Analysis of 1970-1995 Trends in Tropospheric Ozone at Northern Hemisphere Midlatitudes with the GEOS-CHEM Model

[1] The causes of trends in tropospheric ozone at Northern Hemisphere midlatitudes from 1970 to 1995 are investigated with the GEOS-CHEM model, a global three-dimensional model of the troposphere driven by assimilated meteorological observations from the Goddard Earth Observing System (GEOS). This model is used to investigate the sensitivity of tropospheric ozone with respect to (1) changes in the anthropogenic emission of nitrogen oxides and nonmethane hydrocarbons, (2) increases in methane concentrations, (3) variations in the stratospheric source of ozone, (4) changes in solar radiation resulting from stratospheric ozone depletion, and (5) increases in tropospheric temperatures. Model results indicate that local increases in NOx emissions have caused most of the increases seen in lower tropospheric ozone over Europe and Japan. Increases in methane are responsible for roughly one fifth of the anthropogenically induced increase in tropospheric ozone at northern midlatitudes. However, changes in ozone precursors do not adequately explain either the spatial differences in observed ozone trends across midlatitudes or the observed decreases in ozone over Canada throughout the troposphere. We argue that ozone depletion in the lowermost stratosphere is likely to have reduced the stratospheric source by as much as 30% from the early 1970s to the mid 1990s. Model simulations that account for such a reduction along with reported changes in anthropogenic emissions show steep declines of ozone in the upper troposphere and variable increases in the lower troposphere that are more consistent with observations. Differential temperature trends in summer between North America and Europe may account for at least some of the remaining spatial variation in tropospheric ozone trends. Increases in ultraviolet (UV) radiation due to stratospheric ozone depletion do not appear to significantly reduce tropospheric ozone, except at midlatitudes in the Southern Hemisphere following the breakup of the ozone hole.

[1]  I. Isaksen,et al.  Effects of reductions in stratospheric ozone on tropospheric chemistry through changes in photolysis rates , 1994 .

[2]  Changes in solar radiation fluxes after the Pinatubo eruption , 1994 .

[3]  J. Dibb,et al.  Beryllium 7 and Lead 210 in the western hemisphere Arctic atmosphere : Observations from three recent aircraft-based sampling programs , 2019 .

[4]  David W. Fahey,et al.  An estimate of the flux of stratospheric reactive nitrogen and ozone into the troposphere , 1994 .

[5]  C. McLinden,et al.  Stratospheric N2O–NO y system: Testing uncertainties in a three‐dimensional framework , 2001 .

[6]  Global simulation of tropospheric O3-NOx-hydrocarbon chemistry: 1. Model formulation , 1998 .

[7]  P. Rasch,et al.  MOZART, a global chemical transport model for ozone , 1998 .

[8]  P. Groisman,et al.  Cloudiness variations over the former Soviet Union , 2000 .

[9]  Oliver Wild,et al.  Fast-J: Accurate Simulation of In- and Below-Cloud Photolysis in Tropospheric Chemical Models , 2000 .

[10]  A. Bouwman,et al.  Description of EDGAR Version 2.0: A set of global emission inventories of greenhouse gases and ozone-depleting substances for all anthropogenic and most natural sources on a per country basis and on 1 degree x 1 degree grid , 1996 .

[11]  R. Martin,et al.  Sources of tropospheric ozone along the Asian Pacific Rim: An analysis of ozonesonde observations , 2002 .

[12]  E. Dlugokencky,et al.  Atmospheric chemistry and greenhouse gases , 2001 .

[13]  F. Giorgi,et al.  Is ozone pollution affecting crop yields in China? , 1999 .

[14]  Makiko Sato,et al.  GISS analysis of surface temperature change , 1999 .

[15]  S. Baughcum,et al.  Scheduled civil aircraft emission inventories for 1992: Database development and analysis , 1996 .

[16]  Allen S. Lefohn,et al.  THE DIFFICULT CHALLENGE OF ATTAINING EPA'S NEW OZONE STANDARD , 1998 .

[17]  R. McKenzie,et al.  Decay of Mount Pinatubo aerosol at midlatitudes in the northern and southern hemispheres , 1994 .

[18]  Sanford Sillman,et al.  The sensitivity of ozone to nitrogen oxides and hydrocarbons in regional ozone episodes , 1990 .

[19]  D. Jacob,et al.  Global simulation of tropospheric O3-NOx-hydrocarbon chemistry , 1998 .

[20]  D. Jacob,et al.  Asian chemical outflow to the Pacific in spring: Origins, pathways, and budgets , 2001 .

[21]  D. Jacob,et al.  Long‐term trends in ground level ozone over the contiguous United States, 1980–1995 , 1998 .

[22]  I. Isaksen,et al.  Effects of reductions in stratospheric ozone on tropospheric chemistry through changes in photolysis rates: EFFECTS OF REDUCTIONS IN STRATOSPHERIC OZONE , 1994 .

[23]  V. Grewe The origin of ozone , 2005 .

[24]  S. Chandra,et al.  An 11‐year solar cycle in tropospheric ozone from TOMS measurements , 1999 .

[25]  S. Madronich,et al.  Tropospheric Chemistry Changes Due to Increased UV-B Radiation , 1994 .

[26]  P. Kasibhatla,et al.  The global impact of human activity on tropospheric ozone , 1997 .

[27]  Dale P. Kaiser,et al.  Analysis of total cloud amount over China, 1951–1994 , 1998 .

[28]  J. Houghton,et al.  Climate change 1995: the science of climate change. , 1996 .

[29]  Hajime Akimoto,et al.  Distribution of SO2, NOx and CO2 emissions from fuel combustion and industrial activities in Asia with 1° × 1° resolution , 1994 .

[30]  J. Houghton,et al.  Climate change 2001 : the scientific basis , 2001 .

[31]  Paul C. Johnson Assessment of the Contributions of Volatilization and Biodegradation to in Situ Air Sparging Performance , 1998 .

[32]  G. C. Tiao,et al.  Analysis of long-term behavior of ultraviolet radiation measured by Robertson-Berger meters at 14 sites in the United States , 1997 .

[33]  Stuart A. Penkett,et al.  Comparison of calculated and measured peroxide data collected in marine air to investigate prominent features of the annual cycle of ozone in the troposphere , 1998 .

[34]  Jos Lelieveld,et al.  A three-dimensional chemistry/general circulation model simulation of anthropogenically derived ozone in the troposphere and its radiative climate forcing , 1997 .

[35]  B. Hannegan,et al.  Stratospheric ozone in 3-D models : A simple chemistry and the cross-tropopause flux , 2000 .

[36]  P. Crutzen A discussion of the chemistry of some minor constituents in the stratosphere and troposphere , 1973 .

[37]  Michael O. Rodgers,et al.  Correlation of ozone with NOy in photochemically aged air , 1993 .

[38]  D. Jacob,et al.  Export of reactive nitrogen from North America during summertime: Sensitivity to hydrocarbon chemistry , 1998 .

[39]  Yuhang Wang,et al.  Seasonal budgets of reactive nitrogen species and ozone over the United States, and export fluxes to the global atmosphere , 1998 .

[40]  J. Holton,et al.  Stratosphere‐troposphere exchange , 1995 .

[41]  D. Jacob,et al.  Global impact of fossil fuel combustion on atmospheric NOx , 1999 .

[42]  Andrew Gettelman,et al.  Mass fluxes of O3, CH4, N2O and CF2Cl2 in the lower stratosphere calculated from observational data , 1997 .

[43]  Peter H. Stone,et al.  Efficient Three-Dimensional Global Models for Climate Studies: Models I and II , 1983 .

[44]  Stephen D. Piccot,et al.  A global inventory of volatile organic compound emissions from anthropogenic sources , 1992 .

[45]  Sander Houweling,et al.  The impact of nonmethane hydrocarbon compounds on tropospheric photochemistry , 1998 .

[46]  E. Danielsen,et al.  Stratospheric-Tropospheric Exchange Based on Radioactivity, Ozone and Potential Vorticity , 1968 .

[47]  Mark Lawrence,et al.  A model for studies of tropospheric photochemistry: Description, global distributions, and evaluation , 1999 .

[48]  Randel,et al.  Trends in the vertical distribution of ozone , 1999, Science.

[49]  G. Mégie,et al.  Climatology of tropospheric ozone in southern Europe and its relation to potential vorticity , 1994 .

[50]  J. Pages,et al.  Evidence of a long‐term increase in tropospheric ozone from Pic du Midi data series: Consequences: Positive radiative forcing , 1994 .

[51]  Jennifer A. Logan,et al.  An analysis of ozonesonde data for the troposphere : recommendations for testing 3-D models and development of a gridded climatology for tropospheric ozone , 1999 .

[52]  P. Samson,et al.  Impact of temperature on oxidant photochemistry in urban, polluted rural and remote environments , 1995 .

[53]  S. Sillman The relation between ozone, NOx and hydrocarbons in urban and polluted rural environments , 1999 .

[54]  M. Wirth,et al.  Scientific Assessment of Ozone Depletion: 1998 , 1999 .

[55]  J. Kerr,et al.  Evidence for Large Upward Trends of Ultraviolet-B Radiation Linked to Ozone Depletion , 1993, Science.

[56]  Jennifer A. Logan,et al.  Trends in the vertical distribution of ozone: An analysis of ozonesonde data , 1994 .

[57]  D. Stedman,et al.  Tropospheric ozone: Coupling transport and photochemistry , 1977 .

[58]  D. Wardle,et al.  Tropospheric ozone trends over Canada: 1980–1993 , 1995 .

[59]  Yuhang Wang,et al.  Anthropogenic forcing on tropospheric ozone and OH since preindustrial times , 1998 .

[60]  D. Jacob,et al.  Global modeling of tropospheric chemistry with assimilated meteorology : Model description and evaluation , 2001 .

[61]  V. Mohnen,et al.  Project dustorm report: ozone transport, in situ measurements, and meteorological analyses of tropopause folding , 1977 .

[62]  C. McLinden,et al.  Stratospheric N20-NOs system' Testing uncertainties , 2001 .

[63]  D. Jacob,et al.  Uncertainty in preindustrial abundance of tropospheric ozone: Implications for radiative forcing calculations , 2001 .

[64]  Yuhang Wang,et al.  Global simulation of tropospheric O3-NOx-hydrocarbon chemistry: 3. Origin of tropospheric ozone and effects of nonmethane hydrocarbons , 1998 .

[65]  James B. Kerr,et al.  Trends of ozone in the troposphere , 1998 .

[66]  S. Wofsy,et al.  In situ measurements constraining the role of sulphate aerosols in mid-latitude ozone depletion , 1993, Nature.

[67]  Michael O. Rodgers,et al.  Ozone precursor relationships in the ambient atmosphere , 1992 .

[68]  S. Oltmans,et al.  Ozone loss in the lower stratosphere over the United States in 1992-1993: Evidence for heterogeneous chemistry on the Pinatubo aerosol , 1994 .

[69]  D. Jacob,et al.  Constraints from 210Pb and 7Be on wet deposition and transport in a global three‐dimensional chemical tracer model driven by assimilated meteorological fields , 2001 .

[70]  K. Brice,et al.  The spring maximum in photo-oxidants in the Northern Hemisphere troposphere , 1986, Nature.

[71]  F. Vukovich,et al.  On the relationship between high ozone in the rural surface layer and high pressure systems , 1977 .

[72]  C. Junge Global ozone budget and exchange between stratosphere and troposphere , 1962 .

[73]  Hajime Akimoto,et al.  Intercontinental transport of ozone and its precursors in a three-dimensional global CTM , 2001 .

[74]  D. Schimel,et al.  Atmospheric Chemistry and Greenhouse Gases , 1999 .

[75]  Mark Lawrence,et al.  On the background photochemistry of tropospheric ozone , 1999 .

[76]  J. Lelieveld,et al.  A 1°×1° resolution data set of historical anthropogenic trace gas emissions for the period 1890–1990 , 2001 .

[77]  Richard B. Rood,et al.  An assimilated dataset for Earth science applications , 1993 .

[78]  T. Berntsen,et al.  Trend analysis of O3 and CO in the period 1980–1996: A three‐dimensional model study , 2000 .

[79]  S. Mckeen,et al.  A study of the dependence of rural ozone on ozone precursors in the eastern United States , 1991 .

[80]  Paul J. Crutzen,et al.  The origin of ozone in the troposphere , 1978, Nature.

[81]  D. Koch,et al.  Trends in tropospheric aerosol loads and corresponding impact on direct radiative forcing between 1950 and 1990: A model study , 2000 .

[82]  W. Viezee,et al.  The distribution of beryllium‐7 in the troposphere: Implications on stratospheric/tropospheric air exchange , 1980 .

[83]  David A. Neuschuler,et al.  Solar ultraviolet irradiance observed from southern Argentina: September 1990 to March 1991 , 1993 .

[84]  J. Lelieveld,et al.  Model study of the influence of cross-tropopause O3 transports on tropospheric O3 levels , 1997 .

[85]  Edward J. Dlugokencky,et al.  Atmospheric methane at Mauna Loa and Barrow observatories: Presentation and analysis of in situ measurements , 1995 .

[86]  T. Berntsen,et al.  A global three‐dimensional chemical transport model for the troposphere: 1. Model description and CO and ozone results , 1997 .

[87]  P. Crutzen,et al.  Observational and theoretical evidence in support of a significant in‐situ photochemical source of tropospheric ozone , 1979 .

[88]  P. Fabian,et al.  Meridional distribution of ozone in the troposphere and its seasonal variations , 1977 .

[89]  J. Lelieveld,et al.  What controls tropospheric ozone , 2000 .

[90]  Jos Lelieveld,et al.  Distribution and budget of O3 in the troposphere calculated with a chemistry general circulation model. , 1995 .

[91]  R. V. Dorland,et al.  Ozone chemistry changes in the troposphere and consequent radiative forcing of climate. , 1995 .

[92]  Steven L. Baughcum,et al.  Scheduled Civil Aircraft Emission Inventories for 1976 and 1984: Database Development and Analysis , 1996 .

[93]  D. Jacob,et al.  Background ozone over the United States in summer: Origin, trend, and contribution to pollution episodes , 2002 .

[94]  Daniel A. Jaffe,et al.  Influence of Asian emissions on the composition of air reaching the north western United States , 1999 .

[95]  M. Shearer,et al.  Trends of atmospheric methane during the 1960s and 1970s , 1989 .

[96]  T. V. Ommen,et al.  Observed climate variability and change , 2002 .

[97]  J. Dignon,et al.  GLOBAL EMISSIONS OF NITROGEN AND SULFUR OXIDES FROM 1860 TO 1980 , 1989 .

[98]  D. Etheridge,et al.  Changes in tropospheric methane between 1841 and 1978 from a high accumulation‐rate Antarctic ice core , 1992 .

[99]  A. Fiore,et al.  Increasing background ozone in surface air over the United States , 2000 .

[100]  S. Smyth,et al.  Observed distributions of nitrogen oxides in the remote free troposphere from the Nasa Global Tropospheric Experiment Programs , 2000 .

[101]  D. Jacob,et al.  Asian chemical outflow to the Pacific: origins, pathways and budgets , 2000 .

[102]  David Rind,et al.  Chemistry of the Global Troposphere' Fluorocarbons as Tracers of Air Motion , 2007 .

[103]  Daniel J. Jacob,et al.  Factors regulating ozone over the United States and its export to the global atmosphere , 1993 .

[104]  C. Appenzeller,et al.  Seasonal variation of mass transport across the tropopause , 1996 .

[105]  S. Wofsy,et al.  Tropospheric chemistry: A global perspective , 1981 .

[106]  H. Dop,et al.  Photochemical production of ozone in Western Europe (1971–1975) and its relation to meteorology , 1977 .

[107]  G. Brasseur,et al.  IMAGES: A three‐dimensional chemical transport model of the global troposphere , 1995 .

[108]  Xin-Zhong Liang,et al.  Atmospheric ozone as a climate gas , 1995 .

[109]  A. J. Miller,et al.  Global and zonal total ozone variations estimated from ground‐based and satellite measurements: 1964–2000 , 2002 .

[110]  J. Edwards,et al.  Future estimates of tropospheric ozone radiative forcing and methane turnover — The impact of climate change , 2000 .

[111]  S. Oltmans,et al.  Anomalous Antarctic ozone during 1992: Evidence for Pinatubo volcanic aerosol effects , 1993 .

[112]  Thomas E. Graedel,et al.  Global gridded inventories of anthropogenic emissions of sulfur and nitrogen , 1996 .

[113]  R. Martin,et al.  Interannual and seasonal variability of biomass burning emissions constrained by satellite observations , 2003 .

[114]  J. Logan,et al.  Effect of rising Asian emissions on surface ozone in the United States , 1999 .

[115]  David L. Greene,et al.  Aircraft Emissions: Current Inventories and Future Scenarios , 1999 .

[116]  Andreas Volz,et al.  Evaluation of the Montsouris series of ozone measurements made in the nineteenth century , 1988, Nature.