Stratospheric Changes Research Articles

Coupled Stratospheric Ozone and Atlantic Meridional Overturning Circulation Feedbacks on the Northern Hemisphere Midlatitude Jet Response to 4xCO2

Abstract Stratospheric ozone, and its response to anthropogenic forcings, provides an important pathway for the coupling between atmospheric composition and climate. In addition to stratospheric ozone’s radiative impacts, recent studies have shown that changes in the ozone layer due to 4xCO2 have a considerable impact on the Northern Hemisphere (NH) tropospheric circulation, inducing an equatorward shift of the North Atlantic jet during boreal winter. Using simulations produced with the NASA Goddard Institute for Space Studies (GISS) high-top climate model (E2.2), we show that this equatorward shift of the Atlantic jet can induce a more rapid weakening of the Atlantic meridional overturning circulation (AMOC). The weaker AMOC, in turn, results in an eastward acceleration and poleward shift of the Atlantic and Pacific jets, respectively, on longer time scales. As such, coupled feedbacks from both stratospheric ozone and the AMOC result in a two-time-scale response of the NH midlatitude jet to abrupt 4xCO2 forcing: a “fast” response (5–20 years) during which it shifts equatorward and a “total” response (∼100–150 years) during which the jet accelerates and shifts poleward. The latter is driven by a weakening of the AMOC that develops in response to weaker surface zonal winds that result in reduced heat fluxes out of the subpolar gyre and reduced North Atlantic Deep Water formation. Our results suggest that stratospheric ozone changes in the lower stratosphere can have a surprisingly powerful effect on the AMOC, independent of other aspects of climate change.

Sensitivity of the Antarctic Polar Vortex to Temperature Changes in the Lower Subtropical Stratosphere

Sensitivity of the Antarctic Polar Vortex to Temperature Changes in the Lower Subtropical Stratosphere

Antarctic polar vortex dynamics in 2019 and 2020 under the influence of the subtropical stratosphere

The trend of strengthening of the Antarctic polar vortex in late spring and early summer (November–December) has been observed in recent decades. A good example of this trend is the dynamics of the Antarctic polar vortex in 2020 when it existed until the last week of December. In 2019, conversely, on the contrary, an unusually early breakup of the polar vortex occurred, a minor sudden stratospheric warming was recorded. Strengthening (or weakening) of the Antarctic polar vortex occurs as a result of an increase (or decrease) in the stratospheric meridional temperature gradient under conditions of growth (or decline) in the temperature of the lower subtropical stratosphere. We considered the temperature variations in the lower subtropical stratosphere in the spring of 2019 and 2020 and the corresponding response of the Antarctic polar vortex. The dynamics of the Antarctic polar vortex in September–October 2019 and November 2020 was largely synchronized with the temperature changes in the lower subtropical stratosphere relative to climatological means. Using correlation analysis, we show that the Antarctic polar vortex dynamics in December is largely due to the temperature changes in the lower subtropical stratosphere that occurred in the second half of November, which manifested itself in 2020.

Stratospheric Climate Anomalies and Ozone Loss Caused by the Hunga Tonga‐Hunga Ha'apai Volcanic Eruption

AbstractThe Hunga Tonga‐Hunga Ha'apai (HTHH) volcanic eruption in January 2022 injected unprecedented amounts of water vapor (H2O) and a moderate amount of the aerosol precursor sulfur dioxide (SO2) into the Southern Hemisphere (SH) tropical stratosphere. The H2O and aerosol perturbations have persisted during 2022 and early 2023 and dispersed throughout the atmosphere. Observations show large‐scale SH stratospheric cooling, equatorward shift of the Antarctic polar vortex and slowing of the Brewer‐Dobson circulation. Satellite observations show substantial ozone reductions over SH winter midlatitudes that coincide with the largest circulation anomalies. Chemistry‐climate model simulations forced by realistic HTHH inputs of H2O and SO2 qualitatively reproduce the observed evolution of the H2O and aerosol plumes over the first year, and the model exhibits stratospheric cooling, circulation changes and ozone effects similar to observed behavior. The agreement demonstrates that the observed stratospheric changes are caused by the HTHH volcanic influences.

Injection strategy – a driver of atmospheric circulation and ozone response to stratospheric aerosol geoengineering

Abstract. Despite offsetting global mean surface temperature, various studies demonstrated that stratospheric aerosol injection (SAI) could influence the recovery of stratospheric ozone and have important impacts on stratospheric and tropospheric circulation, thereby potentially playing an important role in modulating regional and seasonal climate variability. However, so far, most of the assessments of such an approach have come from climate model simulations in which SO2 is injected only in a single location or a set of locations. Here we use CESM2-WACCM6 SAI simulations under a comprehensive set of SAI strategies achieving the same global mean surface temperature with different locations and/or timing of injections, namely an equatorial injection, an annual injection of equal amounts of SO2 at 15∘ N and 15∘ S, an annual injection of equal amounts of SO2 at 30∘ N and 30∘ S, and a polar strategy injecting SO2 at 60∘ N and 60∘ S only in spring in each hemisphere. We demonstrate that despite achieving the same global mean surface temperature, the different strategies result in contrastingly different magnitudes of the aerosol-induced lower stratospheric warming, stratospheric moistening, strengthening of stratospheric polar jets in both hemispheres, and changes in the speed of the residual circulation. These impacts tend to maximise under the equatorial injection strategy and become smaller as the aerosols are injected away from the Equator into the subtropics and higher latitudes. In conjunction with the differences in direct radiative impacts at the surface, these different stratospheric changes drive different impacts on the extratropical modes of variability (Northern and Southern Annular modes), including important consequences on the northern winter surface climate, and on the intensity of tropical tropospheric Walker and Hadley circulations, which drive tropical precipitation patterns. Finally, we demonstrate that the choice of injection strategy also plays a first-order role in the future evolution of stratospheric ozone under SAI throughout the globe. Overall, our results contribute to an increased understanding of the fine interplay of various radiative, dynamical, and chemical processes driving the atmospheric circulation and ozone response to SAI and lay the foundation for designing an optimal SAI strategy that could form a basis of future multi-model intercomparisons.

Diagnosing observed extratropical stationary wave changes in boreal winter

Stationary waves are time-averaged zonally asymmetric component of the climatological mean atmospheric circulation, primarily due to the unevenly distributed topography and diabatic heating. Stationary waves are subject to influence from long-term external forcing. In this study, the temporal evolution of the winter (January) Northern Hemisphere stationary waves during 1961–2020 is diagnosed with the fifth generation European Centre for Medium-range Weather Forecasts reanalysis data (ERA5), which shows an overall strengthening in amplitude and an eastward shift in phase. A stationary wave model is used to attribute the stationary wave response to changes in the zonal mean basic state (ΔZM) and the zonally asymmetric diabatic heating forcing (). The pattern of stationary wave changes is well captured by the response to ΔZM alone, whereas the contribution of to the amplitude increases in height and becomes dominant in the stratosphere. is also found to be important in driving stationary wave changes in the North Pacific and Western Europe regions. Furthermore, changes in tropospheric stationary waves are probably a result of internal variability, whereas stratospheric changes are more likely to be driven by external forcing.

ENSO Modoki Impacts on the Interannual Variations of Spring Antarctic Stratospheric Ozone

Abstract Using observation and reanalysis data, we investigated the effect of the sea surface temperature anomalies associated with ENSO Modoki from September to October on interannual variations in Antarctic stratospheric ozone from October to November. It was found that the planetary wave anomalies generated by ENSO Modoki in the tropical troposphere propagate to the southern mid- and then high-latitude stratosphere. The planetary wave anomalies have a profound impact on the polar vortex, subsequently affecting the interannual variations in Antarctic stratospheric ozone. Further analysis revealed that the responses of the polar vortex and ozone to ENSO Modoki are mainly modulated by the wave-1 and wave-3 components, and the effect of wave 2 is opposite and offset by those of wave 1 and wave 3. The contribution of the residual waves (after removing waves 1, 2, 3, and the remaining waves) are relatively small. Furthermore, we evaluated the performance of CMIP6 models in simulating the impacts of ENSO Modoki on the southern stratospheric polar vortex and ozone. We selected seven models that include stratospheric processes and stratospheric chemical ozone. We found that all are capable of distinguishing between eastern Pacific ENSO and ENSO Modoki events. However, only GISS-E2-1-G and MPI-ESM-1-2-HAM can simulate the patterns of ozone, circulation, and temperature in the Southern Hemisphere in a manner that closely resembles the reanalysis results. Further analysis indicated that these two models can better simulate the propagation of planetary wave activities in the troposphere forced by ENSO Modoki, whereas the other models produce significantly different results to those obtained from observations. Significance Statement This study found a significant connection between ENSO Modoki and the interannual variability of Antarctic stratospheric ozone in austral spring and investigated the underlying physical mechanisms in detail. In addition, the performances of CMIP6 models in simulating the impact of ENSO Modoki on the southern stratospheric polar vortex and ozone were evaluated. This study not only helps to further understand the characteristics of past Antarctic ozone changes but also helps developers improve the performance of models in simulating Antarctic stratospheric changes.

How the extreme 2019–2020 Australian wildfires affected global circulation and adjustments

Abstract. Wildfires are a significant source of absorbing aerosols in the atmosphere. Extreme fires in particular, such as those during the 2019–2020 Australian wildfire season (Black Summer fires), can have considerable large-scale effects. In this context, the climate impact of extreme wildfires unfolds not only because of the emitted carbon dioxide but also due to smoke aerosol released up to an altitude of 17 km. The overall aerosol effects depend on a variety of factors, such as the amount emitted, the injection height, and the composition of the burned material, and is therefore subject to considerable uncertainty. In the present study, we address the global impact caused by the exceptionally strong and high-reaching smoke emissions from the Australian wildfires using simulations with a global aerosol–climate model. We show that the absorption of solar radiation by the black carbon contained in the emitted smoke led to a shortwave radiative forcing of more than +5 W m−2 in the southern mid-latitudes of the lower stratosphere. Subsequent adjustment processes in the stratosphere slowed down the diabatically driven meridional circulation, thus redistributing the heating perturbation on a global scale. As a result of these stratospheric adjustments, a positive temperature perturbation developed in both hemispheres, leading to additional longwave radiation emitted back to space. According to the model results, this adjustment occurred in the stratosphere within the first 2 months after the event. At the top of the atmosphere (TOA), the net effective radiative forcing (ERF) averaged over the Southern Hemisphere was initially dominated by the instantaneous positive radiative forcing of about +0.5 W m−2, for which the positive sign resulted mainly from the presence of clouds above the Southern Ocean. The longwave adjustments led to a compensation of the initially net positive TOA ERF, which is seen in the Southern Hemisphere, the tropics, and the northern mid-latitudes. The simulated changes in the lower stratosphere also affected the upper troposphere through a thermodynamic downward coupling. Subsequently, increased temperatures were also obtained in the upper troposphere, causing a global decrease in relative humidity, cirrus amount, and the ice water path of about 0.2 %. As a result, surface precipitation also decreased by a similar amount, which was accompanied by a weakening of the tropospheric circulation due to the given energetic constraints. In general, it appears that the radiative effects of smoke from single extreme wildfire events can lead to global impacts that affect the interplay of tropospheric and stratospheric budgets in complex ways. This emphasizes that future changes in extreme wildfires need to be included in projections of aerosol radiative forcing.

Ice Core 17O Reveals Past Changes in Surface Air Temperatures and Stratosphere to Troposphere Mass Exchange

In this study, we have investigated the oxygen isotope compositions (δ17O and δ18O) of modern rain and ice cores using published isotopic data. We find that, contrary to existing interpretations, precipitation δ17O is influenced by two factors: mass-dependent fractionation (MDF), which occurs during ocean evaporation, and mass-independent fractionation (MIF), which happens in the stratosphere. The MDF contribution remains constant and can be understood by studying tropical rain, as the overall movement of mass in the tropics is upward toward the stratosphere. On the other hand, the MIF effect comes from the mixing of stratospheric air in the troposphere, which is a result of the Brewer–Dobson circulation. This MIF effect on precipitation 17O increases from the tropics toward the poles and is observed consistently in modern precipitation and ice cores. The relative δ17O and δ18O composition, denoted as ∆‘17O, in modern precipitation can be calibrated with surface air temperature, creating a new and independent tool for estimating past temperatures. We used this calibration along with the ∆‘17O of Antarctic and Greenland ice cores, and our reconstructed past temperatures are in excellent agreement with those derived from borehole thermometry or gas phase analysis of air trapped in the ice. The ∆‘17O method overcomes the problems associated with using δ18O alone for paleothermometry. Our findings align with climate models that suggest a weakening of the Brewer–Dobson circulation during the Last Glacial Maximum. Furthermore, our approach could be used to monitor future changes in stratosphere–troposphere mass exchange in response to a warming climate caused by increasing greenhouse gases.

Arctic stratosphere changes in the 21st century in the Earth system model SOCOLv4

Two ensemble simulations of a new Earth system model (ESM) SOCOLv4 (SOlar Climate Ozone Links, version 4) for the period from 2015 to 2099 under moderate (SSP2-4.5) and severe (SSP5-8.5) scenarios of greenhouse gas (GHG) emission growth were analyzed to investigate changes in key dynamical processes relevant for Arctic stratospheric ozone. The model shows a 5–10 K cooling and 5%–20% humidity increase in the Arctic lower–upper stratosphere in March (when the most considerable ozone depletion may occur) between 2080–2099 and 2015–2034. The minimal temperature in the lower polar stratosphere in March, which defines the strength of ozone depletion, appears when the zonal mean meridional heat flux in the lower stratosphere in the preceding January–February is the lowest. In the late 21st century, the strengthening of the zonal mean meridional heat flux with a maximum of up to 20 K m/s (∼25%) in the upper stratosphere close to 70°N in January–February is obtained in the moderate scenario of GHG emission, while only a slight increase in this parameter over 50 N–60 N with the maximum up to 5 K m/s in the upper stratosphere and a decrease with the comparable values over the high latitudes is revealed in the severe GHG emission scenario. Although the model simulations confirm the expected ozone layer recovery, particularly total ozone minimum values inside the Arctic polar cap in March throughout the 21st century are characterized by a positive trend in both scenarios, the large-scale negative ozone anomalies in March up to −80 DU–100 DU, comparable to the second lowest ones observed in March 2011 but weaker than record values in March 2020, are possible in the Arctic until the late 21st century. The volume of low stratospheric air with temperatures below the solid nitric acid trihydrate polar stratospheric cloud (PSC NAT) formation threshold is reconstructed from 3D potential vorticity and temperature fields inside the stratospheric polar vortex. A significant positive trend is shown in this parameter in March in the SSP5-8.5 scenario. Furthermore, according to the model data, an increase in the polar vortex isolation throughout the 21st century indicates its possible strengthening in the lower stratosphere. Positive trends of the surface area density (SAD) of PSC NAT particles in March in the lower Arctic stratosphere over the period of 2015–2099 are significant in the severe GHG emission scenario. The polar vortex longitudinal shift toward northern Eurasia is expected in the lower stratosphere in the late 21st century in both scenarios. The statistically significant long-term stratospheric sulfuric acid aerosol trend in March is expected only in the SSP5.8-5 scenario, most probably due to cooler stratosphere and stronger Brewer–Dobson circulation intensification. Both scenarios predict an increase in the residual meridional circulation (RMC) in March by the end of the 21st century. In some regions of the stratosphere, the RMC enhancement under the severe GHG scenario can exceed 20%.

Stratospheric aerosol lidar with a 300 µm diameter superconducting nanowire single-photon detector at 1064 nm.

Stratospheric aerosols play an important role in the atmospheric chemical and radiative balance. To detect the stratospheric aerosol layer, a 1064 nm lidar with high resolution and large dynamic range is developed using a superconducting nanowire single-photon detector (SNSPD). Measurements are typically performed at 1064 nm for its sensitivity to aerosol, whereas detectors are limited by low efficiency and high dark count rate (DCR). SNSPDs are characterized by high efficiency in the infrared wavelength domain, as well as low noise and dead time, which can significantly enhance the signal quality. However, it is still challenging to build an SNSPD with both large active area and high count rate. To improve the maximal count rate (MCR) so as to avoid saturation in the near range, a 16-pixel interleaved SNSPD array and a multichannel data acquisition system are developed. As a reference, a synchronous system working at 532 nm is applied. In a continuous comparison experiment, backscatter ratio profiles are retrieved with resolutions of 90 m/3 min, and the 1064 nm system shows better performance, which is sensitive to aerosols and immune to the contamination of the ozone absorption and density of molecule change in the lower stratosphere.

How Do Stratospheric Perturbations Influence North American Weather Regime Predictions?

Abstract Observational evidence shows changes to North American weather regime occurrence depending on the strength of the lower-stratospheric polar vortex. However, it is not yet clear how this occurs or to what extent an improved stratospheric forecast would change regime predictions. Here we analyze four North American regimes at 500 hPa, constructed in principal component (PC) space. We consider both the location of the regimes in PC space and the linear regression between each PC and the lower-stratospheric zonal-mean winds, yielding a theory of which regime transitions are likely to occur due to changes in the lower stratosphere. Using a set of OpenIFS simulations, we then test the effect of relaxing the polar stratosphere to ERA-Interim on subseasonal regime predictions. The model start dates are selected based on particularly poor subseasonal regime predictions in the European Centre for Medium-Range Weather Forecasts CY43R3 hindcasts. While the results show only a modest improvement to the number of accurate regime predictions, there is a substantial reduction in Euclidean distance error in PC space. The average movement of the forecasts within PC space is found to be consistent with expectation for moderate-to-large lower-stratospheric zonal wind perturbations. Overall, our results provide a framework for interpreting the stratospheric influence on North American regime behavior. The results can be applied to subseasonal forecasts to understand how stratospheric uncertainty may affect regime predictions, and to diagnose which regime forecast errors are likely to be related to stratospheric errors. Significance Statement Predicting the weather several weeks ahead is a major challenge with large potential benefits to society. The strength of the circulation more than 10 km above the Arctic during winter (i.e., the polar vortex) is one source of predictability. This study investigates how forecast error and uncertainty in the polar vortex can impact predictions of large-scale weather patterns called “regimes” over North America. Through statistical analysis of observations and experiments with a weather forecast model, we develop an understanding of which regime changes are more likely to be due to changes in the polar vortex. The results will help forecasters and researchers understand the contribution of the stratosphere to changes in weather patterns, and in assessing and improving weather forecast models.

Stratospheric ozone response to sulfate aerosol and solar dimming climate interventions based on the G6 Geoengineering Model Intercomparison Project (GeoMIP) simulations

Abstract. This study assesses the impacts of stratospheric aerosol intervention (SAI) and solar dimming on stratospheric ozone based on the G6 Geoengineering Model Intercomparison Project (GeoMIP) experiments, called G6sulfur and G6solar. For G6sulfur, an enhanced stratospheric sulfate aerosol burden reflects some of the incoming solar radiation back into space to cool the surface climate, while for G6solar, the reduction in the global solar constant in the model achieves the same goal. Both experiments use the high emissions scenario of SSP5-8.5 as the baseline experiment and define surface temperature from the medium emission scenario of SSP2-4.5 as the target. In total, six Earth system models (ESMs) performed these experiments, and three out of the six models include interactive stratospheric chemistry. The increase in absorbing sulfate aerosols in the stratosphere results in a heating of the lower tropical stratospheric temperatures by between 5 to 13 K for the six different ESMs, leading to changes in stratospheric transport, water vapor, and other related changes. The increase in the aerosol burden also increases aerosol surface area density, which is important for heterogeneous chemical reactions. The resulting changes in the springtime Antarctic ozone between the G6sulfur and SSP5-8.5, based on the three models with interactive chemistry, include an initial reduction in total column ozone (TCO) of 10 DU (ranging between 0–30 DU for the three models) and up to 20 DU (between 10–40 DU) by the end of the century. The relatively small reduction in TCO for the multi-model mean in the first 2 decades results from variations in the required sulfur injections in the models and differences in the complexity of the chemistry schemes. In contrast, in the Northern Hemisphere (NH) high latitudes, no significant changes can be identified due to the large natural variability in the models, with little change in TCO by the end of the century. However, all three models with interactive chemistry consistently simulate an increase in TCO in the NH mid-latitudes up to 20 DU, compared to SSP5-8.5, in addition to the 20 DU increase resulting from increasing greenhouse gases between SSP2-4.5 and SSP5-8.5. In contrast to G6sulfur, G6solar does not significantly change stratospheric temperatures compared to the baseline simulation. Solar dimming results in little change in TCO compared to SSP5-8.5. Only in the tropics does G6solar result in an increase of TCO of up to 8 DU, compared to SSP2-4.5, which may counteract the projected reduction in SSP5-8.5. This work identifies differences in the response of SAI and solar dimming on ozone for three ESMs with interactive chemistry, which are partly due to the differences and shortcomings in the complexity of aerosol microphysics, chemistry, and the description of ozone photolysis. It also identifies that solar dimming, if viewed as an analog to SAI using a predominantly scattering aerosol, would succeed in reducing tropospheric and surface temperatures, but any stratospheric changes due to the high forcing greenhouse gas scenario, including the potential harmful increase in TCO beyond historical values, would prevail.

Weakening of Antarctic stratospheric planetary wave activities in early austral spring since the early 2000s: a response to sea surface temperature trends

Abstract. Using multiple reanalysis datasets and modeling simulations, the trends of Antarctic stratospheric planetary wave activities in early austral spring since the early 2000s are investigated in this study. We find that the stratospheric planetary wave activities in September have weakened significantly since the year 2000, which is mainly related to the weakening of the tropospheric wave sources in the extratropical Southern Hemisphere. As the Antarctic ozone also shows clear shift around the year 2000, the impact of ozone recovery on Antarctic planetary wave activity is also examined through numerical simulations. Significant ozone recovery in the lower stratosphere changes the atmospheric state for wave propagation to some extent, inducing a slight decrease in the vertical wave flux in upper troposphere and lower stratosphere (UTLS). However, the changes in the wave propagation environment in the middle and upper stratosphere over the subpolar region are not significant. The ozone recovery has a minor contribution to the significant weakening of stratospheric planetary wave activity in September. Further analysis indicates that the trend of September sea surface temperature (SST) over 20∘ N–70∘ S is well linked to the weakening of stratospheric planetary wave activities. The model simulations reveal that the SST trend in the extratropical Southern Hemisphere (20–70∘ S) and the tropics (20–20∘ S) induce a weakening of the wave 1 component of tropospheric geopotential height in the extratropical Southern Hemisphere, which subsequently leads to a decrease in stratospheric wave flux. In addition, both reanalysis data and numerical simulations indicate that the Brewer–Dobson circulation (BDC) related to wave activities in the stratosphere has also been weakening in early austral spring since the year 2000 due to the trend of September SST in the tropics and extratropical Southern Hemisphere.

Relationships between Extratropical Precipitation Systems and UTLS Temperatures and Tropopause Height from GPM and GPS-RO

This study characterizes the relationship between extratropical precipitation systems to changes in upper troposphere and lower stratosphere (UTLS) temperature and tropopause height within different environments. Precipitation features (PFs) observed by the Global Precipitation Measurement (GPM) satellite are collocated with GPS radio occultation (RO) temperature profiles from 2014 to 2017 and classified as non-deep stratospheric intrusion (non-DSI; related to convective instability) or deep stratospheric intrusion (DSI; related to strong dynamic effects on the tropopause). Non-DSI PFs introduce warming (up to 1 K) in the upper troposphere, transitioning to strong cooling (up to −3.5 K) around the lapse rate tropopause (LRT), and back to warming (up to 2.5 K, particularly over the ocean) in the lower stratosphere. UTLS temperature anomalies for DSI events are driven predominantly by large scale dynamics, with major cooling (up to −6 K) observed from the mid-troposphere to the LRT, which transitions to strong warming (up to 4 K) in the lower stratosphere. Small and deep non-DSI PFs typically result in a lower LRT (up to 0.4 km), whereas large but weaker PFs lead to a higher LRT with similar magnitudes. DSI events are associated with larger LRT height decreases, with anomalies of almost −2 km near the deepest PFs. These results suggest intricate relationships between precipitation systems and the UTLS temperature structure. Importantly, non-DSI PF temperature anomalies show patterns similar to tropical convection, which provides unification of previous tropical research with extratropical barotropic convective impacts to UTLS temperatures.

Updated total ozone climate normals over the territory of Ukraine

The study presents the results of analysis of spatiotemporal distribution of updated total ozone climate normals for the period of 1991–2020. It analyzes the changes since the last total ozone climate normals estimate conducted for the period of 1981–2010. The daily data retrieved using TOMS and OMI satellite instruments over the territory of Ukraine allowed calculation of multiyear average values, climate normals for each day of the year, amplitudes, phases and determination coefficients for total ozone seasonal variations. Use of the NCEP/NCAR reanalysis data allowed establishment of the relation between total ozone and meridional wind changes in the lower stratosphere. The research shows the existence of the regions with higher/lower total ozone content that are not in line with the characteristics of latitudinal distribution. They are formed due to more frequent recurrence of air advection with ozone content that is not typical for the Ukrainian territory, mostly from January to March. The study describes a typical temporal distribution of the total ozone climate normals varying from 285 to 375 Dobson units (D.u.) and analyzes the statistic patterns of deviations distribution and recurrence of extremely high/low total ozone content. The paper emphasizes a small variation of total ozone over the territory of Ukraine. The authors also researched the features of spatial distribution of seasonal variation amplitudes varying within the range of 42–46 D.u. and the specifics of maximum values periods observed from 19 to 30 of March, depending on a region. It was established that, since the previous update of the climate normals, the total ozone decreased for all months with its maximum decrease of about 8 D.u. in winter. However, no increase of recurrence of ultraviolet radiation high levels was observed. Total ozone changes are mainly associated with shifts of meridional wind values to negative ones. This process indicates the increase of recurrence of air advection from the north. The paper also emphasizes the complexness of total ozone changes during the period of research and the lack of consistency of such changes with the circulation factor of summer months.

An indirect-calibration method for non-target quantification of trace gases applied to a time series of fourth-generation synthetic halocarbons at the Taunus Observatory (Germany)

Abstract. Production and use of many synthetic halogenated trace gases are regulated internationally due to their contribution to stratospheric ozone depletion or climate change. In many applications they have been replaced by shorter-lived compounds, which have become measurable in the atmosphere as emissions increased. Non-target monitoring of trace gases rather than targeted measurements of well-known substances is needed to keep up with such changes in the atmospheric composition. We regularly deploy gas chromatography (GC) coupled to time-of-flight mass spectrometry (TOF-MS) for analysis of flask air samples and in situ measurements at the Taunus Observatory, a site in central Germany. TOF-MS acquires data over a continuous mass range that enables a retrospective analysis of the dataset, which can be considered a type of digital air archive. This archive can be used if new substances come into use and their mass spectrometric fingerprint is identified. However, quantifying new replacement halocarbons can be challenging, as mole fractions are generally low, requiring high measurement precision and low detection limits. In addition, calibration can be demanding, as calibration gases may not contain sufficiently high amounts of newly measured substances or the amounts in the calibration gas may have not been quantified. This paper presents an indirect data evaluation approach for TOF-MS data, where the calibration is linked to another compound which could be quantified in the calibration gas. We also present an approach to evaluate the quality of the indirect calibration method, select periods of stable instrument performance and determine well suited reference compounds. The method is applied to three short-lived synthetic halocarbons: HFO-1234yf, HFO-1234ze(E), and HCFO-1233zd(E). They represent replacements for longer-lived hydrofluorocarbons (HFCs) and exhibit increasing mole fractions in the atmosphere. The indirectly calibrated results are compared to directly calibrated measurements using data from TOF-MS canister sample analysis and TOF-MS in situ measurements, which are available for some periods of our dataset. The application of the indirect calibration method on several test cases can result in uncertainties of around 6 % to 11 %. For hydro(chloro-)fluoroolefines (denoted H(C)FOs), uncertainties up to 23 % are achieved. The indirectly calculated mole fractions of the investigated H(C)FOs at Taunus Observatory range between measured mole fractions at urban Dübendorf and Jungfraujoch stations in Switzerland.

Intercomparison Between Surrogate, Explicit, and Full Treatments of VSL Bromine Chemistry Within the CAM-Chem Chemistry-Climate Model.

Many Chemistry‐Climate Models (CCMs) include a simplified treatment of brominated very short‐lived (VSLBr) species by assuming CH3Br as a surrogate for VSLBr. However, neglecting a comprehensive treatment of VSLBr in CCMs may yield an unrealistic representation of the associated impacts. Here, we use the Community Atmospheric Model with Chemistry (CAM‐Chem) CCM to quantify the tropospheric and stratospheric changes between various VSLBr chemical approaches with increasing degrees of complexity (i.e., surrogate, explicit, and full). Our CAM‐Chem results highlight the improved accuracy achieved by considering a detailed treatment of VSLBr photochemistry, including sea‐salt aerosol dehalogenation and heterogeneous recycling on ice‐crystals. Differences between the full and surrogate schemes maximize in the lowermost stratosphere and midlatitude free troposphere, resulting in a latitudinally dependent reduction of ∼1–7 DU in total ozone column and a ∼5%–15% decrease of the OH/HO2 ratio. We encourage all CCMs to include a complete chemical treatment of VSLBr in the troposphere and stratosphere.

Slow feedbacks resulting from strongly enhanced atmospheric methane mixing ratios in a chemistry–climate model with mixed-layer ocean

Abstract. In a previous study the quasi-instantaneous chemical impacts (rapid adjustments) of strongly enhanced methane (CH4) mixing ratios have been analysed. However, to quantify the influence of the respective slow climate feedbacks on the chemical composition it is necessary to include the radiation-driven temperature feedback. Therefore, we perform sensitivity simulations with doubled and quintupled present-day (year 2010) CH4 mixing ratios with the chemistry–climate model EMAC (European Centre for Medium-Range Weather Forecasts, Hamburg version – Modular Earth Submodel System (ECHAM/MESSy) Atmospheric Chemistry) and include in a novel set-up a mixed-layer ocean model to account for tropospheric warming. Strong increases in CH4 lead to a reduction in the hydroxyl radical in the troposphere, thereby extending the CH4 lifetime. Slow climate feedbacks counteract this reduction in the hydroxyl radical through increases in tropospheric water vapour and ozone, thereby dampening the extension of CH4 lifetime in comparison with the quasi-instantaneous response. Changes in the stratospheric circulation evolve clearly with the warming of the troposphere. The Brewer–Dobson circulation strengthens, affecting the response of trace gases, such as ozone, water vapour and CH4 in the stratosphere, and also causing stratospheric temperature changes. In the middle and upper stratosphere, the increase in stratospheric water vapour is reduced with respect to the quasi-instantaneous response. We find that this difference cannot be explained by the response of the cold point and the associated water vapour entry values but by a weaker strengthening of the in situ source of water vapour through CH4 oxidation. However, in the lower stratosphere water vapour increases more strongly when tropospheric warming is accounted for, enlarging its overall radiative impact. The response of the stratosphere adjusted temperatures driven by slow climate feedbacks is dominated by these increases in stratospheric water vapour as well as strongly decreased ozone mixing ratios above the tropical tropopause, which result from enhanced tropical upwelling. While rapid radiative adjustments from ozone and stratospheric water vapour make an essential contribution to the effective CH4 radiative forcing, the radiative impact of the respective slow feedbacks is rather moderate. In line with this, the climate sensitivity from CH4 changes in this chemistry–climate model set-up is not significantly different from the climate sensitivity in carbon-dioxide-driven simulations, provided that the CH4 effective radiative forcing includes the rapid adjustments from ozone and stratospheric water vapour changes.

Using the climate feedback response analysis method to quantify climate feedbacks in the middle atmosphere

Abstract. Over recent decades it has become clear that the middle atmosphere has a significant impact on surface and tropospheric climate. A better understanding of the middle atmosphere and how it reacts to the current increase in the concentration of carbon dioxide (CO2) is therefore necessary. In this study, we investigate the response of the middle atmosphere to a doubling of the CO2 concentration, and the associated changes in sea surface temperatures (SSTs), using the Whole Atmosphere Community Climate Model (WACCM). We use the climate feedback response analysis method (CFRAM) to calculate the partial temperature changes due to an external forcing and climate feedbacks in the atmosphere. As this method has the unique feature of additivity, these partial temperature changes are linearly addable. In this study, we discuss the direct forcing of CO2 and the effects of the ozone, water vapour, cloud, albedo and dynamical feedbacks. As expected, our results show that the direct forcing of CO2 cools the middle atmosphere. This cooling becomes stronger with increasing height; the cooling in the upper stratosphere is about three times as strong as the cooling in the lower stratosphere. The ozone feedback yields a radiative feedback that mitigates this cooling in most regions of the middle atmosphere. However, in the tropical lower stratosphere, and in some regions of the mesosphere, the ozone feedback has a cooling effect. The increase in the CO2 concentration causes the dynamics to change. The temperature response due to this dynamical feedback is small in terms of the global average, although there are large temperature changes due to this feedback locally. The temperature change in the lower stratosphere is influenced by the water vapour feedback and, to a lesser degree, by the cloud and albedo feedback. These feedbacks play no role in the upper stratosphere and the mesosphere. We find that the effects of the changed SSTs on the middle atmosphere are relatively small compared to the effects of changing the CO2. However, the changes in SSTs are responsible for dynamical feedbacks that cause large temperature changes. Moreover, the temperature response to the water vapour feedback in the lower stratosphere is almost solely due to changes in the SSTs. As CFRAM has not been applied to the middle atmosphere in this way before, this study also serves to investigate the applicability and the limitations of this method. This work shows that CFRAM is a very powerful tool for studying climate feedbacks in the middle atmosphere. However, it should be noted that there is a relatively large error term associated with the current method in the middle atmosphere, which can, to a large extent, be explained by the linearization in the method.