scholarly journals Analysis of HCl and ClO time series in the upper stratosphere using satellite data sets

2011 ◽  
Vol 11 (11) ◽  
pp. 5321-5333 ◽  
Author(s):  
A. Jones ◽  
J. Urban ◽  
D. P. Murtagh ◽  
C. Sanchez ◽  
K. A. Walker ◽  
...  
Keyword(s):  
Time Series ◽  
Satellite Data ◽  
Atmospheric Chemistry ◽  
Linear Trend ◽  
Montreal Protocol ◽  
Data Sets ◽  
Sigma Level ◽  
Chlorine Monoxide ◽  
Significant Downward Trend ◽  
The Tropics

Abstract. Previous analyses of satellite and ground-based measurements of hydrogen chloride (HCl) and chlorine monoxide (ClO) have suggested that total inorganic chlorine in the upper stratosphere is on the decline. We create HCl and ClO time series using satellite data sets extended to November 2008, so that an update can be made on the long term evolution of these two species. We use the HALogen Occultation Experiment (HALOE) and the Atmospheric Chemistry Experiment Fourier Transform Spectrometer (ACE-FTS) data for the HCl analysis, and the Odin Sub-Millimetre Radiometer (SMR) and the Aura Microwave Limb Sounder (Aura-MLS) measurements for the study of ClO. Altitudes between 35 and 45 km and two mid-latitude bands: 30° S–50° S and 30° N–50° N, for HCl, and 20° S–20° N for ClO and HCl are studied. ACE-FTS and HALOE HCl anomaly time series (with QBO and seasonal contributions removed) are combined to produce all instrument average time series, which show HCl to be reducing from peak 1997 values at a linear estimated rate of −5.1 % decade−1 in the Northern Hemisphere and −5.2 % decade−1 in the Southern Hemisphere, while the tropics show a linear trend of −5.8 % per decade (although we do not remove the QBO contribution there due to sparse data). Trend values are significantly different from a zero trend at the 2 sigma level. ClO is decreasing in the tropics by −7.1 % ± 7.8 % decade−1 based on measurements made from December 2001 to November 2008. The statistically significant downward trend found in HCl after 1997 and the apparent downward ClO trend since 2001 (although not statistically significant) confirm how effective the 1987 Montreal protocol objectives and its amendments have been in reducing the total amount of inorganic chlorine.

scholarly journals Analysis of HCl and ClO time series in the upper stratosphere using satellite data sets

2010 ◽  
Vol 10 (4) ◽  
pp. 8623-8655
Author(s):  
A. Jones ◽  
J. Urban ◽  
D. P. Murtagh ◽  
C. Sanchez ◽  
K. A. Walker ◽  
...  
Keyword(s):  
Time Series ◽  
Satellite Data ◽  
Atmospheric Chemistry ◽  
Montreal Protocol ◽  
Data Sets ◽  
Sigma Level ◽  
Chlorine Monoxide ◽  
The Tropics ◽  
Chemistry Experiment

Abstract. Previous analyses of satellite and ground-based measurements of hydrogen chloride (HCl) and chlorine monoxide (ClO) have suggested that total inorganic chlorine in the upper stratosphere is on the decline. We create HCl and ClO time series using satellite data sets with the intension of extending them to beyond November 2008 so that an update can be made on the long term evolution of these two species. We use the HALogen Occultation Experiment (HALOE) and the Atmospheric Chemistry Experiment Fourier Transform Spectrometer (ACE-FTS) data for the HCl analysis, and the Odin Sub-Millimetre Radiometer (SMR) and the Aura Microwave Limb Sounder (Aura-MLS) measurements for the study of ClO. Altitudes between 35 and 45 km and three latitude bands between 60° S–60° N for HCl, and 20° S–20° N for ClO are studied. HCl shows values to be reducing from peak 1997 values by −4.4% in the tropics and between −6.4% to −6.7% per decade in the mid-latitudes. Trend values are significantly different from a zero trend at the 2 sigma level. ClO is decreasing in the tropics by −7.1% ± 7.8%/decade based on measurements made from December 2001. As both of these species contribute most to the chlorine budget at these altitudes then HCl and ClO should decrease at similar rates. The results found here confirm how effective the 1987 Montreal protocol objectives and its amendments have been in reducing the total amount of inorganic chlorine.

scholarly journals Construction of merged satellite total O<sub>3</sub> and NO<sub>2</sub> time series in the tropics for trend studies and evaluation by comparison to NDACC SAOZ measurements

2014 ◽  
Vol 7 (10) ◽  
pp. 3337-3354 ◽  
Author(s):  
M. Pastel ◽  
J.-P. Pommereau ◽  
F. Goutail ◽  
A. Richter ◽  
A. Pazmiño ◽  
...  
Keyword(s):  
Time Series ◽  
Lower Stratosphere ◽  
Atmospheric Composition ◽  
Data Sets ◽  
Composition Change ◽  
Long Time ◽  
Uv Visible ◽  
The Tropics ◽  
Lower Noise ◽  
Total Column

Abstract. Long time series of ozone and NO2 total column measurements in the southern tropics are available from two ground-based SAOZ (Système d'Analyse par Observation Zénithale) UV-visible spectrometers operated within the Network for the Detection of Atmospheric Composition Change (NDACC) in Bauru (22° S, 49° W) in S-E Brazil since 1995 and Reunion Island (21° S, 55° E) in the S-W Indian Ocean since 1993. Although the stations are located at the same latitude, significant differences are observed in the columns of both species, attributed to differences in tropospheric content and equivalent latitude in the lower stratosphere. These data are used to identify which satellites operating during the same period, are capturing the same features and are thus best suited for building reliable merged time series for trend studies. For ozone, the satellites series best matching SAOZ observations are EP-TOMS (1995–2004) and OMI-TOMS (2005–2011), whereas for NO2, best results are obtained by combining GOME version GDP5 (1996–2003) and SCIAMACHY – IUP (2003–2011), displaying lower noise and seasonality in reference to SAOZ. Both merged data sets are fully consistent with the larger columns of the two species above South America and the seasonality of the differences between the two stations, reported by SAOZ, providing reliable time series for further trend analyses and identification of sources of interannual variability in the future analysis.

scholarly journals Flexible approach for quantifying average long-term changes and seasonal cycles of tropospheric trace species

2019 ◽  
Author(s):  
David D. Parrish ◽  
Richard G. Derwent ◽  
Simon O'Doherty ◽  
Peter G. Simmonds
Keyword(s):  
Time Series ◽  
Seasonal Cycle ◽  
Linear Trend ◽  
Power Series Expansion ◽  
Mathematical Representation ◽  
Seasonal Cycles ◽  
Data Sets ◽  
Significant Information ◽  
Long Term Changes

Abstract. We present an approach to derive a systematic mathematical representation of the statistically significant features of the average long-term changes and seasonal cycle of concentrations of trace tropospheric species. The results for two illustrative data sets (time series of baseline concentrations of ozone and N2O at Mace Head, Ireland) indicate that a limited set of seven or eight parameter values provides this mathematical representation for both example species. This method utilizes a power series expansion to extract more information regarding the long-term changes than can be provided by oft-employed linear trend analyses. In contrast, the quantification of average seasonal cycles utilizes a Fourier series analysis that provides less detailed seasonal cycles than are sometimes represented as twelve monthly means; including that many parameters in the seasonal cycle representation is not usually statistically justified, and thereby adds unnecessary noise to the representation and prevents a clear analysis of the statistical uncertainty of the results. The approach presented here is intended to maximize the statistically significant information extracted from analyses of time series of concentrations of tropospheric species regarding their mean long-term changes and seasonal cycles, including non-linear aspects of the long-term trends. Additional implications, advantages and limitations of this approach are discussed.

scholarly journals Global stratospheric fluorine inventory for 2004–2009 from Atmospheric Chemistry Experiment Fourier Transform Spectrometer (ACE-FTS) measurements and SLIMCAT model simulations

2014 ◽  
Vol 14 (1) ◽  
pp. 267-282 ◽  
Author(s):  
A. T. Brown ◽  
M. P. Chipperfield ◽  
N. A. D. Richards ◽  
C. Boone ◽  
P. F. Bernath
Keyword(s):  
Atmospheric Chemistry ◽  
Radiative Forcing ◽  
Transport Model ◽  
Similar Rate ◽  
Montreal Protocol ◽  
Negative Slope ◽  
Mixing Ratios ◽  
Inorganic Species ◽  
The Tropics ◽  
The Impact

Abstract. Fluorine-containing species can be extremely effective atmospheric greenhouse gases. We present fluorine budgets using organic and inorganic species retrieved by the ACE-FTS satellite instrument supplemented with output from the SLIMCAT 3-D chemical transport model. The budgets are calculated between 2004 and 2009 for a number of latitude bands: 70–30° N, 30–00° N, 00° N–30° S, and 30–70° S. At lower altitudes total fluorine profiles are dominated by the contribution from CFC-12, up to an altitude of 20 km in the extra-tropics and 29 km in the tropics; above these altitudes the profiles are dominated by hydrogen fluoride (HF). Our data show that total fluorine profiles at all locations have a negative slope with altitude, providing evidence that overall fluorine emissions (measured by their F content) have been increasing with time. Total stratospheric fluorine is increasing at a similar rate in the tropics: 32.5 ± 4.9 ppt yr−1 (1.31 ± 0.20% per year) in the Northern Hemisphere (NH) and 29.8 ± 5.3 ppt yr−1 (1.21 ± 0.22% per year) in the Southern Hemisphere (SH). Extra-tropical total stratospheric fluorine is also increasing at a similar rate in both the NH and SH: 28.3 ± 2.7 ppt per year (1.12 ± 0.11% per year) in the NH and 24.3 ± 3.1 ppt per year (0.96 ± 0.12% per year) in the SH. The calculation of radiative efficiency-weighted total fluorine allows the changes in radiative forcing between 2004 and 2009 to be calculated. These results show an increase in radiative forcing of between 0.23 ± 0.11% per year and 0.45 ± 0.11% per year, due to the increase in fluorine-containing species during this time. The decreasing trends in the mixing ratios of halons and chlorofluorocarbons (CFCs), due to their prohibition under the Montreal Protocol, have suppressed an increase in total fluorine caused by increasing mixing ratios of hydrofluorocarbons (HFCs). This has reduced the impact of fluorine-containing species on global warming.

scholarly journals Copernicus stratospheric ozone service, 2009–2012: validation, system intercomparison and roles of input data sets

2015 ◽  
Vol 15 (5) ◽  
pp. 2269-2293 ◽  
Author(s):  
K. Lefever ◽  
R. van der A ◽  
F. Baier ◽  
Y. Christophe ◽  
Q. Errera ◽  
...  
Keyword(s):  
Data Assimilation ◽  
Atmospheric Chemistry ◽  
Ozone Depletion ◽  
Total Ozone ◽  
Chemical Constituents ◽  
Stratospheric Ozone ◽  
Atmospheric Composition ◽  
The Arctic ◽  
Data Sets ◽  
The Tropics

Abstract. This paper evaluates and discusses the quality of the stratospheric ozone analyses delivered in near real time by the MACC (Monitoring Atmospheric Composition and Climate) project during the 3-year period between September 2009 and September 2012. Ozone analyses produced by four different chemical data assimilation (CDA) systems are examined and compared: the Integrated Forecast System coupled to the Model for OZone And Related chemical Tracers (IFS-MOZART); the Belgian Assimilation System for Chemical ObsErvations (BASCOE); the Synoptic Analysis of Chemical Constituents by Advanced Data Assimilation (SACADA); and the Data Assimilation Model based on Transport Model version 3 (TM3DAM). The assimilated satellite ozone retrievals differed for each system; SACADA and TM3DAM assimilated only total ozone observations, BASCOE assimilated profiles for ozone and some related species, while IFS-MOZART assimilated both types of ozone observations. All analyses deliver total column values that agree well with ground-based observations (biases < 5%) and have a realistic seasonal cycle, except for BASCOE analyses, which underestimate total ozone in the tropics all year long by 7 to 10%, and SACADA analyses, which overestimate total ozone in polar night regions by up to 30%. The validation of the vertical distribution is based on independent observations from ozonesondes and the ACE-FTS (Atmospheric Chemistry Experiment – Fourier Transform Spectrometer) satellite instrument. It cannot be performed with TM3DAM, which is designed only to deliver analyses of total ozone columns. Vertically alternating positive and negative biases are found in the IFS-MOZART analyses as well as an overestimation of 30 to 60% in the polar lower stratosphere during polar ozone depletion events. SACADA underestimates lower stratospheric ozone by up to 50% during these events above the South Pole and overestimates it by approximately the same amount in the tropics. The three-dimensional (3-D) analyses delivered by BASCOE are found to have the best quality among the three systems resolving the vertical dimension, with biases not exceeding 10% all year long, at all stratospheric levels and in all latitude bands, except in the tropical lowermost stratosphere. The northern spring 2011 period is studied in more detail to evaluate the ability of the analyses to represent the exceptional ozone depletion event, which happened above the Arctic in March 2011. Offline sensitivity tests are performed during this month and indicate that the differences between the forward models or the assimilation algorithms are much less important than the characteristics of the assimilated data sets. They also show that IFS-MOZART is able to deliver realistic analyses of ozone both in the troposphere and in the stratosphere, but this requires the assimilation of observations from nadir-looking instruments as well as the assimilation of profiles, which are well resolved vertically and extend into the lowermost stratosphere.

scholarly journals The SPARC water vapour assessment II: Comparison of stratospheric and lower mesospheric water vapour time series observed from satellites

2018 ◽  
Author(s):  
Farahnaz Khosrawi ◽  
Stefan Lossow ◽  
Gabriele P. Stiller ◽  
Karen H. Rosenlof ◽  
Joachim Urban ◽  
...  
Keyword(s):  
Time Series ◽  
Water Vapour ◽  
Data Sets ◽  
Data Set ◽  
The Future ◽  
Modelling Studies ◽  
The Difference ◽  
The Tropics ◽  
The Antarctic ◽  
Satellite Instruments

Abstract. Time series of stratospheric and lower mesospheric water vapour using 33 data sets from 15 different satellite instruments were compared in the framework of the second SPARC (Stratosphere-troposphere Processes And their Role in Climate) water vapour assessment (WAVAS-II). This comparison aimed to provide a comprehensive overview of the typical uncertainties in the observational database that can be considered in the future in observational and modelling studies addressing e.g stratospheric water vapour trends. The time series comparisons are presented for the three latitude bands, the Antarctic (80°–70° S), the tropics (15° S–15° N) and the northern hemisphere mid-latitudes (50° N–60° N) at four different altitudes (0.1, 3, 10 and 80 hPa) covering the stratosphere and lower mesosphere. The combined temporal coverage of observations from the 15 satellite instruments allowed considering the time period 1986–2014. In addition to the qualitative comparison of the time series, the agreement of the data sets is assessed quantitatively in the form of the spread (i.e. the difference between the maximum and minimum volume mixing ratio among the data sets), the (Pearson) correlation coefficient and the drift (i.e. linear changes of the difference between time series over time). Generally, good agreement between the time series was found in the middle stratosphere while larger differences were found in the lower mesosphere and near the tropopause. Concerning the latitude bands, the largest differences were found in the Antarctic while the best agreement was found for the tropics. From our assessment we find that all data sets can be considered in the future in observational and modelling studies addressing e.g. stratospheric and lower mesospheric water vapour variability and trends when data set specific characteristics (e.g. a drift) and restrictions (e.g. temporal and spatial coverage) are taken into account.

scholarly journals The SPARC Data Initiative: comparisons of CFC-11, CFC-12, HF and SF<sub>6</sub> climatologies from international satellite limb sounders

2016 ◽  
Vol 8 (1) ◽  
pp. 61-78 ◽  
Author(s):  
S. Tegtmeier ◽  
M. I. Hegglin ◽  
J. Anderson ◽  
B. Funke ◽  
J. Gille ◽  
...  
Keyword(s):  
Time Series ◽  
Satellite Data ◽  
Lower Stratosphere ◽  
Atmospheric Transport ◽  
Temporal Structure ◽  
Data Sets ◽  
Upper Troposphere ◽  
Mean Fields ◽  
Mean State

Abstract. A quality assessment of the CFC-11 (CCl3F), CFC-12 (CCl2F2), HF, and SF6 products from limb-viewing satellite instruments is provided by means of a detailed intercomparison. The climatologies in the form of monthly zonal mean time series are obtained from HALOE, MIPAS, ACE-FTS, and HIRDLS within the time period 1991–2010. The intercomparisons focus on the mean biases of the monthly and annual zonal mean fields and aim to identify their vertical, latitudinal and temporal structure. The CFC evaluations (based on MIPAS, ACE-FTS and HIRDLS) reveal that the uncertainty in our knowledge of the atmospheric CFC-11 and CFC-12 mean state, as given by satellite data sets, is smallest in the tropics and mid-latitudes at altitudes below 50 and 20 hPa, respectively, with a 1σ multi-instrument spread of up to ±5 %. For HF, the situation is reversed. The two available data sets (HALOE and ACE-FTS) agree well above 100 hPa, with a spread in this region of ±5 to ±10 %, while at altitudes below 100 hPa the HF annual mean state is less well known, with a spread ±30 % and larger. The atmospheric SF6 annual mean states derived from two satellite data sets (MIPAS and ACE-FTS) show only very small differences with a spread of less than ±5 % and often below ±2.5 %. While the overall agreement among the climatological data sets is very good for large parts of the upper troposphere and lower stratosphere (CFCs, SF6) or middle stratosphere (HF), individual discrepancies have been identified. Pronounced deviations between the instrument climatologies exist for particular atmospheric regions which differ from gas to gas. Notable features are differently shaped isopleths in the subtropics, deviations in the vertical gradients in the lower stratosphere and in the meridional gradients in the upper troposphere, and inconsistencies in the seasonal cycle. Additionally, long-term drifts between the instruments have been identified for the CFC-11 and CFC-12 time series. The evaluations as a whole provide guidance on what data sets are the most reliable for applications such as studies of atmospheric transport and variability, model–measurement comparisons and detection of long-term trends. The data sets will be publicly available from the SPARC Data Centre and through PANGAEA (doi:10.1594/PANGAEA.849223).

scholarly journals Quantifying uncertainties of climate signals related to the 11–year solar cycle. Part I: Annual mean response in heating rates,temperature and ozone

2020 ◽  
Author(s):  
Markus Kunze ◽  
Tim Kruschke ◽  
Ulrike Langematz ◽  
Miriam Sinnhuber ◽  
Thomas Reddmann ◽  
...  
Keyword(s):  
Atmospheric Chemistry ◽  
Climate Model ◽  
Sunspot Cycle ◽  
Spectral Irradiance ◽  
Data Sets ◽  
Heating Rates ◽  
Data Set ◽  
Mixing Ratios ◽  
Solar Signal ◽  
The Tropics

Abstract. Variations of the solar spectral irradiance (SSI) with the 11-year sunspot cycle have been shown to have a significant impact on temperatures and the mixing ratios of atmospheric constituents in the stratosphere and mesosphere. Uncertainties in modelling the effects of SSI variations arise from uncertainties in the empirical models reconstructing the prescribed SSI data set as well as from uncertainties in the chemistry-climate model (CCM) formulation. In this study CCM simulations with the ECHAM MESSy Atmospheric Chemistry (EMAC) model and the Community Earth System Model 1 (CESM1) – Whole Atmosphere Chemistry Climate Model (WACCM) have been performed to quantify the uncertainties of the solar responses in chemistry and dynamics that are due to the usage of five different SSI data sets or the two CCMs. We apply a two-way analysis of variance (ANOVA) to separate the influence of the SSI data sets and the CCMs on the variability of the solar response in shortwave heating rates, temperature and ozone. The ANOVA identifies the SSI data set with the strongest influence on the variability of the solar signal in shortwave heating rates in the upper mesosphere and in the upper stratosphere/lower mesosphere. The strongest influence on the variability of the solar signal in ozone and temperature is identified in the upper stratosphere/lower mesosphere. The largest influence of the CCMs on variability of the solar responses can be identified in the upper mesosphere. The solar response in the lower stratosphere also depends on the CCM used, especially in the tropics and northern hemispheric subtropics and mid latitudes, where the model dynamics modulate the solar responses.

scholarly journals The SPARC water vapour assessment II: comparison of stratospheric and lower mesospheric water vapour time series observed from satellites

2018 ◽  
Vol 11 (7) ◽  
pp. 4435-4463 ◽  
Author(s):  
Farahnaz Khosrawi ◽  
Stefan Lossow ◽  
Gabriele P. Stiller ◽  
Karen H. Rosenlof ◽  
Joachim Urban ◽  
...  
Keyword(s):  
Time Series ◽  
Water Vapour ◽  
Data Sets ◽  
Data Set ◽  
Spatial Coverage ◽  
Modelling Studies ◽  
The Difference ◽  
The Tropics ◽  
The Antarctic ◽  
Satellite Instruments

Abstract. Time series of stratospheric and lower mesospheric water vapour using 33 data sets from 15 different satellite instruments were compared in the framework of the second SPARC (Stratosphere-troposphere Processes And their Role in Climate) water vapour assessment (WAVAS-II). This comparison aimed to provide a comprehensive overview of the typical uncertainties in the observational database that can be considered in the future in observational and modelling studies, e.g addressing stratospheric water vapour trends. The time series comparisons are presented for the three latitude bands, the Antarctic (80∘–70∘ S), the tropics (15∘ S–15∘ N) and the Northern Hemisphere mid-latitudes (50∘–60∘ N) at four different altitudes (0.1, 3, 10 and 80 hPa) covering the stratosphere and lower mesosphere. The combined temporal coverage of observations from the 15 satellite instruments allowed the consideration of the time period 1986–2014. In addition to the qualitative comparison of the time series, the agreement of the data sets is assessed quantitatively in the form of the spread (i.e. the difference between the maximum and minimum volume mixing ratios among the data sets), the (Pearson) correlation coefficient and the drift (i.e. linear changes of the difference between time series over time). Generally, good agreement between the time series was found in the middle stratosphere while larger differences were found in the lower mesosphere and near the tropopause. Concerning the latitude bands, the largest differences were found in the Antarctic while the best agreement was found for the tropics. From our assessment we find that most data sets can be considered in future observational and modelling studies, e.g. addressing stratospheric and lower mesospheric water vapour variability and trends, if data set specific characteristics (e.g. drift) and restrictions (e.g. temporal and spatial coverage) are taken into account.

scholarly journals Global HCFC-22 measurements with MIPAS: retrieval, validation, global distribution and its evolution over 2005–2012

2016 ◽  
Vol 16 (5) ◽  
pp. 3345-3368 ◽  
Author(s):  
M. Chirkov ◽  
G. P. Stiller ◽  
A. Laeng ◽  
S. Kellmann ◽  
T. von Clarmann ◽  
...  
Keyword(s):  
Time Series ◽  
Satellite Data ◽  
Lower Stratosphere ◽  
Positive Trend ◽  
Altitude Range ◽  
Quasi Biennial Oscillation ◽  
Near Surface ◽  
Upper Troposphere ◽  
The Tropics ◽  
Balloon Measurements

Abstract. We report on HCFC-22 data acquired by the Michelson Interferometer for Passive Atmospheric Sounding (MIPAS) in the reduced spectral resolution nominal observation mode. The data cover the period from January 2005 to April 2012 and the altitude range from the upper troposphere (above cloud top altitude) to about 50 km. The profile retrieval was performed by constrained nonlinear least squares fitting of modelled spectra to the measured limb spectral radiances. The spectral ν4-band at 816.5 ± 13 cm−1 was used for the retrieval. A Tikhonov-type smoothing constraint was applied to stabilise the retrieval. In the lower stratosphere, we find a global volume mixing ratio of HCFC-22 of about 185 pptv in January 2005. The rate of linear growth in the lower latitudes lower stratosphere was about 6 to 7 pptv year−1 in the period 2005–2012. The profiles obtained were compared with ACE-FTS satellite data v3.5, as well as with MkIV balloon profiles and cryosampler balloon measurements. Between 13 and 22 km, average agreement within −3 to +5 pptv (MIPAS – ACE) with ACE-FTS v3.5 profiles is demonstrated. Agreement with MkIV solar occultation balloon-borne measurements is within 10–20 pptv below 30 km and worse above, while in situ cryosampler balloon measurements are systematically lower over their full altitude range by 15–50 pptv below 24 km and less than 10 pptv above 28 km. MIPAS HCFC-22 time series below 10 km altitude are shown to agree mostly well to corresponding time series of near-surface abundances from the NOAA/ESRL and AGAGE networks, although a more pronounced seasonal cycle is obvious in the satellite data. This is attributed to tropopause altitude fluctuations and subsidence of polar winter stratospheric air into the troposphere. A parametric model consisting of constant, linear, quasi-biennial oscillation (QBO) and several sine and cosine terms with different periods has been fitted to the temporal variation of stratospheric HCFC-22 for all 10°-latitude/1-to-2-km-altitude bins. The relative linear variation was always positive, with relative increases of 40–70 % decade−1 in the tropics and global lower stratosphere, and up to 120 % decade−1 in the upper stratosphere of the northern polar region and the southern extratropical hemisphere. Asian HCFC-22 emissions have become the major source of global upper tropospheric HCFC-22. In the upper troposphere, monsoon air, rich in HCFC-22, is instantaneously mixed into the tropics. In the middle stratosphere, between 20 and 30 km, the observed trend is inconsistent with the trend at the surface (corrected for the age of stratospheric air), hinting at circulation changes. There exists a stronger positive trend in HCFC-22 in the Southern Hemisphere and a more muted positive trend in the Northern Hemisphere, implying a potential change in the stratospheric circulation over the observation period.

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