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JOURNAL OF GEOPHYSICAL RESEARCH, VOL. 110, D08304, doi:10.1029/2004JD005537, 2005

Tropospheric ozone evolution between 1890 and 1990

J.-F. Lamarque

Atmospheric Chemistry Division, National Center for Atmospheric Research, Boulder, Colorado, USA


P. Hess

Atmospheric Chemistry Division, National Center for Atmospheric Research, Boulder, Colorado, USA


L. Emmons

Atmospheric Chemistry Division, National Center for Atmospheric Research, Boulder, Colorado, USA


L. Buja

Climate and Global Dynamics Division, National Center for Atmospheric Research, Boulder, Colorado, USA


W. Washington

Climate and Global Dynamics Division, National Center for Atmospheric Research, Boulder, Colorado, USA


C. Granier

Service d'Aéronomie, Institut Pierre-Simon Laplace, Paris, France


Abstract

In this study, we have performed a set of simulations to detail the evolution of tropospheric ozone from 1890 to 1990. The simulations are compared with available measurements for present-day conditions and earlier. Using our best estimates of ozone precursors emissions (based on the work by van Aardenne et al. (2001)), we have found a tropospheric ozone burden increase of 71 Tg between 1890 and 1990, an increase of ∼30%. When no anthropogenic emissions in 1890 are considered, this burden increase reaches 88 Tg. The ozone lifetime is shown to have decreased by ∼30%, especially after 1930. It is also shown that the net chemical production in the lower troposphere exceeded that in the free troposphere for the first time in the 1950–1970 period. In addition, the ozone production in this study increased rapidly between 1890 and 1930 and from 1970 to 1990. However, the ozone production efficiency in the troposphere is shown to have decreased during the 20th century, making the troposphere less NOx limited. Finally, a decrease in the OH burden is estimated to be on the order of 8%, matched by a similar increase in the CO lifetime.

Received 21 October 2004; accepted 3 February 2005; published 26 April 2005.

Keywords: tropospheric ozone; preindustrial ozone; ozone budget.

Index Terms: 0365 Atmospheric Composition and Structure: Troposphere: composition and chemistry; 0322 Atmospheric Composition and Structure: Constituent sources and sinks; 0325 Atmospheric Composition and Structure: Evolution of the atmosphere (1610, 8125).

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Citation: Lamarque, J.-F., P. Hess, L. Emmons, L. Buja, W. Washington, and C. Granier (2005), Tropospheric ozone evolution between 1890 and 1990, J. Geophys. Res., 110, D08304, doi:10.1029/2004JD005537.