Gj. Roelofs et J. Lelieveld, DISTRIBUTION AND BUDGET OF O-3 IN THE TROPOSPHERE CALCULATED WITH A CHEMISTRY GENERAL-CIRCULATION MODEL, JOURNAL OF GEOPHYSICAL RESEARCH-ATMOSPHERES, 100(D10), 1995, pp. 20983-20998
We present results of global tropospheric chemistry simulations with t
he coupled chemistry/atmospheric general circulation model ECHAM. Ulti
mately, the model will be used to study climate changes induced by ant
hropogenic influences on the chemistry of the atmosphere; meteorologic
al parameters that are important for the chemistry, such as temperatur
e, humidity, air motions, cloud and lain characteristics, and mixing p
rocesses are calculated on-line. The chemical part of the model descri
bes background tropospheric CH4-CO-NOx-HOx photochemistry. Emissions o
f NO and CO, surface concentrations of CH4, and stratospheric concentr
ations of O-3 and NOy are prescribed as boundary conditions. Calculati
ons of the tropospheric O-3 budget indicate that seasonal variabilitie
s of the photochemical production and of injection from the stratosphe
re are represented realistically, although some aspects of the model s
till need improvement. Comparisons of calculated O-3 surface concentra
tions and O-3 profiles with available measurements show that the model
reproduces O-3 distributions in remote tropical and midlatitudinal si
tes. Also, the model matches typical profiles connected with deep conv
ection in the Intertropical Convergence Zone (ITCZ). However, the mode
l tends to underestimate O-3 concentrations at the poles and in relati
vely polluted regions. These underestimates are caused by the poor rep
resentation of tropopause foldings in midlatitudes, which form a signi
ficant source of tropospheric O-3 from the stratosphere, too weak tran
sport to the poles, and the neglect of higher hydrocarbon chemistry. A
lso, mixing of polluted continental boundary layer air into the free t
roposphere may be underestimated. We discuss how these model deficienc
ies will be improved in the future.