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.
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
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.
Wing Y. Tuet, Yunle Chen, Lu Xu, Shierly Fok, Dong Gao, Rodney J. Weber, and Nga L. Ng
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.
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
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.
Michael R. Giordano, Lars E. Kalnajs, Anita Avery, J. Douglas Goetz, Sean M. Davis, and Peter F. DeCarlo
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.
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
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.
Joel D. Rindelaub, Carlos H. Borca, Matthew A. Hostetler, Jonathan H. Slade, Mark A. Lipton, Lyudmila V. Slipchenko, and Paul B. Shepson
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.
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 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.
Debra Wunch, Geoffrey C. Toon, Jacob K. Hedelius, Nicholas Vizenor, Coleen M. Roehl, Katherine M. Saad, Jean-François L. Blavier, Donald R. Blake, and Paul O. Wennberg
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.
Alexis A. Shusterman, Virginia E. Teige, Alexander J. Turner, Catherine Newman, Jinsol Kim, and Ronald C. Cohen
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.
Jiumeng Liu, Peng Lin, Alexander Laskin, Julia Laskin, Shawn M. Kathmann, Matthew Wise, Ryan Caylor, Felisha Imholt, Vanessa Selimovic, and John E. Shilling
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.
Pascal Renard, Isabelle Canet, Martine Sancelme, Nolwenn Wirgot, Laurent Deguillaume, and Anne-Marie Delort
This paper presents an analysis of unusually long and continuous time series (82 yrs) of visibility in a urban environment, namely Athens. Visibility is shown to be a good proxy to follow the evolution of particulate pollution in the long-term in the absence of direct aerosol measurements that can be compared only over the most recent period. The paper shows interesting evolutions related to the socio-economic local history and, by comparison to a distant island site, demonstrates the major control of large-scale conditions on the aerosol load even in a large and densely populated urban environment.
D. Founda, S. Kazadzis, N. Mihalopoulos, E. Gerasopoulos, M. Lianou, and P. I. Raptis
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.
Z. Z. Kapadia, D. V. Spracklen, S. R. Arnold, D. J. Borman, G. W. Mann, K. J. Pringle, S. A. Monks, C. L. Reddington, F. Benduhn, A. Rap, C. E. Scott, E. W. Butt, and M. Yoshioka
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.
J. J. Harrison, M. P. Chipperfield, C. D. Boone, S. S. Dhomse, P. F. Bernath, L. Froidevaux, J. Anderson, and J. Russell III
Three 30-year simulations of past atmospheric composition changes were performed using different anthropogenic emissions of pollutants accounting or not for the applied air quality legislation and accounting for the year–to–year observed climate and natural emissions variability. The actual benefit of applied legislation along with technological advances is higher than what is usually calculated by a simple comparison of today's atmosphere against a constant anthropogenic emissions simulation.
N. Daskalakis, K. Tsigaridis, S. Myriokefalitakis, G. S. Fanourgakis, and M. Kanakidou
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.
M. D. Willis, J. Burkart, J. L. Thomas, F. Köllner, J. Schneider, H. Bozem, P. M. Hoor, A. A. Aliabadi, H. Schulz, A. B. Herber, W. R. Leaitch, and J. P. D. Abbatt
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.
N. A. J. Schutgens, E. Gryspeerdt, N. Weigum, S. Tsyro, D. Goto, M. Schulz, and P. Stier
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.
N. A. Krotkov, C. A. McLinden, C. Li, L. N. Lamsal, E. A. Celarier, S. V. Marchenko, W. H. Swartz, E. J. Bucsela, J. Joiner, B. N. Duncan, K. F. Boersma, J. P. Veefkind, P. F. Levelt, V. E. Fioletov, R. R. Dickerson, H. He, Z. Lu, and D. G. Streets
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.
L. M. T. Joelsson, J. A. Schmidt, E. J. K. Nilsson, T. Blunier, D. W. T. Griffith, S. Ono, and M. S. Johnson
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.
P. J. Nowack, N. L. Abraham, P. Braesicke, and J. A. Pyle
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.
J. Hansen, M. Sato, P. Hearty, R. Ruedy, M. Kelley, V. Masson-Delmotte, G. Russell, G. Tselioudis, J. Cao, E. Rignot, I. Velicogna, B. Tormey, B. Donovan, E. Kandiano, K. von Schuckmann, P. Kharecha, A. N. Legrande, M. Bauer, and K.-W. Lo
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.
Y. Zhao, L. M. Wingen, V. Perraud, and B. J. Finlayson-Pitts
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.
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
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.
E. D. Sofen, M. J. Evans, and A. C. Lewis
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.
S. P. Burton, J. W. Hair, M. Kahnert, R. A. Ferrare, C. A. Hostetler, A. L. Cook, D. B. Harper, T. A. Berkoff, S. T. Seaman, J. E. Collins, M. A. Fenn, and R. R. Rogers
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).
Y. B. Lim and B. J. Turpin
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.
A. G. Feofilov, C. J. Stubenrauch, and J. Delanoë
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.
D. Liu, B. Quennehen, E. Darbyshire, J. D. Allan, P. I. Williams, J. W. Taylor, S. J.-B. Bauguitte, M. J. Flynn, M. W. Gallagher, K. N. Bower, T. W. Choularton, and H. Coe
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.
Y. Fu and A. P. K. Tai
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.
R. E. Dunmore, J. R. Hopkins, R. T. Lidster, J. D. Lee, M. J. Evans, A. R. Rickard, A. C. Lewis, and J. F. Hamilton
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.
N. R. P. Harris, B. Hassler, F. Tummon, G. E. Bodeker, D. Hubert, I. Petropavlovsikh, 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. Kyrola, M. Laine, S. T. Leblanc, J. C. Lambert, E. Mahieu, A. Maycock, M. de Maziere, A. Parrish, R. Querel, K. H. Rosenlof, C. Roth, C. Sioris, B. Liley, J. Staehelin, R. S. Stolarski, R. Stubi, J. Tamminen, C. Vigouroux, K. A. Walker, H. J. Wang, J. Wild, and J. M. Zawodny
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.
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
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.
K. P. Wyche, P. S. Monks, K. L. Smallbone, J. F. Hamilton, M. R. Alfarra, A. R. Rickard, G. B. McFiggans, M. E. Jenkin, W. J. Bloss, A. C. Ryan, C. N. Hewitt, and A. R. MacKenzie
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.
I. C. Prentice, X. Liang, B. E. Medlyn, and Y.-P. Wang
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.
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
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.
E. K. Bigg, S. Soubeyrand, and C. E. Morris
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.
L. E. Hatch, W. Luo, J. F. Pankow, R. J. Yokelson, C. E. Stockwell, and K. C. Barsanti
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.
S. J. Lawson, P. W. Selleck, I. E. Galbally, M. D. Keywood, M. J. Harvey, C. Lerot, D. Helmig, and Z. Ristovski
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.
D. S. Ward, N. M. Mahowald, and S. Kloster