Abstract

Abstract. High-quality stratospheric ozone profile data sets are a key requirement for accurate quantification and attribution of long-term ozone changes. Satellite instruments provide stratospheric ozone profile measurements over typical mission durations of 5–15 years. Various methodologies have then been applied to merge and homogenise the different satellite data in order to create long-term observation-based ozone profile data sets with minimal data gaps. However, individual satellite instruments use different measurement methods, sampling patterns and retrieval algorithms which complicate the merging of these different data sets. In contrast, atmospheric chemical models can produce chemically consistent long-term ozone simulations based on specified changes in external forcings, but they are subject to the deficiencies associated with incomplete understanding of complex atmospheric processes and uncertain photochemical parameters. Here, we use chemically self-consistent output from the TOMCAT 3-D chemical transport model (CTM) and a random-forest (RF) ensemble learning method to create a merged 42-year (1979–2020) stratospheric ozone profile data set (ML-TOMCAT V1.0). The underlying CTM simulation was forced by meteorological reanalyses, specified trends in long-lived source gases, solar flux and aerosol variations. The RF is trained using the Stratospheric Water and OzOne Satellite Homogenized (SWOOSH) data set over the time periods of the Microwave Limb Sounder (MLS) from the Upper Atmosphere Research Satellite (UARS) (1991–1998) and Aura (2005–2016) missions. We find that ML-TOMCAT shows excellent agreement with available independent satellite-based data sets which use pressure as a vertical coordinate (e.g. GOZCARDS, SWOOSH for non-MLS periods) but weaker agreement with the data sets which are altitude-based (e.g. SAGE-CCI-OMPS, SCIAMACHY-OMPS). We find that at almost all stratospheric levels ML-TOMCAT ozone concentrations are well within uncertainties of the observational data sets. The ML-TOMCAT (V1.0) data set is ideally suited for the evaluation of chemical model ozone profiles from the tropopause to 0.1 hPa and is freely available via https://doi.org/10.5281/zenodo.5651194 (Dhomse et al., 2021).

Highlights

  • With the successful implementation of the Montreal Protocol, various observations confirm reductions in the concentrations of halogenated ozone-depleting substances (ODSs) in the atmosphere (WMO, 2014, 2018)

  • We find that ML-TOMCAT shows excellent agreement with available independent satellite-based data sets which use pressure as a vertical coordinate (e.g. GOZCARDS, Stratospheric Water and OzOne Satellite Homogenized (SWOOSH) for non-Microwave Limb Sounder (MLS) periods) but weaker agreement with the data sets which are altitude-based (e.g. SAGE-CCI-OMPS, SCIAMACHY-OMPS)

  • Significant positive trends have been detected in very shortlived substances (VSLSs) containing chlorine and bromine that are not controlled by the Montreal Protocol (e.g. Hossaini et al, 2015, 2019)

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Summary

Introduction

With the successful implementation of the Montreal Protocol, various observations confirm reductions in the concentrations of halogenated ozone-depleting substances (ODSs) in the atmosphere (WMO, 2014, 2018). Satellite data records confirm a peak in upper-stratospheric HCl (the main chlorine reservoir) around 1997, followed by a steady decline (Anderson et al, 2000; Froidevaux et al, 2006a; Hossaini et al, 2019). Some observational data suggest that there has been a continuous decline in lower-stratospheric ozone (Ball et al, 2018, 2020), which could be attributed to changes in stratospheric dynamics Chipperfield et al, 2018; Wargan et al, 2018; Orbe et al, 2020; Abalos and de la Cámara, 2020). Significant positive trends have been detected in very shortlived substances (VSLSs) containing chlorine and bromine that are not controlled by the Montreal Protocol (e.g. Hossaini et al, 2015, 2019)

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