01 Nov 2021

01 Nov 2021

Review status: this preprint is currently under review for the journal ACP.

Upper stratospheric ClO and HOCl trends (2005–2020): Aura Microwave Limb Sounder and model results

Lucien Froidevaux1, Douglas E. Kinnison2, Michelle L. Santee1, Luis F. Millan1, Nathaniel J. Livesey1, William G. Read1, Charles G. Bardeen2, John J. Orlando2, and Ryan A. Fuller1 Lucien Froidevaux et al.
  • 1Jet Propulsion Laboratory, California Institute of Technology, Pasadena, California, USA
  • 2National Center for Atmospheric Research, Boulder, Colorado, USA

Abstract. We analyze Aura Microwave Limb Sounder (MLS) monthly zonal mean time series of ClO and HOCl between 50° S and 50° N to estimate upper stratospheric trends in these chlorine species from 2005 through 2020. We compare these observations to those from the Whole Atmosphere Community Climate Model version 6 (WACCM6), run under the specified dynamics configuration. The model sampling follows the MLS coverage in space and local time. We use version 5 MLS ClO zonal mean daytime profiles and similarly binned daytime ClO model profiles from 32 to 1.5 hPa. For MLS HOCl, we use the version 5 offline product derived from daily zonal mean radiances rather than averaged Level 2 profiles; MLS HOCl is scientifically useful between 10 and 2 hPa, and the HOCl monthly zonal means are separated into day and night for comparison to WACCM6. We find good agreement (mostly within ~10 %) between the climatological MLS ClO daytime distributions and the model ClO climatology for 2005–2020. The model HOCl climatology, however, underestimates the MLS HOCl climatology by about 30 %. This could well be caused by a combination of fairly large systematic uncertainties in both the model-assumed rate constant for the formation of HOCl and the MLS HOCl retrievals themselves.

The model daytime ClO trends versus latitude and pressure agree quite well with those from MLS. MLS-derived near-global upper stratospheric daytime trends between 7 and 2 hPa are −0.73 ± 0.40 % yr−1 for ClO and –0.39 ± 0.35  % yr−1 for HOCl, with 2σ uncertainty estimates used here. The corresponding model decreases are somewhat faster than observed (although the difference is not statistically significant), with trend values of –0.85 ± 0.45  % yr−1 for ClO and –0.64 ±  0.37  % yr−1 for HOCl. Both data and model results point to a faster trend in ClO than in HOCl. The MLS ClO trends are consistent with past estimates of upper stratospheric ClO trends from satellite and ground-based microwave data. As discussed in the past, trends in other species (in particular, positive trends in CH4 and H2O) can lead to a ClO decrease that is faster than the decrease in total inorganic chlorine. Regarding trends in HOCl, positive trends in HO2 can lead to a faster rate of formation for HOCl as a function of time, which partially offsets the decreasing trend in active chlorine.

The decreasing trends in upper stratospheric ClO and HOCl provide additional confirmation of the effectiveness of the Montreal Protocol and its amendments, which have led to the early stages of an expected long-term ozone recovery from the effects of ozone-depleting substances.

Lucien Froidevaux et al.

Status: open (until 13 Dec 2021)

Comment types: AC – author | RC – referee | CC – community | EC – editor | CEC – chief editor | : Report abuse
  • RC1: 'Comment on acp-2021-880', Anonymous Referee #1, 15 Nov 2021 reply
  • RC2: 'Comment on acp-2021-880', Anonymous Referee #2, 29 Nov 2021 reply

Lucien Froidevaux et al.

Lucien Froidevaux et al.


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Short summary
We analyze satellite-derived distributions of chlorine monoxide (ClO) and hypochlorous acid (HOCl) in the upper atmosphere. For 2005–2020, from 50° S to 50° N and over ~30 to 45 km, ClO and HOCl decreased by −0.7 % and −0.4 % per year, respectively. A detailed model of chemistry and dynamics agrees with these results. These decreases confirm the effectiveness of the 1987 Montreal Protocol, which limited emissions of chlorine- and bromine-containing source gases, in order to protect the ozone layer.