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A comprehensive estimate for loss of atmospheric carbon tetrachloride (CCl4) to the ocean
  • Published Date:
    2016
  • Source:
    Atmospheric Chemistry and Physics, 16(17), 10899-10910.
Filetype[PDF-2.61 MB]


Details:
  • Personal Author:
  • Description:
    Extensive undersaturations of carbon tetrachloride (CCl4) in Pacific, Atlantic, and Southern Ocean surface waters indicate that atmospheric CCl4 is consumed in large amounts by the ocean. Observations made on 16 research cruises between 1987 and 2010, ranging in latitude from 60 degrees N to 77 degrees S, show that negative saturations extend over most of the surface ocean. Corrected for physical effects associated with radiative heat flux, mixing, and air injection, these anomalies were commonly on the order of 5 to 10 %, with no clear relationship to temperature, productivity, or other gross surface water characteristics other than being more negative in association with upwelling. The atmospheric flux required to sustain these undersaturations is 12.4 (9.4-15.4) Gg yr(-1), a loss rate implying a partial atmospheric lifetime with respect to the oceanic loss of 183 (147241) yr and that similar to 18 (14-22) % of atmospheric CCl4 is lost to the ocean. Although CCl4 hydrolyzes in seawater, published hydrolysis rates for this gas are too slow to support such large undersaturations, given our current understanding of air-sea gas exchange rates. The even larger undersaturations in intermediate depth waters associated with reduced oxygen levels, observed in this study and by other investigators, strongly suggest that CCl4 is ubiquitously consumed at mid-depth, presumably by microbiota. Although this subsurface sink creates a gradient that drives a downward flux of CCl4, the gradient alone is not sufficient to explain the observed surface undersaturations. Since known chemical losses are likewise insufficient to sustain the observed undersaturations, this suggests a possible biological sink for CCl4 in surface or near-surface waters of the ocean. The total atmospheric lifetime for CCl4, based on these results and the most recent studies of soil uptake and loss in the stratosphere is now 32 (26-43) yr.
  • DOI:
    http://dx.doi.org/10.5194/acp-16-10899-2016
  • Document Type:
    Journal Article
  • Collection(s):
    NOAA Cooperative Institutes
    Office of Oceanic and Atmospheric Research (OAR)
  • Main Document Checksum:
  • Supporting Files:
    No Additional Files
    1. Summertime surface O-3 behavior and deposition to tundra in the Alaskan Arctic
      Personal Author:
      Van Dam, B.; Helmig, D.; Doskey, P. V.; Oltmans, S. J.;
      Published Date:
      2016
      Source:
      Journal of Geophysical Research-Atmospheres, 121(13), 8055-8066.
      Description:
      Atmospheric turbulence quantities, boundary layer ozone (O-3) levels, and O-3 deposition to the tundra surface were investigated at Toolik Lake, AK, during the 2011 summer season. Beginning immediately after snowmelt, a diurnal cycle of O-3 in the at...
      File Type:
      Filetype[PDF - 2.83 MB]
    2. MIPAS IMK/IAA CFC-11 (CCl3F) and CFC-12 (CCl2F2) measurements: accuracy, precision and long-term stability
      Personal Author:
      Eckert, E.; Laeng, A.; Lossow, S.; Kellmann, S.; Stiller, G.; von Clarmann, T.; Glatthor, N.; Hopfner, M.; Kiefer, M.; Oelhaf, H.; Orphal, J.; Funke, B.; Grabowski, U.; Haenel, F.; Linden, A.; Wetzel, G.; Woiwode, W.; Bernath, P. F.; Boone, C.; Dutton, G. S.; Elkins, J. W.; Engel, A.; Gille, J. C.; Kolonjari, F.; Sugita, T.; Toon, G. C.; Walker, K. A.;
      Published Date:
      2016
      Source:
      Atmospheric Measurement Techniques, 9(7), 3355-3389.
      Description:
      Profiles of CFC-11 (CCl3F) and CFC-12 (CCl2F2) of the Michelson Interferometer for Passive Atmospheric Sounding (MIPAS) aboard the European satellite Envisat have been retrieved from versions MIPAS/4.61 to MI-PAS/4.62 and MIPAS/5.02 to MIPAS/5.06 lev...
      File Type:
      Filetype[PDF - 12.56 MB]
    3. Recent divergences in stratospheric water vapor measurements by frost point hygrometers and the Aura Microwave Limb Sounder
      Personal Author:
      Hurst, D. F.; Read, W. G.; Vomel, H.; Selkirk, H. B.; Rosenlof, K. H.; Davis, S. M.; Hall, E. G.; Jordan, A. F.; Oltmans, S. J.;
      Published Date:
      2016
      Source:
      Atmospheric Measurement Techniques, 9(9), 4447-4457.
      Description:
      Balloon-borne frost point hygrometers (FPs) and the Aura Microwave Limb Sounder (MLS) provide high-quality vertical profile measurements of water vapor in the upper troposphere and lower stratosphere (UTLS). A previous comparison of stratospheric wat...
      File Type:
      Filetype[PDF - 2.10 MB]
    4. The influence of daily meteorology on boreal fire emissions and regional trace gas variability
      Personal Author:
      Wiggins, E. B.; Veraverbeke, S.; Henderson, J. M.; Karion, A.; Miller, J. B.; Lindaas, J.; Commane, R.; Sweeney, C.; Luus, K. A.; Tosca, M. G.; Dinardo, S. J.; Wofsy, S.; Miller, C. E.; Randerson, J. T.;
      Published Date:
      2016
      Source:
      Journal of Geophysical Research-Biogeosciences, 121(11), 2793-2810.
      Description:
      Relationships between boreal wildfire emissions and day-to-day variations in meteorological variables are complex and have important implications for the sensitivity of high-latitude ecosystems to climate change. We examined the influence of environm...
      File Type:
      Filetype[PDF - 2.44 MB]
    5. Separation of biospheric and fossil fuel fluxes of CO2 by atmospheric inversion of CO2 and (CO2)-C-14 measurements: Observation System Simulations
      Personal Author:
      Basu, S.; Miller, J. B.; Lehman, S.;
      Published Date:
      2016
      Source:
      Atmospheric Chemistry and Physics, 16(9), 5665-5683.
      Description:
      National annual total CO2 emissions from combustion of fossil fuels are likely known to within 5-10aEuro-% for most developed countries. However, uncertainties are inevitably larger (by unknown amounts) for emission estimates at regional and monthly ...
      File Type:
      Filetype[PDF - 6.92 MB]
    6. Investigating Alaskan methane and carbon dioxide fluxes using measurements from the CARVE tower
      Personal Author:
      Karion, A.; Sweeney, C.; Miller, J. B.; Andrews, A. E.; Commane, R.; Dinardo, S.; Henderson, J. M.; Lindaas, J.; Lin, J. C.; Luus, K. A.; Newberger, T.; Tans, P.; Wofsy, S. C.; Wolter, S.; Miller, C. E.;
      Published Date:
      2016
      Source:
      Atmospheric Chemistry and Physics, 16(8), 5383-5398.
      Description:
      Northern high-latitude carbon sources and sinks, including those resulting from degrading permafrost, are thought to be sensitive to the rapidly warming climate. Because the near-surface atmosphere integrates surface fluxes over large ( aEuro-500-100...
      File Type:
      Filetype[PDF - 3.56 MB]
    7. Regional atmospheric CO2 inversion reveals seasonal and geographic differences in Amazon net biome exchange
      Personal Author:
      Alden, C. B.; Miller, J. B.; Gatti, L. V.; Gloor, M. M.; Guan, K.; Michalak, A. M.; van der Laan-Luijkx, I. T.; Touma, D.; Andrews, A.; Basso, L. S.; Correia, C. S. C.; Domingues, L. G.; Joiner, J.; Krol, M. C.; Lyapustin, A. I.; Peters, W.; Shiga, Y. P.; Thoning, K.; van der Velde, I. R.; van Leeuwen, T. T.; Yadav, V.; Diffenbaugh, N. S.;
      Published Date:
      2016
      Source:
      Global Change Biology, 22(10), 3427-3443.
      Description:
      Understanding tropical rainforest carbon exchange and its response to heat and drought is critical for quantifying the effects of climate change on tropical ecosystems, including global climate-carbon feedbacks. Of particular importance for the globa...
      File Type:
      Filetype[PDF - 1.22 MB]
    8. Airborne methane remote measurements reveal heavy-tail flux distribution in Four Corners region
      Personal Author:
      Frankenberg, C.; Thorpe, A. K.; Thompson, D. R.; Hulley, G.; Kort, E. A.; Vance, N.; Borchardt, J.; Krings, T.; Gerilowski, K.; Sweeney, C.; Conley, S.; Bue, B. D.; Aubrey, A. D.; Hook, S.; Green, R. O.;
      Published Date:
      2016
      Source:
      Proceedings of the National Academy of Sciences of the United States of America, 113(35), 9734-9739.
      Description:
      Methane (CH4) impacts climate as the second strongest anthropogenic greenhouse gas and air quality by influencing tropospheric ozone levels. Space-based observations have identified the Four Corners region in the Southwest United States as an area of...
      File Type:
      Filetype[PDF - 1.96 MB]
    9. New approaches to quantifying aerosol influence on the cloud radiative effect
      Personal Author:
      Feingold, G.; McComiskey, A.; Yamaguchi, T.; Johnson, J. S.; Carslaw, K. S.; Schmidt, K. S.;
      Published Date:
      2016
      Source:
      Proceedings of the National Academy of Sciences of the United States of America, 113(21), 5812-5819.
      Description:
      The topic of cloud radiative forcing associated with the atmospheric aerosol has been the focus of intense scrutiny for decades. The enormity of the problem is reflected in the need to understand aspects such as aerosol composition, optical propertie...
      File Type:
      Filetype[PDF - 1006.31 KB]
    10. No significant increase in long-term CH4 emissions on North Slope of Alaska despite significant increase in air temperature
      Personal Author:
      Sweeney, C.; Dlugokencky, E.; Miller, C. E.; Wofsy, S.; Karion, A.; Dinardo, S.; Chang, R. Y. W.; Miller, J. B.; Bruhwiler, L.; Crotwell, A. M.; Newberger, T.; McKain, K.; Stone, R. S.; Wolter, S. E.; Lang, P. E.; Tans, P.;
      Published Date:
      2016
      Source:
      Geophysical Research Letters, 43(12), 6604-6611.
      Description:
      Continuous measurements of atmospheric methane (CH4) mole fractions measured by NOAA's Global Greenhouse Gas Reference Network in Barrow, AK (BRW), show strong enhancements above background values when winds come from the land sector from July to Dec...
      File Type:
      Filetype[PDF - 536.86 KB]
    11. Detecting regional patterns of changing CO2 flux in Alaska
      Personal Author:
      Parazoo, N. C.; Commane, R.; Wofsy, S. C.; Koven, C. D.; Sweeney, C.; Lawrence, D. M.; Lindaas, J.; Chang, R. Y. W.; Miller, C. E.;
      Published Date:
      2016
      Source:
      Proceedings of the National Academy of Sciences of the United States of America, 113(28), 7733-7738.
      Description:
      With rapid changes in climate and the seasonal amplitude of carbon dioxide (CO2) in the Arctic, it is critical that we detect and quantify the underlying processes controlling the changing amplitude of CO2 to better predict carbon cycle feedbacks in ...
      File Type:
      Filetype[PDF - 1.21 MB]
    12. Evaluation of wetland methane emissions across North America using atmospheric data and inverse modeling
      Personal Author:
      Miller, S. M.; Commane, R.; Melton, J. R.; Andrews, A. E.; Benmergui, J.; Dlugokencky, E. J.; Janssens-Maenhout, G.; Michalak, A. M.; Sweeney, C.; Worthy, D. E. J.;
      Published Date:
      2016
      Source:
      Biogeosciences, 13(4), 1329-1339.
      Description:
      Existing estimates of methane (CH4) fluxes from North American wetlands vary widely in both magnitude and distribution. In light of these differences, this study uses atmospheric CH4 observations from the US and Canada to analyze seven different bott...
      File Type:
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    13. O-3, CH4, CO2, CO, NO2 and NMHC aircraft measurements in the Uinta Basin oil and gas region under low and high ozone conditions in winter 2012 and 2013
      Personal Author:
      Oltmans, S. J.; Karion, A.; Schnell, R. C.; Petron, G.; Helmig, D.; Montzka, S. A.; Wolter, S.; Neff, D.; Miller, B. R.; Hueber, J.; Conley, S.; Johnson, B. J.; Sweeney, C.;
      Published Date:
      2016
      Source:
      Elementa-Science of the Anthropocene, 4: 000132.
      Description:
      Instrumented aircraft measuring air composition in the Uinta Basin, Utah, during February 2012 and January-February 2013 documented dramatically different atmospheric ozone (O-3) mole fractions. In 2012 O-3 remained near levels of similar to 40 ppb i...
      File Type:
      Filetype[PDF - 6.01 MB]
    14. Controlled weather balloon ascents and descents for atmospheric research and climate monitoring
      Personal Author:
      Krauchi, A.; Philipona, R.; Romanens, G.; Hurst, D. F.; Hall, E. G.; Jordan, A. F.;
      Published Date:
      2016
      Source:
      Atmospheric Measurement Techniques, 9(3), 929-938.
      Description:
      In situ upper-air measurements are often made with instruments attached to weather balloons launched at the surface and lifted into the stratosphere. Present-day balloon-borne sensors allow near-continuous measurements from the Earth's surface to abo...
      File Type:
      Filetype[PDF - 5.50 MB]
    15. Atmospheric histories and global emissions of halons H-1211 (CBrClF2), H-1301 (CBrF3), and H-2402 (CBrF2CBrF2)
      Personal Author:
      Vollmer, M. K.; Muhle, J.; Trudinger, C. M.; Rigby, M.; Montzka, S. A.; Harth, C. M.; Miller, B. R.; Henne, S.; Krummel, P. B.; Hall, B. D.; Young, D.; Kim, J.; Arduini, J.; Wenger, A.; Yao, B.; Reimann, S.; O'Doherty, S.; Maione, M.; Etheridge, D. M.; Li, S. L.; Verdonik, D. P.; Park, S.; Dutton, G.; Steele, L. P.; Lunder, C. R.; Rhee, T. S.; Hermansen, O.; Schmidbauer, N.; Wang, R. H. J.; Hill, M.; Salameh, P. K.; Langenfelds, R. L.; Zhou, L. X.; Blunier, T.; Schwander, J.; Elkins, J. W.; Butler, J. H.; Simmonds, P. G.; Weiss, R. F.; Prinn, R. G.; Fraser, P. J.;
      Published Date:
      2016
      Source:
      Journal of Geophysical Research-Atmospheres, 121(7), 3663-3686.
      Description:
      We report ground-based atmospheric measurements and emission estimates for the halons H-1211 (CBrClF2), H-1301 (CBrF3), and H-2402 (CBrF2CBrF2) from the AGAGE (Advanced Global Atmospheric Gases Experiment) and the National Oceanic and Atmospheric Adm...
      File Type:
      Filetype[PDF - 2.26 MB]
    16. Inverse modeling of GOSAT-retrieved ratios of total column CH4 and CO2 for 2009 and 2010
      Personal Author:
      Pandey, S.; Houweling, S.; Krol, M.; Aben, I.; Chevallier, F.; Dlugokencky, E. J.; Gatti, L. V.; Gloor, E.; Miller, J. B.; Detmers, R.; Machida, T.; Rockmann, T.;
      Published Date:
      2016
      Source:
      Atmospheric Chemistry and Physics, 16(8), 5043-5062.
      Description:
      This study investigates the constraint provided by greenhouse gas measurements from space on surface fluxes. Imperfect knowledge of the light path through the atmosphere, arising from scattering by clouds and aerosols, can create biases in column mea...
      File Type:
      Filetype[PDF - 3.49 MB]
    17. Regional Methane Emission Estimation Based on Observed Atmospheric Concentrations (2002-2012)
      Personal Author:
      Patra, P. K.; Saeki, T.; Dlugokencky, E. J.; Ishijima, K.; Umezawa, T.; Ito, A.; Aoki, S.; Morimoto, S.; Kort, E. A.; Crotwell, A.;
      Published Date:
      2016
      Source:
      Journal of the Meteorological Society of Japan, 94(1), 91-113.
      Description:
      Methane (CH4) plays important roles in atmospheric chemistry and short-term forcing of climate. A clear understanding of atmospheric CH4's budget of emissions and losses is required to aid sustainable management of Earth's future environment. We used...
      File Type:
      Filetype[PDF - 16.15 MB]
    18. The CU 2-D-MAX-DOAS instrument - Part 2: Raman scattering probability measurements and retrieval of aerosol optical properties
      Personal Author:
      Ortega, I.; Coburn, S.; Berg, L. K.; Lantz, K.; Michalsky, J.; Ferrare, R. A.; Hair, J.; Hostetler, C. A.; Volkamer, R.;
      Published Date:
      2016
      Source:
      Atmospheric Measurement Techniques, 9(8), 3893-3910.
      Description:
      The multiannual global mean of aerosol optical depth at 550 nm (AOD(550))over land is similar to 0.19, and that over oceans is similar to 0.13. About 45% of the Earth surface shows AOD550 smaller than 0.1. There is a need for measurement techniques t...
      File Type:
      Filetype[PDF - 3.76 MB]
    19. Low-CCN concentration air masses over the eastern North Atlantic: Seasonality, meteorology, and drivers
      Personal Author:
      Wood, R.; Stemmler, J. D.; Remillard, J.; Jefferson, A.;
      Published Date:
      2017
      Source:
      Journal of Geophysical Research-Atmospheres, 122(2), 1203-1223.
      Description:
      A 20 month cloud condensation nucleus concentration (N-CCN) data set from Graciosa Island (39 degrees N, 28 degrees W) in the remote North Atlantic is used to characterize air masses with low cloud condensation nuclei (CCN) concentrations. Low-CCN ev...
      File Type:
      Filetype[PDF - 6.32 MB]
    20. The Stratospheric Water and Ozone Satellite Homogenized (SWOOSH) database: a long-term database for climate studies
      Personal Author:
      Davis, S. M.; Rosenlof, K. H.; Hassler, B.; Hurst, D. F.; Read, W. G.; Vomel, H.; Selkirk, H.; Fujiwara, M.; Damadeo, R.;
      Published Date:
      2016
      Source:
      Earth System Science Data, 8(2), 461-490.
      Description:
      In this paper, we describe the construction of the Stratospheric Water and Ozone Satellite Homogenized (SWOOSH) database, which includes vertically resolved ozone and water vapor data from a subset of the limb profiling satellite instruments operatin...
      File Type:
      Filetype[PDF - 11.92 MB]
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