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Dry deposition to the surface is one of the main removal pathways of tropospheric ozone (O₃). We quantified for the first time the impact of O₃ deposition to the Arctic sea ice on the planetary boundary layer (PBL) O₃ concentration and budget using year-round flux and concentration observations from the Multidisciplinary drifting Observatory for the Study of Arctic Climate (MOSAiC) campaign and simulations with a single-column atmospheric chemistry and meteorological model (SCM). Based on eddy-covariance O₃ surface flux observations, we find a median surface resistance on the order of 20,000 s m¯¹, resulting in a dry deposition velocity of approximately 0.005 cm s¯¹. This surface resistance is up to an order of magnitude larger than traditionally used values in many atmospheric chemistry and transport models. The SCM is able to accurately represent the yearly cycle, with maxima above 40 ppb in the winter and minima around 15 ppb at the end of summer. However, the observed springtime ozone depletion events are not captured by the SCM. In winter, the modelled PBL O₃ budget is governed by dry deposition at the surface mostly compensated by downward turbulent transport of O₃ towards the surface. Advection, which is accounted for implicitly by nudging to reanalysis data, poses a substantial, mostly negative, contribution to the simulated PBL O₃ budget in summer. During episodes with low wind speed (<5 m s¯¹) and shallow PBL (<50 m), the 7-day mean dry deposition removal rate can reach up to 1.0 ppb h¯¹. Our study highlights the importance of an accurate description of dry deposition to Arctic sea ice in models to quantify the current and future O₃ sink in the Arctic, impacting the tropospheric O₃ budget, which has been modified in the last century largely due to anthropogenic activities.

Dry deposition to the surface is one of the main removal pathways of tropospheric ozone (O3). We quantified for the first time the impact of O3 deposition to the Arctic sea ice on the planetary boundary layer (PBL) O3 concentration and budget using year-round flux and concentration observations from the Multidisciplinary drifting Observatory for the Study of Arctic Climate (MOSAiC) campaign and simulations with a single-column atmospheric chemistry and meteorological model (SCM). Based on eddy-covariance O3 surface flux observations, we find a median surface resistance on the order of 20,000 s m−1, resulting in a dry deposition velocity of approximately 0.005 cm s−1. This surface resistance is up to an order of magnitude larger than traditionally used values in many atmospheric chemistry and transport models. The SCM is able to accurately represent the yearly cycle, with maxima above 40 ppb in the winter and minima around 15 ppb at the end of summer. However, the observed springtime ozone depletion events are not captured by the SCM. In winter, the modelled PBL O3 budget is governed by dry deposition at the surface mostly compensated by downward turbulent transport of O3 towards the surface. Advection, which is accounted for implicitly by nudging to reanalysis data, poses a substantial, mostly negative, contribution to the simulated PBL O3 budget in summer. During episodes with low wind speed (

With the Arctic rapidly changing, the needs to observe, understand, and model the changes are essential. To support these needs, an annual cycle of observations of atmospheric properties, processes, and interactions were made while drifting with the sea ice across the central Arctic during the Multidisciplinary drifting Observatory for the Study of Arctic Climate (MOSAiC) expedition from October 2019 to September 2020. An international team designed and implemented the comprehensive program to document and characterize all aspects of the Arctic atmospheric system in unprecedented detail, using a variety of approaches, and across multiple scales. These measurements were coordinated with other observational teams to explore cross-cutting and coupled interactions with the Arctic Ocean, sea ice, and ecosystem through a variety of physical and biogeochemical processes. This overview outlines the breadth and complexity of the atmospheric research program, which was organized into 4 subgroups: atmospheric state, clouds and precipitation, gases and aerosols, and energy budgets. Atmospheric variability over the annual cycle revealed important influences from a persistent large-scale winter circulation pattern, leading to some storms with pressure and winds that were outside the interquartile range of past conditions suggested by long-term reanalysis. Similarly, the MOSAiC location was warmer and wetter in summer than the reanalysis climatology, in part due to its close proximity to the sea ice edge. The comprehensiveness of the observational program for characterizing and analyzing atmospheric phenomena is demonstrated via a winter case study examining air mass transitions and a summer case study examining vertical atmospheric evolution. Overall, the MOSAiC atmospheric program successfully met its objectives and was the most comprehensive atmospheric measurement program to date conducted over the Arctic sea ice. The obtained data will support a broad range of coupled-system

With the Arctic rapidly changing, the needs to observe, understand, and model the changes are essential. To support these needs, an annual cycle of observations of atmospheric properties, processes, and interactions were made while drifting with the sea ice across the central Arctic during the Multidisciplinary drifting Observatory for the Study of Arctic Climate (MOSAiC) expedition from October 2019 to September 2020. An international team designed and implemented the comprehensive program to document and characterize all aspects of the Arctic atmospheric system in unprecedented detail, using a variety of approaches, and across multiple scales. These measurements were coordinated with other observational teams to explore crosscutting and coupled interactions with the Arctic Ocean, sea ice, and ecosystem through a variety of physical and biogeochemical processes. This overview outlines the breadth and complexity of the atmospheric research program, which was organized into 4 subgroups: atmospheric state, clouds and precipitation, gases and aerosols, and energy budgets. Atmospheric variability over the annual cycle revealed important influences from a persistent large-scale winter circulation pattern, leading to some storms with pressure and winds that were outside the interquartile range of past conditions suggested by long-term reanalysis. Similarly, the MOSAiC location was warmer and wetter in summer than the reanalysis climatology, in part due to its close proximity to the sea ice edge. The comprehensiveness of the observational program for characterizing and analyzing atmospheric phenomena is demonstrated via a winter case study examining air mass transitions and a summer case study examining vertical atmospheric evolution. Overall, the MOSAiC atmospheric program successfully met its objectives and was the most comprehensive atmospheric measurement program to date conducted over the Arctic sea ice. The obtained data will support a broad range of coupled-system s

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.

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 in boreal winter (e.g. Rex et al. 2014), we set up an atmospheric research station in Palau (7°N 134°E) as part of the StratoClim campaign. Our analysis of regular balloon-borne tropospheric ozone observations at Palau from 01/2016-12/2019 gives unprecedented insights into transport processes and air mass origin in the TWP. We confirm 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 (ATLAS) 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 controversial hypothesis of several studies which attribute ozone enhancement against the ozone-poor 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 de

A comprehensive analysis of the temporal evolution of tropospheric ozone in Antarctica using more than 25 years of surface and ozonesonde measurements reveals significant changes in tropospheric ozone there. It shows a positive trend in ozone at the surface lower and mid-troposphere, but a negative trend in the upper troposphere. We also find significant links between different climate modes and tropospheric ozone in Antarctica and observe that changes in residual overturning circulation, the strength of the polar vortex, and stratosphere-troposphere exchange make noticeable variability in tropospheric ozone. Therefore, this study alerts increasing ozone concentration in Antarctica, which would have a profound impact on the future climate of the region as tropospheric ozone has warming feedback to the Earth’s climate.

Throughout spring and summer 2020, ozone stations in the northern extratropics recorded unusually low ozone in the free troposphere. From April to August, and from 1 to 8 kilometers altitude, ozone was on average 7% (≈4 nmol/mol) below the 2000 to 2020 climatological mean. Such low ozone, over several months, and at so many stations, has not been observed in any previous year since at least 2000. Atmospheric composition analyses from the Copernicus Atmosphere Monitoring Service and simulations from the NASA GMI model indicate that the large 2020 springtime ozone depletion in the Arctic stratosphere contributed less than one quarter of the observed tropospheric anomaly. The observed anomaly is consistent with recent chemistry-climate model simulations, which assume emissions reductions similar to those caused by the COVID-19 crisis. COVID-19 related emissions reductions appear to be the major cause for the observed reduced free tropospheric ozone in 2020.

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.

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.

Ozonesonde data from four sites are analyzed in relation to 191 solar protons events (SPEs) from 1989-2016. Analysis shows ozone depletion (~10-35 km altitude) commencing following the SPEs. Seasonally-corrected ozone data demonstrate that depletions occur only in winter/early-spring above sites where the northern hemisphere polar vortex (PV) can be present. A rapid reduction in stratospheric ozone is observed with the maximum decrease occurring ~10-20 days after SPEs. Ozone levels remain depleted in excess of 30 days. No depletion is observed above sites completely outside the PV. No depletion is observed in relation to 191 random epochs at any site at any time of year. Results point to the role of indirect ozone destruction, most likely via the rapid descent of long-lived NOx species in the PV during the polar winter.

We validate the Ozone Monitoring Instrument (OMI) Ozone Profile (PROFOZ) product from October 2004 through December 2014 retrieved by the Smithsonian Astrophysical Observatory (SAO) algorithm against ozonesonde observations. We also evaluate the effects of OMI row anomaly (RA) on the retrieval by dividing the dataset into before and after the occurrence of serious OMI RA, i.e., pre-RA (2004–2008) and post-RA (2009–2014). The retrieval shows good agreement with ozonesondes in the tropics and midlatitudes and for pressure < ∼ 50 hPa in the high latitudes. It demonstrates clear improvement over the a priori down to the lower troposphere in the tropics and down to an average of ∼ 550 (300) hPa at middle (high) latitudes. In the tropics and midlatitudes, the profile mean biases (MBs) are less than 6 %, and the standard deviations (SDs) range from 5 to 10 % for pressure < ∼ 50 hPa to less than 18 % (27 %) in the tropics (midlatitudes) for pressure > ∼ 50 hPa after applying OMI averaging kernels to ozonesonde data. The MBs of the stratospheric ozone column (SOC, the ozone column from the tropopause pressure to the ozonesonde burst pressure) are within 2 % with SDs of < 5 % and the MBs of the tropospheric ozone column (TOC) are within 6 % with SDs of 15 %. In the high latitudes, the profile MBs are within 10 % with SDs of 5–15 % for pressure < ∼ 50 hPa but increase to 30 % with SDs as great as 40 % for pressure > ∼ 50 hPa. The SOC MBs increase up to 3 % with SDs as great as 6 % and the TOC SDs increase up to 30 %. The comparison generally degrades at larger solar zenith angles (SZA) due to weaker signals and additional sources of error, leading to worse performance at high latitudes and during the midlatitude winter. Agreement also degrades with increasing cloudiness for pressure > ∼ 100 hPa and varies with cross-track position, especially with large MBs and SDs at extreme off-nadir positions. In the tropics and midlatitudes, the post-RA comparison is considerably wo

We validate the Ozone Monitoring Instrument (OMI) ozone-profile (PROFOZ) product from October 2004 through December 2014 retrieved by the Smithsonian Astrophysical Observatory (SAO) algorithm against ozonesonde observations. We also evaluate the effects of OMI Row anomaly (RA) on the retrieval by dividing the data set into before and after the occurrence of serious OMI RA, i.e., pre-RA (2004–2008) and post-RA (2009–2014). The retrieval shows good agreement with ozonesondes in the tropics and mid-latitudes and for pressure < ~ 50 hPa in the high latitudes. It demonstrates clear improvement over the a priori down to the lower troposphere in the tropics and down to an average of ~ 550 (300) hPa at middle (high latitudes). In the tropics and mid-latitudes, the profile mean biases (MBs) are less than 6 %, and the standard deviations (SDs) range from 5–10 % for pressure < ~ 50 hPa to less than 18 % (27 %) in the tropics (mid-latitudes) for pressure > ~ 50 hPa after applying OMI averaging kernels to ozonesonde data. The MBs of the stratospheric ozone column (SOC) are within 2 % with SDs of < 5 % and the MBs of the tropospheric ozone column (TOC) are within 6 % with SDs of 15 %. In the high latitudes, the profile MBs are within 10 % with SDs of 5–15 % for pressure < ~ 50 hPa, but increase to 30 % with SDs as great as 40 % for pressure > ~ 50 hPa. The SOC MBs increase up to 3 % with SDs as great as 6 % and the TOC SDs increase up to 30 %. The comparison generally degrades at larger solar-zenith angles (SZA) due to weaker signals and additional sources of error, leading to worse performance at high latitudes and during the mid-latitude winter. Agreement also degrades with increasing cloudiness for pressure > ~ 100 hPa and varies with cross-track position, especially with large MBs and SDs at extreme off-nadir positions. In the tropics and mid-latitudes, the post-RA comparison is considerably worse with larger SDs reaching 2 % in the stratosphere and 8 % in the troposphere and