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Inorganic Chlorine Partitioning in the Summer Lower Stratosphere: Modeled and Measured [ClONO2/HCl] During POLARISWe examine inorganic chlorine (Cly) 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 [ClONO2]/[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 HO2 chemistry. We find that inorganic chlorine photochemistry alone overestimates observed [ClONO2]/[HCl] by approximately 55-60% at mid and high latitudes. On the basis of POLARIS studies of the inorganic chlorine budget, [ClO]/[ClONO2], and an intercomparison with balloon observations, the most direct explanation for the model-measurement discrepancy in Cly 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 ClONO2 measurement (too low). The high precision of our simulation (+/-15% 1-sigma for [ClONO2]/[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.
Document ID
20010062494
Acquisition Source
Ames Research Center
Document Type
Reprint (Version printed in journal)
External Source(s)
Authors
Voss, P. B.
(Harvard Univ. Southboro, MA United States)
Stimpfle, R. M.
(Harvard Univ. Southboro, MA United States)
Cohen, R. C.
(Harvard Univ. Southboro, MA United States)
Hanisco, T. F.
(Harvard Univ. Southboro, MA United States)
Bonne, G. P.
(Harvard Univ. Southboro, MA United States)
Perkins, K. K.
(Harvard Univ. Southboro, MA United States)
Lanzendorf, E. J.
(Harvard Univ. Southboro, MA United States)
Anderson, J. G.
(Harvard Univ. Southboro, MA United States)
Salawitch, R. J.
(Jet Propulsion Lab., California Inst. of Tech. Pasadena, CA United States)
Date Acquired
August 20, 2013
Publication Date
January 27, 2001
Publication Information
Publication: Journal of Geophysical Research
Publisher: American Geophysical Union
Volume: 106
Issue: D2
ISSN: 0148-0227
Subject Category
Geophysics
Report/Patent Number
Paper-2000JD900494
Funding Number(s)
CONTRACT_GRANT: NAG1-2007
CONTRACT_GRANT: NAG2-1300
Distribution Limits
Public
Copyright
Other

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