Convective transport over the central United States and its role in regional CO and ozone budgets

We have constructed a regional budget for boundary layer carbon monoxide over the central United States (32.5°–50°N, 90°–105°W), emphasizing a detailed evaluation of deep convective vertical fluxes appropriate for the month of June. Deep convective venting of the boundary layer (upward) dominates other components of the CO budget, e.g., downward convective transport, loss of CO by oxidation, anthropogenic emissions, and CO produced from oxidation of methane, isoprene, and anthropogenic nonmethane hydrocarbons (NMHCs). Calculations of deep convective venting are based on the method of Pickering et al. [1992a] which uses a satellite-derived deep convective cloud climatology along with transport statistics from convective cloud model simulations of observed prototype squall line events. This study uses analyses of convective episodes in 1985 and 1989 and CO measurements taken during several midwestern field campaigns. Deep convective venting of the boundary layer over this moderately polluted region provides a net (upward minus downward) flux of 18.1×108kg CO month−1 to the free troposphere during early summer, assuming the June statistics are typical. Shallow cumulus and synoptic-scale weather systems together make a comparable contribution (total net flux 16.2×108 kg CO month−1). Boundary layer venting of CO with other O3 precursors leads to efficient free tropospheric O3 formation. We estimate that deep convective transport of CO and other precursors over the central United States in early summer leads to a gross production of 0.66–1.1 Gmol O3 d−1 in good agreement with estimates of O3 production from boundary layer venting in a continental-scale model [Jacob et al., 1993a, b]. In this respect the central U.S. region acts as a “chimney” for the country, and presumably this O3 contributes to high background levels of O3 in the eastern United States and O3 export to the North Atlantic.

[1]  R. Dickerson,et al.  Modification of a Commercial Gas Filter Correlation CO Detector for Enhanced Sensitivity , 1988 .

[2]  R. Dickerson,et al.  Trace gas transport in the vicinity of frontal convective clouds , 1988 .

[3]  R. Dickerson,et al.  Model calculations of tropospheric ozone production potential following observed convective events , 1990 .

[4]  H. Sievering,et al.  Airborne sampling of selected trace chemicals above the central United States , 1989 .

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

[6]  C. Sui,et al.  Heating, Moisture, and Water Budgets of Tropical and Midlatitude Squall Lines: Comparisons and Sensitivity to Longwave Radiation , 1993 .

[7]  Joanne Simpson,et al.  Goddard Cumulus Ensemble Model. Part I: Model Description , 1993 .

[8]  Anne M. Thompson,et al.  Free tropospheric ozone production following entrainment of urban plumes into deep convection , 1992 .

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

[10]  M. Chin,et al.  Relationship of ozone and carbon monoxide over North America , 1994 .

[11]  D. Jacob,et al.  Simulation of summertime ozone over North America , 1993 .

[12]  John S. Holloway,et al.  Export of North American Ozone Pollution to the North Atlantic Ocean , 1993, Science.

[13]  George C. Holzworth,et al.  ESTIMATES OF MEAN MAXIMUM MIXING DEPTHS IN THE CONTIGUOUS UNITED STATES , 1964 .

[14]  A. Gertler,et al.  Comparison of the SCAQS Tunnel Study with Other On Road Vehicle Emission Data , 1990 .

[15]  R. Dickerson,et al.  Tropospheric Chemistry Over the Lower Great Plains of the United States 2. Trace Gas Profiles and Distributions , 1992 .

[16]  Russell R. Dickerson,et al.  Trace gas concentrations and meteorology in rural Virginia: 1. Ozone and carbon monoxide , 1991 .

[17]  Alan C. Lloyd,et al.  A chemical mechanism for use in long‐range transport/acid deposition computer modeling , 1986 .

[18]  R. Dickerson,et al.  Clear-sky vertical profiles of trace gases as influenced by upstream convective activity , 1989 .

[19]  P. Hanst,et al.  Carbon monoxide production in photooxidation of organic molecules in the air , 1980 .

[20]  B. Anderson,et al.  Airborne boundary layer flux measurements of trace species over Canadian boreal forest and northern wetland regions , 1994 .

[21]  V. Kirchhoff,et al.  Surface carbon monoxide measurements in Amazonia , 1990 .

[22]  Jack Fishman,et al.  Distribution of tropospheric ozone determined from satellite data , 1990 .

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

[24]  R. Dickerson,et al.  Thunderstorms: An Important Mechanism in the Transport of Air Pollutants , 1987, Science.

[25]  Alan Stern The Pluto reconnaissance flyby mission , 1993 .

[26]  W. Tao,et al.  A regional estimate of convective transport of CO from biomass burning , 1992 .

[27]  David D. Parrish,et al.  Assessment of pollutant emission inventories by principal component analysis of ambient air measurements , 1992 .

[28]  Roland B. Stull,et al.  A Fair-Weather Cumulus Cloud Classification Scheme for Mixed-Layer Studies , 1985 .

[29]  W. Rossow,et al.  ISCCP Cloud Data Products , 1991 .

[30]  P. Crutzen,et al.  Estimates on the production of CO and H2 from the oxidation of hydrocarbon emissions from vegetation , 1978 .

[31]  D. Fahey,et al.  Ozone production in the rural troposphere and the implications for regional and global ozone distributions , 1987 .

[32]  B. Doddridge,et al.  The gradient of meteorological and chemical variables across the tropopause , 1994 .

[33]  Dennis L. Hartmann,et al.  Spurious changes in the ISCCP dataset , 1993 .

[34]  Wolfgang Seiler,et al.  The cycle of atmospheric CO. , 1974 .