Articles | Volume 18, issue 11
Atmos. Chem. Phys., 18, 7757–7780, 2018
© Author(s) 2018. This work is distributed under
the Creative Commons Attribution 4.0 License.
the Creative Commons Attribution 4.0 License.
04 Jun 2018
Research article | 04 Jun 2018
Stable sulfur isotope measurements to trace the fate of SO2 in the Athabasca oil sands region
Neda Amiri et al.
No articles found.
Kevin Douglas Easterbrook, Mitchell Anthony Vona, Kiana Nayebi-Astaneh, Amanda McKenzie Miller, and Hans Dieter Osthoff
Atmos. Chem. Phys. Discuss.,
Preprint under review for ACPShort summary
The trace gas peroxypropionyl nitrate (PPN) is generated in photochemical smog, phytotoxic, a strong eye irritant, and possibly mutagenic. Here, its solubility and reactivity in water and in octanol was investigated using a bubble flow apparatus, yielding its Henry's law constant and octanol-water partition coefficient (Kow). The results allow the fate of PPN to be more accurately constrained in atmospheric chemical transport models, including its uptake on clouds, organic aerosol, and leaves.
Nicholas J. Gingerysty and Hans D. Osthoff
Atmos. Meas. Tech., 13, 4159–4167,Short summary
The generation of clean calibration gases is critical for accurate ambient air measurements. Here, we describe a source of HONO vapour dynamically generated from reaction of HCl and NaNO2. The output was characterized by Fourier transform infrared (FTIR) and thermal-dissociation cavity ring-down spectroscopy (TD-CRDS) and was stable, tuneable, and > 95 % pure. We show how generation of unwanted side products (NO, NO2, and ClNO) can be avoided.
Zoë Y. W. Davis, Udo Frieß, Kevin B. Strawbridge, Monika Aggarwaal, Sabour Baray, Elijah G. Schnitzler, Akshay Lobo, Vitali E. Fioletov, Ihab Abboud, Chris A. McLinden, Jim Whiteway, Megan D. Willis, Alex K. Y. Lee, Jeff Brook, Jason Olfert, Jason O'Brien, Ralf Staebler, Hans D. Osthoff, Cristian Mihele, and Robert McLaren
Atmos. Meas. Tech., 13, 1129–1155,Short summary
Here, we evaluate a ground-based remote sensing method (MAX-DOAS) for measuring total pollutant loading and vertical profiles of pollution in the lower atmosphere by comparing our method to a variety of other measurement methods (lidar, sunphotometer, active DOAS, and aircraft measurements). Measurements were made in the Athabasca Oil Sands Region in Alberta, Canada. The complex dataset provided a rare opportunity to evaluate the performance of MAX-DOAS under varying atmospheric conditions.
Nick Jordan and Hans D. Osthoff
Atmos. Meas. Tech., 13, 273–285,Short summary
We describe a new spectrometer for quantification of HONO and NO2 in ambient air, called HODOR. The instrument uses an LED and two highly reflective mirrors to increase the effective optical absorption path to ~6 km. The accuracy of concentration retrievals was validated using parallel measurements by a single wavelength cavity ring-down spectrometer of laboratory-generated gas mixtures. The instrument's precision suffices for quantification of HONO and NO2 in an urban environment.
Roya Ghahreman, Wanmin Gong, Martí Galí, Ann-Lise Norman, Stephen R. Beagley, Ayodeji Akingunola, Qiong Zheng, Alexandru Lupu, Martine Lizotte, Maurice Levasseur, and W. Richard Leaitch
Atmos. Chem. Phys., 19, 14455–14476,Short summary
Atmospheric DMS(g) is a climatically important compound and the main source of biogenic sulfate in the Arctic. Its abundance in the Arctic increases during summer due to greater ice-free sea surface and higher biological activity. In this study, we implemented DMS(g) in a regional air quality forecast model configured for the Arctic. The study showed a significant impact from DMS(g) on sulfate aerosols, particularly in the 50–100 nm size range, in the Arctic marine boundary layer during summer.
Alex K. Y. Lee, Max G. Adam, John Liggio, Shao-Meng Li, Kun Li, Megan D. Willis, Jonathan P. D. Abbatt, Travis W. Tokarek, Charles A. Odame-Ankrah, Hans D. Osthoff, Kevin Strawbridge, and Jeffery R. Brook
Atmos. Chem. Phys., 19, 12209–12219,Short summary
This work provides the first direct field evidence that anthropogenic organo-nitrate contributed up to half of secondary organic aerosol (SOA) mass that was freshly produced within the emission plumes of oil sands facilities in Alberta, Canada. The findings illustrate the central role of organo-nitrate in SOA production from the oil and gas industry, with relevance for other urban and industrial regions with significant intermediate-volatility organic compounds (IVOCs) and NOx emissions.
Rashed Mahmood, Knut von Salzen, Ann-Lise Norman, Martí Galí, and Maurice Levasseur
Atmos. Chem. Phys., 19, 6419–6435,Short summary
This study evaluates impacts of surface seawater dimethylsulfide on Arctic sulfate aerosol budget, changes in cloud droplet number concentration (CDNC), and cloud radiative forcing under current and future sea ice conditions using an atmospheric global climate model. In the future, sulfate wet removal efficiency is increased by enhanced precipitation; however, simulated aerosol nucleation rates are higher, which result in an overall increase in CDNC and negative cloud radiative forcing.
Jonathan P. D. Abbatt, W. Richard Leaitch, Amir A. Aliabadi, Allan K. Bertram, Jean-Pierre Blanchet, Aude Boivin-Rioux, Heiko Bozem, Julia Burkart, Rachel Y. W. Chang, Joannie Charette, Jai P. Chaubey, Robert J. Christensen, Ana Cirisan, Douglas B. Collins, Betty Croft, Joelle Dionne, Greg J. Evans, Christopher G. Fletcher, Martí Galí, Roya Ghahreman, Eric Girard, Wanmin Gong, Michel Gosselin, Margaux Gourdal, Sarah J. Hanna, Hakase Hayashida, Andreas B. Herber, Sareh Hesaraki, Peter Hoor, Lin Huang, Rachel Hussherr, Victoria E. Irish, Setigui A. Keita, John K. Kodros, Franziska Köllner, Felicia Kolonjari, Daniel Kunkel, Luis A. Ladino, Kathy Law, Maurice Levasseur, Quentin Libois, John Liggio, Martine Lizotte, Katrina M. Macdonald, Rashed Mahmood, Randall V. Martin, Ryan H. Mason, Lisa A. Miller, Alexander Moravek, Eric Mortenson, Emma L. Mungall, Jennifer G. Murphy, Maryam Namazi, Ann-Lise Norman, Norman T. O'Neill, Jeffrey R. Pierce, Lynn M. Russell, Johannes Schneider, Hannes Schulz, Sangeeta Sharma, Meng Si, Ralf M. Staebler, Nadja S. Steiner, Jennie L. Thomas, Knut von Salzen, Jeremy J. B. Wentzell, Megan D. Willis, Gregory R. Wentworth, Jun-Wei Xu, and Jacqueline D. Yakobi-Hancock
Atmos. Chem. Phys., 19, 2527–2560,Short summary
The Arctic is experiencing considerable environmental change with climate warming, illustrated by the dramatic decrease in sea-ice extent. It is important to understand both the natural and perturbed Arctic systems to gain a better understanding of how they will change in the future. This paper summarizes new insights into the relationships between Arctic aerosol particles and climate, as learned over the past five or so years by a large Canadian research consortium, NETCARE.
Nick Jordan, Connie Z. Ye, Satyaki Ghosh, Rebecca A. Washenfelder, Steven S. Brown, and Hans D. Osthoff
Atmos. Meas. Tech., 12, 1277–1293,Short summary
A new spectrometer to measure abundances of the atmospheric trace gases nitrogen dioxide and iodine is described. The spectrometer uses a light-emitting diode between 470 and 540 nm and two highly reflective mirrors to yield an effective absorption path of 6.3 km. We remeasured scattering cross sections of common atmospheric gases in the cyan region and present sample NO2 measurements that agreed with those made with a laser-based instrument.
Travis W. Tokarek, Charles A. Odame-Ankrah, Jennifer A. Huo, Robert McLaren, Alex K. Y. Lee, Max G. Adam, Megan D. Willis, Jonathan P. D. Abbatt, Cristian Mihele, Andrea Darlington, Richard L. Mittermeier, Kevin Strawbridge, Katherine L. Hayden, Jason S. Olfert, Elijah G. Schnitzler, Duncan K. Brownsey, Faisal V. Assad, Gregory R. Wentworth, Alex G. Tevlin, Douglas E. J. Worthy, Shao-Meng Li, John Liggio, Jeffrey R. Brook, and Hans D. Osthoff
Atmos. Chem. Phys., 18, 17819–17841,Short summary
Measurements of air pollutants at a ground site near Fort McKay in the Athabasca oil sands region in the summer of 2013 are presented. A large number of intermediate-volatility organic compounds (IVOCs) were observed; these molecules were shown previously to generate atmospheric particles downwind of the region. A principal component analysis was performed to identify major pollution source types, including which source(s) is(are) associated with IVOC emissions (e.g., freshly mined bitumen).
Youssef M. Taha, Matthew T. Saowapon, Faisal V. Assad, Connie Z. Ye, Xining Chen, Natasha M. Garner, and Hans D. Osthoff
Atmos. Meas. Tech., 11, 4109–4127,Short summary
Nitrogen oxides are commonly measured by selective thermal dissociation (TD) to NO2, which can be quantified by optical absorption. Quantification of peroxynitrates (RO2NO2) by TD methods, however, is challenging in ambient air since NO2 is usually more abundant than RO2NO2. Here, a method to boost the sensitivity of TD instruments by chemical amplification following addition of ~ 1 % ethane and ~ 1 ppm NO to the inlet is presented. Advantages and disadvantages of the new method are discussed.
Hans D. Osthoff, Charles A. Odame-Ankrah, Youssef M. Taha, Travis W. Tokarek, Corinne L. Schiller, Donna Haga, Keith Jones, and Roxanne Vingarzan
Atmos. Chem. Phys., 18, 6293–6315,Short summary
The nocturnal nitrogen oxides dinitrogen pentoxide (N2O5) and its heterogeneous uptake product nitryl chloride (ClNO2) can have profound impacts on air quality, yet their abundances and chemistry are only sparsely constrained by field measurements. Here, we present the first measurements of N2O5 and ClNO2 in the Lower Fraser Valley of British Columbia, Canada. Concentrations were lower than have been observed elsewhere. Morning peaks indicate higher ClNO2 production above the measurement site.
Roya Ghahreman, Ann-Lise Norman, Betty Croft, Randall V. Martin, Jeffrey R. Pierce, Julia Burkart, Ofelia Rempillo, Heiko Bozem, Daniel Kunkel, Jennie L. Thomas, Amir A. Aliabadi, Gregory R. Wentworth, Maurice Levasseur, Ralf M. Staebler, Sangeeta Sharma, and W. Richard Leaitch
Atmos. Chem. Phys., 17, 8757–8770,Short summary
We present spring and summertime vertical profile measurements of Arctic dimethyl sulfide (DMS), together with model simulations to consider what these profiles indicate about DMS sources and lifetimes in the Arctic. Our results highlight the role of local open water as the source of DMS(g) during July 2014 and the influence of long-range transport of DMS(g) from further afield in the Arctic during April 2015.
Nga Lee Ng, Steven S. Brown, Alexander T. Archibald, Elliot Atlas, Ronald C. Cohen, John N. Crowley, Douglas A. Day, Neil M. Donahue, Juliane L. Fry, Hendrik Fuchs, Robert J. Griffin, Marcelo I. Guzman, Hartmut Herrmann, Alma Hodzic, Yoshiteru Iinuma, José L. Jimenez, Astrid Kiendler-Scharr, Ben H. Lee, Deborah J. Luecken, Jingqiu Mao, Robert McLaren, Anke Mutzel, Hans D. Osthoff, Bin Ouyang, Benedicte Picquet-Varrault, Ulrich Platt, Havala O. T. Pye, Yinon Rudich, Rebecca H. Schwantes, Manabu Shiraiwa, Jochen Stutz, Joel A. Thornton, Andreas Tilgner, Brent J. Williams, and Rahul A. Zaveri
Atmos. Chem. Phys., 17, 2103–2162,Short summary
Oxidation of biogenic volatile organic compounds by NO3 is an important interaction between anthropogenic and natural emissions. This review results from a June 2015 workshop and includes the recent literature on kinetics, mechanisms, organic aerosol yields, and heterogeneous chemistry; advances in analytical instrumentation; the current state NO3-BVOC chemistry in atmospheric models; and critical needs for future research in modeling, field observations, and laboratory studies.
Brian M. Lerner, Jessica B. Gilman, Kenneth C. Aikin, Elliot L. Atlas, Paul D. Goldan, Martin Graus, Roger Hendershot, Gabriel A. Isaacman-VanWertz, Abigail Koss, William C. Kuster, Richard A. Lueb, Richard J. McLaughlin, Jeff Peischl, Donna Sueper, Thomas B. Ryerson, Travis W. Tokarek, Carsten Warneke, Bin Yuan, and Joost A. de Gouw
Atmos. Meas. Tech., 10, 291–313,Short summary
Whole air sampling followed by analysis by gas chromatography is a common technique for characterization of trace volatile organic compounds in the atmosphere. We describe a new automated gas chromatograph–mass spectrograph which uses a Stirling cooler for sample preconcentration at −165 °C without the need for a cryogen such as liquid nitrogen. We also discuss potential sources of artifacts from our electropolished stainless steel sampling system and present results from two field campaigns.
Maria Zatko, Joseph Erbland, Joel Savarino, Lei Geng, Lauren Easley, Andrew Schauer, Timothy Bates, Patricia K. Quinn, Bonnie Light, David Morison, Hans D. Osthoff, Seth Lyman, William Neff, Bin Yuan, and Becky Alexander
Atmos. Chem. Phys., 16, 13837–13851,Short summary
This manuscript presents chemical and optical observations collected in the air and snow during UBWOS2014 in eastern Utah. These observations are used to calculate fluxes of reactive nitrogen associated with snow nitrate photolysis. Snow-sourced reactive nitrogen fluxes are compared to reactive nitrogen emission inventories to find that snow-sourced reactive nitrogen is a minor contributor to the reactive nitrogen budget, and thus wintertime ground-level ozone formation, in the Uintah Basin.
Roghayeh Ghahremaninezhad, Ann-Lise Norman, Jonathan P. D. Abbatt, Maurice Levasseur, and Jennie L. Thomas
Atmos. Chem. Phys., 16, 5191–5202,Short summary
Aerosols in six size fractions (> 0.49–7.0 microns) were collected in the Arctic (July 2014). The isotopic composition of sulfate aerosols was measured to determine the role of biogenic and anthropogenic sources in the growth of aerosols. More than 63 % of the average sulfate concentration in the fine aerosols (> 0.49 microns) was from biogenic sources. For some samples, the S isotope ratio values for SO2 and fine aerosols were close together, suggesting the same source for SO2 and aerosol sulfur.
Bin Yuan, John Liggio, Jeremy Wentzell, Shao-Meng Li, Harald Stark, James M. Roberts, Jessica Gilman, Brian Lerner, Carsten Warneke, Rui Li, Amy Leithead, Hans D. Osthoff, Robert Wild, Steven S. Brown, and Joost A. de Gouw
Atmos. Chem. Phys., 16, 2139–2153,Short summary
We describe high-resolution measurements of nitrated phenols using a time-of-flight chemical ionization mass spectrometer (ToF-CIMS). Strong diurnal profiles were observed for nitrated phenols, with concentration maxima at night. Box model simulations were able to reproduce the measured nitrated phenols.
N. D. Rider, Y. M. Taha, C. A. Odame-Ankrah, J. A. Huo, T. W. Tokarek, E. Cairns, S. G. Moussa, J. Liggio, and H. D. Osthoff
Atmos. Meas. Tech., 8, 2737–2748,Short summary
A photochemical source of peroxycarboxylic nitric anhydrides (PANs) in which a dialkyl ketone (acetone, diethyl-, di-isopropyl, or di-n-propyl ketone) in the presence of oxygen and nitric oxide is photodissociated by arrays of ultraviolet light-emitting diodes (UV-LEDs) is described. The source output was analyzed by gas chromatography and thermal dissociation cavity ring-down spectroscopy and modeled using the Master Chemical Mechanism.
T. W. Tokarek, J. A. Huo, C. A. Odame-Ankrah, D. Hammoud, Y. M. Taha, and H. D. Osthoff
Atmos. Meas. Tech., 7, 3263–3283,
C. J. Young, R. A. Washenfelder, P. M. Edwards, D. D. Parrish, J. B. Gilman, W. C. Kuster, L. H. Mielke, H. D. Osthoff, C. Tsai, O. Pikelnaya, J. Stutz, P. R. Veres, J. M. Roberts, S. Griffith, S. Dusanter, P. S. Stevens, J. Flynn, N. Grossberg, B. Lefer, J. S. Holloway, J. Peischl, T. B. Ryerson, E. L. Atlas, D. R. Blake, and S. S. Brown
Atmos. Chem. Phys., 14, 3427–3440,
Related subject area
Subject: Isotopes | Research Activity: Field Measurements | Altitude Range: Troposphere | Science Focus: Chemistry (chemical composition and reactions)Atmospheric methane isotopes identify inventory knowledge gaps in the Surat Basin, Australia, coal seam gas and agricultural regionsPhotolytic modification of seasonal nitrate isotope cycles in East AntarcticaMethane (CH4) sources in Krakow, Poland: insights from isotope analysisIsotopic signatures of major methane sources in the coal seam gas fields and adjacent agricultural districts, Queensland, AustraliaMeasurement report: Nitrogen isotopes (δ15N) and first quantification of oxygen isotope anomalies (Δ17O, δ18O) in atmospheric nitrogen dioxideMeasurement report: Spatial variability of northern Iberian rainfall stable isotope values – investigating atmospheric controls on daily and monthly timescalesIsotopic constraints on atmospheric sulfate formation pathways in the Mt. Everest region, southern Tibetan PlateauBaffin Bay sea ice extent and synoptic moisture transport drive water vapor isotope (δ18O, δ2H, and deuterium excess) variability in coastal northwest GreenlandNew evidence for atmospheric mercury transformations in the marine boundary layer from stable mercury isotopesThe isotopic composition of atmospheric nitrous oxide observed at the high-altitude research station Jungfraujoch, SwitzerlandDeposition, recycling, and archival of nitrate stable isotopes between the air–snow interface: comparison between Dronning Maud Land and Dome C, AntarcticaOxygen and sulfur mass-independent isotopic signatures in black crusts: the complementary negative Δ33S reservoir of sulfate aerosols?Atmospheric radiocarbon measurements to quantify CO2 emissions in the UK from 2014 to 2015An improved estimate for the δ13C and δ18O signatures of carbon monoxide produced from atmospheric oxidation of volatile organic compoundsSeasonality in the Δ33S measured in urban aerosols highlights an additional oxidation pathway for atmospheric SO2The Δ17O and δ18O values of atmospheric nitrates simultaneously collected downwind of anthropogenic sources – implications for polluted air massesA very limited role of tropospheric chlorine as a sink of the greenhouse gas methaneDetection and variability of combustion-derived vapor in an urban basinTriple oxygen isotopes indicate urbanization affects sources of nitrate in wet and dry atmospheric depositionIsotopic constraints on heterogeneous sulfate production in Beijing hazeEstimation of the fossil fuel component in atmospheric CO2 based on radiocarbon measurements at the Beromünster tall tower, SwitzerlandConstraining N2O emissions since 1940 using firn air isotope measurements in both hemispheresSeasonal variations of triple oxygen isotopic compositions of atmospheric sulfate, nitrate, and ozone at Dumont d'Urville, coastal AntarcticaCarbon isotopic signature of coal-derived methane emissions to the atmosphere: from coalification to alterationIsotopic composition for source identification of mercury in atmospheric fine particlesIsotopic constraints on the role of hypohalous acids in sulfate aerosol formation in the remote marine boundary layerIn situ observations of the isotopic composition of methane at the Cabauw tall tower siteOxygen isotope mass balance of atmospheric nitrate at Dome C, East Antarctica, during the OPALE campaignIsotopic effects of nitrate photochemistry in snow: a field study at Dome C, AntarcticaStable carbon isotope ratios of ambient secondary organic aerosols in TorontoWAIS Divide ice core suggests sustained changes in the atmospheric formation pathways of sulfate and nitrate since the 19th century in the extratropical Southern HemisphereStable carbon isotope ratios of toluene in the boundary layer and the lower free troposphereEmission ratio and isotopic signatures of molecular hydrogen emissions from tropical biomass burningCan the carbon isotopic composition of methane be reconstructed from multi-site firn air measurements?Air–snow transfer of nitrate on the East Antarctic Plateau – Part 1: Isotopic evidence for a photolytically driven dynamic equilibrium in summerChemical characterization and stable carbon isotopic composition of particulate Polycyclic Aromatic Hydrocarbons issued from combustion of 10 Mediterranean woodsQuantification of the carbonaceous matter origin in submicron marine aerosol by 13C and 14C isotope analysisTemporal and spatial variability of the stable isotopic composition of atmospheric molecular hydrogen: observations at six EUROHYDROS stationsContinuous isotopic composition measurements of tropospheric CO2 at Jungfraujoch (3580 m a.s.l.), Switzerland: real-time observation of regional pollution eventsAnthropogenic imprints on nitrogen and oxygen isotopic composition of precipitation nitrate in a nitrogen-polluted city in southern ChinaAnalysis of 13C and 18O isotope data of CO2 in CARIBIC aircraft samples as tracers of upper troposphere/lower stratosphere mixing and the global carbon cycleTracing the fate of atmospheric nitrate deposited onto a forest ecosystem in Eastern Asia using Δ17OPhotolysis imprint in the nitrate stable isotope signal in snow and atmosphere of East Antarctica and implications for reactive nitrogen cyclingSources and transport of Δ14C in CO2 within the Mexico City Basin and vicinity
Bryce F. J. Kelly, Xinyi Lu, Stephen J. Harris, Bruno G. Neininger, Jorg M. Hacker, Stefan Schwietzke, Rebecca E. Fisher, James L. France, Euan G. Nisbet, David Lowry, Carina van der Veen, Malika Menoud, and Thomas Röckmann
Atmos. Chem. Phys. Discuss.,
Revised manuscript accepted for ACPShort summary
This study explores using the composition of methane of in-flight atmospheric air samples for greenhouse gas inventory verification. The air samples were collected above one of the largest coal seam gas production regions in the world. Adjacent to these gas fields are coal mines, Australia's largest cattle feedlot and over a million grazing cattle. The results are also used to identify methane mitigation opportunities.
Pete D. Akers, Joël Savarino, Nicolas Caillon, Olivier Magand, and Emmanuel Le Meur
Nitrate in Antarctic ice cores could be used to reconstruct past atmospheric conditions, but nitrate isotopes in deep ice are greatly altered from the seasonal nitrate cycles in the atmosphere. We sampled nitrate along an 850 km Antarctic transect that better preserves the atmospheric cycles. This shows that the degree of the isotopic transformation is related to snow accumulation rate, and nitrate isotopes can potentially reconstruct past changes in snowfall if sampled properly.
Malika Menoud, Carina van der Veen, Jaroslaw Necki, Jakub Bartyzel, Barbara Szénási, Mila Stanisavljević, Isabelle Pison, Philippe Bousquet, and Thomas Röckmann
Atmos. Chem. Phys., 21, 13167–13185,Short summary
Using measurements of methane isotopes in ambient air and a 3D atmospheric transport model, in Krakow, Poland, we mainly detected fossil-fuel-related sources, coming from coal mining in Silesia and from the use of natural gas in the city. Emission inventories report large emissions from coal mine activity in Silesia, which is in agreement with our measurements. However, methane sources in the urban area of Krakow related to the use of fossil fuels might be underestimated in the inventories.
Xinyi Lu, Stephen J. Harris, Rebecca E. Fisher, James L. France, Euan G. Nisbet, David Lowry, Thomas Röckmann, Carina van der Veen, Malika Menoud, Stefan Schwietzke, and Bryce F. J. Kelly
Atmos. Chem. Phys., 21, 10527–10555,Short summary
Many coal seam gas (CSG) facilities in the Surat Basin, Australia, are adjacent to other sources of methane, including agricultural, urban, and natural seeps. This makes it challenging to estimate the amount of methane being emitted into the atmosphere from CSG facilities. This research demonstrates that measurements of the carbon and hydrogen stable isotopic composition of methane can distinguish between and apportion methane emissions from CSG facilities, cattle, and many other sources.
Sarah Albertin, Joël Savarino, Slimane Bekki, Albane Barbero, and Nicolas Caillon
Atmos. Chem. Phys., 21, 10477–10497,Short summary
We report an efficient method to collect atmospheric NO2 adapted for multi-isotopic analysis and present the first NO2 triple oxygen and double nitrogen isotope measurements. Atmospheric samplings carried out in Grenoble, France, highlight the NO2 isotopic signature sensitivity to the local NOx emissions and chemical regimes. These preliminary results are very promising for using the combination of Δ17O and δ15N of NO2 as a probe of the atmospheric NOx emissions and chemistry.
Ana Moreno, Miguel Iglesias, Cesar Azorin-Molina, Carlos Pérez-Mejías, Miguel Bartolomé, Carlos Sancho, Heather Stoll, Isabel Cacho, Jaime Frigola, Cinta Osácar, Arsenio Muñoz, Antonio Delgado-Huertas, Ileana Bladé, and Françoise Vimeux
Atmos. Chem. Phys., 21, 10159–10177,Short summary
We present a large and unique dataset of the rainfall isotopic composition at seven sites from northern Iberia to characterize their variability at daily and monthly timescales and to assess the role of climate and geographic factors in the modulation of δ18O values. We found that the origin, moisture uptake along the trajectory and type of precipitation play a key role. These results will help to improve the interpretation of δ18O paleorecords from lacustrine carbonates or speleothems.
Kun Wang, Shohei Hattori, Mang Lin, Sakiko Ishino, Becky Alexander, Kazuki Kamezaki, Naohiro Yoshida, and Shichang Kang
Atmos. Chem. Phys., 21, 8357–8376,Short summary
Sulfate aerosols play an important climatic role and exert adverse effects on the ecological environment and human health. In this study, we present the triple oxygen isotopic composition of sulfate from the Mt. Everest region, southern Tibetan Plateau, and decipher the formation mechanisms of atmospheric sulfate in this pristine environment. The results indicate the important role of the S(IV) + O3 pathway in atmospheric sulfate formation promoted by conditions of high cloud water pH.
Pete D. Akers, Ben G. Kopec, Kyle S. Mattingly, Eric S. Klein, Douglas Causey, and Jeffrey M. Welker
Atmos. Chem. Phys., 20, 13929–13955,Short summary
Water vapor isotopes recorded for 2 years in coastal northern Greenland largely reflect changes in sea ice cover, with distinct values when Baffin Bay is ice covered in winter vs. open in summer. Resulting changes in moisture transport, surface winds, and air temperature also modify the isotopes. Local glacial ice may thus preserve past changes in the Baffin Bay sea ice extent, and this will help us better understand how the Arctic environment and water cycle responds to global climate change.
Ben Yu, Lin Yang, Linlin Wang, Hongwei Liu, Cailing Xiao, Yong Liang, Qian Liu, Yongguang Yin, Ligang Hu, Jianbo Shi, and Guibin Jiang
Atmos. Chem. Phys., 20, 9713–9723,Short summary
We found that Br atoms in the marine boundary layer are the most probable oxidizer that transform gaseous elemental mercury into gaseous oxidized mercury, according to the mercury isotopes in the total gaseous mercury. On the other hand, Br or Cl atoms are not the primary oxidizers that produced oxidized mercury on particles. This study showed that mercury isotopes can provide new evidence that help us to fully understand the transformations of atmospheric mercury.
Longfei Yu, Eliza Harris, Stephan Henne, Sarah Eggleston, Martin Steinbacher, Lukas Emmenegger, Christoph Zellweger, and Joachim Mohn
Atmos. Chem. Phys., 20, 6495–6519,Short summary
We observed the isotopic composition of nitrous oxide in the unpolluted air at Jungfraujoch for 5 years. Our results indicate a clear seasonal pattern in the isotopic composition, corresponding with that in atmospheric nitrous oxide levels. This is most likely due to temporal variations in both emission processes and air mass sources for Jungfraujoch. Our findings are of importance to global nitrous oxide modelling and to better understanding of long-term trends in atmospheric nitrous oxide.
V. Holly L. Winton, Alison Ming, Nicolas Caillon, Lisa Hauge, Anna E. Jones, Joel Savarino, Xin Yang, and Markus M. Frey
Atmos. Chem. Phys., 20, 5861–5885,Short summary
The transfer of the nitrogen stable isotopic composition in nitrate between the air and snow at low accumulation sites in Antarctica leaves an UV imprint in the snow. Quantifying how nitrate isotope values change allows us to interpret longer ice core records. Based on nitrate observations and modelling at Kohnen, East Antarctica, the dominant factors controlling the nitrate isotope signature in deep snow layers are the depth of light penetration into the snowpack and the snow accumulation rate.
Isabelle Genot, David Au Yang, Erwan Martin, Pierre Cartigny, Erwann Legendre, and Marc De Rafelis
Atmos. Chem. Phys., 20, 4255–4273,Short summary
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.
Angelina Wenger, Katherine Pugsley, Simon O'Doherty, Matt Rigby, Alistair J. Manning, Mark F. Lunt, and Emily D. White
Atmos. Chem. Phys., 19, 14057–14070,Short summary
We present 14CO2 observations at a background site in Ireland and a tall tower site in the UK. These data have been used to calculate the contribution of fossil fuel sources to atmospheric CO2 mole fractions from the UK and Ireland. 14CO2 emissions from nuclear industry sites in the UK cause a higher uncertainty in the results compared to observations in other locations. The observed ffCO2 at the site was not significantly different from simulated values based on the bottom-up inventory.
Isaac J. Vimont, Jocelyn C. Turnbull, Vasilii V. Petrenko, Philip F. Place, Colm Sweeney, Natasha Miles, Scott Richardson, Bruce H. Vaughn, and James W. C. White
Atmos. Chem. Phys., 19, 8547–8562,Short summary
Stable isotopes of Carbon Monoxide (CO) and radiocarbon carbon dioxide were measured over three summers at Indianapolis, Indiana, US, and for 1 year at a site thought to be strongly influenced by CO from oxidized volatile organic compounds (VOCs) in South Carolina, US. The Indianapolis results were used to provide an estimate of the carbon and oxygen isotopic signatures of CO produced from oxidized VOCs. This updated estimate agrees well with the data from South Carolina during the summer.
David Au Yang, Pierre Cartigny, Karine Desboeufs, and David Widory
Atmos. Chem. Phys., 19, 3779–3796,Short summary
Sulfates present in urban aerosols collected worldwide usually exhibit 33S-anomalies whose origin remains unclear. Besides, the sulfate concentration is not very well modelled nowadays, which, coupled with the isotopic composition anomaly on the 33S, would highlight the presence of at least an additional oxidation pathway, different from O2+TMI, O3, OH, H2O2 and NO2. We suggest here the implication of two other possible oxidation pathways.
Martine M. Savard, Amanda S. Cole, Robert Vet, and Anna Smirnoff
Atmos. Chem. Phys., 18, 10373–10389,Short summary
Improving air quality requires understanding of the atmospheric processes transforming nitrous oxides emitted by human activities into nitrates, an N form that may degrade natural ecosystems. Isotopes (∆17O, δ18O) are characterized in separate wet, particulate and gaseous nitrates for the first time. The gas ranges are distinct from those of the other nitrates, and the plume dynamics emerge as crucial in interpreting the results, which unravel key processes behind the distribution of nitrates.
Sergey Gromov, Carl A. M. Brenninkmeijer, and Patrick Jöckel
Atmos. Chem. Phys., 18, 9831–9843,Short summary
Using the observational data on 13C (CO) and 13C (CH4) from the extra-tropical Southern Hemisphere (ETSH) and EMAC model we (1) provide an independent, observation-based evaluation of Cl atom concentration variations in the ETSH throughout 1994–2000, (2) show that the role of tropospheric Cl as a sink of CH4 is seriously overestimated in the literature, (3) demonstrate that the 13C/12C ratio of CO is a sensitive indicator for the isotopic composition of reacted CH4 and therefore for its sources.
Richard P. Fiorella, Ryan Bares, John C. Lin, James R. Ehleringer, and Gabriel J. Bowen
Atmos. Chem. Phys., 18, 8529–8547,Short summary
Fossil fuel combustion produces water; where fossil fuel combustion is concentrated in urban areas, this humidity source may represent ~ 10 % of total humidity. In turn, this water vapor addition may alter urban meteorology, though the contribution of combustion vapor is difficult to measure. Using stable water isotopes, we estimate that up to 16 % of urban humidity may arise from combustion when the atmosphere is stable during winter, and develop recommendations for application in other cities.
David M. Nelson, Urumu Tsunogai, Dong Ding, Takuya Ohyama, Daisuke D. Komatsu, Fumiko Nakagawa, Izumi Noguchi, and Takashi Yamaguchi
Atmos. Chem. Phys., 18, 6381–6392,Short summary
Atmospheric nitrate may be produced locally and/or come from upwind regions. To address this issue we measured oxygen and nitrogen isotopes of wet and dry nitrate deposition at nearby urban and rural sites. Our results suggest that, relative to nitrate in wet deposition in urban environments and wet and dry deposition in rural environments, nitrate in dry deposition in urban environments results from local NOx emissions more so than wet deposition, which is transported longer distances.
Pengzhen He, Becky Alexander, Lei Geng, Xiyuan Chi, Shidong Fan, Haicong Zhan, Hui Kang, Guangjie Zheng, Yafang Cheng, Hang Su, Cheng Liu, and Zhouqing Xie
Atmos. Chem. Phys., 18, 5515–5528,Short summary
We use observations of the oxygen isotopic composition of sulfate aerosol as a fingerprint to quantify various sulfate formation mechanisms during pollution events in Beijing, China. We found that heterogeneous reactions on aerosols dominated sulfate production in general; however, in-cloud reactions would dominate haze sulfate production when cloud liquid water content was high. The findings also suggest the heterogeneity of aerosol acidity should be parameterized in models.
Tesfaye A. Berhanu, Sönke Szidat, Dominik Brunner, Ece Satar, Rüdiger Schanda, Peter Nyfeler, Michael Battaglia, Martin Steinbacher, Samuel Hammer, and Markus Leuenberger
Atmos. Chem. Phys., 17, 10753–10766,Short summary
Fossil fuel CO2 is the major contributor of anthropogenic CO2 in the atmosphere, and accurate quantification is essential to better understand the carbon cycle. Such accurate quantification can be conducted based on radiocarbon measurements. In this study, we present radiocarbon measurements from a tall tower site in Switzerland. From these measurements, we have observed seasonally varying fossil fuel CO2 contributions and a biospheric CO2 component that varies diurnally and seasonally.
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
Atmos. Chem. Phys., 17, 4539–4564,Short summary
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.
Sakiko Ishino, Shohei Hattori, Joel Savarino, Bruno Jourdain, Susanne Preunkert, Michel Legrand, Nicolas Caillon, Albane Barbero, Kota Kuribayashi, and Naohiro Yoshida
Atmos. Chem. Phys., 17, 3713–3727,Short summary
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.
Giulia Zazzeri, Dave Lowry, Rebecca E. Fisher, James L. France, Mathias Lanoisellé, Bryce F. J. Kelly, Jaroslaw M. Necki, Charlotte P. Iverach, Elisa Ginty, Miroslaw Zimnoch, Alina Jasek, and Euan G. Nisbet
Atmos. Chem. Phys., 16, 13669–13680,Short summary
Methane emissions estimates from the coal sector are highly uncertain. Precise δ13C isotopic signatures of methane sources can be used in atmospheric models for a methane budget assessment. Emissions from both underground and opencast coal mines in the UK, Australia and Poland were sampled and isotopically characterised using high-precision measurements of δ13C values. Representative isotopic signatures were provided, taking into account specific ranks of coal and mine type.
Qiang Huang, Jiubin Chen, Weilin Huang, Pingqing Fu, Benjamin Guinot, Xinbin Feng, Lihai Shang, Zhuhong Wang, Zhongwei Wang, Shengliu Yuan, Hongming Cai, Lianfang Wei, and Ben Yu
Atmos. Chem. Phys., 16, 11773–11786,Short summary
Atmospheric airborne mercury is of particular concern because, once inhaled, both Hg and its vectors might have adverse effects on human beings. In this study, we attempted to identify the sources of PM2.5-Hg in Beijing, China, using Hg isotopic composition. Large range and seasonal variations in both mass-dependent and mass-independent fractionations of Hg isotopes in haze particles demonstrate the usefulness of Hg isotopes for directly tracing the sources and its vectors in the atmosphere.
Qianjie Chen, Lei Geng, Johan A. Schmidt, Zhouqing Xie, Hui Kang, Jordi Dachs, Jihong Cole-Dai, Andrew J. Schauer, Madeline G. Camp, and Becky Alexander
Atmos. Chem. Phys., 16, 11433–11450,Short summary
The formation mechanisms of sulfate in the marine boundary layer are not well understood, which could result in large uncertainties in aerosol radiative forcing. We measure the oxygen isotopic composition (Δ17O) of sulfate collected in the MBL and analyze with a global transport model. Our results suggest that 33–50 % of MBL sulfate is formed via oxidation of S(IV) by hypohalous acids HOBr / HOCl in the aqueous phase, and the daily-mean HOBr/HOCl concentrations are on the order of 0.01–0.1 ppt.
Thomas Röckmann, Simon Eyer, Carina van der Veen, Maria E. Popa, Béla Tuzson, Guillaume Monteil, Sander Houweling, Eliza Harris, Dominik Brunner, Hubertus Fischer, Giulia Zazzeri, David Lowry, Euan G. Nisbet, Willi A. Brand, Jaroslav M. Necki, Lukas Emmenegger, and Joachim Mohn
Atmos. Chem. Phys., 16, 10469–10487,Short summary
A dual isotope ratio mass spectrometric system (IRMS) and a quantum cascade laser absorption spectroscopy (QCLAS)-based technique were deployed at the Cabauw experimental site for atmospheric research (CESAR) in the Netherlands and performed in situ, high-frequency (approx. hourly) measurements for a period of more than 5 months, yielding a combined dataset with more than 2500 measurements of both δ13C and δD.
Joël Savarino, William C. Vicars, Michel Legrand, Suzanne Preunkert, Bruno Jourdain, Markus M. Frey, Alexandre Kukui, Nicolas Caillon, and Jaime Gil Roca
Atmos. Chem. Phys., 16, 2659–2673,Short summary
Atmospheric nitrate is collected on the East Antarctic ice sheet. Nitrogen and oxygen stable isotopes and concentrations of nitrate are measured. Using a box model, we show that there is s systematic discrepancy between observations and model results. We suggest that this discrepancy probably results from unknown NOx chemistry above the Antarctic ice sheet. However, possible misconception in the stable isotope mass balance is not completely excluded.
T. A. Berhanu, J. Savarino, J. Erbland, W. C. Vicars, S. Preunkert, J. F. Martins, and M. S. Johnson
Atmos. Chem. Phys., 15, 11243–11256,Short summary
In this field study at Dome C, Antarctica, we investigated the effect of solar UV photolysis on the stable isotopes of nitrate in snow via comparison of two identical snow pits while exposing only one to solar UV. From the difference between the average isotopic fractionations calculated for each pit, we determined a purely photolytic nitrogen isotopic fractionation of -55.8‰, in good agreement with what has been recently determined in a laboratory study.
M. Saccon, A. Kornilova, L. Huang, S. Moukhtar, and J. Rudolph
Atmos. Chem. Phys., 15, 10825–10838,
E. D. Sofen, B. Alexander, E. J. Steig, M. H. Thiemens, S. A. Kunasek, H. M. Amos, A. J. Schauer, M. G. Hastings, J. Bautista, T. L. Jackson, L. E. Vogel, J. R. McConnell, D. R. Pasteris, and E. S. Saltzman
Atmos. Chem. Phys., 14, 5749–5769,
J. Wintel, E. Hösen, R. Koppmann, M. Krebsbach, A. Hofzumahaus, and F. Rohrer
Atmos. Chem. Phys., 13, 11059–11071,
F. A. Haumann, A. M. Batenburg, G. Pieterse, C. Gerbig, M. C. Krol, and T. Röckmann
Atmos. Chem. Phys., 13, 9401–9413,
C. J. Sapart, P. Martinerie, E. Witrant, J. Chappellaz, R. S. W. van de Wal, P. Sperlich, C. van der Veen, S. Bernard, W. T. Sturges, T. Blunier, J. Schwander, D. Etheridge, and T. Röckmann
Atmos. Chem. Phys., 13, 6993–7005,
J. Erbland, W. C. Vicars, J. Savarino, S. Morin, M. M. Frey, D. Frosini, E. Vince, and J. M. F. Martins
Atmos. Chem. Phys., 13, 6403–6419,
A. Guillon, K. Le Ménach, P.-M. Flaud, N. Marchand, H. Budzinski, and E. Villenave
Atmos. Chem. Phys., 13, 2703–2719,
D. Ceburnis, A. Garbaras, S. Szidat, M. Rinaldi, S. Fahrni, N. Perron, L. Wacker, S. Leinert, V. Remeikis, M. C. Facchini, A. S. H. Prevot, S. G. Jennings, M. Ramonet, and C. D. O'Dowd
Atmos. Chem. Phys., 11, 8593–8606,
A. M. Batenburg, S. Walter, G. Pieterse, I. Levin, M. Schmidt, A. Jordan, S. Hammer, C. Yver, and T. Röckmann
Atmos. Chem. Phys., 11, 6985–6999,
B. Tuzson, S. Henne, D. Brunner, M. Steinbacher, J. Mohn, B. Buchmann, and L. Emmenegger
Atmos. Chem. Phys., 11, 1685–1696,
Y. T. Fang, K. Koba, X. M. Wang, D. Z. Wen, J. Li, Y. Takebayashi, X. Y. Liu, and M. Yoh
Atmos. Chem. Phys., 11, 1313–1325,
S. S. Assonov, C. A. M. Brenninkmeijer, T. J. Schuck, and P. Taylor
Atmos. Chem. Phys., 10, 8575–8599,
U. Tsunogai, D. D. Komatsu, S. Daita, G. A. Kazemi, F. Nakagawa, I. Noguchi, and J. Zhang
Atmos. Chem. Phys., 10, 1809–1820,
M. M. Frey, J. Savarino, S. Morin, J. Erbland, and J. M. F. Martins
Atmos. Chem. Phys., 9, 8681–8696,
S. A. Vay, S. C. Tyler, Y. Choi, D. R. Blake, N. J. Blake, G. W. Sachse, G. S. Diskin, and H. B. Singh
Atmos. Chem. Phys., 9, 4973–4985,
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