Atmospheric Chemistry and Physics
www.atmos-chem-phys.net
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2008
10.5194/acp-8-1635-2008
http://www.atmos-chem-phys.net/8/1635/2008/
http://www.atmos-chem-phys.net/8/1635/2008/acp-8-1635-2008.html
http://www.atmos-chem-phys.net/8/1635/2008/acp-8-1635-2008.pdf
1635
1648
2008-03-18
NO<sub>2</sub> climatology in the northern subtropical region: diurnal, seasonal and interannual variability
M. Gil
gilm@inta.es
M. Yela
L. N. Gunn
A. Richter
I. Alonso
M. P. Chipperfield
E. Cuevas
J. Iglesias
M. Navarro
O. Puentedura
S. Rodríguez
Area de Investigación e Instrumentación Atmosférica, INTA, Torrejón de Ardoz, Spain
Institute for Atmospheric Science, School of Earth and Environment, University of Leeds, Leeds, UK
Institute of Environmental Physics, University of Bremen, Bremen, Germany
Centro de Investigación Atmosférica de Izaña, INM, Sta. Cruz de Tenerife, Spain
Daily NO<sub>2</sub> vertical column density (VCD) has been routinely measured by
zenith sky spectroscopy at the subtropical station of Izaña (28° N,
16° W) since 1993 in the framework of the Network for the Detection of
Atmospheric Composition Change (NDACC). Based on 14 years of data the first
low latitude NO<sub>2</sub> VCD climatology has been established and the main
characteristics from short timescales of one day to interannual variability
are presented. Instrumental descriptions and different sources of errors are
described in detail. The observed diurnal cycle follows that expected by
gas-phase NO<sub>x</sub> chemistry, as can be shown by the good agreement with a
vertically integrated chemical box model, and is modulated by solar
radiation. The seasonal evolution departs from the phase of the hours of
daylight, indicating the signature of upper stratospheric temperature
changes. From the data record (1993–2006) no significant long-term trends in
NO<sub>2</sub> VCD can be inferred. Comparison of the ground-based data sets with
nadir-viewing satellite spectrometers shows excellent agreement for
SCIAMACHY with differences between both datasets of 1.1%. GOME displays
unrealistic features with the largest discrepancies during summer. The
ground-based data are compared with long-term output of the SLIMCAT 3-D
chemical transport model (CTM). The basic model, forced by ECMWF (ERA-40)
analyses, captures the observed NO<sub>2</sub> annual cycle but significantly
underestimates the spring/summer maximum (by 12% at sunset and up to
25% at sunrise). In a model run which uses assimilation of satellite
CH<sub>4</sub> profiles to constrain the model long-lived tracers the agreement is
significantly improved. This improvement in modelled column NO<sub>2</sub> is due
to better modelled NO<sub>y</sub> profiles and points to transport errors in the ECMWF
ERA-40 reanalyses.
Bernhard, G., Evans, R. D., Labow, G. J., and Oltmans, S. J.: Bias in Dobson total ozone measurements at high latitudes due to approximations in calculations of ozone absorption coefficients and air mass, J. Geophys. Res., 110, D10305, doi:10.1029/2004JD005559, 2005.
Bovensmann, H., Burrows, J. P., Buchwitz, M., Frerick, J., No\"el, S., Rozanov, V. V., Chance, K. V., and Goede, A. H. P.: SCIAMACHY – Mission objectives and measurement modes, J. Atmos. Sci., 56(2), 127–150, 1999.
Bogumil, K., Orphal, J., Flaud, J.-M., and Burrows, J.-P.: Vibrational progressions in the visible and near ultraviolet absorption spectrum of ozone, Chem. Phys. Lett., 349, 241–248, 2001.
Bogumil, K., Orphal, J., Homann, T., Voigt, S., Spietz, P., Fleischmann, O. C., Vogel, A., Hartmann, M., Bovensmann, H., Frerick, J., and Burrows, J. P.: Measurements of molecular absorption spectra with the SCIAMACHY pre-flight model: Instrument characterization and reference data for atmospheric remote-sensing in the 230–2380 nm region, J. Photoch. Photobio. A, 157, 167–184, 2003.
Brewer, A. W., McElroy C. T., and Kerr, J. B.: Nitrogen dioxide concentration in the atmosphere, Nature, 246, 129–133, 1973.
Burrows, J. P., Dehn, A., Deters, B., Himmelmann, S., Richter, A., Voigt, S., and Orphal, J.: Atmospheric remote-sensing reference data from GOME: Part 1. Temperature-dependent absorption cross-sections of NO<sub>2</sub> in the 231–794 nm range, J. Quant. Spectrosc. Ra., 60, 1025–1031, 1998.
Chipperfield, M. P.: Multiannual simulations with a three-dimensional chemical transport model, J. Geophys. Res., 104, 1781–1805, 1999.
Chipperfield, M. P., Khattatov, B. V., and Lary, D. J.: Sequential assimilation of stratospheric chemical observations in a three-dimensional model, J. Geophys. Res. 107, 4585, doi:10.1029/2002JD002110, 2002.
Chipperfield, M. P.: New Version of the TOMCAT/SLIMCAT Off-Line Chemical Transport Model: Intercomparison of Stratospheric Tracer Experiments, Q. J. Roy Meteor. Soc., 132, 1179–1203, doi:10.1256/qj.05.51, 2006.
Denis, L., Roscoe, H. K., Chipperfield, M. P., Van Roozendael, M., and Goutail, F.: A new software suite for NO<sub>2</sub> vertical profile retrieval from ground-based zenith-sky spectrometers, J. Quant. Spectrosc. Ra., 92, 3, 321–333, 2005.
Dobber, M. R., Dirksen, R., Voors, R., Mount, G. H., and Levelt, P.: Ground-based zenith sky abundances and in situ gas cross sections for ozone and nitrogen dioxide with the Earth Observing System Aura Ozone Monitoring Instrument, Appl. Optics, 44, 2846–2856, 2005.
ESA (European Space Agency): GOME Global Ozone Measuring Experiment Users Manual, ESA SP-1182, ESA/ESTEC, Noordwijk, 1995.
Fayt, C. and Van Roozendael, M.: WinDOAS 2.1. User Manual, IASB-BIRA, 2001.
Feng, W., Chipperfield, M. P., Dorf, M., Pfeilsticker, K., and Ricaud, P.: Mid-latitude Ozone Changes: Studies with a 3-D CTM Forced by ERA-40 Analyses, Atmos. Chem. Phys., 7, 2357–2369, 2007.
Greenblatt, G. D., Orlando, J. J., Burkholder, J. B., and Ravishankara, A. R.: Absorption Measurements of Oxygen Between 330 and 1140 nm, J. Geophys. Res., 95, 18 577–18 581, 1990.
Hendrick, F., Van Roozendael, M., Lambert, J.-C., and de Mazière, M.: Validation of MIPAS NO<sub>2</sub> profiles and columns using ground-based zenith-sky UV-visible observations, Geophys. Res. Abstr., 6, 10-2-2004, EGU 2004.
Johnston, P. V., McKenzie, R. L., Keys, J. G., and Matthews, W. A.: Observations of depleted stratospheric NO<sub>2</sub> following the Pinatubo volcanic eruption, Geophys. Res. Lett., 19, 211–213, 1992.
Khattatov, B. V., Lamarque, J. F., Lvjak, L. V., Menard, R., Levelt, P., Tie, X. X., Brasseur, G. P., and Gille, J. C.: Assimilation of satellite observations of long-lived chemical species in global chemistry transport models, J. Geophys. Res., 105, 29 135–29 144, 2000.
Koike, M., Kondo, Y., Matthews, W. A., Johnston, P. V., and Yamazaki, K.: Decrease of stratospheric NO<sub>2</sub> at 44° N caused by Pinatubo Volcanic aerosols, Geophys. Res. Lett., 20, 1975–1978, 1993.
Lambert, J.-C., Van Roozendael, M., Simon, P. C., De Mazière, M., Pommereau, J.-P., Goutail, F., and Sarkissian, A.: Pole-to-pole validation of GOME level-2 products with ground-based networks, Earth Observation Quarterly, 58, 6–8, 1998.
Lambert, J.-C., Granville, J., Van Roozendael, M., Müller, J.-F., Goutail, F., Pommereau, J.-P., Sarkissian, A., Johnston, P. V., and Russell III, J. M.: Global Behavior of Atmospheric NO<sub>2</sub> as Derived from the Integrated Use of Satellite, Ground-based Network and Balloon Observations, Atmospheric Ozone, XIX Quadrennial Ozone Symposium, Sapporo, Hokkaido, Japan, 3–8 July 2000.
Lambert, J.-C., Blumenstock, T., Boersma, F., Bracher, A., De Maziere, M., Demoulin, P., De Smedt, I., Eskes, H., Gil, M., Goutail, Granville, J., F., Hendrick, F., Ionov, D. V., Johnston, P. V., Kostadinov, I., Kreher, K., Kyrö, E., Martin, R., Meier, A., Navarro-Comas, M., Petritoli, A., Pommereau, J.-P., Richter, A., Roscoe, H. K., Sioris, C., Sussmann, R., Van Roozendael, M., Wagner, T., Wood, S., and Yela, M.: Geophysical validation of SCIAMACHY NO2 vertical columns: overview of early 2004 results, Proc. of the Second Workshop on the Atmospheric Chemistry Validation of ENVISAT (ACVE-2), ESA ESRIN, Frascati, Italy, 3–7 May 2004, ESA SP-562, 2004.
Lambert, J.-C., Granville, J., Hendrick, F., Andersen, S. B., Dorokhov, V., Gerard, P., Gil, M., Goutail, F., Gruzdev, A. N., Held, G., Ionov, D. V., Johnston, P. V., Kostadinov, I., Kreher, K., Kyro, E., Lerot, C., Leveau, J., Navarro-Comas, M., Petritoli, A., Pommereau, J.-P., Richter, A., Roscoe, H. K., Semenov, V. K., Stebel, K., Van Roozendael, M., Vaughan, G., Wagner, T., Wittrock, F., and Yela, M.: Transfer of GOME Data Processor (GDP) version 4.0 to SCIAMACHY Off-line (OL) processor version 3.0: Pole-to-pole delta-validation of NO<sub>2</sub> column data with the NDACC/UV-Visible network, Proc. of the Third Workshop on the Atmospheric Chemistry Validation of Envisat (ACVE-3), ESA SP-642, 2007.
Lee, A. M., Roscoe, H. K., Oldham, D. J., Squires, J. A. C., Sarkissian A., and Pommereau, J.-.P.: Improvements to the accuracy of measurements of NO<sub>2</sub> by zenith-sky visible spectrometers, J. Quant. Spectrosc. Ra., 52, 5, 649–657, 1994.
Liley, J. B., Johnston, P. V., McKenzie, R. L., Thomas, A. J., and Boyd, I. S.: Stratospheric NO<sub>2</sub> variations from a long time series at Lauder, New Zealand, J. Geophys. Res., 105(D9), 11 633–11 640, doi:10.1029/1999JD901157, 2000.
Minschwaner, K., Salawitch, R., and McElroy, M.: Absorption of solar radiation by O<sub>2</sub>: Implications for O<sub>3</sub> and lifetimes of N<sub>2</sub>O, CFCl<sub>3</sub> and CF<sub>2</sub>Cl<sub>2</sub>, J. Geophys. Res., 98, 10 543–10 561, 1993.
NDACC: http://www.ndsc.ncep.noaa.gov/, last access: March 2008, 2007.
Noxon, J. F.: Nitrogen Dioxide in the stratosphere and troposphere measured by ground-based absorption spectroscopy, Science, 189, 547–549, 1975.
Orphal, J. A.: Critical Review of the Absorption Cross-Sections of O<sub>3</sub> and NO<sub>2</sub> in the 240–790 nm Region, Part 2. Nitrogen Dioxide, ESA Technical Note MO-TN-ESA-GO-0302, 2002.
Piters, A. J. M., Bramstedt, K., Lambert, J.-C., and Kirchhoff, B.: Overview of SCIAMACHY validation: 2002–2004, Atmos. Chem. Phys., 6, 127–148, 2006.
Richter, A. and Burrows, J. P.: Retrieval of Tropospheric NO<sub>2</sub> from GOME Measurements, Adv. Space Res., 29(11), 1673–1683, 2002.
Richter, A., Wittrock, F., Weber, M., Beirle, S., Kühl, S., Platt, U., Wagner, T., Wilms-Grabe, W., and Burrows, J. P.: GOME observations of stratospheric trace gas distributions during the splitting vortex event in the Antarctic winter 2002 Part I: Measurements, J. Atmos. Sci., 62(3), 778–785, 2005a.
Richter, A., Burrows, J. P., Nüß, H., Granier, C., and Niemeier, U.: Increase in tropospheric nitrogen dioxide over China observed from space, Nature, 437, 129–132, doi:10.1038/nature04092, 2005b.
Richter, A., Kreher, K., Johnston, P. V., Wittrock, F., and Burrows, J. P.: Validation of GOME O<sub>3</sub>, NO<sub>2</sub>, BrO, and OClO Measurements in Southern High Latitudes, Procc. of the Fifth European Workshop on Stratospheric Ozone, European Commission, Air Pollution research report 73, 719–722, 2000.
Richter, A., Burrows, J. P., Fietkau, S., Medeke, T., Notholt, J., Oetjen, H., Sierk, B., Warneke, T., Wittrock, F., Dix, B., Friess, U., Wagner, T., Blumenstock, T., Griesfeller, A., Sussmann, R., Rockmann, A., and Schultz, A.: A Scientific NO<sub>2</sub> product from Sciamachy: First Results and validation. Proc. of the Second Workshop on the Atmospheric Chemistry Validation of ENVISAT (ACVE-2), ESA ESRIN, Frascati, Italy, 3–7 May 2004, ESA SP-562, 2004.
Rinsland, C. P., Weisenstein, D. K., Ko, M. K. W., Scott, C. J., Chiou, L. S., Mahieu, E., Zander, R., and Demoulin, P.: Post-Mount Pinatubo eruption ground-based infrared stratospheric column measurements of HNO<sub>3</sub>, NO, and NO<sub>2</sub> and their comparison with model calculations, J. Geophys. Res., 108(D15), 4437, doi:10.1029/2002JD002965, 2003.
Roscoe, H. K., Johnston, P. V., Van Roozendael, M., Richter, A., Sarkissian, A., Roscoe, J., Preston, K. E., Lambert, J. C., Hermans, C., Decuyper, W., Dzienus, S., Winterrath, T., Burrows, J., Goutail, F., Pommereau, J. P., D'Almeida, E., Hottier, J., Coureul, C., Didier, R., Pundt, I., Bartlett, L. M., McElroy, C. T., Kerr, J. E., Elokhov, A., Giovanelli, G., Ravegnani, F., Premuda, M., Kostadinov, I., Erle, F., Wagner, T., Pfeilsticker, K., Kenntner, M., Marquard, L. C., Gil, M., Puentedura, O., Yela, M., Arlander, D. W., Kastad Hoiskar, B. A., Tellefsen, C. W., Karlsen Tornqvist, K., Heese, B., Jones, R. L., Aliwell, S. R., and Freshwater, R. A.: Slant column measurements of O3 and NO2 during the NDSC intercomparison of zenith-sky UV-visible spectrometers in june 1996, J. Atmos. Chem., 32, 281–314, 1999.
SAOZ: http://www.aero.jussieu.fr/themes/CA/Reseau_SAOZ.html, 2007.
Sarkissian, A., Fish, D., Van Roozendael, M., Gil, M., Chen, H. B., Wang, P., Pommereau, J. P., and Lenoble, J.: Ozone and NO<sub>2</sub> air-mass factors for zenith-sky spectrometers: Intercomparison of calculations with different radiative transfer models, Geophys. Res. Lett., 22, 1113–1116, 1995a.
Sarkissian, A., Roscoe, H. K., and Fish, D.: Ozone measurements by zenith-sky spectrometers: an evaluation of errors in air-mass factors calculated by radiative transfer models, J. Quant. Spectrosc. Ra., 54, 471–480, 1995b.
Schneider, M., Blumenstock, T., Chipperfield, M. P., Hase, F., Kouker, W., Reddmann, T., Ruhnke, R., Cuevas, E., and Fischer, H.: Subtropical trace gas profiles determined by ground-based FTIR spectroscopy at Izaña (28° N, 16° W): Five-year record, error analysis, and comparison with 3-D CTMs, Atmos. Chem., Phys., 5, 153–167, 2005.
Solomon, S., Russell III, J. M., and Gordley, L. L.: Observations of the diurnal variation of Nitrogen dioxide in the stratosphere, J. Geophys. Res., 91(D5), 5455–5464, 1986.
Solomon, S., Schmeltekopft, A. L., and Sanders, R. W.: On the interpretation of zenith sky absorption measurements, J. Geophys. Res., 92(D7), 8311–8319, 1987.
Solomon, S., Sanders, R. W., Jakoubek, R. O., Arpag, K. H., Stephens, S. L., Keys, J. G., and Garcia, R. R.: Visible and near-ultraviolet spectroscopy at McMurdo Station, Antarctica. 10. Reductions of statospheric NO<sub>2</sub> due to Pinatubo aerosols, J. Geophys. Res., 99(D2), 3509–3516, 1994.
Struthers, H., Kreher, K., Austin, J., Schonfield, R., Bodecker, G., Johnston, P., Shiona, H., and Thomas, A.: Past and future suimulations of NO<sub>2</sub> from a coupled chemistry-climate model in comparison with observations, Atmos. Chem. Phys., 4, 2227–2239, 2004.
Sussmann, R., Stremme, W., Burrows, J. P., Richter, A., Seiler, W., and Rettinger, M.: Stratospheric and tropospheric NO<sub>2</sub> variability on the diurnal and annual scale: a combined retrieval from ENVISAT/SCIAMACHY and solar FTIR at the Permanent Ground-Truthing Facility Zugspitze/Garmisch, Atmos. Chem. Phys., 5, 2657–2677, 2005.
Van Roozendael, M., De Mazière, M., Hermans, C., Simon, P. C., Pommereau, J.-P., Goutail, F., Tie, X.X., Brasseur, G., and Granier, C.: Ground-Based observations of stratospheric NO<sub>2</sub> at high and mid-latitudes in Europe after the Mount Pinatubo eruption, J. Geophys Res., 102(D15), 19 171–19 176, 1997.
Vandaele, A. C., Hermans, C., Simon, P .C., Carleer, M., Colins, R., Fally, S., Mérienne, M. F., Jenouvrier, A., and Coquart, B.: Measurements of the NO<sub>2</sub> absorption cross-sections from 42000 cm<sup>−1</sup> to 10000 cm<sup>−1</sup> (238–1000 nm) at 220 K and 294 K, J. Quant. Spectrosc. Radiat. Transfer, 59, 171–184, 1998.
Vandaele, A. C., Fayt, C., Hendrick, F., Hermans, C., Humbled, F., Van Roozendael, M., Gil, M., Navarro, M., Puentedura, O., Yela, M., Braathen, G., Stebel, K., Tørnkvist, K., Johnston, P., Kreher, K., Goutail, F., Mieville, A., Pommereau, J.-P., Khaikine, S., Richter, A., Oetjen, H., Wittrock, F., Bugarski, S., Friess, U., Pfeilsticker, K., Sinreich, R., Wagner, T., Corlett, G., and Leigh, R.: An intercomparison campaign of ground-based UV-Visible measurements of NO<sub>2</sub>, BrO, and OClO slant columns. I. NO<sub>2</sub>, J. Geophys. Res., 110(D8), D08305, doi:10.1029/2004JD005423, 2005.
Wetzel, G., Bracher, A., Funke, B., Goutail, F., Hendrick, F., Lambert, J.-C., Mikuteit, S., Piccolo, C., Pirre, M., Bazureau, A., Belotti, C., Blumenstock, T., De Mazière, M., Fischer, H., Huret, N., Ionov, D., López-Puertas, M., Maucher, G., Oelhaf, H., Pommereau, J.-P., Ruhnke, R., Sinnhuber, M., Stiller, G., Van Roozendael, M., and Zhang, G.: Validation of MIPAS-ENVISAT NO<sub>2</sub> operational data, Atmos. Chem. Phys., 7, 3261–3284, 2007.
WMO (World Meteorological Organization): Scientific Assessment of Ozone Depletion, 2002, Global Ozone Research and Monitoring Project, Report No 47, 2003.
WMO (World Meteorological Organization): Scientific Assessment of Ozone Depletion: 2006, Global Ozone Research and Monitoring Project, Report No 50, 2007.
Yela, M., Gil, M., Navarro, M., Rodriguez, S., Cuevas E., and Romero, C.: Meridional transport in the subtropics during winter as seen by NO<sub>2</sub> column record, Air Pollution Report 66, EUR 18032EN, edited by: Harris, N. R. P., Kilbane-Dawe, I., and Amanatidis, G. T., 88–91, 1998.
Yela., M., Gil, M., Rodríguez, S., Araujo, J., Ochoa, H., Díaz, S., and Deferrari, G.: Unusual behavior of stratospheric NO<sub>2</sub> during splitting vortex event in the Antarctic winter 2002: Comparison with a 10-years NO<sub>2</sub> climatology at three Antarctic and sub Antarctic sites, Proc. Quadrennial Ozone Symposium, 1055, 1–8 June 2004, Kos, Greece, 2004.