scholarly journals An evaluation of chemistry's role in the winter-spring ozone maximum found in the northern midlatitude free troposphere

1999 ◽  
Vol 104 (D3) ◽  
pp. 3655-3667 ◽  
Author(s):  
J. J. Yienger ◽  
A. A. Klonecki ◽  
H. Levy ◽  
W. J. Moxim ◽  
G. R. Carmichael
1988 ◽  
Vol 27 (3) ◽  
pp. 269-279 ◽  
Author(s):  
G. S. Kent ◽  
U. O. Farrukh ◽  
P. H. Wang ◽  
A. Deepak

2010 ◽  
Vol 10 (21) ◽  
pp. 10639-10654 ◽  
Author(s):  
C. S. Bretherton ◽  
R. Wood ◽  
R. C. George ◽  
D. Leon ◽  
G. Allen ◽  
...  

Abstract. Multiplatform airborne, ship-based, and land-based observations from 16 October–15 November 2008 during the VOCALS Regional Experiment (REx) are used to document the typical structure of the Southeast Pacific stratocumulus-topped boundary layer and lower free troposphere on a~transect along 20° S between the coast of Northern Chile and a buoy 1500 km offshore. Strong systematic gradients in clouds, precipitation and vertical structure are modulated by synoptically and diurnally-driven variability. The boundary layer is generally capped by a strong (10–12 K), sharp inversion. In the coastal zone, the boundary layer is typically 1 km deep, fairly well mixed, and topped by thin, nondrizzling stratocumulus with accumulation-mode aerosol and cloud droplet concentrations exceeding 200 cm−3. Far offshore, the boundary layer depth is typically deeper (1600 m) and more variable, and the vertical structure is usually decoupled. The offshore stratocumulus typically have strong mesoscale organization, much higher peak liquid water paths, extensive drizzle, and cloud droplet concentrations below 100 cm−3, sometimes with embedded pockets of open cells with lower droplet concentrations. The lack of drizzle near the coast is not just a microphysical response to high droplet concentrations; smaller cloud depth and liquid water path than further offshore appear comparably important. Moist boundary layer air is heated and mixed up along the Andean slopes, then advected out over the top of the boundary layer above adjacent coastal ocean regions. Well offshore, the lower free troposphere is typically much drier. This promotes strong cloud-top radiative cooling and stronger turbulence in the clouds offshore. In conjunction with a slightly cooler free troposphere, this may promote stronger entrainment that maintains the deeper boundary layer seen offshore. Winds from ECMWF and NCEP operational analyses have an rms difference of only 1 m s−1 from collocated airborne leg-mean observations in the boundary layer and 2 m s−1 above the boundary layer. This supports the use of trajectory analysis for interpreting REx observations. Two-day back-trajectories from the 20° S transect suggest that eastward of 75° W, boundary layer (and often free-tropospheric) air has usually been exposed to South American coastal aerosol sources, while at 85° W, neither boundary-layer or free-tropospheric air has typically had such contact.


2013 ◽  
Author(s):  
Jonathan Duplissy ◽  
Joonas Merikanto ◽  
Karine Sellegri ◽  
Clemence Rose ◽  
Eija Asmi ◽  
...  

2008 ◽  
Vol 8 (11) ◽  
pp. 2999-3014 ◽  
Author(s):  
A. van Donkelaar ◽  
R. V. Martin ◽  
W. R. Leaitch ◽  
A. M. Macdonald ◽  
T. W. Walker ◽  
...  

Abstract. We interpret a suite of satellite, aircraft, and ground-based measurements over the North Pacific Ocean and western North America during April–May 2006 as part of the Intercontinental Chemical Transport Experiment Phase B (INTEX-B) campaign to understand the implications of long-range transport of East Asian emissions to North America. The Canadian component of INTEX-B included 33 vertical profiles from a Cessna 207 aircraft equipped with an aerosol mass spectrometer. Long-range transport of organic aerosols was insignificant, contrary to expectations. Measured sulfate plumes in the free troposphere over British Columbia exceeded 2 μg/m3. We update the global anthropogenic emission inventory in a chemical transport model (GEOS-Chem) and use it to interpret the observations. Aerosol Optical Depth (AOD) retrieved from two satellite instruments (MISR and MODIS) for 2000–2006 are analyzed with GEOS-Chem to estimate an annual growth in Chinese sulfur emissions of 6.2% and 9.6%, respectively. Analysis of aircraft sulfate measurements from the NASA DC-8 over the central Pacific, the NSF C-130 over the east Pacific and the Cessna over British Columbia indicates most Asian sulfate over the ocean is in the lower free troposphere (800–600 hPa), with a decrease in pressure toward land due to orographic effects. We calculate that 56% of the measured sulfate between 500–900 hPa over British Columbia is due to East Asian sources. We find evidence of a 72–85% increase in the relative contribution of East Asian sulfate to the total burden in spring off the northwest coast of the United States since 1985. Campaign-average simulations indicate anthropogenic East Asian sulfur emissions increase mean springtime sulfate in Western Canada at the surface by 0.31 μg/m3 (~30%) and account for 50% of the overall regional sulfate burden between 1 and 5 km. Mean measured daily surface sulfate concentrations taken in the Vancouver area increase by 0.32 μg/m3 per 10% increase in the simulated fraction of Asian sulfate, and suggest current East Asian emissions episodically degrade local air quality by more than 1.5 μg/m3.


2015 ◽  
Vol 15 (12) ◽  
pp. 7085-7102 ◽  
Author(s):  
N. L. Wagner ◽  
C. A. Brock ◽  
W. M. Angevine ◽  
A. Beyersdorf ◽  
P. Campuzano-Jost ◽  
...  

Abstract. Vertical profiles of submicron aerosol from in situ aircraft-based measurements were used to construct aggregate profiles of chemical, microphysical, and optical properties. These vertical profiles were collected over the southeastern United States (SEUS) during the summer of 2013 as part of two separate field studies: the Southeast Nexus (SENEX) study and the Study of Emissions and Atmospheric Composition, Clouds, and Climate Coupling by Regional Surveys (SEAC4RS). Shallow cumulus convection was observed during many profiles. These conditions enhance vertical transport of trace gases and aerosol and create a cloudy transition layer on top of the sub-cloud mixed layer. The trace gas and aerosol concentrations in the transition layer were modeled as a mixture with contributions from the mixed layer below and the free troposphere above. The amount of vertical mixing, or entrainment of air from the free troposphere, was quantified using the observed mixing ratio of carbon monoxide (CO). Although the median aerosol mass, extinction, and volume decreased with altitude in the transition layer, they were ~10 % larger than expected from vertical mixing alone. This enhancement was likely due to secondary aerosol formation in the transition layer. Although the transition layer enhancements of the particulate sulfate and organic aerosol (OA) were both similar in magnitude, only the enhancement of sulfate was statistically significant. The column integrated extinction, or aerosol optical depth (AOD), was calculated for each individual profile, and the transition layer enhancement of extinction typically contributed less than 10 % to the total AOD. Our measurements and analysis were motivated by two recent studies that have hypothesized an enhanced layer of secondary aerosol aloft to explain the summertime enhancement of AOD (2–3 times greater than winter) over the southeastern United States. The first study attributes the layer aloft to secondary organic aerosol (SOA) while the second study speculates that the layer aloft could be SOA or secondary particulate sulfate. In contrast to these hypotheses, the modest enhancement we observed in the transition layer was not dominated by OA and was not a large fraction of the summertime AOD.


2016 ◽  
Vol 16 (3) ◽  
pp. 702-716 ◽  
Author(s):  
Evelyn Freney ◽  
Sellegri Karine Sellegri Karine ◽  
Asmi Eija ◽  
Rose Clemence ◽  
Chauvigne Aurelien ◽  
...  

2017 ◽  
Vol 17 (17) ◽  
pp. 10259-10268 ◽  
Author(s):  
Lorena Moreira ◽  
Klemens Hocke ◽  
Niklaus Kämpfer

Abstract. Stratospheric and middle-mesospheric ozone profiles above Bern, Switzerland (46.95° N, 7.44° E; 577 m) have been continually measured by the GROMOS (GROund-based Millimeter-wave Ozone Spectrometer) microwave radiometer since 1994. GROMOS is part of the Network for the Detection of Atmospheric Composition Change (NDACC). A new version of the ozone profile retrievals has been developed with the aim of improving the altitude range of retrieval profiles. GROMOS profiles from this new retrieval version have been compared to coincident ozone profiles obtained by the satellite limb sounder Aura Microwave Limb Sounder (MLS). The study covers the stratosphere and middle mesosphere from 50 to 0.05 hPa (from 21 to 70 km) and extends over the period from July 2009 to November 2016, which results in more than 2800 coincident profiles available for the comparison. On average, GROMOS and MLS comparisons show agreement generally over 20 % in the lower stratosphere and within 2 % in the middle and upper stratosphere for both daytime and nighttime, whereas in the mesosphere the mean relative difference is below 40 % during the daytime and below 15 % during the nighttime. In addition, we have observed the annual variation in nighttime ozone in the middle mesosphere, at 0.05 hPa (70 km), characterized by the enhancement of ozone during wintertime for both ground-based and space-based measurements. This behaviour is related to the middle-mesospheric maximum in ozone (MMM).


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