ALBERT

Description: Ozone loss pathways and their rates in the ozone quasi-biennial oscillation (QBO), which is simulated by a chemistry-climate model developed by the Meteorological Research Institute of Japan, are evaluated using an ob- jective pathway analysis program (PAP). The analyzed chemical system contains catalytic cycles caused by NOx , HOx , ClOx , Ox , and BrOx . PAP quantified the rates of all significant catalytic ozone loss cycles, and evaluated the partitioning among these cycles. The QBO amplitude of the sum of all cycles amounts to about 4 and 14 % of the annual mean of the total ozone loss rate at 10 and 20 hPa, respectively. The contribution of catalytic cycles to the QBO of the ozone loss rate is found to be as follows: NOx cycles contribute the largest fraction (50 – 85 %) of the QBO amplitude of the total ozone loss rate; HOx cycles are the second-largest (20 – 30 %) below 30 hPa and the third-largest (about 10 %) above 20 hPa; Ox cycles rank third (5 – 20 %) below 30 hPa and second (about 20 %) above 20 hPa; ClOx cycles rank fourth (5 – 10 %); and BrOx cycles are almost negligible. The relative contribution of the NOx and Ox cycles to the QBO amplitude of ozone loss differs by up to 10 % and 20 %, respectively, from their contribution to the annual mean ozone loss rate. The ozone QBO at 20 hPa is mainly driven by ozone transport, which then alters the ozone loss rate. In contrast, the ozone QBO at 10 hPa is driven chemically by NOx and the temperature dependence of [O]/[O3], which results from the temperature dependence of the reaction O + O2 + M → O3 + M. In addition, the ozone QBO at 10 hPa is influenced by the overhead ozone column, which affects [O]/[O3] (through ozone photolysis) and the ozone production rate (through oxygen photolysis).

Description: Motivated by previous measurements of very low tropospheric ozone concentrations in the Tropical West Pacific (TWP) and the implied low oxidizing capacity of this key region for transport into the stratosphere (e.g. Rex et al. 2014), we set up an atmospheric research station in Palau (7° N 134° E). Our analysis of regular balloon-borne tropospheric ozone observations at Palau from 01/2016-10/2019 confirms the year-round dominance of a low ozone background in the mid-troposphere. Layers of enhanced ozone are often anti-correlated with water vapor and occur frequently. Moreover, the occurrence of respective layers shows a strong seasonality. Dry and ozone-rich air masses between 5 and 10 km altitude were observed in 71 % of the profiles from February until April compared to 25 % from August until October. By defining monthly atmospheric background profiles for ozone and relative humidity based on observed statistics, we found that the deviations from this background reveal a bimodal distribution of RH anomalies. A previously proposed universal bimodal structure of free tropospheric ozone in the TWP could not be verified (Pan et al. 2015). Back trajectory calculations confirm that throughout the year the mid-tropospheric background is controlled by local convective processes and the origin of air masses is thus close to or East of Palau in the Pacific Ocean. Dry and ozone-rich air originates in tropical Asia and reaches Palau in anticyclonic conditions over an area stretching from India to the Philippines. This supports the hypothesis of several studies which attribute ozone enhancement against the low ozone background to remote pollution events on the ground such as biomass burning (e.g. Andersen et al. 2016). A potential vorticity analysis revealed no stratospheric influence and we thus propose large-scale descent within the tropical troposphere as responsible for dehydration of air masses on their way to Palau.

Description: In the Antarctic ozone hole, ozone mixing ratios have been decreasing to extremely low values of 0.01–0.1 ppm in nearly all spring seasons since the late 1980s, corresponding to 95–99% local chemical loss. In contrast, Arctic ozone loss has been much more limited and mixing ratios have never before fallen below 0.5 ppm. In Arctic spring 2020, however, ozonesonde measurements in the most depleted parts of the polar vortex show a highly depleted layer, with ozone loss averaged over sondes peaking at 93% at 18 km. Typical minimum mixing ratios of 0.2 ppm were observed, with individual profiles showing values as low as 0.13 ppm (96% loss). The reason for the unprecedented chemical loss was an unusually strong, long-lasting, and cold polar vortex, showing that for individual winters the effect of the slow decline of ozone-depleting substances on ozone depletion may be counteracted by low temperatures.

Description: The winter 2019/2020 showed the lowest ozone mixing ratios ever observed in the Arctic winter stratosphere. It was the coldest Arctic stratospheric winter on record and was characterized by an unusually strong and long-lasting polar vortex. We study the chemical evolution and ozone depletion in the winter 2019/2020 using the global Chemistry and Transport Model ATLAS. We examine whether the chemical processes in 2019/2020 are more characteristic of typical conditions in Antarctic winters or in average Arctic winters. Model runs for the winter 2019/2020 are compared to simulations of the Arctic winters 2004/2005, 2009/2010, and 2010/2011 and of the Antarctic winters 2006 and 2011, to assess differences in chemical evolution in winters with different meteorological conditions. In some respects, the winter 2019/2020 (and also the winter 2010/2011) was a hybrid between Arctic and Antarctic conditions, for example, with respect to the fraction of chlorine deactivation into HCl versus ClONO2, the amount of denitrification, and the importance of the heterogeneous HOCl + HCl reaction for chlorine activation. The pronounced ozone minimum of less than 0.2 ppm at about 450 K potential temperature that was observed in about 20% of the polar vortex area in 2019/2020 was caused by exceptionally long periods in the history of these air masses with low temperatures in sunlight. Based on a simple extrapolation of observed loss rates, only an additional 21-46 h spent below the upper temperature limit for polar stratospheric cloud formation and in sunlight would have been necessary to reduce ozone to near zero values (0.05 ppm) in these parts of the vortex.