A study of stratospheric chlorine partitioning based on new satellite measurements and modeling

M. L. Santee; I. A. MacKenzie; G. L. Manney; M. P. Chipperfield; P. F. Bernath; K. A. Walker; C. D. Boone; L. Froidevaux; N. J. Livesey; J. W. Waters

doi:10.1029/2007JD009057

A study of stratospheric chlorine partitioning based on new satellite measurements and modeling

M. L. Santee, I. A. MacKenzie, G. L. Manney, M. P. Chipperfield, P. F. Bernath, K. A. Walker, C. D. Boone, L. Froidevaux, N. J. Livesey, J. W. Waters

Chemistry

Research output: Contribution to journal › Literature review › peer-review

Abstract

Two recent satellite instruments, the Microwave Limb Sounder (MLS) on Aura and the Atmospheric Chemistry Experiment Fourier Transform Spectrometer (ACE-FTS) on SCISAT-1, provide an unparalleled opportunity to investigate stratospheric chlorine partitioning. We use measurements of ClO, HCl, ClONO2, and other species from MLS and ACE-FTS to study the evolution of reactive and reservoir chlorine throughout the lower stratosphere during two Arctic and two Antarctic winters characterizing both relatively cold and relatively warm and disturbed conditions in each hemisphere. At middle latitudes, and at high latitudes at the beginning of winter, HCl greatly exceeds ClONO2, representing similar to 0.7-0.8 of estimated total inorganic chlorine. Nearly complete chlorine activation is seen inside the winter polar vortices. In the Arctic, chlorine recovery follows different paths in the two winters: In 2004/2005, deactivation initially takes place through reformation of ClONO2, then both reservoirs are produced concurrently but ClONO2 continues to significantly exceed HCl, and finally slow repartitioning between ClONO2 and HCl occurs; in 2005/2006, HCl and ClONO2 rise at comparable rates in some regions. In the Antarctic, chlorine deactivation proceeds in a similar manner in both winters, with a rapid rise in HCl accompanying the decrease in ClO. The measurements are compared to customized runs of the SLIMCAT three-dimensional chemical transport model. Measured and modeled values typically agree well outside the winter polar regions. In contrast, partly because of the equilibrium scheme used to parameterize polar stratospheric clouds, the model overestimates the magnitude, spatial extent, and duration of chlorine activation inside the polar vortices.

Original language	English
Article number	D12307
Pages (from-to)	-
Number of pages	25
Journal	Journal of Geophysical Research
Volume	113
Issue number	D12
DOIs	https://doi.org/10.1029/2007JD009057
Publication status	Published - 25 Jun 2008

Keywords

CHEMICAL-TRANSPORT MODEL
HALOGEN OCCULTATION EXPERIMENT
ATMOSPHERIC TRACE GASES
ARCTIC WINTER 2002/2003
POLAR VORTEX
OZONE LOSS
FTIR MEASUREMENTS
CLO DIMER
SOUTHERN-HEMISPHERE
ANTARCTIC VORTEX

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10.1029/2007JD009057

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title = "A study of stratospheric chlorine partitioning based on new satellite measurements and modeling",

abstract = "Two recent satellite instruments, the Microwave Limb Sounder (MLS) on Aura and the Atmospheric Chemistry Experiment Fourier Transform Spectrometer (ACE-FTS) on SCISAT-1, provide an unparalleled opportunity to investigate stratospheric chlorine partitioning. We use measurements of ClO, HCl, ClONO2, and other species from MLS and ACE-FTS to study the evolution of reactive and reservoir chlorine throughout the lower stratosphere during two Arctic and two Antarctic winters characterizing both relatively cold and relatively warm and disturbed conditions in each hemisphere. At middle latitudes, and at high latitudes at the beginning of winter, HCl greatly exceeds ClONO2, representing similar to 0.7-0.8 of estimated total inorganic chlorine. Nearly complete chlorine activation is seen inside the winter polar vortices. In the Arctic, chlorine recovery follows different paths in the two winters: In 2004/2005, deactivation initially takes place through reformation of ClONO2, then both reservoirs are produced concurrently but ClONO2 continues to significantly exceed HCl, and finally slow repartitioning between ClONO2 and HCl occurs; in 2005/2006, HCl and ClONO2 rise at comparable rates in some regions. In the Antarctic, chlorine deactivation proceeds in a similar manner in both winters, with a rapid rise in HCl accompanying the decrease in ClO. The measurements are compared to customized runs of the SLIMCAT three-dimensional chemical transport model. Measured and modeled values typically agree well outside the winter polar regions. In contrast, partly because of the equilibrium scheme used to parameterize polar stratospheric clouds, the model overestimates the magnitude, spatial extent, and duration of chlorine activation inside the polar vortices.",

keywords = "CHEMICAL-TRANSPORT MODEL, HALOGEN OCCULTATION EXPERIMENT, ATMOSPHERIC TRACE GASES, ARCTIC WINTER 2002/2003, POLAR VORTEX, OZONE LOSS, FTIR MEASUREMENTS, CLO DIMER, SOUTHERN-HEMISPHERE, ANTARCTIC VORTEX",

author = "Santee, {M. L.} and MacKenzie, {I. A.} and Manney, {G. L.} and Chipperfield, {M. P.} and Bernath, {P. F.} and Walker, {K. A.} and Boone, {C. D.} and L. Froidevaux and Livesey, {N. J.} and Waters, {J. W.}",

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doi = "10.1029/2007JD009057",

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journal = "Journal of Geophysical Research",

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publisher = "Wiley-Blackwell",

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T1 - A study of stratospheric chlorine partitioning based on new satellite measurements and modeling

AU - Santee, M. L.

AU - MacKenzie, I. A.

AU - Manney, G. L.

AU - Chipperfield, M. P.

AU - Bernath, P. F.

AU - Walker, K. A.

AU - Boone, C. D.

AU - Froidevaux, L.

AU - Livesey, N. J.

AU - Waters, J. W.

PY - 2008/6/25

Y1 - 2008/6/25

N2 - Two recent satellite instruments, the Microwave Limb Sounder (MLS) on Aura and the Atmospheric Chemistry Experiment Fourier Transform Spectrometer (ACE-FTS) on SCISAT-1, provide an unparalleled opportunity to investigate stratospheric chlorine partitioning. We use measurements of ClO, HCl, ClONO2, and other species from MLS and ACE-FTS to study the evolution of reactive and reservoir chlorine throughout the lower stratosphere during two Arctic and two Antarctic winters characterizing both relatively cold and relatively warm and disturbed conditions in each hemisphere. At middle latitudes, and at high latitudes at the beginning of winter, HCl greatly exceeds ClONO2, representing similar to 0.7-0.8 of estimated total inorganic chlorine. Nearly complete chlorine activation is seen inside the winter polar vortices. In the Arctic, chlorine recovery follows different paths in the two winters: In 2004/2005, deactivation initially takes place through reformation of ClONO2, then both reservoirs are produced concurrently but ClONO2 continues to significantly exceed HCl, and finally slow repartitioning between ClONO2 and HCl occurs; in 2005/2006, HCl and ClONO2 rise at comparable rates in some regions. In the Antarctic, chlorine deactivation proceeds in a similar manner in both winters, with a rapid rise in HCl accompanying the decrease in ClO. The measurements are compared to customized runs of the SLIMCAT three-dimensional chemical transport model. Measured and modeled values typically agree well outside the winter polar regions. In contrast, partly because of the equilibrium scheme used to parameterize polar stratospheric clouds, the model overestimates the magnitude, spatial extent, and duration of chlorine activation inside the polar vortices.

AB - Two recent satellite instruments, the Microwave Limb Sounder (MLS) on Aura and the Atmospheric Chemistry Experiment Fourier Transform Spectrometer (ACE-FTS) on SCISAT-1, provide an unparalleled opportunity to investigate stratospheric chlorine partitioning. We use measurements of ClO, HCl, ClONO2, and other species from MLS and ACE-FTS to study the evolution of reactive and reservoir chlorine throughout the lower stratosphere during two Arctic and two Antarctic winters characterizing both relatively cold and relatively warm and disturbed conditions in each hemisphere. At middle latitudes, and at high latitudes at the beginning of winter, HCl greatly exceeds ClONO2, representing similar to 0.7-0.8 of estimated total inorganic chlorine. Nearly complete chlorine activation is seen inside the winter polar vortices. In the Arctic, chlorine recovery follows different paths in the two winters: In 2004/2005, deactivation initially takes place through reformation of ClONO2, then both reservoirs are produced concurrently but ClONO2 continues to significantly exceed HCl, and finally slow repartitioning between ClONO2 and HCl occurs; in 2005/2006, HCl and ClONO2 rise at comparable rates in some regions. In the Antarctic, chlorine deactivation proceeds in a similar manner in both winters, with a rapid rise in HCl accompanying the decrease in ClO. The measurements are compared to customized runs of the SLIMCAT three-dimensional chemical transport model. Measured and modeled values typically agree well outside the winter polar regions. In contrast, partly because of the equilibrium scheme used to parameterize polar stratospheric clouds, the model overestimates the magnitude, spatial extent, and duration of chlorine activation inside the polar vortices.

KW - CHEMICAL-TRANSPORT MODEL

KW - HALOGEN OCCULTATION EXPERIMENT

KW - ATMOSPHERIC TRACE GASES

KW - ARCTIC WINTER 2002/2003

KW - POLAR VORTEX

KW - OZONE LOSS

KW - FTIR MEASUREMENTS

KW - CLO DIMER

KW - SOUTHERN-HEMISPHERE

KW - ANTARCTIC VORTEX

UR - http://www.scopus.com/inward/record.url?scp=50049124399&partnerID=8YFLogxK

U2 - 10.1029/2007JD009057

DO - 10.1029/2007JD009057

M3 - Literature review

SN - 0148-0227

VL - 113

SP - -

JO - Journal of Geophysical Research

JF - Journal of Geophysical Research

IS - D12

M1 - D12307

ER -

A study of stratospheric chlorine partitioning based on new satellite measurements and modeling

Abstract

Keywords

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