Fifty years of balloon-borne ozone profile measurements at Uccle, Belgium: a short history, the scientific relevance, and the achievements in understanding the vertical ozone distribution

Abstract

Starting in 1969 and comprising three launches a week, the Uccle (Brussels, Belgium) ozonesonde dataset is one of longest and densest in the world. Moreover, as the only major change was the switch from Brewer-Mast (BM) to electrochemical concentration cell (ECC) ozonesonde types in 1997 (when the emissions of ozone-depleting substances peaked), the Uccle time series is very homogenous. In this paper, we briefly describe the efforts that were undertaken during the first 3 decades of the 50 years of ozonesonde observations to guarantee the homogeneity between ascent and descent profiles, under changing environmental conditions (e.g. SO2), and between the different ozonesonde types. This paper focuses on the 50-year-long Uccle ozonesonde dataset and aims to demonstrate its past, present, and future relevance to ozone research in two application areas: (i) the assessment of the temporal evolution of ozone from the surface to the (middle) stratosphere, and (ii) as the backbone for validation and stability analysis of both stratospheric and tropospheric satellite ozone retrievals. Using the Long-term Ozone Trends and Uncertainties in the Stratosphere (LOTUS) multiple linear regression model (SPARC/IO3C/GAW, 2019), we found that the stratospheric ozone concentrations at Uccle have declined at a significant rate of around 2 % per decade since 1969, which is also rather consistent over the different stratospheric levels. This overall decrease can mainly be assigned to the 1969–1996 period with a rather consistent rate of decrease of around −4 % per decade. Since 2000, a recovery of between +1 % per decade and +3 % per decade of the stratospheric ozone levels above Uccle has been observed, although it is not significant and is not seen for the upper stratospheric levels measured by ozonesondes. Throughout the entire free troposphere, a very consistent increase in the ozone concentrations of 2 % per decade to 3 % per decade has been measured since both 1969 and 1995, with the trend since 1995 being in almost perfect agreement with the trends derived from the In-service Aircraft for a Global Observing System (IAGOS) ascent/descent profiles at Frankfurt. As the number of tropopause folding events in the Uccle time series has increased significantly over time, increased stratosphere-to-troposphere transport of recovering stratospheric ozone might partly explain these increasing tropospheric ozone concentrations, despite the levelling-off of (tropospheric) ozone precursor emissions and notwithstanding the continued increase in mean surface ozone concentrations. Furthermore, we illustrate the crucial role of ozonesonde measurements for the validation of satellite ozone profile retrievals. With the operational validation of the Global Ozone Monitoring Experiment-2 (GOME-2), we show how the Uccle dataset can be used to evaluate the performance of a degradation correction for the MetOp-A/GOME-2 UV (ultraviolet) sensors. In another example, we illustrate that the Microwave Limb Sounder (MLS) overpass ozone profiles in the stratosphere agree within ±5 % with the Uccle ozone profiles between 10 and 70 hPa. Another instrument on the same Aura satellite platform, the Tropospheric Emission Spectrometer (TES), is generally positively biased with respect to the Uccle ozonesondes in the troposphere by up to ∼ 10 ppbv, corresponding to relative differences of up to ∼ 15 %. Using the Uccle ozonesonde time series as a reference, we also demonstrate that the temporal stability of those last two satellite retrievals is excellent.