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Inorganic chlorine partitioning in the summer lower stratosphere: Modeled and measured [ClONO_2]/[HCl] during POLARIS

Voss, P. B. and Stimpfle, R. M. and Cohen, R. C. and Hanisco, T. F. and Bonne, G. P. and Perkins, K. K. and Lanzendorf, E. J. and Anderson, J. G. and Salawitch, R. J. and Webster, C. R. and Scott, D. C. and May, R. D. and Wennberg, P. O. and Newman, P. A. and Lait, L. R. and Elkins, J. W. and Bui, T. P. (2001) Inorganic chlorine partitioning in the summer lower stratosphere: Modeled and measured [ClONO_2]/[HCl] during POLARIS. Journal of Geophysical Research D, 106 (D2). pp. 1713-1732. ISSN 0148-0227. https://resolver.caltech.edu/CaltechAUTHORS:20140625-083843890

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Abstract

We examine inorganic chlorine (Cl_y,) partitioning in the summer lower stratosphere using in situ ER-2 aircraft observations made during the Photochemistry of Ozone Loss in the Arctic Region in Summer (POLARIS) campaign. New steady state and numerical models estimate [ClONO_2]/[HCl] using currently accepted photochemistry. These models are tightly constrained by observations with OH (parameterized as a function of solar zenith angle) substituting for modeled HO_2 chemistry. We find that inorganic chlorine photochemistry alone overestimates observed [ClONO_2]/[HCl] by approximately 55–60% at mid and high latitudes. On the basis of POLARIS studies of the inorganic chlorine budget, [ClO]/[ClONO_2], and an intercomparison with balloon observations, the most direct explanation for the model-measurement discrepancy in Cl_y, partitioning is an error in the reactions, rate constants, and measured species concentrations linking HCl and ClO (simulated [ClO]/[HCl] too high) in combination with a possible systematic error in the ER-2 ClONO_2 measurement (too low). The high precision of our simulation (±15% 1σ for [ClONO_2]/[HCl], which is compared with observations) increases confidence in the observations, photolysis calculations, and laboratory rate constants. These results, along with other findings, should lead to improvements in both the accuracy and precision of stratospheric photochemical models.


Item Type:Article
Related URLs:
URLURL TypeDescription
http://dx.doi.org/10.1029/2000JD900494DOIArticle
http://onlinelibrary.wiley.com/doi/10.1029/2000JD900494/abstractPublisherArticle
ORCID:
AuthorORCID
Wennberg, P. O.0000-0002-6126-3854
Alternate Title:Inorganic chlorine partitioning in the summer lower stratosphere: Modeled and measured [ClONO2]/[HCl] during POLARIS
Additional Information:© 2001 American Geophysical Union. Received March 14, 2000; revised July 24, 2000; accepted August 8, 2000. Paper number 2000JD900494. We thank NASA's Upper Atmosphere Research Program as well as the researchers pilots, crew, and managers of NASA's ER-2 program for supporting the POLARIS campaign. This work was funded under NASA grants NAG-1-2007 and NAG-2-1300. We thank J. J. Margitan for the ER-2 O_3 data. P. B. Voss is grateful for support from NASA's Global Change Fellowship Program.
Funders:
Funding AgencyGrant Number
NASANAG-1-2007
NASANAG-2-1300
NASA Global Change FellowshipUNSPECIFIED
Issue or Number:D2
Record Number:CaltechAUTHORS:20140625-083843890
Persistent URL:https://resolver.caltech.edu/CaltechAUTHORS:20140625-083843890
Official Citation:Voss, P. B., et al. (2001), Inorganic chlorine partitioning in the summer lower stratosphere: Modeled and measured [ClONO2]/[HCl] during POLARIS, J. Geophys. Res., 106(D2), 1713–1732, doi:10.1029/2000JD900494.
Usage Policy:No commercial reproduction, distribution, display or performance rights in this work are provided.
ID Code:46497
Collection:CaltechAUTHORS
Deposited By: Ruth Sustaita
Deposited On:25 Jun 2014 17:01
Last Modified:03 Oct 2019 06:44

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