Stratospheric Column Ozone Research Articles

Wavelet Analysis of Ozone Driving Factors Based on ~20 Years of Ozonesonde Measurements in Beijing

A long-term vertical ozone observational dataset has been provided during 2001–2019 by ozonesonde measurements in Beijing on the North China Plain. Previous studies using this dataset primarily focused on the vertical characteristics of climatological ozone and its variation; however, the driving factors of ozone variation have not been well discussed. In this study, by applying the wavelet analysis method (including continuous wavelet transform and cross wavelet) and sliding correlation coefficients to ~20 years of ozonesonde measurements collected in Beijing, we analyzed the dominant modes of ozone column variability within three height ranges over Beijing (total column ozone: TOT; stratospheric column ozone: SCO; and tropospheric column ozone: TCO). Moreover, we also preliminarily discussed the relationship between these three ozone columns and the El Niño Southern Oscillation (ENSO), Quasi-biennial Oscillation (QBO), and 11-year solar activity cycle. The results revealed that the ozone columns within the three height ranges predominantly adhered to interannual variability patterns, and the short-term variabilities in TOT and SCO may have been related to eruptive volcanic activity. In comparison to the TOT and SCO, the TCO was more susceptible to the forcing influences of high-frequency factors such as pollutant transport. Similar to the results in other mid-latitude regions, strong ENSO and QBO signals were revealed in the interannual ozone column variability over Beijing. The TOT and SCO showed positive anomalous responses to ENSO warm-phase events, and the peak of the ENSO warm phase led the winter peaks of the TOT and SCO by approximately 3–6 months. During the strong cold–warm transition phase in 2009–2012, the TOT and SCO showed a significant positive correlation with the ENSO index. The strong seasonality of the meridional circulation process driven by the QBO led to a significant positive correlation between the QBO index and the TOT and SCO in the interannual cycle, except for two periods of abnormal QBO fluctuations in 2010–2012 and 2015–2017, whereas the TCO showed a time-lagged correlation of approximately 3 months in the annual cycle relative to the QBO due to the influence of the thermodynamic tropopause. In addition, analysis of the F10.7 index and the ozone columns revealed that the ozone columns over Beijing exhibited lagged responses to the peaks of sunspot activity, and there was no obvious correlation between ozone columns and 11-year solar activity cycle. Given the complex driving mechanism of the climatic factors on local ozone variability, the preliminary results obtained in this study still require further validation using longer time series of observational data and the combination of chemical models and more auxiliary data.

High Spatial Resolution Ozone Profiles Retrieved from the First Chinese Ultraviolet–Visible Hyperspectral Satellite Instrument

Understanding the vertical distribution of ozone is crucial when assessing both its horizontal and vertical transport, as well as when analyzing the physical and chemical properties of the atmosphere. One of the most effective ways to obtain high spatial resolution ozone profiles is through satellite observations. The Environmental Trace Gases Monitoring Instrument (EMI) deployed on the Gaofen-5 satellite is the first Chinese ultraviolet–visible hyperspectral spectrometer. However, retrieving ozone profiles using backscattered radiance values measured by the EMI is challenging due to unavailable measurement errors and a low signal-to-noise ratio. The algorithm developed for the Tropospheric Monitoring Instrument did not allow us to retrieve 87% of the EMI pixels. Therefore, we developed an algorithm specific to the characteristics of the EMI. The fitting residuals are smaller than 0.3% in most regions. The retrieved ozone profiles were in good agreement with ozonesonde data, with maximum mean biases of 20% at five latitude bands. By applying EMI averaging kernels to the ozonesonde profiles, the integrated stratospheric column ozone and tropospheric column ozone also showed excellent agreement with ozonesonde data. The lower layers (0–7.5 km) of the EMI ozone profiles reflected the seasonal variation in surface ozone derived from the China National Environmental Monitoring Center (CNEMC). However, the upper layers (9.7–16.7 km) of the ozone profiles show different trends, with the ozone peak occurring at an altitude of 9.7–16.7 km in March, 2019. A stratospheric intrusion event in central China from August 11 to 15, 2019, is captured using the EMI ozone profiles, potential vorticity data, and relative humidity data. The increase in the CNEMC ozone concentration showed that downward transport enhanced surface ozone pollution.

Synergy of Using Nadir and Limb Instruments for Tropospheric Ozone Monitoring (SUNLIT)

Abstract. Satellite measurements in nadir and limb viewing geometry provide a complementary view of the atmosphere. An effective combination of the limb and nadir measurements can give new information about atmospheric composition. In this work, we present tropospheric ozone column datasets that have been created using a combination of total ozone columns from OMI (Ozone Monitoring Instrument) and TROPOMI (TROPOspheric Monitoring Instrument) with stratospheric ozone column datasets from several available limb-viewing instruments: MLS (Microwave Limb Sounder), OSIRIS (Optical Spectrograph and InfraRed Imaging System), MIPAS (Michelson Interferometer for Passive Atmospheric Sounding), SCIAMACHY (SCanning Imaging Spectrometer for Atmospheric CHartographY), OMPS-LP (Ozone Mapping and Profiles Suite – Limb Profiler), and GOMOS (Global Ozone Monitoring by Occultation of Stars). We have developed further the methodological aspects of the assessment of tropospheric ozone using the residual method supported by simulations with the chemistry transport model SILAM (System for Integrated modeLling of Atmospheric coMposition). It has been shown that the accurate assessment of ozone in the upper troposphere and the lower stratosphere (UTLS) is of high importance for detecting the ground-level ozone patterns. The stratospheric ozone column is derived from a combination of ozone profiles from several satellite instruments in limb-viewing geometry. We developed a method for the data homogenization, which includes the removal of biases and a posteriori estimation of random uncertainties, thus making the data from different instruments compatible with each other. The high-horizontal- and vertical-resolution dataset of ozone profiles is created via interpolation of the limb profiles from each day to a 1∘×1∘ horizonal grid. A new kriging-type interpolation method, which takes into account data uncertainties and the information about natural ozone variations from the SILAM-adjusted ozone field, has been developed. To mitigate the limited accuracy and coverage of the limb profile data in the UTLS, a smooth transition to the model data is applied below the tropopause. This allows for the estimation of the stratospheric ozone column with full coverage of the UTLS. The derived ozone profiles are in very good agreement with collocated ozonesonde measurements. The residual method was successfully applied to OMI and TROPOMI clear-sky total ozone data in combination with the stratospheric ozone column from the developed high-resolution limb profile dataset. The resulting tropospheric ozone column is in very good agreement with other satellite data. The global distributions of tropospheric ozone exhibit enhancements associated with the regions of high tropospheric ozone production. The main datasets created are (i) a monthly 1∘×1∘ global tropospheric ozone column dataset (from ground to 3 km below the tropopause) using OMI and limb instruments, (ii) a monthly 1∘×1∘ global tropospheric ozone column dataset using TROPOMI and limb instruments, and (iii) a daily 1∘×1∘ interpolated stratospheric ozone column from limb instruments. Other datasets, which are created as an intermediate step of creating the tropospheric ozone column data, are (i) a daily 1∘×1∘ clear-sky and total ozone column from OMI and TROPOMI, (ii) a daily 1∘×1∘ homogenized and interpolated dataset of ozone profiles from limb instruments, and (iii) a daily 1∘×1∘ dataset of ozone profiles from SILAM simulations with adjustment to satellite data. These datasets can be used in various studies related to variability and trends in ozone distributions in both the troposphere and the stratosphere. The datasets are processed from the beginning of OMI and TROPOMI measurements until December 2020 and are planned to be regularly extended in the future.

Kolmogorov Complexity Analysis and Prediction Horizon of the Daily Erythemal Dose Time Series

Influenced by stratospheric total ozone column (TOC), cloud cover, aerosols, albedo, and other factors, levels of daily erythemal dose (Her) in a specific geographic region show significant variability in time and space. To investigate the degree of randomness and predictability of Her time series from ground-based observations in Novi Sad, Serbia, during the 2003–2012 time period, we used a set of information measures: Kolmogorov complexity, Kolmogorov complexity spectrum, running Kolmogorov complexity, the largest Lyapunov exponent, Lyapunov time, and Kolmogorov time. The result reveals that fluctuations in daily Her are moderately random and exhibit low levels of chaotic behavior. We found a larger number of occurrences of deviation from the mean in the time series during the years with lower values of Her (2007–2009, 2011–2012), which explains the higher complexity. Our analysis indicated that the time series of daily values of Her show a tendency to increase the randomness when the randomness of cloud cover and TOC increases, which affects the short-term predictability. The prediction horizon of daily Her values in Novi Sad given by the Lyapunov time corrected for randomness by Kolmogorov is between 1.5 and 3.5 days.

Characterizing ozone throughout the atmospheric column over the tropical Andes from in situ and remote sensing observations

In this study, we characterize atmospheric ozone over the tropical Andes in the boundary layer, the free troposphere, and the stratosphere; we quantify each contribution to total column ozone, and we evaluate the performance of the multi-sensor reanalysis (MSR2) in the region. Thus, we present data taken in Ecuador and Peru (2014–2019). The contribution from the surface was determined by integrating ozone concentrations measured in Quito and Cuenca (Ecuador) up to boundary layer height. In addition, tropospheric and stratospheric column ozone were quantified from ozone soundings (38) launched from Quito during the study time period. Profiles were compared against soundings at Natal (SHADOZ network) for being the closest observational reference with sufficient data in 2014–2019. Data were also compared against stratospheric mixing ratios from the Aura Microwave Limb Sounder (Aura MLS). Findings demonstrate that the stratospheric component of total column ozone over the Andes (225.2 ± 8.9 Dobson Units [DU]) is at similar levels as those observed at Natal (223.3 ± 8.6 DU), and observations are comparable to Aura MLS data. In contrast, the tropospheric contribution is lower over the Andes (20.2 ± 4.3 DU) when compared to Natal (35.4 ± 6.4 DU) due to a less deep and cleaner troposphere. From sounding extrapolation of Quito profiles down to sea level, we determined that altitude deducts about 5–7 DU from the total column, which coincides with a 3%–4% overestimation of the MSR2 over Quito and Marcapomacocha (Peru). In addition, when MSR2 data are compared along a transect that crosses from the Amazon over Quito, the Ecuadorian coast side, and into the Pacific, observations are not significantly different among the three first locations. Results point to coarse reanalysis resolution not being suitable to resolve the formidable altitude transition imposed by the Andes mountain chain. This work advances our knowledge of atmospheric ozone over the study region and provides a robust time series of upper air measurements for future evaluations of satellite and reanalysis products.

Evaluation of the interactive stratospheric ozone (O3v2) module in the E3SM version 1 Earth system model

Abstract. Stratospheric ozone affects climate directly as the predominant heat source in the stratosphere and indirectly through chemical reactions controlling other greenhouse gases. The U.S. Department of Energy's Energy Exascale Earth System Model version 1 (E3SMv1) implemented a new ozone chemistry module that improves the simulation of the sharp tropopause gradients, replacing a version based partly on long-term average climatologies that poorly represented heating rates in the lowermost stratosphere. The new O3v2 module extends seamlessly into the troposphere and preserves the naturally sharp cross-tropopause gradient, with 20 %–40 % less ozone in this region. Additionally, O3v2 enables the diagnosis of stratosphere–troposphere exchange flux of ozone, a key budget term lacking in E3SMv1. Here, we evaluate key features in ozone abundance and other closely related quantities in atmosphere-only E3SMv1 simulations driven by observed sea surface temperatures (SSTs, years 1990–2014), comparing them with satellite observations of ozone and also with the University of California, Irvine chemistry transport model (UCI CTM) using the same stratospheric chemistry scheme but driven by European Centre forecast fields for the same period. In terms of stratospheric column ozone, O3v2 shows reduced mean bias and improved northern midlatitude variability, but it is not quite as good as the UCI CTM. As expected, SST-forced E3SMv1 simulations cannot synchronize with observed quasi-biennial oscillations (QBOs), but they do show the typical QBO pattern seen in column ozone. This new O3v2 E3SMv1 model mostly retains the same climate state and climate sensitivity as the previous version, and we recommend its use for other climate models that still use ozone climatologies.

Verification of the Atmospheric Infrared Sounder (AIRS) and the Microwave Limb Sounder (MLS) ozone algorithms based on retrieved daytime and night-time ozone

Abstract. Ozone (O3) plays a significant role in weather and climate on regional to global spatial scales. Most studies on the variability in the total column of O3 (TCO) are typically carried out using daytime data. Based on knowledge of the chemistry and transport of O3, significant deviations between daytime and night-time O3 are only expected either in the planetary boundary layer (PBL) or high in the stratosphere or mesosphere, with little effect on the TCO. Hence, we expect the daytime and night-time TCO to be very similar. However, a detailed evaluation of satellite measurements of daytime and night-time TCO is still lacking, despite the existence of long-term records of both. Thus, comparing daytime and night-time TCOs provides a novel approach to verifying the retrieval algorithms of instruments such as the Atmospheric Infrared Sounder (AIRS) and the Microwave Limb Sounder (MLS). In addition, such a comparison also helps to assess the value of night-time TCO for scientific research. Applying this verification on the AIRS and the MLS data, we identified inconsistencies in observations of O3 from both satellite instruments. For AIRS, daytime–night-time differences were found over oceans resembling cloud cover patterns and over land, mostly over dry land areas, which is likely related to infrared surface emissivity. These differences point to issues with the representation of both processes in the AIRS retrieval algorithm. For MLS, a major issue was identified with the “ascending–descending” orbit flag, used to discriminate night-time and daytime MLS measurements. Disregarding this issue, MLS day–night differences were significantly smaller than AIRS day–night differences, providing additional support for the retrieval method origin of AIRS in stratospheric column ozone (SCO) day–night differences. MLS day–night differences are dominated by the upper-stratospheric and mesospheric diurnal O3 cycle. These results provide useful information for improving infrared O3 products.

Using Machine Learning to Make Computationally Inexpensive Projections of 21st Century Stratospheric Column Ozone Changes in the Tropics

Stratospheric ozone projections in the tropics, modeled using the UKESM1 Earth system model, are explored under different Shared Socioeconomic Pathways (SSPs). Consistent with other studies, it is found that tropical stratospheric column ozone does not return to 1980s values by the end of the 21st century under any SSP scenario as increased ozone mixing ratios in the tropical upper stratosphere are offset by continued ozone decreases in the tropical lower stratosphere. Stratospheric column ozone is projected to be largest under SSP scenarios with the smallest change in radiative forcing, and smallest for SSP scenarios with larger radiative forcing, consistent with a faster Brewer-Dobson circulation at high greenhouse gas loadings. This study explores the use of machine learning (ML) techniques to make accurate, computationally inexpensive projections of tropical stratospheric column ozone. Four ML techniques are investigated: Ridge regression, Lasso regression, Random Forests and Extra Trees. All four techniques investigated here are able to make projections of future tropical stratospheric column ozone which agree well with those made by the UKESM1 Earth system model, often falling within the ensemble spread of UKESM1 simulations for a broad range of SSPs. However, all techniques struggle to make accurate projects for the final decades of the SSP5-8.5 scenario. Accurate projections can only be achieved when the ML methods are trained on sufficient data, including both historical and future simulations. When trained only on historical data, the projections made using models based on ML techniques fail to accurately predict tropical stratospheric ozone changes. Results presented here indicate that, when sufficiently trained, ML models have the potential to make accurate, computationally inexpensive projections of tropical stratospheric column ozone. Further development of these models may reduce the computational burden placed on fully coupled chemistry-climate and Earth system models and enable the exploration of tropical stratospheric column ozone recovery under a much broader range of future emissions scenarios.

Ozone profile retrievals from TROPOMI: Implication for the variation of tropospheric ozone during the outbreak of COVID-19 in China

During the outbreak of the coronavirus disease 2019 (COVID-19) in China in January and February 2020, production and living activities were drastically reduced to impede the spread of the virus, which also caused a strong reduction of the emission of primary pollutants. However, as a major species of secondary air pollutant, tropospheric ozone did not reduce synchronously, but instead rose in some region. Furthermore, higher concentrations of ozone may potentially promote the rates of COVID-19 infections, causing extra risk to human health. Thus, the variation of ozone should be evaluated widely. This paper presents ozone profiles and tropospheric ozone columns from ultraviolet radiances detected by TROPOospheric Monitoring Instrument (TROPOMI) onboard Sentinel 5 Precursor (S5P) satellite based on the principle of optimal estimation method. We compare our TROPOMI retrievals with global ozonesonde observations, Fourier Transform Spectrometry (FTS) observation at Hefei (117.17°E, 31.7°N) and Global Positioning System (GPS) ozonesonde sensor (GPSO3) ozonesonde profiles at Beijing (116.46°E, 39.80°N). The integrated Tropospheric Ozone Column (TOC) and Stratospheric Ozone Column (SOC) show excellent agreement with validation data. We use the retrieved TOC combining with tropospheric vertical column density (TVCD) of NO2 and HCHO from TROPOMI to assess the changes of tropospheric ozone during the outbreak of COVID-19 in China. Although NO2 TVCD decreased by 63%, the retrieved TOC over east China increase by 10% from the 20-day averaged before the lockdown on January 23, 2020 to 20-day averaged after it. Because the production of ozone in winter is controlled by volatile organic compounds (VOCs) indicated by monitored HCHO, which did not present evident change during the lockdown, the production of ozone did not decrease significantly. Besides, the decrease of NOx emission weakened the titration of ozone, causing an increase of ozone.

Stratospheric ozone trends for 1985–2018: sensitivity to recent large variability

Abstract. The Montreal Protocol, and its subsequent amendments, has successfully prevented catastrophic losses of stratospheric ozone, and signs of recovery are now evident. Nevertheless, recent work has suggested that ozone in the lower stratosphere (< 24 km) continued to decline over the 1998–2016 period, offsetting recovery at higher altitudes and preventing a statistically significant increase in quasi-global (60∘ S–60∘ N) total column ozone. In 2017, a large lower stratospheric ozone resurgence over less than 12 months was estimated (using a chemistry transport model; CTM) to have offset the long-term decline in the quasi-global integrated lower stratospheric ozone column. Here, we extend the analysis of space-based ozone observations to December 2018 using the BASICSG ozone composite. We find that the observed 2017 resurgence was only around half that modelled by the CTM, was of comparable magnitude to other strong interannual changes in the past, and was restricted to Southern Hemisphere (SH) midlatitudes (60–30∘ S). In the SH midlatitude lower stratosphere, the data suggest that by the end of 2018 ozone is still likely lower than in 1998 (probability ∼80 %). In contrast, tropical and Northern Hemisphere (NH) ozone continue to display ongoing decreases, exceeding 90 % probability. Robust tropical (>95 %, 30∘ S–30∘ N) decreases dominate the quasi-global integrated decrease (99 % probability); the integrated tropical stratospheric column (1–100 hPa, 30∘ S–30∘ N) displays a significant overall ozone decrease, with 95 % probability. These decreases do not reveal an inefficacy of the Montreal Protocol; rather, they suggest that other effects are at work, mainly dynamical variability on long or short timescales, counteracting the positive effects of the Montreal Protocol on stratospheric ozone recovery. We demonstrate that large interannual midlatitude (30–60∘) variations, such as the 2017 resurgence, are driven by non-linear quasi-biennial oscillation (QBO) phase-dependent seasonal variability. However, this variability is not represented in current regression analyses. To understand if observed lower stratospheric ozone decreases are a transient or long-term phenomenon, progress needs to be made in accounting for this dynamically driven variability.

Modeling the Effect of Potential Nitric Acid Removal During Convective Injection of Water Vapor Over the Central United States on the Chemical Composition of the Lower Stratosphere.

Tropopause‐penetrating convection is a frequent seasonal feature of the Central United States climate. This convection presents the potential for consistent transport of water vapor into the upper troposphere and lower stratosphere (UTLS) through the lofting of ice, which then sublimates. Water vapor enhancements associated with convective ice lofting have been observed in both in situ and satellite measurements. These water vapor enhancements can increase the probability of sulfate aerosol‐catalyzed heterogeneous reactions that convert reservoir chlorine (HCl and ClONO2) to free radical chlorine (Cl and ClO) that leads to catalytic ozone loss. In addition to water vapor transport, lofted ice may also scavenge nitric acid and further impact the chlorine activation chemistry of the UTLS. We present a photochemical model that resolves the vertical chemical structure of the UTLS to explore the effect of water vapor enhancements and potential additional nitric acid removal. The model is used to define the response of stratospheric column ozone to the range of convective water vapor transported and the temperature variability of the lower stratosphere currently observed over the Central United States in conjunction with potential nitric acid removal and to scenarios of elevated sulfate aerosol surface area density representative of possible future volcanic eruptions or solar radiation management. We find that the effect of HNO3 removal is dependent on the magnitude of nitric acid removal and has the greatest potential to increase chlorine activation and ozone loss under UTLS conditions that weakly favor the chlorine activation heterogeneous reactions by reducing NOx sources.

Estimates of ozone return dates from Chemistry-Climate Model Initiative simulations

Abstract. >We analyse simulations performed for the Chemistry-Climate Model Initiative (CCMI) to estimate the return dates of the stratospheric ozone layer from depletion caused by anthropogenic stratospheric chlorine and bromine. We consider a total of 155 simulations from 20 models, including a range of sensitivity studies which examine the impact of climate change on ozone recovery. For the control simulations (unconstrained by nudging towards analysed meteorology) there is a large spread (±20 DU in the global average) in the predictions of the absolute ozone column. Therefore, the model results need to be adjusted for biases against historical data. Also, the interannual variability in the model results need to be smoothed in order to provide a reasonably narrow estimate of the range of ozone return dates. Consistent with previous studies, but here for a Representative Concentration Pathway (RCP) of 6.0, these new CCMI simulations project that global total column ozone will return to 1980 values in 2049 (with a 1σ uncertainty of 2043–2055). At Southern Hemisphere mid-latitudes column ozone is projected to return to 1980 values in 2045 (2039–2050), and at Northern Hemisphere mid-latitudes in 2032 (2020–2044). In the polar regions, the return dates are 2060 (2055–2066) in the Antarctic in October and 2034 (2025–2043) in the Arctic in March. The earlier return dates in the Northern Hemisphere reflect the larger sensitivity to dynamical changes. Our estimates of return dates are later than those presented in the 2014 Ozone Assessment by approximately 5–17 years, depending on the region, with the previous best estimates often falling outside of our uncertainty range. In the tropics only around half the models predict a return of ozone to 1980 values, around 2040, while the other half do not reach the 1980 value. All models show a negative trend in tropical total column ozone towards the end of the 21st century. The CCMI models generally agree in their simulation of the time evolution of stratospheric chlorine and bromine, which are the main drivers of ozone loss and recovery. However, there are a few outliers which show that the multi-model mean results for ozone recovery are not as tightly constrained as possible. Throughout the stratosphere the spread of ozone return dates to 1980 values between models tends to correlate with the spread of the return of inorganic chlorine to 1980 values. In the upper stratosphere, greenhouse gas-induced cooling speeds up the return by about 10–20 years. In the lower stratosphere, and for the column, there is a more direct link in the timing of the return dates of ozone and chlorine, especially for the large Antarctic depletion. Comparisons of total column ozone between the models is affected by different predictions of the evolution of tropospheric ozone within the same scenario, presumably due to differing treatment of tropospheric chemistry. Therefore, for many scenarios, clear conclusions can only be drawn for stratospheric ozone columns rather than the total column. As noted by previous studies, the timing of ozone recovery is affected by the evolution of N2O and CH4. However, quantifying the effect in the simulations analysed here is limited by the few realisations available for these experiments compared to internal model variability. The large increase in N2O given in RCP 6.0 extends the ozone return globally by ∼ 15 years relative to N2O fixed at 1960 abundances, mainly because it allows tropical column ozone to be depleted. The effect in extratropical latitudes is much smaller. The large increase in CH4 given in the RCP 8.5 scenario compared to RCP 6.0 also lengthens ozone return by ∼ 15 years, again mainly through its impact in the tropics. Overall, our estimates of ozone return dates are uncertain due to both uncertainties in future scenarios, in particular those of greenhouse gases, and uncertainties in models. The scenario uncertainty is small in the short term but increases with time, and becomes large by the end of the century. There are still some model–model differences related to well-known processes which affect ozone recovery. Efforts need to continue to ensure that models used for assessment purposes accurately represent stratospheric chemistry and the prescribed scenarios of ozone-depleting substances, and only those models are used to calculate return dates. For future assessments of single forcing or combined effects of CO2, CH4, and N2O on the stratospheric column ozone return dates, this work suggests that it is more important to have multi-member (at least three) ensembles for each scenario from every established participating model, rather than a large number of individual models.

Stratospheric Response in the First Geoengineering Simulation Meeting Multiple Surface Climate Objectives

AbstractWe describe here changes in stratospheric dynamics and chemistry in a first century‐long sulfate aerosol geoengineering simulation in which the mean surface temperature and the interhemispheric and equator‐to‐pole surface temperature gradients were kept near their 2020 levels despite the RCP8.5 emission scenario. Simulations were carried out with the Community Earth System Model, version 1 with the Whole Atmosphere Community Climate Model as its atmospheric component [CESM1(WACCM)] coupled to a feedback algorithm controlling the magnitude of sulfur dioxide (SO2) injections at four injection latitudes. We find that, throughout the entire geoengineering simulation, the lower stratospheric temperatures increase by ∼0.19 K per Tg SO2 injection per year or ∼10 K with ∼40 Tg SO2/year total SO2 injection. These temperature changes are associated with a strengthening of the polar jets in the stratosphere and weakening of the mean zonal wind in the lower stratosphere subtropics and throughout the troposphere, associated with weaker storm track activity. In the geoengineering simulation the quasi‐biennial oscillation of the tropical lower stratospheric winds remains close to the presently observed quasi‐biennial oscillation, even for large amounts of SO2 injection. Water vapor in the stratosphere increases substantially: by 25% with ∼20 Tg SO2/year annual injection and by up to 90% with a ∼40 Tg SO2/year injection. Stratospheric column ozone in the geoengineering simulation is predicted to recover to or supersede preozone hole conditions by the end of the century.

Evidence for a continuous decline in lower stratospheric ozone offsetting ozone layer recovery

Abstract. Ozone forms in the Earth's atmosphere from the photodissociation of molecular oxygen, primarily in the tropical stratosphere. It is then transported to the extratropics by the Brewer–Dobson circulation (BDC), forming a protective ozone layer around the globe. Human emissions of halogen-containing ozone-depleting substances (hODSs) led to a decline in stratospheric ozone until they were banned by the Montreal Protocol, and since 1998 ozone in the upper stratosphere is rising again, likely the recovery from halogen-induced losses. Total column measurements of ozone between the Earth's surface and the top of the atmosphere indicate that the ozone layer has stopped declining across the globe, but no clear increase has been observed at latitudes between 60° S and 60° N outside the polar regions (60–90°). Here we report evidence from multiple satellite measurements that ozone in the lower stratosphere between 60° S and 60° N has indeed continued to decline since 1998. We find that, even though upper stratospheric ozone is recovering, the continuing downward trend in the lower stratosphere prevails, resulting in a downward trend in stratospheric column ozone between 60° S and 60° N. We find that total column ozone between 60° S and 60° N appears not to have decreased only because of increases in tropospheric column ozone that compensate for the stratospheric decreases. The reasons for the continued reduction of lower stratospheric ozone are not clear; models do not reproduce these trends, and thus the causes now urgently need to be established.

Validation of 10-year SAO OMI ozone profile (PROFOZ) product using Aura MLS measurements

Abstract. We validate the Ozone Monitoring Instrument (OMI) ozone profile (PROFOZ v0.9.3) product including ozone profiles between 0.22 and 261 hPa and stratospheric ozone columns (SOCs) down to 100, 215, and 261 hPa from October 2004 through December 2014 retrieved by the Smithsonian Astrophysical Observatory (SAO) algorithm against the latest Microwave Limb Sound (MLS) v4.2x data. 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 RA, i.e., pre-RA (2004–2008) and post-RA (2009–2014). During the pre-RA period, OMI ozone profiles agree very well with MLS data. After applying OMI averaging kernels to MLS data, the global mean biases (MBs) are within 3 % between 0.22 and 100 hPa, negative biases are within 3–9 % for lower layers, and the standard deviations (SDs) are 3.5–5 % from 1 to 40 hPa, 6–10 % for upper layers, and 5–20 % for lower layers. OMI shows biases dependent on latitude and solar zenith angle (SZA), but MBs and SDs are mostly within 10 % except for low and high altitudes of high latitudes and SZAs. Compared to the retrievals during the pre-RA period, OMI retrievals during the post-RA period degrade slightly between 5 and 261 hPa with MBs and SDs typically larger by 2–5 %, and degrade much more for pressure less than ∼ 5 hPa, with larger MBs by up to 8 % and SDs by up to 15 %, where the MBs are larger by 10–15 % south of 40∘ N due to the blockage effect of RA and smaller by 15–20 % north of 40∘ N due to the solar contamination effect of RA. The much worse comparisons at high altitudes indicate the UV1 channel of pixels that are not flagged as RA is still affected by the RA. During the pre-RA period, OMI SOCs show very good agreement with MLS data with global mean MBs within 0.6 % and SDs of 1.9 % for SOCs down to 215 and 261 hPa and of 2.30 % for SOC down to 100 hPa. Despite clearly worse ozone profile comparisons during the post-RA period, OMI SOCs only slightly degrade, with SDs larger by 0.4–0.6 % mostly due to looser spatial coincidence criteria as a result of missing data from RA and MBs larger by 0.4–0.7 %. Our retrieval comparisons indicate significant bias trends, especially during the post-RA period. The spatiotemporal variation of our retrieval performance suggests the need to improve OMI's radiometric calibration to maintain the long-term stability and spatial consistency of the PROFOZ product.

Diagnosing the radiative and chemical contributions to future changes in tropical column ozone with the UM-UKCA chemistry–climate model

Abstract. Chemical and dynamical drivers of trends in tropical total-column ozone (TCO3) for the recent past and future periods are explored using the UM-UKCA (Unified Model HadGEM3-A (Hewitt et al., 2011) coupled with the United Kingdom Chemistry and Aerosol scheme) chemistry–climate model. A transient 1960–2100 simulation is analysed which follows the representative concentration pathway 6.0 (RCP6.0) emissions scenario for the future. Tropical averaged (10° S–10° N) TCO3 values decrease from the 1970s, reach a minimum around 2000 and return to their 1980 values around 2040, consistent with the use and emission of halogenated ozone-depleting substances (ODSs), and their later controls under the Montreal Protocol. However, when the ozone column is subdivided into three partial columns (PCO3) that cover the upper stratosphere (PCO3US), lower stratosphere (PCO3LS) and troposphere (PCO3T), significant differences in the temporal behaviour of the partial columns are seen. Modelled PCO3T values under the RCP6.0 emissions scenario increase from 1960 to 2000 before remaining approximately constant throughout the 21st century. PCO3LS values decrease rapidly from 1960 to 2000 and remain constant from 2000 to 2050, before gradually decreasing further from 2050 to 2100 and never returning to their 1980s values. In contrast, PCO3US values decrease from 1960 to 2000, before increasing rapidly throughout the 21st century and returning to 1980s values by ∼ 2020, and reach significantly higher values by 2100. Using a series of idealised UM-UKCA time-slice simulations with concentrations of well-mixed greenhouse gases (GHGs) and halogenated ODS species set to either year 2000 or 2100 levels, we examine the main processes that drive the PCO3 responses in the three regions and assess how these processes change under different emission scenarios. Finally, we present a simple, linearised model to describe the future evolution of tropical stratospheric column ozone values based on terms representing time-dependent abundances of GHG and halogenated ODS.

Impact of volcanic aerosols on stratospheric ozone recovery

AbstractWe use transient GFDL‐CM3 chemistry‐climate model simulations over the 2006–2100 period to show how the influence of volcanic aerosols on the extent and timing of ozone recovery varies with (a) future greenhouse gas scenarios (Representative Concentration Pathway (RCP)4.5 and RCP8.5) and (b) halogen loading. Current understanding is that elevated volcanic aerosols reduce ozone under high halogen loading but increase ozone under low halogen loading when the chemistry is more NOx dominated. With extremely low aerosol loadings (designated here as “background”), global stratospheric ozone burden is simulated to return to 1980 levels around 2050 in the RCP8.5 scenario but remains below 1980 levels throughout the 21st century in the RCP4.5 scenario. In contrast, with elevated volcanic aerosols, ozone column recovers more quickly to 1980 levels, with recovery dates ranging from the mid‐2040s in RCP8.5 to the mid‐2050s to early 2070s in RCP4.5. The ozone response in both future emission scenarios increases with enhanced volcanic aerosols. By 2100, the 1980 baseline‐adjusted global stratospheric ozone column is projected to be 20–40% greater in RCP8.5 and 110–200% greater in RCP4.5 with elevated volcanic aerosols compared to simulations with the extremely low background aerosols. The weaker ozone enhancement at 2100 in RCP8.5 than in RCP4.5 in response to elevated volcanic aerosols is due to a factor of 2.5 greater methane in RCP8.5 compared with RCP4.5. Our results demonstrate the substantial uncertainties in stratospheric ozone projections and expected recovery dates induced by volcanic aerosol perturbations that need to be considered in future model ozone projections.

Validation of 10-year SAO OMI Ozone Profile (PROFOZ) product using ozonesonde observations

Abstract. 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 worse with larger SDs reaching 2 % in the stratosphere and 8 % in the troposphere and up to 6 % in TOC. There are systematic differences that vary with latitude compared to the pre-RA comparison. The retrieval comparison demonstrates good long-term stability during the pre-RA period but exhibits a statistically significant trend of 0.14–0.7 % year−1 for pressure < ∼ 80 hPa, 0.7 DU year−1 in SOC, and −0. 33 DU year−1 in TOC during the post-RA period. The spatiotemporal variation of retrieval performance suggests the need to improve OMI's radiometric calibration especially during the post-RA period to maintain the long-term stability and reduce the latitude/season/SZA and cross-track dependency of retrieval quality.

Ozone structure over the equatorial Andes from balloon-borne observations and zonal connection with two tropical sea level sites

In this paper we present first-time measurements of ozone profiles from a high altitude station in Quito, Ecuador (0.19°S, 78.4°W, and 2391 masl) taken from June 2014 to September 2015. We interpret ozone observations in the troposphere, tropopause, and stratosphere through a zonal comparison with data from stations in the Atlantic and Pacific (Natal and San Cristobal from the SHADOZ network). Tropospheric ozone concentrations above the Andes are lower than ozone over San Cristobal and Natal for similar time periods. Ozone variability and pollution layers are also reduced in the troposphere above the Andes. We explain these differences in terms of reduced contributions from the boundary layer and from horizontal transport. In the tropical tropopause layer, ozone is well-mixed up to near the cold point tropopause level. In this regard, our profiles do not show constraints to deep mixing above 14 km, as has been consistently observed at other tropical stations. Total column ozone and stratospheric column ozone are comparable among the three sites. However, the contribution of tropospheric column ozone to total column ozone is significantly lower above the Andes. Our comparisons provide a connection between observations from tropical stations in equatorial South America separated by the wide continental mass. Identified differences in ozone throughout the atmospheric column demonstrate the global benefit of having an ozone sounding station at the equatorial Andes in support of global monitoring networks.

Representation of the Community Earth System Model (CESM1) CAM4-chem within the Chemistry-Climate Model Initiative (CCMI)

Abstract. The Community Earth System Model (CESM1) CAM4-chem has been used to perform the Chemistry Climate Model Initiative (CCMI) reference and sensitivity simulations. In this model, the Community Atmospheric Model version 4 (CAM4) is fully coupled to tropospheric and stratospheric chemistry. Details and specifics of each configuration, including new developments and improvements are described. CESM1 CAM4-chem is a low-top model that reaches up to approximately 40 km and uses a horizontal resolution of 1.9° latitude and 2.5° longitude. For the specified dynamics experiments, the model is nudged to Modern-Era Retrospective Analysis for Research and Applications (MERRA) reanalysis. We summarize the performance of the three reference simulations suggested by CCMI, with a focus on the last 15 years of the simulation when most observations are available. Comparisons with selected data sets are employed to demonstrate the general performance of the model. We highlight new data sets that are suited for multi-model evaluation studies. Most important improvements of the model are the treatment of stratospheric aerosols and the corresponding adjustments for radiation and optics, the updated chemistry scheme including improved polar chemistry and stratospheric dynamics and improved dry deposition rates. These updates lead to a very good representation of tropospheric ozone within 20 % of values from available observations for most regions. In particular, the trend and magnitude of surface ozone is much improved compared to earlier versions of the model. Furthermore, stratospheric column ozone of the Southern Hemisphere in winter and spring is reasonably well represented. All experiments still underestimate CO most significantly in Northern Hemisphere spring and show a significant underestimation of hydrocarbons based on surface observations.