References

ACP

Atmospheric Chemistry and Physics

ACP

1680-7324

Copernicus GmbH

Göttingen, Germany

10.5194/acp-9-175-2009

Spatial distribution of Δ14CO2 across Eurasia: measurements from the TROICA-8 expedition

Turnbull

J. C.

¹ ² Miller

J. B.

² ³ Lehman

S. J.

¹ Hurst

² ³ Peters

² ³ Tans

P. P.

² Southon

⁴ Montzka

S. A.

² Elkins

J. W.

² Mondeel

D. J.

² Romashkin

P. A.

⁵ Elansky

⁶ Skorokhod

⁶

INSTAAR and Dept of Geological Sciences, University of Colorado, Boulder, Colorado, USA

NOAA/ESRL, Boulder, Colorado, USA

CIRES, University of Colorado, Boulder, Colorado, USA

Dept. of Earth System Science, University of California, Irvine, USA

NCAR, Broomfield, Colorado, USA

A.M. Obukhov Institute of Atmospheric Physics RAS, Moscow, Russia

12 01 2009

9 1 175 187

This is an open-access article ditributed under the terms of the Creative Commons Attribution License, which permits unrestricted use, distribution, and reproduction in any medium, provided the original author and source are credited.

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Because fossil fuel derived CO2 is the only source of atmospheric CO2 that is devoid of 14C, atmospheric measurements of Δ14CO2 can be used to constrain fossil fuel emission estimates at local and regional scales. However, at the continental scale, uncertainties in atmospheric transport and other sources of variability in Δ14CO2 may influence the fossil fuel detection capability. We present a set of Δ14CO2 observations from the train-based TROICA-8 expedition across Eurasia in March–April 2004. Local perturbations in Δ14CO2 are caused by easily identifiable sources from nuclear reactors and localized pollution events. The remaining data show an increase in Δ14CO2 from Western Russia (40° E) to Eastern Siberia (120° E), consistent with depletion in 14CO2 caused by fossil fuel CO2 emissions in heavily populated Europe, and gradual dispersion of the fossil fuel plume across Northern Asia. Other trace gas species which may be correlated with fossil fuel CO2 emissions, including carbon monoxide, sulphur hexafluoride, and perchloroethylene, were also measured and the results compared with the Δ14CO2 measurements. The sulphur hexafluoride longitudinal gradient is not significant relative to the measurement uncertainty. Carbon monoxide and perchloroethylene show large-scale trends of enriched values in Western Russia and decreasing values in Eastern Siberia, consistent with fossil fuel emissions, but exhibit significant spatial variability, especially near their primary sources in Western Russia. The clean air Δ14CO2 observations are compared with simulated spatial gradients from the TM5 atmospheric transport model. We show that the change in Δ14CO2 across the TROICA transect is due almost entirely to emissions of fossil fuel CO2, but that the magnitude of this Δ14CO2 gradient is relatively insensitive to modest uncertainties in the fossil fuel flux. In contrast, the Δ14CO2 gradient is more sensitive to the modeled representation of vertical mixing, suggesting that Δ14CO2 may be a useful tracer for training mixing in atmospheric transport models.

References 1

% vor jede Referenz Andreae, M. O. and Merlet, P.: Emission of trace gases and aerosols from biomass burning, Global Biogeochem. Cy., 15, 955–966, 2001.

% vor jede Referenz Bakwin, P. S., Hurst, D. F., Tans, P. P., and Elkins, J. W.: Anthropogenic sources of halocarbons, sulfur hexafluoride, carbon monoxide, and methane in the southeastern United States, J. Geophys. Res., 102, 15915–15925, 1997.

% vor jede Referenz Barnes, D. H., Wofsy, S. C., Fehlau, B. P., Gottlieb, E. W., Elkins, J. W., Dutton, G. S., and Montzka, S. A.: Urban/industrial pollution for the New York City – Washington D.C. corridor, 1996–1998: 1. Providing independent verification of CO and PCE emissions inventories, J. Geophys. Res., 108, 4185, doi:10.1029/2001JD001116, 2003.

% vor jede Referenz Belikov, I., Brenninkmeijer, C. A. M., Elansky, N., and Ral'ko, A.: Methane, carbon monoxide, and carbon dioxide concentrations measured in the atmospheric surface layer over continental Russia in the TROICA experiments, Izvestiya, Atmospheric and Ocean Physics, 42, 46–59, 2006.

% vor jede Referenz Blasing, T., Broniak, C., and Marland, G.: The annual cycle of fossil-fuel carbon dioxide emissions in the United States, Tellus, 57B, 107–115, 2005.

% vor jede Referenz Crutzen, P. J., Elansky, N., Hahn, M., Golitsyn, G., Brenninkmeijer, C. A. M., Scharffe, D., Belikov, I., Maiss, M., Bergamaschi, P., Rockmann, T., Grisenko, A., and Sevostyanov, V.: Trace gas measurements between Moscow and Vladivostok using the Trans-Siberian railroad, J. Atmos. Chem., 29, 179–194, 1998.

% vor jede Referenz Denning, A. S., Holzer, M., Gurney, K. R., Heimann, M., Law, R. M., Rayner, P. J., Fung, I. Y., Fan, S., Taguchi, S., Friedlingstein, P., Balkanski, Y., Taylor, J., Maiss, M., and Levin, I.: Three-dimensional transport and concentration of SF$_6$: A model intercomparison study (TransCom 2), Tellus, 51B, 266–297, 1999.

% vor jede Referenz HYSPLIT (HYbrid Single-Particle Lagrangian Integrated Trajectory): Model access via NOAA ARL READY Website, http://www.arl.noaa.gov/ready/hysplit4.html, 2003.

% vor jede Referenz Gibson, J., Kållberg, P., Uppala, S., Hernandez, A., Nomura, A., and Serrano, E.: ERA-15 description, Centre europeen por les previsions meteorologique a moyen terme, 1999.

% vor jede Referenz Gloor, M., Bakwin, P. S., Hurst, D. F., Lock, L., Draxler, R., and Tans, P. P.: What is the footprint of a tall tower?, J. Geophys. Res., 106, 17831–17840, 2001.

% vor jede Referenz Godwin, H.: Half-life of radiocarbon, Nature, 195, p. 984, 1962.

% vor jede Referenz Gurney, K. R., Law, R. M., Denning, A. S., Rayner, P. J., Baker, D., Bousquet, P., Bruhwiler, L., Chen, Y.-H., Ciais, P., Fan, S., Fung, I. Y., Gloor, M., Heimann, M., Higuchi, K., John, J., Maki, T., Maksyutov, S., Masarie, K. A., Peylin, P., Prather, M., Pak, B. C., Randerson, J., Sarmiento, J. L., Taguchi, S., Takahashi, T., and Yuen, C.-W.: Towards robust regional estimates of CO2 sources and sinks using atmospheric transport models, Nature, 415, 626–630, 2002.

% vor jede Referenz Hsueh, D. Y., Krakauer, N. Y., Randerson, J. T., Xu, X., Trumbore, S. E., and Southon, J. R.: Regional patterns of radiocarbon and fossil fuel-derived CO2 in surface air across North America, Geophys. Res. Lett., 34, LO2816, doi:10.1029/2006GL027032, 2007.

% vor jede Referenz Hurst, D. F., Lin, J., Romashkin, P. A., Daube, B. C., Gerbig, C., Matross, D. M., Wofsy, S. C., Hall, B. D., and Elkins, J. W.: Continuing global significance of emissions of Montreal Protocol restricted halocarbons in the USA and Canada, J. Geophys. Res., 111, D15302, doi:15310.11029/12005JD006785, 2006.

% vor jede Referenz Hurst, D. F., Romashkin, P. A., Elkins, J. W., Oberlander, E., Elansky, N., Belikov, I., Granberg, I., Golitsyn, G., Grisenko, A., Brenninkmeijer, C. A. M., and Crutzen, P. J.: Emissions of ozone-depleting substances in Russia during 2001, J. Geophys. Res., 109, 14303–14311, 2004.

% vor jede Referenz Krol, M., Houweling, S., Bregman, B., van den Broek, M., Segers, A., van Velthoven, P., Peters, W., Dentener, F., and Bergamaschi, P.: The two-way nested global chemistry-transport zoom model TM5: algorithm and applications, Atmos. Chem. Phys., 5, 417–432, 2005.

% vor jede Referenz Lal, D.: Theoretically expected variations in the terrestrial cosmic-ray production rates of isotopes, in: Proceedings of the International school of Physics, Solar-terrestrial relationships and the Earth environment in the last millennia, edited by: Castagnoli, G. C., North Holland Publishing Company, Amsterdam, 216–233, 1988.

% vor jede Referenz Levin, I. and Karstens, U.: Inferring high-resolution fossil fuel CO2 records at continental sites from combined $^14$CO2 and CO observations, Tellus, 59B, 245–250, 2007.

% vor jede Referenz Levin, I. and Kromer, B.: Twenty years of atmospheric $^14$CO2 observations at Schauinsland station, Germany, Radiocarbon, 39, 205–221, 1997.

% vor jede Referenz Levin, I. and Kromer, B.: The tropospheric $^14$CO2 level in mid-latitudes of the Northern Hemisphere (1959–2003), Radiocarbon, 46, 1261–1272, 2004.

% vor jede Referenz Levin, I., Kromer, B., Barabase, M., and Munnich, K. O.: Environmental distribution and long-term dispersion of reactor $^14$CO2 around two German nuclear power plants, Health Phys., 54, 149–156, 1988.

% vor jede Referenz Levin, I., Kromer, B., Schmidt, M., and Sartorius, H.: A novel approach for independent budgeting of fossil fuel CO2 over Europe by $^14$CO2 observations, Geophys. Res. Lett., 30, 2194, doi:10.1029/2003GL018477, 2003.

% vor jede Referenz Levin, I., Kromer, B., Schoch-Fischer, H., Bruns, M., Munnich, M., Berdau, D., Vogel, J. C., and Munnich, K. O.: 25 years of tropospheric $^14$C observations in central Europe, Radiocarbon, 27, 1–19, 1985.

% vor jede Referenz Levin, I. and Rödenbeck, C.: Can the envisaged reductions in fossil fuel CO$_2 $emissions be detected using atmospheric observations?, Naturwissenschaften, doi:10.1007/s00114-00007-00313-00114, 2007.

% vor jede Referenz Magnusson, A., Stenström, K., Skog, G., Adliene, D., Adlys, G., Hellborg, R., Olariu, A., Zakaria, M., Rääf, C., and Mattsson, S.: Levels of $^14$C in the terrestrial environment in the vicinity of two European nuclear power plants, Radiocarbon, 46, 863–868, 2004.

% vor jede Referenz Manning, M. R., Lowe, D. C., Melhuish, W. H., Sparks, R. J., Wallace, G., Brenninkmeijer, C. A. M., and McGill, R. C.: The use of radiocarbon measurements in atmospheric sciences, \mboxRadiocarbon, 32, 37–58, 1990.

% vor jede Referenz Marland, G., Boden, T. A., and Andres, R. J.: Global, regional and national CO2 emissions, in: Trends: A compedium of data on global change, Carbon Dioxide Information Analysis Center, Oak Ridge National Laboratory, US Department of Energy, Oak Ridge, TN, 2006.

% vor jede Referenz Masarik, J. and Beer, J.: Simulation of particle fluxes and cosmogenic nuclide formation in the Earth's atmosphere, J. Geophys. Res., 104, 12099–13012, 1999.

% vor jede Referenz Meijer, H. A. J., Smid, H. M., Perez, E., and Keizer, M. G.: Isotopic characterization of anthropogenic CO2 emissions using isotopic and radiocarbon analysis, Phys. Chem. Earth, 21, 483–487, 1996.

% vor jede Referenz Montzka, S. A., Myers, R. C., Butler, J. H., Elkins, J. W., and Cummings, S.: Global tropospheric distribution and calibration scale of HCFC-22, Geophys. Res. Lett., 20, 703–706, 1993.

% vor jede Referenz Nakamura, T., Nakazawa, T., Honda, H., Kitagawa, H., Machida, T., Ikeda, A., and Matsumoto, E.: Seasonal variations in $^14$C concentrations of stratospheric CO2 measured with accelerator mass spectrometry, Nucl. Instrum. Methods, B92, 413–416, 1994.

% vor jede Referenz Nydal, R. and Lövseth, K.: Tracing bomb $^14$C in the atmosphere 1962–1980, J. Geophys. Res., 88, 3621–3642, 1983.

% vor jede Referenz Olivier, J. G. J. and Berdowski, J. J. M.: Global emissions sources and sinks, in: The Climate System, edited by: Berdowski, J., Guicherit, R., and Heij, B., Balkema Publishers/Swets and Zeitlinger Publishers, Lisse, The Netherlands, 33–78, 2001.

% vor jede Referenz Olivier, J. G. J., Berdowski, J. J. M., Peters, J., Bakker, J., Visschedijk, A., and Bloos, J.: Applications of EDGAR, Including a description of EDGAR V3.0: reference database with trend data for 1970–1995, RIVM, BilthovenRIVM report 773301001 NRP report 410200051, 2001.

% vor jede Referenz Peters, W., Krol, M. C., Dlugokencky, E. J., Dentener, F. J., Bergamaschi, P., Dutton, G. S., Velthoven, P. v., Miller, J. B., Bruhwiler, L., and Tans, P. P.: Toward regional-scale modeling using the two-way nested global model TM5: Characterization of transport using SF$_6$, J. Geophys. Res., 109, 19314–19331, doi:10.1029/2004JD005020, 2004.

% vor jede Referenz Potosnak, M. J., Wofsy, S. C., Denning, A. S., Conway, T. J., Munger, J. W., and Barnes, D. H.: Influence of biotic exchange and combustion sources on atmospheric CO2 concentrations in New England from observations at a forest flux tower, J. Geophys. Res., 104, 9561–9569, 1999.

% vor jede Referenz Prentice, I. C., Farquhar, G. D., Fasham, M., Goulden, M. L., Heimann, M., Jaramillo, V., Kheshgi, H. S., Le Quere, C., Scholes, R. J., and Wallace, D. W.: The Carbon Cycle and Atmospheric Carbon Dioxide, in: Climate Change 2001: Third Assessment Report, Intergovernmental Panel on Climate Change, IPCC, 183–237, 2001.

% vor jede Referenz Randerson, J., Enting, I. G., Schuur, E. A. G., Caldeira, K., and Fung, I. Y.: Seasonal and latitudinal variability of troposphere $\Delta^14$CO2: post bomb contributions from fossil fuels, oceans, the stratosphere, and the terrestrial biosphere, Global Biogeochem. Cy., 16, 1112, doi:1110.1029/2002GB001876, 2002.

% vor jede Referenz Randerson, J. T., Thompson, M. V., Conway, T. J., Fung, I. Y., and Field, C.: The contribution of terrestrial source and sinks to trends in the seasonal cycle of atmospheric carbon dioxide, Global Biogeochem. Cy., 11, 535–560, 1997.

% vor jede Referenz Rivier, L., Ciais, P., Hauglustaine, D., Bakwin, P. S., Bousquet, P., Peylin, P., and Klonecki, A.: Evaluation of SF$_6$, C2Cl4 and CO as surrogate tracers for fossil fuel CO2 in the Northern Hemisphere using a chemistry transport model, J. Geophys. Res., 111, 16311, doi:16310.11029/12005JD006725, 2006.

% vor jede Referenz Romashkin, P. A., Hurst, D. F., Elkins, J. W., Dutton, G. S., Fahey, D., Dunn, R., Moore, F. L., Myers, R. C., and Hall, B. D.: In situ measurements of long-lived tracer gases in the lower stratosphere by gas chromatography, J. Atmos. Ocean. Tech., 18, 1195–1204, 2001.

% vor jede Referenz Rozanski, K., Levin, I., Stock, J., Falcon, R., and Rubio, F.: Atmospheric (CO2)-C-14 variations in the Equatorial region, Radiocarbon, 37, 509–515, 1995.

% vor jede Referenz Stephens, B. B., Gurney, K. R., Tans, P. P., Sweeney, C., Peters, W., Bruhwiler, L., Ciais, P., Ramonet, M., Bousquet, P., Nakazawa, T., Aoki, S., Machida, T., Inoue, G., Vinnichenko, N., Lloyd, J., Jordan, A., Heimann, M., Shibistowa, O., Langenfelds, R. L., Steele, L. P., Francey, R. J., and Denning, A. S.: Weak northern and strong tropical land carbon uptake from vertical profiles of atmospheric CO2, Science, 316, 1732–1735, 2007.

% vor jede Referenz Stuiver, M. and Polach, H. A.: Discussion: Reporting of $^14$C data, Radiocarbon, 19, 355–363, 1977.

% vor jede Referenz Takahashi, T., Sutherland, S. C., Sweeney, C., Poisson, A., Metzl, N., Tilbrook, B., Bates, N. R., Wanninkhof, R., Feely, R. A., Sabine, C., Olafsson, J., and Yukihiro, N.: Global sea-air CO2 flux based on climatological surface ocean $p$CO2, and seasonal biological and temperature effects, Deep Sea Res. II, 49, 1601–1622, 2002.

% vor jede Referenz Tans, P. P. and Conway, T. J.: Monthly Atmospheric CO2 Mixing Ratios from the NOAA CMDL Carbon Cycle Cooperative Global Air Sampling Network, 1968–2002, in: Trends: A Compendium of Data on Global Change, Carbon Dioxide Information Analysis Center, Oak Ridge National Laboratory, US Department of Energy, Oak Ridge, Tenn., USA, 2005.

% vor jede Referenz Tarasova, O., Brenninkmeijer, C. A. M., Assonov, S., Elansky, N., Röckmann, T., and Brass, M.: Atmospheric CH4 along the trans-Siberian railroad (TROICA) and river Ob: Source identification using stable isotopes, Atmos. Environ., 40, 5617–5628, 2006.

% vor jede Referenz Thompson, M. V. and Randerson, J. T.: Impulse response functions of terrestrial carbon cycle models: method and application, Global Change Biol., 5, 371–394, 1999.

% vor jede Referenz Trumbore, S. E.: Potential responses of soil organic carbon to global environmental change, Proc. Natl. Acad. Sci., 94, 8284–8291, 1997.

% vor jede Referenz Turnbull, J. C., Lehman, S. J., Miller, J. B., Sparks, R. J., Southon, J. R., and Tans, P. P.: A new high precision $^14$CO2 time series for North American continental air, J. Geophys. Res., 112, D11310, doi:11310.11029/12006JD008184, 2007.

% vor jede Referenz Turnbull, J. C., Miller, J. B., Lehman, S. J., Tans, P. P., Sparks, R. J., and Southon, J. R.: Comparison of $^14$CO2, CO and SF$_6$ as tracers for determination of recently added fossil fuel CO2 in the atmosphere and implications for biological CO2 exchange, Geophys. Res. Lett., 33, L01817, doi:01810.01029/02005GL024213, 2006.

% vor jede Referenz UNSCEAR: Sources and effects of ionizing radiation, UNSCEAR 2000 report to the General Assembly, with scientific annexes, 1, Annex C, 2000.

% vor jede Referenz USEPA: Trends in greenhouse gas emissions and sinks: 1990–2002, in: EPA 2004 Summary Report GHG emissions inventory 2004, USEPA, 2004.

% vor jede Referenz Wanninkhof, R.: Relationship between wind-speed and gas-exchange over the ocean, J. Geophys. Res., 97, 7373–7382, 1992.

% vor jede Referenz Wofsy, S. C., Fan, S.-M., Blake, D., Bradshaw, J., Sandholm, S., Singh, H., Sachse, G., and Harriss, R.: Factors influencing atmospheric composition over subarctic North America during summer, J. Geophys. Res., 99, 1887–0897, 1994.

% vor jede Referenz Yang, Z., Washenfelder, R., Keppel-Aleks, G., Krakauer, N. Y., Randerson, J. T., Tans, P. P., Sweeney, C., and Wennberg, P.: New constraints on Northern Hemisphere growing season net flux, Geophys. Res. Lett., 34, L12807, doi:10.1029/2007GL029742, 2007.

% vor jede Referenz Zondervan, A. and Meijer, H. A. J.: Isotopic characterisation of CO2 sources during regional pollution events using isotopic and radiocarbon analysis, Tellus, 48B, 601–612, 1996.