Reply on RC1

Abstract. The short- and long-term variability of the surface spectral solar ultraviolet (UV) irradiance is investigated across Italy using high-quality ground-based measurements from three locations: Aosta (45.7∘ N, 7.4∘ E, 570 m a.s.l.), Rome (41.9∘ N, 12.5∘ E, 15 75 m a.s.l.), and Lampedusa (35.5∘ N, 12.6∘ E, 50 m a.s.l.). The three sites are characterized by different environmental conditions and represent almost the full latitudinal extent of the Italian territory. Data of two periods were analysed: 2006–2020 (all sites) and 1996–2020 (Rome only). The main objective of this study is to quantify the effect of the geopotential height (GPH) at 250 hPa on total ozone, and spectral irradiance at 307.5 and 324 nm. We first show that monthly anomalies in GPH, total ozone, and spectral irradiances are correlated amongst the three sites, suggesting that Italy is often affected by the same synoptical weather systems. We further find statistically significant anticorrelations between GPH and monthly anomalies in total ozone for all stations and months. Conversely, we identify positive correlations between GPH and monthly anomalies in spectral irradiance at 307.5 nm for most months. The influence of GPH on short-term variability also hold for long-term trends. For example, long-term changes in total ozone over the period 2006–2020 were associated with changes in GPH for all stations. This suggests that observed negative trends in total ozone were mainly driven by changes in lower-stratospheric ozone as upper-stratospheric ozone was increasing over this period. For several months of the year, positive trends in UV irradiance were observed, and we found that these trends were predominantly caused by changes in clouds and/or aerosols instead of total ozone. For the longer period of 1996–2020, a statistically significant annualized decrease in total ozone of ∼ 0.1 % per year was identified for Rome and could subsequently be attributed to decreasing lower-stratospheric ozone. While positive trends in spectral irradiance at 307.5 nm were observed for several months of this extended period, the negative trend in total ozone did not lead to a positive trend in the spectral irradiance at 307.5 nm in the deseasonalized data. Our study provides evidence that dynamical processes taking place in the troposphere lead to significant variability in total ozone and surface solar UV irradiance.

In this study the short- and long-term variability of the surface spectral solar ultraviolet (UV) irradiance are investigated over Italy using high quality ground based measurements from three sites located at quite different environmental conditions, and covering the full latitudinal extent of the Italian territory: Aosta (45.7° N, 7.4° E, 570 m a.s.l.), Rome (41.9° N, 12.5° E, 75 m a.s.l.), and Lampedusa (35.5° N, 12.6° E, 50 m a.s.l.). The variability of the irradiances at 307.5 nm, 324 nm, and of the ratio between the 307.5 nm and the 324 nm irradiances were investigated with respect to the corresponding variability in total ozone and the geopotential height at 250 hPa (GPH). The study was performed for two periods: 2006–2020 for all stations, and 1996–2020 only for Rome. A statistically significant correlation between the GPH and total ozone monthly anomalies was found for all stations and all seasons of the year. A corresponding statistically significant correlation was also found in most cases between the GPH and the 307.5 nm irradiance monthly anomalies. The correlation between GPH anomalies at different sites was statistically significant, possibly explaining the strong and significant correlation between the total ozone monthly anomalies at the three sites. A statistically significant decrease of total ozone, of ~0.1 %/year was found for Rome for the period 1996–2020, which however did not induce increasing trends in irradiance at 307.5 nm (neither increasing trends in the ratio between the 307.5 nm and the 324 nm irradiances) at SZA = 67°. Further analyses revealed positive trends in the ratio and the 307.5 nm irradiance at smaller solar zenith angles (SZA), which can be attributed to the fact that total ozone decrease is driven by a decrease in the lower stratosphere while upper stratospheric ozone increases, and the effect of changes of upper stratospheric ozone becoming disproportionately larger for increasing SZA. It was also showed that long-term changes in total ozone follow changes in GPH, which is an additional indication that negative trends in total ozone are mainly driven by changes in lower stratospheric ozone. An anti-correlation between the GPH long-term changes and total ozone was also evident for all stations in 2006–2020. Positive trends in UV irradiance for this latter period which were possibly driven by changes in clouds and/or aerosols were found for Rome and Aosta. This study clearly points out the significance of dynamical processes which take place in the troposphere for the variability of total ozone and surface solar UV irradiance.

Variability of sunspot cycle QBO and total ozone over high altitude western Himalayan regions

Abstract. We present the first spatial analysis of "fingerprints" of the El Niño/Southern Oscillation (ENSO) and atmospheric aerosol load after major volcanic eruptions (El Chichón and Mt. Pinatubo) in extreme low and high (termed ELOs and EHOs, respectively) and mean values of total ozone for the northern and southern mid-latitudes (defined as the region between 30° and 60° north and south, respectively). Significant influence on ozone extremes was found for the warm ENSO phase in both hemispheres during spring, especially towards low latitudes, indicating the enhanced ozone transport from the tropics to the extra-tropics. Further, the results confirm findings of recent work on the connection between the ENSO phase and the strength and extent of the southern ozone "collar". For the volcanic eruptions the analysis confirms findings of earlier studies for the northern mid-latitudes and gives new insights for the Southern Hemisphere. The results provide evidence that the negative effect of the eruption of El Chichón might be partly compensated by a strong warm ENSO phase in 1982–1983 at southern mid-latitudes. The strong west-east gradient in the coefficient estimates for the Mt. Pinatubo eruption and the analysis of the relationship between the AAO and ENSO phase, the extent and the position of the southern ozone "collar" and the polar vortex structure provide clear evidence for a dynamical "masking" of the volcanic signal at southern mid-latitudes. The paper also analyses the contribution of atmospheric dynamics and chemistry to long-term total ozone changes. Here, quite heterogeneous results have been found on spatial scales. In general the results show that EESC and the 11-yr solar cycle can be identified as major contributors to long-term ozone changes. However, a strong contribution of dynamical features (El Niño/Southern Oscillation (ENSO), North Atlantic Oscillation (NAO), Antarctic Oscillation (AAO), Quasi-Biennial Oscillation (QBO)) to ozone variability and trends is found at a regional level. For the QBO (at 30 and 50 hPa), strong influence on total ozone variability and trends is found over large parts of the northern and southern mid-latitudes, especially towards equatorial latitudes. Strong influence of ENSO is found over the Northern and Southern Pacific, Central Europe and central southern mid-latitudes. For the NAO, strong influence on column ozone is found over Labrador/Greenland, the Eastern United States, the Euro-Atlantic Sector, and Central Europe. For the NAO's southern counterpart, the AAO, strong influence on ozone variability and long-term changes is found at lower southern mid-latitudes, including the southern parts of South America and the Antarctic Peninsula, and central southern mid-latitudes.

Cloud cover is one of the important climate indicators. The characteristics of the cloud cover regime can be used to determine the peculiarities of atmospheric circulation, the planetary albedo of the climate system, the effective radiation of the underlying surface and the possible distribution of precipitation, so quantifying changes in cloud cover in modern conditions is relevant. Changes in circulation indices should affect changes in both the quantitative indicators of cloud cover and the repeatability of the main cloud types. An analysis of climatic studies of cloud cover and its actual changes over the territory of Ukraine, which were carried out by Ukrainian scientists, showed that they are based only on ground-based observations. The features of the spatial distribution of individual characteristics were obtained using long-term observations of the same length at all weather stations of the Ukrainian hydrometeorological network. Ukrainian studies of cloud cover fluctuations due to climate change are based on ground observations. Moreover, the length of the rows depends on the goal of the study and the time of its completion. This paper is devoted to the analysis of total and low cloudiness for each month between different decades in relation to the climate norm (1981-2010). The input data for this study was total cloud cover and low cloud cover from ERA5 [https://cds.climate.copernicus.eu/cdsapp#!/dataset/reanalysis-era5-single-levels-monthly-means?tab=overview] for each month of the year for the period 1981-2020 years. The horizontal grid resolution was 0.25 degrees. The data of total and low cloud cover measured in points (from 0 to 10) were also used, which were obtained from the archive of Ukrainian hydrometeorological observation network, which is situated in the Borys Sreznevsky Central Geophysical Observatory. The average monthly data from 15 meteorological stations for the period from 1981 to 2020 were collected: Kyiv, Kharkiv, Odesa, Dnipro, Zaporizhzhia, Kryvyi Rih, Lviv, as well as Kropyvnytskyi, Lutsk, Mykolaiv, Sumy, Uzhhorod, Kherson, Chernivtsi, and Chernihiv. An analysis of cloud cover changes over the past four decades (1981-1990, 1991-2000, 2001-2010, 2011-2020) compared to the climate norm of 1981-2010 showed that they were oscillating over the territory of Ukraine. In some decades both a decrease and an increase of total and low cloudiness were observed in different parts of the country. However, for certain months, there are tendencies toward a decrease in cloud cover over time. These tendencies are most typical for spring and summer. Partially similar changes can be noted for the autumn-winter period. The decrease of low cloud cover prevails over the total cloud cover.

Abstract. Depletion of the stratospheric ozone layer remains an ongoing environmental issue, with increasing stratospheric chlorine from very short-lived substances (VSLS) recently emerging as a potential but uncertain threat to its future recovery. Here the impact of chlorinated VSLS (Cl-VSLS) on past ozone is quantified, for the first time, using the UM–UKCA (Unified Model–United Kingdom Chemistry and Aerosol) chemistry-climate model. Model simulations nudged to reanalysis fields show that in the second decade of the 21st century Cl-VSLS reduced total column ozone by, on average, ∼ 2–3 DU (Dobson unit) in the springtime high latitudes and by ∼0.5 DU in the annual mean in the tropics. The largest ozone reductions were simulated in the Arctic in the springs of 2011 and 2020. During the recent cold Arctic winter of 2019/20 Cl-VSLS resulted in local ozone reductions of up to ∼7 % in the lower stratosphere and of ∼7 DU in total column ozone by the end of March. Despite nearly doubling of Cl-VSLS contribution to stratospheric chlorine over the early 21st century, the inclusion of Cl-VSLS in the nudged simulations does not substantially modify the magnitude of the simulated recent ozone trends and, thus, does not help to explain the persistent negative ozone trends that have been observed in the extra-polar lower stratosphere. The free-running simulations, on the other hand, suggest Cl-VSLS-induced amplification of the negative tropical lower-stratospheric ozone trend by ∼20 %, suggesting a potential role of the dynamical feedback from Cl-VSLS-induced chemical ozone loss. Finally, we calculate the ozone depletion potential of dichloromethane, the most abundant Cl-VSLS, at 0.0107. Our results illustrate a so-far modest but nonetheless non-negligible role of Cl-VSLS in contributing to the stratospheric ozone budget over the recent past that if continues could offset some of the gains achieved by the Montreal Protocol.

Analysis of the monthly mean interannual variations of the total ozone (Total Ozone Mapping Spectrometer (TOMS, TOMS‐Meteor 3)), surface air temperature (National Centres for Environmental Prediction and Atmospheric Research (NCEP/NCAR) reanalysis) and their relations is conducted by means of the singular value decomposition (SVD) for each month December–March 1979–1994. It is shown that the total ozone increase (decrease) occurs almost over those geographical regions where cooling (warming) is observed both on the interannual and longer time‐scales Strong non‐local correlations were indicated between the total ozone changes over England in January and surface temperature variations in western Siberia, southern European Russia and the Azores in February. Similar relations occur for the total ozone (February) and surface temperature (March) changes. These results can be used for the empirical extended‐range forecasts of the anomalously cold winters in Europe and Russia using the total ozone data. Possible mechanisms for this non‐local linkage and its relation to the Arctic Oscillation are discussed.

The morphology of temperature trends in the south polar stratosphere from 1979‐1985 is detailed. A significant cooling has occurred in the stratosphere over this period. South polar October mean temperatures have declined 18°K at 24 km over the seven year period. A large fraction of this decline occurs as a result of including 1979 temperatures in the trend. The years 1979 and 1982 differ from other years in that they include large mid‐October wave events which produce significantly warmer polar temperatures. Nevertheless, a significant temperature decline has still occurred in the stratosphere even when the dynamically active years are not included. Comparing two relatively dynamically quiet years, 1980 and 1985, the largest temperature decrease in the 30 mb temperature field occurs not at the pole but in the sub‐polar temperature maximum centered near 60°S. The changes in temperature of both the maximum and the polar low regions correlate fairly well with total ozone changes observed by TOMS.

A global three-dimensional chemical transport model is being developed for forecasting total ozone. The model includes detailed stratospheric chemistry and transport and couples with a dynamical module of the Meteorological Research Institute/Japan Meteorological Agency 1998 (MRI/JMA98) general circulation model, which can yield realistic atmospheric fields through a meteorological assimilation system. Its predictability on total ozone is investigated for up to 4 weeks from 1997 to 2000. Global root-mean-square errors (rmses) of a control run are approximately 10 DU (3% of total ozone) throughout a year; the control run results are used as initial values for hindcast experiments. Rmses of the hindcast experiments globally range from 10 to 30 DU. The anomaly correlation between the 5-day forecasts and satellite measurements is approximately 0.6 throughout a year in the mid- and high latitudes of both the Northern and Southern Hemispheres. Thus, the model has potential for utilization on total ozone forecasts up to 5 days. In the northern mid- and high latitudes, the model produces better total ozone forecasts than the persistence up to 2 weeks, indicating that the deterministic limit of the total ozone forecasts is durationally comparable to that of weather forecasts. Good correlations between changes in total ozone and 100-hPa geopotential height reveal that the predictability of the dynamical field in the lower stratosphere critically affects the predictability of total ozone.

In this study we present an updated perspective on near-global total ozone trends for the period 1995–2020. We use the GOME-type Total Ozone Essential Climate Variable (GTO-ECV) satellite data record which has been extended and generated as part of the European Space Agency’s Climate Change Initiative (ESA-CCI) and European Union Copernicus Climate Change Service (EU-C3S) ozone projects. The focus of our work is the analysis of regional patterns in the ozone trend as well as the investigation of its seasonal dependence. In the Southern Hemisphere we found regions that indicate statistically significant positive trends increasing from 0.6 ± 0.5 % decade−1 in the subtropics to 1.0 ± 0.9 % decade−1 in the middle latitudes and 2.8 ± 2.6 % decade−1 in the latitude band 60°–70° S. In the middle latitudes of the Northern Hemisphere the trend exhibits distinct regional patterns, i.e. latitudinal and longitudinal structures. Significant positive trends (∼1.5 ± 1.0 % decade−1) over the North Atlantic region as well as negative trends (−1.0 ± 1.0 % decade−1) over Eastern Europe were found. Moreover, these trends indicate a correlation with long-term changes in tropopause pressure. Total ozone trends in the tropics are not significant. Regarding the seasonal dependence of the trends we found only very small variations over the course of the year. However, we identified different behavior depending on latitude. In the latitude band 40°–70° N the positive trend maximizes in boreal winter from December to February. In the middle latitudes of the Southern Hemisphere (35°–50° S) the trend is maximum from March to May. Further south toward the high latitudes (55°–70° S) the trend denotes a relatively strong seasonal cycle which varies from 2 % decade−1 in December and January to 3.8 % decade−1 in June and July.

On timescales less than a month, negative (positive) 100 hPa temperature anomalies (deviations from seasonal means) and positive (negative) 100 hPa height anomalies at northern midlatitudes are associated with negative (positive) total ozone anomalies owing to vertical and horizontal advective transport of ozone. We apply linear regression relationships between total ozone and 100 hPa temperature and height together with observed monthly temperature and height anomalies to estimate the component of total ozone variability at northern midlatitudes that results from month‐to‐month differences in advective transport. At 45°N, this empirical method simulates a large part of the observed monthly zonal mean total ozone variability over the period 1979–1991. In order to estimate the advective transport contribution to total ozone trends, we apply a multiple regression statistical model to empirical model time series for latitudes of 10°N to 60°N. These empirical model trends result from long‐term changes in ozone advective transport which are calculated on a month‐to‐month basis. The resulting model trend component at northern midlatitudes in February has a longitude dependence consistent with that of the observed ozone trends and has a latitude dependence that also agrees with that of the observed trends, peaking at midlatitudes and decreasing at higher latitudes. Subtracting the estimated advective contribution from the observed trends yields a residual meridional trend profile that agrees more closely in latitude dependence and amplitude with two‐dimensional stratospheric model estimates.

Abstract. Continuous measurements of total ozone (by Dobson spectrophotometers) across the contiguous United States began in the early 1960s. Here, we analyze temporal and spatial variability and trends in total ozone from the five US sites with long-term records. While similar long-term ozone changes are detected at all five sites, we find differences in the patterns of ozone variability on shorter timescales. In addition to standard evaluation techniques, STL-decomposition methods (Seasonal Trend decomposition of time series based on LOESS (LOcally wEighted Scatterplot Smoothing)) are used to address temporal variability and "fingerprints" of dynamical features in the Dobson data. Methods from statistical extreme value theory (EVT) are used to characterize days with high and low total ozone (termed EHOs and ELOs, respectively) at each station and to analyze temporal changes in the frequency of ozone extremes and their relationship to dynamical features such as the North Atlantic Oscillation (NAO) and El Niño–Southern Oscillation. A comparison of the fingerprints detected in the frequency distribution of the extremes with those for standard metrics (i.e., the mean) shows that more fingerprints are found for the extremes, particularly for the positive phase of the NAO, at all five US monitoring sites. Results from the STL decomposition support the findings of the EVT analysis. Finally, we analyze the relative influence of low- and high-ozone events on seasonal mean column ozone at each station. The results show that the influence of ELOs and EHOs on seasonal mean column ozone can be as much as ±5 %, about as large as the overall long-term decadal ozone trends.

Stratospheric circulation is a critical part of the Arctic ozone cycle. Sudden stratospheric warming events (SSWs) manifest the strongest alteration of stratospheric dynamics. Changes in planetary wave propagation vigorously influence zonal mean zonal wind, temperature, and tracer concentrations in the stratosphere over the high latitudes. In this study, we examine six major SSWs from 2004 to 2020 using the Modern-Era Retrospective analysis for Research and Applications, Version 2 (MERRA-2). Using the unique density of observations around the Greenland sector at high latitudes, we perform comprehensive comparisons of high latitude observations with the MERRA-2 ozone dataset during the six major SSWs. Our results show that MERRA-2 captures the high variability of mid stratospheric ozone fluctuations during SSWs over high latitudes. However, larger uncertainties are observed in the lower stratosphere and troposphere. The zonally averaged stratospheric ozone shows a dramatic increase of 9–29 % in total column ozone (TCO) near the time of each SSW, which lasts up to two months. The SSWs exhibit a more significant impact on ozone over high northern latitudes when the polar vortex is mostly elongated as seen in 2009 and 2018 compared to the events in which the polar vortex is displaced towards Europe. The regional impact of SSWs over Greenland has a similar structure as the zonal average, however, exhibits more intense ozone anomalies which is reflected by 15–37 % increase in TCO. The influence of SSW on mid stratospheric ozone levels persists longer than their impact on temperature. This paper is focused on the increased (suppressed) wave activity before (after) the SSWs and their impact on ozone variability at high latitudes. This includes an investigation of the different terms of tracer continuity using MERRA-2 parameters, which emphasizes the key role of vertical advection on mid-stratospheric ozone during the SSWs.

Abstract. Despite decades of effort, the drivers of global long-term trends in tropospheric ozone are not well understood, impacting estimates of ozone radiative forcing and the global ozone budget. We analyze tropospheric ozone trends since 1980 using ozonesondes and remote surface measurements around the globe and investigate the ability of two atmospheric chemical transport models, GEOS-Chem and MERRA2-GMI, to reproduce these trends. Global tropospheric ozone trends measured at 25 ozonesonde sites from 1990–2017 (nine sites since 1980s) show increasing trends averaging 1.8 ± 1.3 ppb per decade across sites in the free troposphere (800–400 hPa). Relative trends in sondes are more pronounced closer to the surface (3.5 % per decade above 700 hPa, 4.3 % per decade below 700 hPa on average), suggesting the importance of surface emissions (anthropogenic, soil NOx, impacts on biogenic volatile organic compounds (VOCs) from land use changes, etc.) in observed changes. While most surface sites (148 of 238) in the United States and Europe exhibit decreases in high daytime ozone values due to regulatory efforts, 73 % of global sites outside these regions (24 of 33 sites) show increases from 1990–2014 that average 1.4 ± 0.9 ppb per decade. In all regions, increasing ozone trends both at the surface and aloft are at least partially attributable to increases in 5th percentile ozone, which average 1.8 ± 1.3 ppb per decade and reflect the global increase of baseline ozone in rural areas. Observed ozone percentile distributions at the surface have shifted notably across the globe: all regions show increases in low tails (i.e., below 25th percentile), North America and Europe show decreases in high tails (above 75th percentile), and the Southern Hemisphere and Japan show increases across the entire distribution. Three model simulations comprising different emissions inventories, chemical schemes, and resolutions, sampled at the same locations and times of observations, are not able to replicate long-term ozone trends either at the surface or free troposphere, often underestimating trends. We find that ∼75 % of the average ozone trend from 800–400 hPa across the 25 ozonesonde sites is captured by MERRA2-GMI, and <20 % is captured by GEOS-Chem. MERRA2-GMI performs better than GEOS-Chem in the northern midlatitude free troposphere, reproducing nearly half of increasing trends since 1990 and capturing stratosphere–troposphere exchange (STE) determined via a stratospheric ozone tracer. While all models tend to capture the direction of shifts in the ozone distribution and typically capture changes in high and low tails, they tend to underestimate the magnitude of the shift in medians. However, each model shows an 8 %–12 % (or 23–32 Tg) increase in total tropospheric ozone burden from 1980 to 2017. Sensitivity simulations using GEOS-Chem and the stratospheric ozone tracer in MERRA2-GMI suggest that in the northern midlatitudes and high latitudes, dynamics such as STE are most important for reproducing ozone trends in models in the middle and upper troposphere, while emissions are more important closer to the surface. Our model evaluation for the last 4 decades reveals that the recent version of the GEOS-Chem model underpredicts free tropospheric ozone across this long time period, particularly in winter and spring over midlatitudes to high latitudes. Such widespread model underestimation of tropospheric ozone highlights the need for better understanding of the processes that transport ozone and promote its production.

Abstract. Within the European project UFTIR (Time series of Upper Free Troposphere observations from an European ground-based FTIR network), six ground-based stations in Western Europe, from 79° N to 28° N, all equipped with Fourier Transform infrared (FTIR) instruments and part of the Network for the Detection of Atmospheric Composition Change (NDACC), have joined their efforts to evaluate the trends of several direct and indirect greenhouse gases over the period 1995–2004. The retrievals of CO, CH4, C2H6, N2O, CHClF2, and O3 have been optimized. Using the optimal estimation method, some vertical information can be obtained in addition to total column amounts. A bootstrap resampling method has been implemented to determine annual partial and total column trends for the target gases. The present work focuses on the ozone results. The retrieved time series of partial and total ozone columns are validated with ground-based correlative data (Brewer, Dobson, UV-Vis, ozonesondes, and Lidar). The observed total column ozone trends are in agreement with previous studies: 1) no total column ozone trend is seen at the lowest latitude station Izaña (28° N); 2) slightly positive total column trends are seen at the two mid-latitude stations Zugspitze and Jungfraujoch (47° N), only one of them being significant; 3) the highest latitude stations Harestua (60° N), Kiruna (68° N) and Ny-Ålesund (79° N) show significant positive total column trends. Following the vertical information contained in the ozone FTIR retrievals, we provide partial columns trends for the layers: ground-10 km, 10–18 km, 18–27 km, and 27–42 km, which helps to distinguish the contributions from dynamical and chemical changes on the total column ozone trends. We obtain no statistically significant trends in the ground-10 km layer for five out of the six ground-based stations. We find significant positive trends for the lowermost stratosphere at the two mid-latitude stations, and at Ny-Ålesund. We find smaller, but significant trends for the 18–27 km layer at Kiruna, Harestua, Jungfraujoch, and Izaña. The results for the upper layer are quite contrasted: we find significant positive trends at Kiruna, Harestua, and Jungfraujoch, and significant negative trends at Zugspitze and Izaña. These ozone partial columns trends are discussed and compared with previous studies.