales of a few days and therefore provides new insights into wave intermittency phenomena, which can help to improve model simulations.
Substantial differences exist in current estimates of agricultural ammonia emissions in China, hindering understanding of their environmental consequences. This study applies both bottom-up and top-down methods to better quantify agricultural ammonia sources in China using observations from satellite and surface networks interpreted by a chemical transport model. Our estimate of annual Chinese anthropogenic ammonia emission is 11.7 tg (teragram) for 2008 with a strong seasonality peak in summer.
Isabell Krisch, Peter Preusse, Jörn Ungermann, Andreas Dörnbrack, Stephen D. Eckermann, Manfred Ern, Felix Friedl-Vallon, Martin Kaufmann, Hermann Oelhaf, Markus Rapp, Cornelia Strube, and Martin Riese
Using the infrared limb imager GLORIA, the 3-D structure of mesoscale gravity waves in the lower stratosphere was measured for the first time, allowing for a complete 3-D characterization of the waves. This enables the precise determination of the sources of the waves in the mountain regions of Iceland with backward ray tracing. Forward ray tracing shows oblique propagation, an effect generally neglected in global atmospheric models.
The generalized linear regression model (GLM), even based only on meteorological parameters, could be satisfactory to estimate the contribution of meteorological conditions in reducing air pollution and hence the contribution of control strategies in reducing air pollution. Using the GLM, we found that the meteorological conditions and pollution control strategies contributed 30 % and 28 % to the reduction of the PM2.5 concentration during APEC 2014 and 38 % and 25 % during Parade 2015.
Understanding tropospheric ozone chemistry has been at the centre of the field of atmospheric chemistry for the last 30 years. However, our conceptual approach to diagnosing ozone production in global models has not advanced in this time. Our work presents a new and powerful approach for diagnosing tropospheric ozone production, providing a significant enhancement in our ability to understand the processes controlling ozone and how we can validate our assessment of these processes.
This study shows that agricultural emissions are important for air quality and their reduction can effectively reduce the concentration of fine particles and their associated premature mortality. Therefore, emission control policies, especially in North America and Europe, should also involve strong ammonia emission decreases to optimally reduce fine-particle concentration.
David E. Oram, Matthew J. Ashfold, Johannes C. Laube, Lauren J. Gooch, Stephen Humphrey, William T. Sturges, Emma Leedham-Elvidge, Grant L. Forster, Neil R. P. Harris, Mohammed Iqbal Mead, Azizan Abu Samah, Siew Moi Phang, Chang-Feng Ou-Yang, Neng-Huei Lin, Jia-Lin Wang, Angela K. Baker, Carl A. M. Brenninkmeijer, and David Sherry
We have observed large amounts of man-made chlorine compounds in E and SE Asia and in the upper tropical troposphere. These relatively short-lived compounds are not controlled by the Montreal Protocol, but if significant quantities were able to reach the stratosphere, the long-term recovery of stratospheric ozone would be delayed. We have also identified an important atmospheric transport mechanism that can rapidly transport these chemicals from E Asia to the upper troposphere via the tropics.
Wolfgang Steinbrecht, Lucien Froidevaux, Ryan Fuller, Ray Wang, John Anderson, Chris Roth, Adam Bourassa, Doug Degenstein, Robert Damadeo, Joe Zawodny, Stacey Frith, Richard McPeters, Pawan Bhartia, Jeannette Wild, Craig Long, Sean Davis, Karen Rosenlof, Viktoria Sofieva, Kaley Walker, Nabiz Rahpoe, Alexei Rozanov, Mark Weber, Alexandra Laeng, Thomas von Clarmann, Gabriele Stiller, Natalya Kramarova, Sophie Godin-Beekmann, Thierry Leblanc, Richard Querel, Daan Swart, Ian Boyd, Klemens Hocke, Niklaus Kämpfer, Eliane Maillard Barras, Lorena Moreira, Gerald Nedoluha, Corinne Vigouroux, Thomas Blumenstock, Matthias Schneider, Omaira García, Nicholas Jones, Emmanuel Mahieu, Dan Smale, Michael Kotkamp, John Robinson, Irina Petropavlovskikh, Neil Harris, Birgit Hassler, Daan Hubert, and Fiona Tummon
Thanks to the 1987 Montreal Protocol and its amendments, ozone-depleting chlorine (and bromine) in the stratosphere has declined slowly since the late 1990s. Improved and extended long-term ozone profile observations from satellites and ground-based stations confirm that ozone is responding as expected and has increased by about 2 % per decade since 2000 in the upper stratosphere, around 40 km altitude. At lower altitudes, however, ozone has not changed significantly since 2000.
This study reports the distinct effects of street canyons on new particle formation (NPF) under warm or cold ambient temperature conditions because of on-road vehicle emissions; i.e., stronger condensation sinks are responsible for the reduced NPF in the springtime, but efficient nucleation and partitioning of gaseous species contribute to the enhanced NPF in the wintertime. The oxidization of biogenic organics is suggested to play an important role in growing new particles.
We assess NOx emission trends over Chinese cities based on satellite NO2 observations using a method independent of chemical transport models. NOx emissions over 48 Chinese cities have decreased significantly since 2011. Cities with different dominant emission sources (i.e. power, industrial, and transportation sectors) showed variable emission decline timelines that corresponded to the schedules for emission control in different sectors.
We introduce a novel 3-D method of measuring atmospheric gravity waves, based around a 3-D Stockwell transform. Our method lets us measure new properties, including wave intrinsic frequencies and phase and group velocities. We apply it to data from the AIRS satellite instrument over the Southern Andes for two consecutive winters. Our results show clear evidence that the waves measured are primarily orographic in origin, and that their group velocity vectors are focused into the polar night jet.
Thibaud Thonat, Marielle Saunois, Philippe Bousquet, Isabelle Pison, Zeli Tan, Qianlai Zhuang, Patrick M. Crill, Brett F. Thornton, David Bastviken, Ed J. Dlugokencky, Nikita Zimov, Tuomas Laurila, Juha Hatakka, Ove Hermansen, and Doug E. J. Worthy
Atmospheric methane simulations in the Arctic have been made for 2012 and compared to continuous observations at six measurement sites. All methane sources significantly affect the measurements at all stations, at least at the synoptic scale, except for biomass burning. An appropriate modelling framework combined with continuous observations of atmospheric methane enables us to gain knowledge on regional methane sources, including those which are usually poorly represented, such as freshwater.
Opposite trends in aerosol loading between the lower and upper planetary boundary layer are found on a wide range of timescales and from different types of data acquired by various platforms in China. The reversal trend is consistent with the strong vertical gradients in the aerosol-induced atmospheric heating rate that unevenly modifies the atmospheric temperature profile and alters the stability differently. The findings have multiple implications in understanding and combating air pollution.
While it is widely recognized that air pollutants adversely affect human health and climate change, their impacts on the regional carbon balance are less well understood. We apply an Earth system model to quantify the combined effects of ozone and aerosol particles on net primary production in China. Ozone vegetation damage dominates over the aerosol effects, leading to a substantial net suppression of land carbon uptake in the present and future worlds.
Markella Prokopiou, Patricia Martinerie, Célia J. Sapart, Emmanuel Witrant, Guillaume Monteil, Kentaro Ishijima, Sophie Bernard, Jan Kaiser, Ingeborg Levin, Thomas Blunier, David Etheridge, Ed Dlugokencky, Roderik S. W. van de Wal, and Thomas Röckmann
Nitrous oxide is the third most important anthropogenic greenhouse gas with an increasing mole fraction. To understand its natural and anthropogenic sources
we employ isotope measurements. Results show that while the N2O mole fraction increases, its heavy isotope content decreases. The isotopic changes observed underline the dominance of agricultural emissions especially at the early part of the record, whereas in the later decades the contribution from other anthropogenic sources increases.
Radiosonde observations (RAOBs) have provided the only long-term global in situ temperature measurements since 1958. In this study, we use Global Positioning System (GPS) radio occultation (RO) temperature data from 2006 to 2014 to characterize the inter-seasonal and interannual variability of temperature biases in the lower stratosphere. Results from this study also demonstrate the feasibility to use RO data to correct RAOB temperature biases for different sensor types.
The potential of airborne radiance measurements in the sideward and nadir directions for cirrus remote sensing is investigated. Therefore radiative transfer simulations were used and the sensitivity of upward radiance with respect to optical thickness, effective radius, surface albedo, wavelength and viewing angle was studied. It was shown that sideward observations lead to more accurate retrieval results. Investigating a case study of ML-CIRRUS, these findings are confirmed.
We show the first simultaneous observations of triple oxygen isotopic compositions of atmospheric sulfate, nitrate, and ozone at Dumont d'Urville, coastal Antarctica. The contrasting seasonal trends between oxygen isotopes of ozone and those of sulfate and nitrate indicate that these signatures in sulfate and nitrate are mainly controlled by changes in oxidation chemistry. We also discuss the specific oxidation chemistry induced by the unique phenomena at the site.
Gunnar Myhre, Wenche Aas, Ribu Cherian, William Collins, Greg Faluvegi, Mark Flanner, Piers Forster, Øivind Hodnebrog, Zbigniew Klimont, Marianne T. Lund, Johannes Mülmenstädt, Cathrine Lund Myhre, Dirk Olivié, Michael Prather, Johannes Quaas, Bjørn H. Samset, Jordan L. Schnell, Michael Schulz, Drew Shindell, Ragnhild B. Skeie, Toshihiko Takemura, and Svetlana Tsyro
Over the past decades, the geographical distribution of emissions of substances that alter the atmospheric energy balance has changed due to economic growth and pollution regulations. Here, we show the resulting changes to aerosol and ozone abundances and their radiative forcing using recently updated emission data for the period 1990–2015, as simulated by seven global atmospheric composition models. The global mean radiative forcing is more strongly positive than reported in IPCC AR5.
Currently the Cape Point GAW GEM record is a very sought-after data record for international modelers and scientist alike, as the data set of 20 years represents the longest record in the Southern Hemisphere (SH). CPT was the only monitoring site on the African continent and one of eight GMOS ground-based monitoring sites located in the SH. The increasing Hg trend observed at CPT is of global importance as treaties such as the Minamata Convention on Mercury is there to combat Hg pollution.
Claudia Di Biagio, Paola Formenti, Yves Balkanski, Lorenzo Caponi, Mathieu Cazaunau, Edouard Pangui, Emilie Journet, Sophie Nowak, Sandrine Caquineau, Meinrat O. Andreae, Konrad Kandler, Thuraya Saeed, Stuart Piketh, David Seibert, Earle Williams, and Jean-François Doussin
Modeling the interaction of dust with long-wave (LW) radiation is still a challenge due to the scarcity of information on their refractive index. In this paper, we present a unique dataset of dust refractive indices obtained from in situ measurements in a large smog chamber. Our results show that the dust LW refractive index varies strongly from source to source due to particle composition changes. We recommend taking this variability into account in climate and remote sensing applications.
We model pre-industrial to present day changes using the GEOS-Chem global chemical transport model with halogens (Cl, Br, I). The model better captures pre-industrial O3 observations with halogens included. Halogens buffer the tropospheric forcing of O3 (RFTO3) from pre-industrial to present day, reducing RFTO3 by 0.087 Wm−2. This reduction is greater than that from halogens on stratospheric O3 (−0.05 Wm−2). This suggests that models that do not include halogens will overestimate RFTO3by ~ 25%.
Global surface emissions of nitrogen oxides (NOx) over a 10-year period (2005–2014) are estimated from assimilation of multiple satellite datasets. We present detailed distributions of the estimated NOx emission distributions for all major regions, the diurnal, seasonal, and decadal variability. The estimated emissions show a positive trend over India, China, and the Middle East, and a negative trend over the United States, southern Africa, and western Europe.
Tamás Kovács, Wuhu Feng, Anna Totterdill, John M. C. Plane, Sandip Dhomse, Juan Carlos Gómez-Martín, Gabriele P. Stiller, Florian J. Haenel, Christopher Smith, Piers M. Forster, Rolando R. García, Daniel R. Marsh, and Martyn P. Chipperfield
Sulfur hexafluoride (SF6) is a very potent greenhouse gas, which is present in the atmosphere only through its industrial use, for example as an electrical insulator. To estimate accurately the impact of SF6 emissions on climate we need to know how long it persists in the atmosphere before being removed. Previous estimates of the SF6 lifetime indicate a large degree of uncertainty. Here we use a detailed atmospheric model to calculate a current best estimate of the SF6 lifetime.
Secondary organic aerosols (SOA) comprise a significant fraction of particulate matter (PM) and may have health implications. The water-soluble oxidative potentials of various SOA systems were determined using dithiothreitol consumption. Results from this study demonstrate that precursor identity was more influential than reaction condition in determining SOA oxidative potential and highlight a need to consider SOA contributions from anthropogenic hydrocarbons to PM-induced health effects.
Zhaofeng Tan, Hendrik Fuchs, Keding Lu, Andreas Hofzumahaus, Birger Bohn, Sebastian Broch, Huabin Dong, Sebastian Gomm, Rolf Häseler, Lingyan He, Frank Holland, Xin Li, Ying Liu, Sihua Lu, Franz Rohrer, Min Shao, Baolin Wang, Ming Wang, Yusheng Wu, Limin Zeng, Yinsong Zhang, Andreas Wahner, and Yuanhang Zhang
In this study, we performed accurate OH measurements as well as selective HO2 and RO2 measurements at a rural site in North China Plain with state-of-the-art instruments newly developed. We confirmed the previous discovery on the enhancement of the OH in low NOx with which little O3 production was associated, and we found a missing RO2 source in high NOx which promoted higher O3 production. Our results are of vital importance for ozone abatement strategies currently under discussion for China.
This paper summarizes two field measurements of particles and gases made in coastal Antarctica and represents the first real-time composition measurements of particles in this understudied area of the world. Using the combined data from both field measurements, we find that there is a constant background of particles in coastal Antarctica and that they are mostly sulfate. Seasonal transitions from winter to spring add additional particles, and that from spring to summer adds additional sulfate.
Martyn P. Chipperfield, Qing Liang, Matthew Rigby, Ryan Hossaini, Stephen A. Montzka, Sandip Dhomse, Wuhu Feng, Ronald G. Prinn, Ray F. Weiss, Christina M. Harth, Peter K. Salameh, Jens Mühle, Simon O'Doherty, Dickon Young, Peter G. Simmonds, Paul B. Krummel, Paul J. Fraser, L. Paul Steele, James D. Happell, Robert C. Rhew, James Butler, Shari A. Yvon-Lewis, Bradley Hall, David Nance, Fred Moore, Ben R. Miller, James W. Elkins, Jeremy J. Harrison, Chris D. Boone, Elliot L. Atlas, and Emmanuel Mahieu
Carbon tetrachloride (CCl4) is a compound which, when released into the atmosphere, can cause depletion of the stratospheric ozone layer. Its emissions are controlled under the Montreal Protocol, and its atmospheric abundance is slowly decreasing. However, this decrease is not as fast as expected based on estimates of its emissions and its atmospheric lifetime. We have used an atmospheric model to look at the uncertainties in the CCl4 lifetime and to examine the impact on its atmospheric decay.
This study provides new insight into the hydrolysis reaction mechanism, which was elucidated for atmospherically relevant organic nitrates using kinetic measurements, product identification, and theoretical calculations. The results help broaden our knowledge of the organic chemistry that impacts the fate of NOx, ozone production, aerosol phase processing, and aerosol composition.
Yee Jun Tham, Zhe Wang, Qinyi Li, Hui Yun, Weihao Wang, Xinfeng Wang, Likun Xue, Keding Lu, Nan Ma, Birger Bohn, Xin Li, Simonas Kecorius, Johannes Größ, Min Shao, Alfred Wiedensohler, Yuanhang Zhang, and Tao Wang
This work addresses the unclear global significance of chlorine activation processes in the troposphere. The first high-quality measurement data set of ClNO2 in northern China revealed strong ClNO2 production in the residual layers, and demonstrated its significant effects on radical budget and ozone production. Our findings imply the widespread effects of ClNO2 over the polluted regions of northern China, which may increase photochemical and haze pollution.
This paper investigates the cause of the known underestimate of bottom-up inventories of methane in California's South Coast Air Basin (SoCAB). We use total column measurements of methane, ethane, carbon monoxide, and other trace gases beginning in the late 1980s to calculate emissions and attribute sources of excess methane to the atmosphere. We conclude that more than half of the excess methane to the SoCAB atmosphere is attributable to processed natural gas.
We describe the design of and first results from the BErkeley Atmospheric CO2 Observation Network, a distributed instrument of 28 CO2 sensors stationed across and around the city of Oakland, California at ~ 2 km intervals. We evaluate the network via 4 performance parameters (cost, reliability, precision, systematic uncertainty) and find this high density technique to be sufficiently cost-effective and rigorous to inform understanding of small-scale urban emissions relevant to climate regulation.
Light absorbing organic aerosols (BrC) absorb sunlight thereby influencing climate; however, understanding of the link between their optical properties and environmental variables remains limited. Our chamber experiment results suggest that variables including NOx concentration, RH level, and photolysis time have considerable influence on secondary BrC optical properties. The results contribute to a more accurate characterization of the impacts of aerosols on climate, especially in urban areas.
A total of 480 microorganisms collected from 39 clouds sampled in France were isolated and identified. This unique collection was screened for biosurfactant production by measuring the surface tension. 41 % of the tested strains were active producers. Pseudomonas, the most frequently detected genus in clouds, was the dominant group for the production of biosurfactants. Further, the potential impact of the production of biosurfactants by cloud microorganisms on atmospheric processes is discussed.
Historical time series are unique sources of information for past climate and atmospheric composition change. The 82-year time series of visibility data collected at the National Observatory of Athens (NOA) was an excellent proxy for the long-term evolution of particulate pollution in the eastern Mediterranean, at times when direct aerosol measurements were missing. Evolution of particulate pollution of both local and regional origin is nicely reflected on visibility records of NOA.
Zarashpe Z. Kapadia, Dominick V. Spracklen, Steve R. Arnold, Duncan J. Borman, Graham W. Mann, Kirsty J. Pringle, Sarah A. Monks, Carly L. Reddington, François Benduhn, Alexandru Rap, Catherine E. Scott, Edward W. Butt, and Masaru Yoshioka
Using a coupled tropospheric chemistry-aerosol microphysics model this research paper investigates the effect of variations in aviation fuel sulfur content (FSC) on surface PM2.5 concentrations, increases in aviation-induced premature mortalities, low-level cloud condensation nuclei and radiative effect.
When investigating the climatic impact of variations in FSC the ozone direct radiative effect, aerosol direct radiative effect and aerosol cloud albedo effect are quantified.
HF, the dominant stratospheric fluorine reservoir, results from the atmospheric degradation of anthropogenic species such as CFCs, HCFCs, and HFCs. All are strong greenhouse gases, and CFCs and HCFCs deplete stratospheric ozone.
We report the comparison of HF global distributions and trends measured by the ACE-FTS and HALOE satellite instruments with the output of SLIMCAT, a chemical transport model. The global HF trends reveal a slowing down in the rate of increase of HF since the 1990s.
Megan D. Willis, Julia Burkart, Jennie L. Thomas, Franziska Köllner, Johannes Schneider, Heiko Bozem, Peter M. Hoor, Amir A. Aliabadi, Hannes Schulz, Andreas B. Herber, W. Richard Leaitch, and Jonathan P. D. Abbatt
We present a case study focused on an aerosol growth event observed in the Canadian High Arctic during summer. Using measurements of aerosol chemical and physical properties we find evidence for aerosol growth into cloud condensation nuclei-active sizes, through marine-influenced secondary organic aerosol formation. Understanding the mechanisms that control the formation and growth of aerosol is crucial for our ability to predict cloud properties, and therefore radiative balance and climate.
We show that evaluating global aerosol model data with observations of very different spatial scales (200 vs. 10 km) can lead to large discrepancies, solely due to different spatial sampling. Strategies for reducing these sampling errors are developed and tested using a set of high-resolution model simulations.
Nickolay A. Krotkov, Chris A. McLinden, Can Li, Lok N. Lamsal, Edward A. Celarier, Sergey V. Marchenko, William H. Swartz, Eric J. Bucsela, Joanna Joiner, Bryan N. Duncan, K. Folkert Boersma, J. Pepijn Veefkind, Pieternel F. Levelt, Vitali E. Fioletov, Russell R. Dickerson, Hao He, Zifeng Lu, and David G. Streets
We examine changes in SO2 and NO2 over the world's most polluted regions during the first decade of Aura OMI observations. Over the eastern US, both NO2 and SO2 levels decreased by 40 % and 80 %, respectively. OMI confirmed large reductions in SO2 over eastern Europe's largest coal power plants. The North China Plain has the world's most severe SO2 pollution, but a decreasing trend been observed since 2011, with a 50 % reduction in 2012–2014. India's SO2 and NO2 levels are growing at a fast pace.
We present experimental kinetic isotope effects (KIE) for the OH oxidation of CH3D and 13CH3D and their temperature dependence. Our determination of the 13CH3D + OH KIE is novel and we find no "clumped" isotope effect within the experimental uncertainty.
Various forms of solar radiation management (SRM) have been proposed to counteract man-made climate change. However, all these countermeasures could have unintended side-effects. We add a novel perspective to this discussion by showing how atmospheric ozone changes under solar geoengineering could affect UV exposure and air pollution. This would have implications for human health and ecology. Atmospheric composition changes are therefore important to consider in the evaluation of any SRM scheme.
James Hansen, Makiko Sato, Paul Hearty, Reto Ruedy, Maxwell Kelley, Valerie Masson-Delmotte, Gary Russell, George Tselioudis, Junji Cao, Eric Rignot, Isabella Velicogna, Blair Tormey, Bailey Donovan, Evgeniya Kandiano, Karina von Schuckmann, Pushker Kharecha, Allegra N. Legrande, Michael Bauer, and Kwok-Wai Lo
We use climate simulations, paleoclimate data and modern observations to infer that continued high fossil fuel emissions will yield cooling of Southern Ocean and North Atlantic surfaces, slowdown and shutdown of SMOC & AMOC, increasingly powerful storms and nonlinear sea level rise reaching several meters in 50–150 years, effects missed in IPCC reports because of omission of ice sheet melt and an insensitivity of most climate models, likely due to excessive ocean mixing.
A significant fraction of airborne particles, which have significant impacts on human health, visibility, and climate, are formed from the oxidation of gaseous precursors to generate low-volatility products. We show here that a sesquiterpene, α-cedrene, efficiently forms high-viscosity semisolid particles with complex composition via mechanisms that involve the highly reactive Criegee intermediate and that high molecular weight products play an important role in new particle formation.
M. Mallet, F. Dulac, P. Formenti, P. Nabat, J. Sciare, G. Roberts, J. Pelon, G. Ancellet, D. Tanré, F. Parol, C. Denjean, G. Brogniez, A. di Sarra, L. Alados-Arboledas, J. Arndt, F. Auriol, L. Blarel, T. Bourrianne, P. Chazette, S. Chevaillier, M. Claeys, B. D'Anna, Y. Derimian, K. Desboeufs, T. Di Iorio, J.-F. Doussin, P. Durand, A. Féron, E. Freney, C. Gaimoz, P. Goloub, J. L. Gómez-Amo, M. J. Granados-Muñoz, N. Grand, E. Hamonou, I. Jankowiak, M. Jeannot, J.-F. Léon, M. Maillé, S. Mailler, D. Meloni, L. Menut, G. Momboisse, J. Nicolas, T. Podvin, V. Pont, G. Rea, J.-B. Renard, L. Roblou, K. Schepanski, A. Schwarzenboeck, K. Sellegri, M. Sicard, F. Solmon, S. Somot, B Torres, J. Totems, S. Triquet, N. Verdier, C. Verwaerde, F. Waquet, J. Wenger, and P. Zapf
The aim of this article is to present an experimental campaign over the Mediterranean focused on aerosol-radiation measurements and modeling. Results indicate an important atmospheric loading associated with a moderate absorbing ability of mineral dust. Observations suggest a complex vertical structure and size distributions characterized by large aerosols within dust plumes. The radiative effect is highly variable, with negative forcing over the Mediterranean and positive over northern Africa.
As an air pollutant, O3 is monitored photometrically to assess compliance with air quality legislation. A recent study found a 1.8% reduction in its absorption cross section, which would lead to an equivalent increase in observed O3 concentrations. We estimate this would increase the number of sites out of compliance with air quality regulations in the EU and US by 20%. We draw attention to how small changes in gas metrology impacts attainment and compliance with legal air quality standards.
The manuscript describes measurements of particle depolarization ratio from the NASA airborne HSRL-2 at three wavelengths, for two dust cases and a smoke case. Differences in the spectral dependence of particle depolarization ratio are due to the sizes of the non-spherical particles, large for dust and small for smoke. The large depolarization at 355nm for smoke has not been previously reported and may impact aerosol typing when only a single wavelength is available.
This paper demonstrates organic peroxide and peroxyhemiacetal formation during aqueous photooxidation of methylglyoxal using ultra-high-resolution Fourier transform ion cyclotron resonance electrospray ionization mass spectrometry (FTICR-MS). Then, we provide simulation results of organic peroxide/peroxyhemiacetal formation in clouds and wet aerosols and discuss organic peroxides as a source of condensed-phase OH radicals and as a contributor to aqueous secondary organic aerosol (SOA).
We discuss the shape of ice water content (IWC) vertical profiles in high ice clouds and its effect on radiative properties of these clouds, both in short- and in long-wave bands (SW and LW). We suggest a set of primitive shapes (rectangular, isosceles trapezoid, lower and upper triangle) and propose a statistical parameterization using ice water path (IWP) as a single parameter. We estimate and explain simulated differences in LW/SW atmospheric radiances for suggested IWC shapes.
We show that during the springtime of 2013, the anthropogenic pollution particularly from sources in Asia, contributed significantly to black carbon across the European Arctic free troposphere. In contrast to previous studies, the contribution from open wildfires was minimal. Given that Asian pollution is likely to continue to rise over the coming years, it is likely that the radiative forcing in the Arctic will also continue to increase.
Historical land cover and land use change alone between 1980 and 2010 could lead to reduced summertime surface ozone by up to 4ppbv in East Asia. Climate change alone could lead to an increase in summertime ozone by 2-10ppbv in most of East Asia. Land cover change could offset part of the climate effect and lead to a previously unknown public health benefit. The sensitivity of surface ozone to land cover change is more dependent on dry deposition than isoprene emission in most of East Asia.
N. R. P. Harris, B. Hassler, F. Tummon, G. E. Bodeker, D. Hubert, I. Petropavlovskikh, W. Steinbrecht, J. Anderson, P. K. Bhartia, C. D. Boone, A. Bourassa, S. M. Davis, D. Degenstein, A. Delcloo, S. M. Frith, L. Froidevaux, S. Godin-Beekmann, N. Jones, M. J. Kurylo, E. Kyrölä, M. Laine, S. T. Leblanc, J.-C. Lambert, B. Liley, E. Mahieu, A. Maycock, M. de Mazière, A. Parrish, R. Querel, K. H. Rosenlof, C. Roth, C. Sioris, J. Staehelin, R. S. Stolarski, R. Stübi, J. Tamminen, C. Vigouroux, K. A. Walker, H. J. Wang, J. Wild, and J. M. Zawodny
Trends in the vertical distribution of ozone are reported for new and recently revised data sets. The amount of ozone-depleting compounds in the stratosphere peaked in the second half of the 1990s. We examine the trends before and after that peak to see if any change in trend is discernible. The previously reported decreases are confirmed. Furthermore, the downward trend in upper stratospheric ozone has not continued. The possible significance of any increase is discussed in detail.
Technological shifts between fuel sources have had unexpected impacts on atmospheric composition and these significant changes can go undetected if source-specific monitoring infrastructure is not in place. We present chemically comprehensive, continuous measurements of organic compounds in a developed megacity (London), that show diesel-related hydrocarbons can dominate reactive carbon and ozone formation potential, highlighting a serious underestimation of this source in emission inventories.
P. S. Monks, A. T. Archibald, A. Colette, O. Cooper, M. Coyle, R. Derwent, D. Fowler, C. Granier, K. S. Law, G. E. Mills, D. S. Stevenson, O. Tarasova, V. Thouret, E. von Schneidemesser, R. Sommariva, O. Wild, and M. L. Williams
Ozone holds a certain fascination in atmospheric science. It is ubiquitous in the atmosphere, central to tropospheric oxidation chemistry, and yet harmful to human and ecosystem health as well as being an important greenhouse gas. It is not emitted into the atmosphere but is a byproduct of the very oxidation chemistry it largely initiates. This review examines current understanding of the processes regulating tropospheric ozone at global to local scales from both measurements and models.
This paper describes a new ensemble methodology for the statistical analysis of atmospheric gas- & particle-phase composition data sets. The methodology reduces the huge amount of data derived from many chamber experiments to show that organic reactivity & resultant particle formation can be mapped into unique clusters in statistical space. The model generated is used to map more realistic plant mesocosm oxidation data, the projection of which gives insight into reactive pathways & precursors.
Land surface models (LSMs) describe how carbon and water fluxes react to environmental change. They are key component of climate models, yet they differ enormously. Many perform poorly, despite having many parameters. We outline a development strategy emphasizing robustness, reliability and realism, none of which is guaranteed by complexity alone. We propose multiple constraints, benchmarking and data assimilation, and representing unresolved processes stochastically, as tools in this endeavour.
F. Tummon, B. Hassler, N. R. P. Harris, J. Staehelin, W. Steinbrecht, J. Anderson, G. E. Bodeker, A. Bourassa, S. M. Davis, D. Degenstein, S. M. Frith, L. Froidevaux, E. Kyrölä, M. Laine, C. Long, A. A. Penckwitt, C. E. Sioris, K. H. Rosenlof, C. Roth, H.-J. Wang, and J. Wild
Understanding ozone trends in the vertical is vital in terms of assessing the success of the Montreal Protocol. This paper compares and analyses the long-term trends in stratospheric ozone from seven new merged satellite data sets. The data sets largely agree well with each other, particularly for the negative trends seen in the early period 1984-1997. For the 1998-2011 period there is less agreement, but a clear shift from negative to mostly positive trends.
We show that atmospheric load of ice nuclei is enhanced for up to 20 days after key rainfall events. The rate of enhancement decreases exponentially with time. Rainfall quantity and frequency are increased for a similar duration and with similar exponential decreases thereby supporting the notion of rainfall feedback.
We reveal series of significant feedback in rainfall patterns across Australia over the past century and marked changes in feedback patterns, and we indicate their locations.
This work represents the first application of two-dimensional gas chromatography to broadly characterize the gas-phase emissions of biomass burning, including comparisons among the emissions from burns of selected conifer, grass, crop residue, and peat fuel types. In these smoke samples, over 700 compounds were detected, which are discussed in the context of potential secondary organic aerosol formation.
Glyoxal and methylglyoxal are short-lived organic trace gases and important precursors of secondary organic aerosol. Measurements over oceans are sparse. We present the first in situ glyoxal and methylglyoxal observations over remote temperate oceans, alongside observations of precursor gases. Precursor gases cannot explain observed mixing ratios, highlighting an unknown source. We show a large discrepancy between calculated vertical column densities of glyoxal and those retrieved by satellite.
While climate change mitigation policy often focuses on the energy sector, we find that 40% of the historical human-caused change in the Earth’s radiative balance can be attributed to land use activities, such as deforestation and agriculture. Since pressure on land resources is expected to increase, we compute a theoretical upper bound on the radiative balance impacts from future land use which suggests that both energy policy and land policy are necessary to minimize future climate change.
Sulfuric acid plays a major role in the formation of aerosol particles and clouds. Measurements at the west coast of Ireland reveal that oxidation of SO2 by OH explains only 20%, on average, of H2SO4 formation in coastal marine air. Additional sources may be (a) oxidation by Criegee intermediates produced photolytically and/or (b) formation from SO3 instead of SO2 in the oxidation of dimethyl sulfide, suggesting an important role of marine emissions in the self-cleaning power of the atmosphere.
S. M. Khaykin, I. Engel, H. Vömel, I. M. Formanyuk, R. Kivi, L. I. Korshunov, M. Krämer, A. D. Lykov, S. Meier, T. Naebert, M. C. Pitts, M. L. Santee, N. Spelten, F. G. Wienhold, V. A. Yushkov, and T. Peter
P. Stier, N. A. J. Schutgens, N. Bellouin, H. Bian, O. Boucher, M. Chin, S. Ghan, N. Huneeus, S. Kinne, G. Lin, X. Ma, G. Myhre, J. E. Penner, C. A. Randles, B. Samset, M. Schulz, T. Takemura, F. Yu, H. Yu, and C. Zhou
G. Myhre, B. H. Samset, M. Schulz, Y. Balkanski, S. Bauer, T. K. Berntsen, H. Bian, N. Bellouin, M. Chin, T. Diehl, R. C. Easter, J. Feichter, S. J. Ghan, D. Hauglustaine, T. Iversen, S. Kinne, A. Kirkevåg, J.-F. Lamarque, G. Lin, X. Liu, M. T. Lund, G. Luo, X. Ma, T. van Noije, J. E. Penner, P. J. Rasch, A. Ruiz, Ø. Seland, R. B. Skeie, P. Stier, T. Takemura, K. Tsigaridis, P. Wang, Z. Wang, L. Xu, H. Yu, F. Yu, J.-H. Yoon, K. Zhang, H. Zhang, and C. Zhou
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