A global climate‐chemistry model study of present‐day tropospheric chemistry and radiative forcing from changes in tropospheric O 3 since the preindustrial period
We present simulations of present‐day tropospheric O 3 and of changes in its concentrations and the associated radiative forcing since the industrial revolution. Numerical experiments were conducted using a global tropospheric climate‐chemistry model (GCCM) developed by incorporating the University...
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Veröffentlicht in: | Journal of Geophysical Research: Atmospheres 2004-06, Vol.109 (D11) |
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Hauptverfasser: | , , , , |
Format: | Artikel |
Sprache: | eng |
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Zusammenfassung: | We present simulations of present‐day tropospheric O
3
and of changes in its concentrations and the associated radiative forcing since the industrial revolution. Numerical experiments were conducted using a global tropospheric climate‐chemistry model (GCCM) developed by incorporating the University of Oslo (UiO) photochemical module (a reduced tracer scheme that lumps nonmethane volatile organic compounds (NMVOCs) to simulate the CO‐NO
x
‐HO
x
‐O
3
system) into State University of New York at Albany–Community Climate Model 3 (SUNYA CCM3). The GCCM was run with emissions of pollutants corresponding to two periods, the early 1990s and the preindustrial period, and the simulated tropospheric O
3
is used for off‐line calculations of radiative forcing. The study consists of two parts: an evaluation of the GCCM‐simulated present‐day distributions of tropospheric chemical species with sensitivity experiments to test the effects of NO production by lightning and stratospheric O
3
influx on the simulated results, and the radiative forcing due to O
3
changes since the industrial revolution. The model can reproduce the temporal and spatial variations of O
3
precursors, including CO and NO
x
(NO + NO
2
), in the Northern Hemisphere (NH), although there are biases such as the larger CO concentrations in the Southern Hemisphere (SH) and the smaller NO
x
concentrations in the tropical middle‐upper troposphere. The simulated OH concentrations are sensitive to the NO production by lightning. The simulated concentrations of tropospheric OH have a global and annual average of about 9.8 × 10
5
molecules/cm
3
(corresponding to a tropospheric CH
4
lifetime due to OH of 8.6 years), when the annual production of NO by lightning is about 6 TgN/yr. Compared with O
3
sonde climatology, the model can simulate the seasonal variations of lower to middle tropospheric O
3
within the observed interannual variations when the stratospheric O
3
influx is about 600 Tg/yr, although detailed biases exist in the middle troposphere during fall to winter and in the continental boundary layer during summer. The present‐day tropospheric O
3
burden is calculated to be about 376 Tg (or 34 DU) with a net tropospheric chemical production of about 513 Tg/yr. Using realistic stratospheric O
3
concentrations instead of a prescribed O
3
influx as the upper boundary condition enhances the model biases in the extratropical upper‐middle tropospheric O
3
concentrations. The model calculates a globally and annua |
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ISSN: | 0148-0227 |
DOI: | 10.1029/2003JD003998 |