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____________________________Near Tropopause Halogen
Heterogeneous Chemistry Indicators using Occultation Observations and
CESM1 (WACCM) Simulations________________________________
Doug Kinnison, (NCAR, USA)Susan Solomon and Catherine Wilka (MIT, USA)
Special Thanks to Lynn Harvey (LASP, USA)
Whole Atmosphere Working Group , 19 June 2018
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Hypothesis: Occultation NO2 observations (e.g., SAGEII, SAGEIII-Meteor, and
SAGEIII-ISS) can be used as an indicator of near tropopause heterogeneous halogen activation.
Heterogeneous Chemistry: Heterogeneous halogen reactions on sulfate converts NO2 to reservoir
species, e.g.,NO2 + ClO + M => ClONO2 +M, ClONO2 + hv => ClO + NO2 (fast recycling)
ClONO2 + HCl (het) => HNO3 + Cl2 ClONO2 + H2O (het) => HNO3 + HOCl
Approach: Compare profile output from SAGE instruments to two SD-WACCM
(MERRA) simulations: 1) with sulfate halogen chemistry; 2) without sulfate halogen chemistry. Water-Ice Het chemistry is turned off.
The N2O5 + H2O => 2HNO3 heterogeneous reaction is included in all simulations, i.e., only looking at the halogen impact.
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With and Without Heterogeneous Halogen Chemistry
Monsoon Region• Lat: 0-30N, • Lon: 0-180E• Period: July• SAGEII• Solomon et al.,
JGR, 2017.
Subpolar Region1• Lat: 45S-60S• Lon: 0-360.• Period: Sept.-Oct. • SAGEIII-Meteor
Subpolar Region2• Lat: 50S-67S• Lon: 0-360• Period: Oct-Nov• SAGEIII-ISS
SD-WACCM/MERRA 24-hour average results shown above.
Three illustrious regions are shown.
SAGEII
SAGEIII-Meteor SAGEIII-ISS
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Northern Hemisphere, Summer, Monsoon Region
Solomon, S., D. E. Kinnison, R. R. Garcia, J. Bandoro1, M. Mills, C. Wilka, R. R. Neely III, A. Schmidt, J. Barnes, J-P Vernier, M. Hopfner, Monsoon circulations and tropical heterogeneous chlorine chemistry in the stratosphere, Geophys. Res. Lett., doi:10.1002/2016GL071778, 2016.
July, 2011
Transport processes associated with the summer monsoon can create a”perfect storm” in which abundances of HCl can be brought into contactwith liquid sulfate aerosols near the cold tropical tropopause leading toheterogeneous chemical activation. Solomon et al., 2016.
HCl => ClO
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Why SAGEII
Tick Marks are the 15th of the given month.
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July *** Lat: 0-30N *** Lon: 0-180E *** 1984-2005Observations
Total Profiles = 1049
Temperatures are <200K in the Lower Stratosphere (red line).
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July *** Lat: 0-30N *** Lon: 0-180E *** 1984-2005Model
Model species profiles are in good agreement in absolute magnitude with SAGEII.
SAGEII limit
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July *** Lat: 0-30N *** Lon: 0-180E *** 1984-2005Model
Red dashed lines show region where halogen heterogeneous activation occurs.
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July *** Lat: 0-30N *** Lon: 0-180E *** 1984-2005Model NoHet
Without halogen heterogeneous chemistry NO2 depletion is reduced.
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July *** Lat: 0-30N *** Lon: 0-180E *** lev: 118-68hPa
PDFs were created for region between the previous slide red dashed lines.
total points = 2702 25 pptv bin width
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July *** Lat: 0-30N *** Lon: 0-180E *** lev: 118-68hPa
OBS and WACCM have a higher frequency of low NO2
OBS and WACCM have a lower frequency of high NO2 relative to NoHet
total points = 2702 25 pptv bin width
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Tick Marks are the 15th of the given month.
SAGE III - Meteor
SAGEIII-Meteor has better Vertical Resolution, Extent, and Accuracy than SAGEII
Southern Hemisphere, Spring, Subpolar Region 1
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1 Sept – 15 Oct ** Lat 56-48S ** Lon 0-360 ** 2003-2005Observations
Temperatures are <200K in the Lower Stratosphere (red line).
Total Profiles = 2045
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1 Sept – 15 Oct ** Lat 56-48S ** Lon 0-360 ** 2003-2005Model
Model species profiles are in good agreement in absolute magnitude with SAGEIII-M.
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1 Sept – 15 Oct ** Lat 56-48S ** Lon 0-360 ** 2003-2005Model
Red dashed lines show region where NO2 PDFs will be derived.
Log Scale
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Sept – Oct ** Lat: 56-48S ** Lon: 0-360 ** 2003-2005Model NoHet
Without halogen heterogeneous chemistry NO2 depletion is reduced.
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Sept-Oct ** Lat: 56-48S ** Lon; 0-360 ** lev; 170-72hPa
total points = 8064
OBS have a higher frequency of low NO2 relative to WACCM?
25 pptv bin width
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Lat: 56-48S *** Lon: 0-360 *** lev: 170-72hPa
OBS and WACCM have a higher frequency of low NO2
OBS and WACCM have a lower frequency of high NO2 relative to NoHet
total points = 8064 25 pptv bin width
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Tick Marks are the 15th of the given month.
SAGE III - ISS
SAGEIII-ISS has better global coverage than SAGEIII-Meteor.
Southern Hemisphere, Spring, Subpolar Region 2
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15 Oct - 15 Nov *** Lat 67-50S *** Lon 0-360 *** 2017
This comparison is later in the year and higher in latitude than the SAGEIII-Meteor.
H2O Vapor not available.
Observations
Total Profiles = 238
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15 Oct - 15 Nov *** Lat 67-50S *** Lon 0-360 *** 2017Model
Model NO2 profiles are in good agreement in absolute magnitude with SAGEIII-ISS.
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15 Oct - 15 Nov *** Lat 67-50S *** Lon 0-360 *** 2017Model
Less Chlorine activation shown in the years 2003-2005 (SAGEIII-Meteor comparison).
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15 Oct - 15 Nov *** Lat 67-50S *** Lon: 0-360 *** 2017Model NoHet
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Oct-Nov ** Lat: 67-50S ** Lon: 0-360 ** lev; 180-72hPa
Excellent Model / SAGEIII – ISS agreement.
total points = 1179 25 pptv bin width
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Oct-Nov ** Lat: 67-50S ** Lon; 0-360 ** lev; 180-72hPa
OBS and WACCM have a higher frequency of low NO2 versus the NoHet simulation.
total points = 1179 25 pptv bin width
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Summary
• We have shown that NO2 occultation observations (SAGEII, SAGEIII-Meteor, and SAGEIII-ISS) in conjunction with 3-D chemistry climate model results can identify regions where sulfate heterogeneous chemistry is operating in the near tropopause region. This work examined the subtropical and subpolar regions.
• This approach may also be useful in identifying the aerosol / PSC type (e.g., sulfate vs water-ice) based on temperature and H2O vapor considerations.
• This approach can also be applied to ozone and HCl.
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Sulfate Aerosol Reaction Probability as function of H2O vapor