Dj. Jacob et al., FACTORS REGULATING OZONE OVER THE UNITED-STATES AND ITS EXPORT TO THEGLOBAL ATMOSPHERE, JOURNAL OF GEOPHYSICAL RESEARCH-ATMOSPHERES, 98(D8), 1993, pp. 14817-14826
The factors regulating summertime O3 over the United States and its ex
port to the global atmosphere are examined with a 3-month simulation u
sing a continental scale, three-dimensional photochemical model. It is
found that reducing NO(x) emissions by 50% from 1985 levels would dec
rease rural O3 concentrations over the eastern United States by about
15% under almost all meteorological conditions, while reducing anthrop
ogenic hydrocarbon emissions by 50% would have less than a 4% effect e
xcept in the largest urban plumes. The strongly NO(x)-limited conditio
ns in the model reflect the dominance of rural areas as sources of O3
on the regional scale. The correlation between O3 concentrations and t
emperature observed at eastern U.S. sites is attributed in part to the
association of high temperatures with regional stagnation, and in par
t to an actual dependence of O3 production on temperature driven prima
rily by conversion of NO(x) to peroxyacetylnitrate (PAN). The net numb
er of O3 molecules produced per molecule of NO(x) consumed (net O3 Pro
duction efficiency, accounting for both chemical production and chemic
al loss of O3) has a mean value of 6.3 in the U.S. boundary layer, it
is 3 times higher in the western United States than in the east becaus
e of lower NO(x) concentrations in the west. Approximately 70% of the
net chemical production of O3 in the U.S. boundary layer is exported (
the rest is deposited). Only 6% of the NO(x) emitted in the United Sta
tes is exported out of the U.S. boundary layer as NO(x) or PAN, but th
is export contributes disproportionately to total U.S. influence on gl
obal tropospheric O3 because of the high O3 production efficiency per
unit NO(x) in the remote troposphere. It is estimated that export of U
.S. pollution supplies 8 Gmol O3 d-1 to the global troposphere in summ
er, including 4 Gmol d-1 from direct export of O3 out of the U.S. boun
dary layer and 4 Gmol d-1 from production of O3 downwind of the United
States due to exported NO(x). This U.S. pollution source can be compa
red to estimates of 18-28 Gmol d-1 for the cross-tropopause transport
of O3 over the entire northern hemisphere in summer.