A new method to detect long term trends of methane (CH4) and nitrous oxide (N2O) total columns measured within the NDACC ground-based high resolution solar FTIR network
remote sensing; atmospheric composition and trends; FTIR spectrometer
Abstract :
[en] Total columns measured with the ground-based solar FTIR technique are highly variable in time due to atmospheric chemistry and dynamics in the atmosphere above the measurement station. In this paper, a multiple regression model with anomalies of air pressure, total columns of hydrogen fluoride (HF) and carbon monoxide (CO) and tropopause height are used to reduce the variability in the methane (CH4) and nitrous oxide (N2O) total columns to estimate reliable linear trends with as small uncertainties as possible. The method is developed at the Harestua station (60 N, 11 E, 600m a.s.l.) and used on three other European FTIR stations, i.e. Jungfraujoch (47 N, 8 E, 3600m a.s.l.), Zugspitze (47 N, 11 E, 3000m a.s.l.), and Kiruna (68 N, 20 E, 400m a.s.l.). Linear CH4 trends between 0.13±0.01-0.25±0.02%yr-1 were estimated for all stations in the 1996-2009 period. A piecewise model with three separate linear trends, connected at change points, was used to estimate the short term fluctuations in the CH4 total columns. This model shows a growth in 1996–1999 followed by a period of steady state until 2007. From 2007 until 2009 the atmospheric CH4 amount increases between 0.57±0.22–1.15±0.17%yr-1. Linear N2O trends between 0.19±0.01–0.40±0.02%yr-1 were estimated for all stations in the 1996-2007 period, here with the strongest trend at Harestua and Kiruna and the lowest at the Alp stations. From the N2O total columns crude tropospheric and stratospheric partial columns were derived, indicating that the observed difference in the N2O trends between the FTIR sites is of stratospheric origin. This agrees well with the N2O measurements by the SMR instrument onboard the Odin satellite showing the highest trends at Harestua, 0.98±0.28%yr-1, and considerably smaller trends at lower latitudes, 0.27±0.25%yr-1. The multiple regression model was compared with two other trend methods, the ordinary linear regression and a Bootstrap algorithm. The multiple regression model estimated CH4 and N2O trends that differed up to 31% compared to the other two methods and had uncertainties that were up to 300% lower. Since the multiple regression method were carefully validated this stresses the importance to account for variability in the total columns when estimating trend from solar FTIR data.
Disciplines :
Earth sciences & physical geography
Author, co-author :
Angelbratt, J.
Mellqvist, J.
Blumenstock, T.
Borsdorff, T.
Brohede, S.
Duchatelet, Pierre ; Université de Liège - ULiège > Département d'astrophys., géophysique et océanographie (AGO) > Groupe infra-rouge de phys. atmosph. et solaire (GIRPAS)
Forster, F.
Hase, F.
Mahieu, Emmanuel ; Université de Liège - ULiège > Département d'astrophys., géophysique et océanographie (AGO) > Groupe infra-rouge de phys. atmosph. et solaire (GIRPAS)
A new method to detect long term trends of methane (CH4) and nitrous oxide (N2O) total columns measured within the NDACC ground-based high resolution solar FTIR network
Bates, D. R. and Hays, P. B.: Atmospheric Nitrous Oxide, Planet. Space Sci., 15, 189-197, 1967.
Davidson, E. A.: The contribution of manure and fertilizer nitrogen to atmospheric nitrous oxide since 1860, Nat. Geosci., 2, 659- 662, doi:10.1038/Ngeo608, 2009.
DeMazière, M., Vigouroux, C., Gardiner, T., Coleman, M., Woods, P., Ellingsen, K., Gauss, M., Isaksen, I., Blumenstock, T., Hase, F., Kramer, I., Camy-peyret, C., Chelin, P., Mahieu, E., De-moulin, P., Duchatelet, P., Mellqvist, J., Strandberg, A., Velazco, V., Notholt, J., Sussmann, R., Stremme, W., and Rockmann, A.: The exploitation of ground-based Fourier transform infrared observations for the evaluation of tropospheric trends of greenhouse gases over Europe, Environm. Sci., 2, 283-293, 2005.
Dlugokencky, E. J., Steele, L. P., Lang, P. M., and Masarie, K. A.: The Growth-Rate and Distribution of Atmospheric Methane, J. Geophys. Res.-Atmos., 99, 17021-17043, 1994.
Dlugokencky, E. J., Houweling, S., Bruhwiler, L., Masarie, K. A., Lang, P. M., Miller, J. B., and Tans, P. P.: Atmospheric methane levels off: Temporary pause or a new steady-state?, Geophys. Res. Lett., 30, 1992, doi:10.1029/2003gl018126, 2003.
Dlugokencky, E. J., Bruhwiler, L., White, J. W. C., Emmons, L. K., Novelli, P. C., Montzka, S. A., Masarie, K. A., Lang, P. M., Crotwell, A. M., Miller, J. B., and Gatti, L. V.: Observational constraints on recent increases in the atmospheric CH4 burden, Geophys. Res. Lett., 36, L18803, doi:10.1029/2009gl039780, 2009.
Efron, B. and Tibshirani, R.: An introduction to the bootstrap, Monographs on statistics and applied probability, 57, Chapman & Hall, New York, USA, xvi, 436 pp., 1993.
Gardiner, T., Forbes, A., de Mazière, M., Vigouroux, C., Mahieu, E., Demoulin, P., Velazco, V., Notholt, J., Blumenstock, T., Hase, F., Kramer, I., Sussmann, R., Stremme, W., Mellqvist, J., Strand-berg, A., Ellingsen, K., and Gauss, M.: Trend analysis of greenhouse gases over Europe measured by a network of ground-based remote FTIR instruments, Atmos. Chem. Phys., 8, 6719-6727, doi:10.5194/acp-8-6719-2008, 2008.
Hase, F., Blumenstock, T., and Paton-Walsh, C.: Analysis of the instrumental line shape of high-resolution Fourier transform IR spectrometers with gas cell measurements and new retrieval software, Appl. Optics, 38, 3417-3422, 1999. (Pubitemid 129568232)
Hase, F., Hannigan, J. W., Coffey, M. T., Goldman, A., Hopfner, M., Jones, N. B., Rinsland, C. P., and Wood, S. W.: Intercompar-ison of retrieval codes used for the analysis of high-resolution, ground-based FTIR measurements, J. Quant. Spectrosc. Ra., 87, 25-52, doi:10.1016/j.jqsrt.2003.12.008, 2004. (Pubitemid 38536698)
Haszpra, L., Barcza, Z., Hidy, D., Szilagyi, I., Dlugokencky, E., and Tans, R.: Trends and temporal variations of major greenhouse gases at a rural site in Central Europe, Atmos. Environ., 42, 8707-8716, doi:10.1016/j.atmosenv. 2008.09.012, 2008.
IPCC: Contribution of Working Group I to the Fourth Assessment Report of the Intergovernmental Panel on Climate Change, 2007, Cambridge University Press, Cambridge, United Kingdom and New York, NY, USA, 2007.
Jackowicz-Korczynski, M., Christensen, T. R., Backstrand, K., Crill, P., Friborg, T., Mastepanov, M., and Strom, L.: Annual cycle of methane emission from a subarctic peatland, J. Geophys. Res.-Biogeo., 115, G02009, doi:10.1029/2008jg000913, 2010.
Jones, A., Urban, J., Murtagh, D. P., Eriksson, P., Brohede, S., Haley, C., Degenstein, D., Bourassa, A., von Savigny, C., Sonkaew, T., Rozanov, A., Bovensmann, H., and Burrows, J.: Evolution of stratospheric ozone and water vapour time series studied with satellite measurements, Atmos. Chem. Phys., 9, 6055-6075, doi:10.5194/acp-9-6055-2009, 2009.
Li, F., Newman, P. A., and Stolarski, R. S.: Relationships between the Brewer-Dobson circulation and the southern annular mode during austral summer in coupled chemistry-climate model simulations, J. Geophys. Res.-Atmos., 115, D15106, doi:10.1029/2009jd012876, 2010.
Mellqvist, J., Galle, B., Blumenstock, T., Hase, F., Yashcov, D., Notholt, J., Sen, B., Blavier, J.-F., Toon, G. C., and Chip-perfield, M. P.: Ground-Based FTIR observations of chlorine activation and ozone depletion inside the Arctic vortex during the winter of 1999/2000, J. Geophys. Res., 107, 8263, doi:10.1029/2001JD001080, 2002.
Montgomery, D. C., Jennings, C. L., and Kulahci, M.: Introduction to time series analysis and forecasting, in: Wiley series in probability and statistics, edited by: Hoboken, N. J., Wiley-Interscience, xi, 445 pp., 2008.
Murtagh, D., Frisk, U., Merino, F., Ridal, M., Jonsson, A., Stegman, J., Witt, G., Eriksson, P., Jimenez, C., Megie, G., de la Noe, J., Ricaud, P., Baron, P., Pardo, J. R., Hauchcorne, A., Llewellyn, E. J., Degenstein, D. A., Gattinger, R. L., Lloyd, N. D., Evans, W. F. J., McDade, I. C., Haley, C. S., Sioris, C., von Savigny, C., Solheim, B. H., McConnell, J. C., Strong, K., Richardson, E. H., Leppelmeier, G. W., Kyrola, E., Auvinen, H., and Oikarinen, L.: An overview of the Odin atmospheric mission, Can. J. Phys., 80, 309-319, doi:10.1139/P01-157, 2002.
Neter, J., Wasserman, W., and Kutner, M. H.: Applied linear statistical models : regression, analysis of variance, and experimental designs, 3rd edn., Irwin, Homewood, IL, xvi, 1181 pp., 1990.
Rinsland, C. P., Jones, N. B., Connor, B. J., Logan, J. A., Pougatchev, N. S., Goldman, A., Murcray, F. J., Stephen, T. M., Pine, A. S., Zander, R., Mahieu, E., and Demoulin, P.: Northern and southern hemisphere ground-based infrared spectroscopic measurements of tropospheric carbon monoxide and ethane, J. Geophys. Res.-Atmos., 103, 28197-28217, 1998. (Pubitemid 128700273)
Rinsland, C. P., Chiou, L., Boone, C., Bernath, P., Mahieu, E., and Zander, R.: Trend of lower stratospheric methane (CH4) from atmospheric chemistry experiment (ACE) and atmospheric trace molecule spectroscopy (ATMOS) measurements, J. Quant. Spec- trosc. Ra., 110, 1066-1071, doi:10.1016/j.jqsrt. 2009.03.024, 2009.
Rodgers, C. D.: Inverse Methods for Atmospheric Sounding, Series on Atmospheric, Oceanic and Planetary Physics, 2, 55-63, 2000.
Simpson, I. J., Rowland, F. S., Meinardi, S., and Blake, D. R.: Influence of biomass burning during recent fluctuations in the slow growth of global tropospheric methane, Geophys. Res. Lett., 33, L22808, doi:10.1029/2006gl027330, 2006. (Pubitemid 47386176)
Strong, K., Wolff, M. A., Kerzenmacher, T. E., Walker, K. A., Bernath, P. F., Blumenstock, T., Boone, C., Catoire, V., Cof-fey, M., De Mazire, M., Demoulin, P., Duchatelet, P., Dupuy, E., Hannigan, J., Hpfner, M., Glatthor, N., Griffith, D. W. T., Jin, J. J., Jones, N., Jucks, K., Kuellmann, H., Kuttippurath, J., Lambert, A., Mahieu, E., McConnell, J. C., Mellqvist, J., Mikuteit, S., Murtagh, D. P., Notholt, J., Piccolo, C., Raspollini, P., Ri-dolfi, M., Robert, C., Schneider, M., Schrems, O., Semeniuk, K., Senten, C., Stiller, G. P., Strandberg, A., Taylor, J., Tétard, C., Toohey, M., Urban, J., Warneke, T., and Wood, S.: Validation of ACE-FTS N2O measurements, Atmos. Chem. Phys., 8, 4759-4786, doi:10.5194/acp-8-4759-2008, 2008.
Sussmann, R. and Borsdorff, T.: Technical Note: Interference errors in infrared remote sounding of the atmosphere, Atmos. Chem. Phys., 7, 3537-3557, doi:10.5194/acp-7-3537-2007, 2007. (Pubitemid 47151110)
Sussmann, R., Stremme, W., Buchwitz, M., and de Beek, R.: Validation of ENVISAT/SCIAMACHY columnar methane by solar FTIR spectrometry at the Ground-Truthing Station Zugspitze, Atmos. Chem. Phys., 5, 2419-2429, doi:10.5194/acp-5-2419-2005, 2005. (Pubitemid 41479779)
Tiao, G. C., Reinsel, G. C., Xu, D. M., Pedrick, J. H., Zhu, X. D., Miller, A. J., Deluisi, J. J., Mateer, C. L., and Wuebbles, D. J.: Effects of Autocorrelation and Temporal Sampling Schemes on Estimates of Trend and Spatial Correlation, J. Geophys. Res.-Atmos., 95, 20507-20517, 1990.
Toon, G. C., Blavier, J.-F., Sen, B., Salawitch, R. J., G. B. Osterman, Notholt, J., Rex, M., McElroy, C. T., and Russell, J. M.: Ground-based observations of Arctic O3 loss during spring and summer 1997, J. Geophys. Res., 104, 497-510, 1997.
Twomey, S.: Introduction to the mathematics of inversion in remote sensing and indirect measurements, Dover Publications, Mine-ola, N.Y., x, 237 pp., 1996.
Urban, J., Lautie, N., Le Flochmoen, E., Jimenez, C., Eriksson, P., de La Noe, J., Dupuy, E., Ekstrom, M., El Amraoui, L., Frisk, U., Murtagh, D., Olberg, M., and Ricaud, P.: Odin/SMR limb observations of stratospheric trace gases: Level 2 processing of ClO, N2O, HNO3, and O-3, J. Geophys. Res.-Atmos., 110, D14307, doi:10.1029/2004jd005741, 2005a. (Pubitemid 41320631)
Urban, J., Lautie, N., Le Flochmoen, E., Jimenez, C., Eriksson, P., de La Noe, J., Dupuy, E., El Amraoui, L., Frisk, U., Jegou, F., Murtagh, D., Olberg, M., Ricaud, P., Camy-Peyret, C., Du-four, G., Payan, S., Huret, N., Pirre, M., Robinson, A. D., Harris, N. R. P., Bremer, H., Kleinbohl, A., Kullmann, K., Kunzi, K., Kuttippurath, J., Ejiri, M. K., Nakajima, H., Sasano, Y., Sugita, W., Yokota, T., Piccolo, C., Raspollini, P., and Ridolfi, M.: Odin/SMR limb observations of stratospheric trace gases: Validation of N2O, J. Geophys. Res.-Atmos., 110, D09301, doi:10.1029/2004jd005394, 2005b. (Pubitemid 40923956)
Urban, J., Murtagh, D., Lautié, N., Barret, B., Dupuy, E., de La Noë, J., Eriksson, P., Frisk, U., Jones, A., Le Flochmoën, E., Olberg, M., Piccolo, C., Ricaud, P., and Rösevall, J.: Odin/SMR Limb Observations of Trace Gases in the Polar Lower Stratosphere during 2004-2005, Proc. ESA First Atmospheric Science Conference, edited by: Lacoste, H., ESA-SP-628, ISBN-92-9092-939-1, 2006.
Weatherhead, E. C., Reinsel, G. C., Tiao, G. C., Meng, X. L., Choi, D. S., Cheang, W. K., Keller, T., DeLuisi, J., Wuebbles, D. J., Kerr, J. B., Miller, A. J., Oltmans, S. J., and Frederick, J. E.: Factors affecting the detection of trends: Statistical considerations and applications to environmental data, J. Geophys. Res.-Atmos., 103, 17149-17161, 1998.
Vigouroux, C., De Mazière, M., Demoulin, P., Servais, C., Hase, F., Blumenstock, T., Kramer, I., Schneider, M., Mellqvist, J., Strandberg, A., Velazco, V., Notholt, J., Sussmann, R., Stremme, W., Rockmann, A., Gardiner, T., Coleman, M., and Woods, P.: Evaluation of tropospheric and stratospheric ozone trends over Western Europe from ground-based FTIR network observations, Atmos. Chem. Phys., 8, 6865-6886, doi:10.5194/acp-8-6865-2008, 2008.
Yurganov, L. N., Blumenstock, T., Grechko, E. I., Hase, F., Hyer, E. J., Kasischke, E. S., Koike, M., Kondo, Y., Kramer, I., Leung, F. Y., Mahieu, E., Mellqvist, J., Notholt, J., Novelli, P. C., Rinsland, C. P., Scheel, H. E., Schulz, A., Strandberg, A., Suss-mann, R., Tanimoto, H., Velazco, V., Zander, R., and Zhao, Y.: A quantitative assessment of the 1998 carbon monoxide emission anomaly in the Northern Hemisphere based on total column and surface concentration measurements, J. Geophys. Res.-Atmos., 109, D15305, doi:10.1029/2004jd004559, 2004. (Pubitemid 39411963)
Yurganov, L. N., Duchatelet, P., Dzhola, A. V., Edwards, D. P., Hase, F., Kramer, I., Mahieu, E., Mellqvist, J., Notholt, J., Nov-elli, P. C., Rockmann, A., Scheel, H. E., Schneider, M., Schulz, A., Strandberg, A., Sussmann, R., Tanimoto, H., Velazco, V., Drummond, J. R., and Gille, J. C.: Increased Northern Hemispheric carbon monoxide burden in the troposphere in 2002 and 2003 detected from the ground and from space, Atmos. Chem. Phys., 5, 563-573, doi:10.5194/acp-5-563-2005, 2005. (Pubitemid 40405305)
