scholarly journals Supplementary material to "Age Spectra and Other Transport Diagnostics in the North American Monsoon UTLS from SEAC<sup>4</sup>RS In Situ Trace Gas Measurements"

Author(s):  
Eric A. Ray ◽  
Elliot L. Atlas ◽  
Sue Schauffler ◽  
Sofia Chelpon ◽  
Laura Pan ◽  
...  
2021 ◽  
Author(s):  
Eric A. Ray ◽  
Elliot L. Atlas ◽  
Sue Schauffler ◽  
Sofia Chelpon ◽  
Laura Pan ◽  
...  

Abstract. The upper troposphere and lower stratosphere (UTLS) during the summer monsoon season over North America (NAM) is influenced by the transport of air from a variety of source regions over a wide range of time scales (hours to years). Age spectra are useful for characterizing the transport into such a region and in this study we use and build on recently developed techniques to infer age spectra from trace gas measurements with photochemical lifetimes from days to centuries. We show that the measurements taken by the Whole Air Sampler instrument during the SEAC4RS campaign can be used to not only derive age spectra, but also path-integrated lifetimes of each of the trace gases and surface source regions. The method used here can also clearly identify and adjust for measurement outliers that were influenced by polluted surface source regions. The results are generally consistent with expected transport features of the NAM but also provide a range of transport diagnostics that have not previously been computed solely from in situ measurements. These methods may be applied to many other existing in situ datasets and the transport diagnostics can be compared with chemistry-climate model transport in the UTLS.


2021 ◽  
Author(s):  
Valentin Lauther ◽  
Johannes Wintel ◽  
Emil Gerhardt ◽  
Andrea Rau ◽  
Peter Hoor ◽  
...  

&lt;p&gt;Chlorinated very short-lived substances (Cl-VSLS) are not controlled by the Montreal Protocol but the recent emission increase of the Cl-VSLS CH&lt;sub&gt;2&lt;/sub&gt;Cl&lt;sub&gt;2&lt;/sub&gt; (Dichloromethane) and CHCl&lt;sub&gt;3&lt;/sub&gt; (Chloroform) is believed to significantly increase the stratospheric chlorine loading from VSLS. Provided efficient transport of Cl-VSLS from the source region into the stratosphere further emission increases could ultimately even cause a significant delay of the predicted recovery date of the ozone layer to pre-1980 values. During the WISE (Wave-driven ISentropic Exchange) campaign in autumn 2017 excessive probing of the UTLS (upper troposphere lower stratosphere) region above Western Europe and the Atlantic Ocean was conducted from aboard the HALO (High Altitude and Long range) research aircraft. We use real-time in situ WISE measurements of CH&lt;sub&gt;2&lt;/sub&gt;Cl&lt;sub&gt;2&lt;/sub&gt; and CHCl&lt;sub&gt;3&lt;/sub&gt; from HAGAR-V (High Altitude Gas AnalyzeR &amp;#8211; 5 channel version) in correlation with N&lt;sub&gt;2&lt;/sub&gt;O from UMAQS (University of Mainz Airborne QCL Spectrometer), as well as CLaMS (Chemical Lagrangian Model of the Stratosphere) global 3-dimensional simulations of air mass origin tracers and backward trajectories to identify the most efficient transport mechanisms for Cl-VSLS entering the LS region in northern hemispheric summer.&lt;/p&gt;&lt;p&gt;The WISE measurements reveal two distinct transport pathways into the UTLS region of particularly CH&lt;sub&gt;2&lt;/sub&gt;Cl&lt;sub&gt;2&lt;/sub&gt;-rich and CH&lt;sub&gt;2&lt;/sub&gt;Cl&lt;sub&gt;2&lt;/sub&gt;-poor air. CH&lt;sub&gt;2&lt;/sub&gt;Cl&lt;sub&gt;2&lt;/sub&gt;-rich air could be identified to be transported by the Asian summer monsoon within about 4-10 weeks from its source regions in Asia into the stratosphere above the Atlantic Ocean at around 380 K and above. CH&lt;sub&gt;2&lt;/sub&gt;Cl&lt;sub&gt;2&lt;/sub&gt;-poor air could be identified to be mainly uplifted to potential temperatures of about 365 K by the North American monsoon above the region of Central America with transport times of only 2-5 weeks. In addition, we could link backward trajectories of CH&lt;sub&gt;2&lt;/sub&gt;Cl&lt;sub&gt;2&lt;/sub&gt;-poor air in the LS region to be uplifted by the category 5 hurricane Maria in September 2017. Based on all analyzed WISE measurements, we found that almost all young (transport time &lt; 4 months) air masses were uplifted either above Asia or above Central America, emphasizing not only the impact of the Asian summer monsoon on the stratospheric tracer distribution but also that of the North American monsoon and hurricanes.&lt;/p&gt;&lt;p&gt;The measurements of both CH&lt;sub&gt;2&lt;/sub&gt;Cl&lt;sub&gt;2&lt;/sub&gt; and CHCl&lt;sub&gt;3&lt;/sub&gt; show the lowest stratospheric mixing ratios originating in the region of Central America and enhanced mixing ratios from Asia (enhancements &gt; 100 % and &gt; 50 %, respectively). However, the source distribution of CHCl&lt;sub&gt;3&lt;/sub&gt; is much less clear than that of CH&lt;sub&gt;2&lt;/sub&gt;Cl&lt;sub&gt;2&lt;/sub&gt; and inconspicuous CH&lt;sub&gt;2&lt;/sub&gt;Cl&lt;sub&gt;2&lt;/sub&gt; measurements can also contain enhanced CHCl&lt;sub&gt;3&lt;/sub&gt; mixing ratios. Nevertheless, the anthropogenic impact on CHCl&lt;sub&gt;3&lt;/sub&gt; -rich air from Asia is clearly visible in the measurements and we believe it is likely that a future increase of Asian CHCl&lt;sub&gt;3&lt;/sub&gt; emissions could lead to similarly large stratospheric enhancements as already observed for CH&lt;sub&gt;2&lt;/sub&gt;Cl&lt;sub&gt;2&lt;/sub&gt;. Consequently, this would further increase ozone depletion from stratospheric chlorine deposition of VSLS.&lt;/p&gt;


2012 ◽  
Vol 12 (22) ◽  
pp. 11003-11026 ◽  
Author(s):  
M. C. Barth ◽  
J. Lee ◽  
A. Hodzic ◽  
G. Pfister ◽  
W. C. Skamarock ◽  
...  

Abstract. To study the meteorology and chemistry that is associated with the early stages of the North American Monsoon, the Weather Research and Forecasting model coupled with Chemistry (WRF-Chem) is applied for the first time at high resolution (4 km grid spacing, allowing for explicit representation of convection) over a large region (continental US and northern Mexico) for a multi-week (15 July to 7 August 2006) integration. Evaluation of model results shows that WRF-Chem reasonably represents the large-scale meteorology and strong convective storms, but tends to overestimate weak convection. In the upper troposphere, the WRF-Chem model predicts ozone (O3) and carbon monoxide (CO) to within 10–20% of aircraft and sonde measurements. Comparison of UT O3 and CO frequency distributions between WRF-Chem and satellite data indicates that WRF-Chem is lofting CO too frequently from the boundary layer (BL). This excessive lofting should also cause biases in the WRF-Chem ozone frequency distribution; however it agrees well with satellite data suggesting that either the chemical production of O3 in the model is overpredicted or there is too much stratosphere to troposphere transport in the model. Analysis of different geographic regions (West Coast, Rocky Mountains, Central Plains, Midwest, and Gulf Coast) reveals that much of the convective transport occurs in the Rocky Mountains, while much of the UT ozone chemical production occurs over the Gulf Coast and Midwest regions where both CO and volatile organic compounds (VOCs) are abundant in the upper troposphere and promote the production of peroxy radicals. In all regions most of the ozone chemical production occurs within 24 h of the air being lofted from the boundary layer. In addition, analysis of the anticyclone and adjacent air indicates that ozone mixing ratios within the anticyclone region associated with the North American Monsoon and just outside the anticyclone are similar. Increases of O3 within the anticyclone are strongly coincident with entrainment of stratospheric air into the anticyclone, but also are from in situ O3 chemical production. In situ O3 production is up to 17% greater within the anticyclone than just outside the anticyclone when the anticyclone is over the southern US indicating that the enhancement of O3 is most pronounced over regions with abundant VOCs.


2012 ◽  
Vol 12 (7) ◽  
pp. 16407-16455 ◽  
Author(s):  
M. C. Barth ◽  
J. Lee ◽  
A. Hodzic ◽  
G. Pfister ◽  
W. C. Skamarock ◽  
...  

Abstract. In this study, the Weather Research and Forecasting model coupled with Chemistry (WRF-Chem) is applied at 4 km horizontal grid spacing to study the meteorology and chemistry over the continental US and Northern Mexico region for the 15 July to 7 August 2006 period, which coincides with the early stages of the North American Monsoon. Evaluation of model results shows that WRF-Chem reasonably represents the large-scale meteorology and strong convective storms, but tends to overestimate weak convection. In the upper troposphere, the WRF-Chem model predicts ozone and carbon monoxide (CO) to within 10–20% of aircraft and sonde measurements. However, the frequency distribution from satellite data indicates that WRF-Chem is lofting too much CO from the boundary layer (BL). Because ozone mixing ratios agree well with these same satellite data, it suggests that chemical production of O3 in the model is overpredicted and compensates for the excess convective lofting of BL air. Analysis of different geographic regions (West Coast, Rocky Mountains, Central Plains, Midwest, and Gulf Coast) reveals that much of the convective transport occurs in the Rocky Mountains, while much of the UT ozone chemical production occurs over the Gulf Coast and Midwest regions where both CO and volatile organic compounds (VOCs) are abundant in the upper troposphere and promote the production of peroxy radicals. In all regions most of the ozone chemical production occurs within 24 h of the air being lofted from the boundary layer. In addition, analysis of the anticyclone and adjacent air indicates that ozone mixing ratios within the anticyclone region associated with the North American Monsoon and just outside the anticyclone are similar. Increases of O3 within the anticyclone are strongly coincident with entrainment of stratospheric air into the anticyclone, but also are from in situ O3 chemical production. In situ O3 production is up to 17% greater within the anticyclone than just outside the anticyclone when the anticyclone is over the Southern US indicating that the enhancement of O3 is most pronounced over regions with abundant VOCs.


Ecohydrology ◽  
2008 ◽  
Vol 1 (3) ◽  
pp. 225-238 ◽  
Author(s):  
Enrique R. Vivoni ◽  
Alex J. Rinehart ◽  
Luis A. Méndez-Barroso ◽  
Carlos A. Aragón ◽  
Gautam Bisht ◽  
...  

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