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 ◽  
...  

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.

2015 ◽  
Vol 15 (10) ◽  
pp. 14783-14841
Author(s):  
M. Chirkov ◽  
G. P. Stiller ◽  
A. Laeng ◽  
S. Kellmann ◽  
T. von Clarmann ◽  
...  

Abstract. We report on HCFC-22 data acquired by the Michelson Interferometer for Passive Atmospheric Sounding (MIPAS) in reduced spectral resolution nominal mode in the period from January 2005 to April 2012 from version 5.02 level-1b spectral data and covering an 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 measured limb spectral radiances to modelled spectra. 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 linear growth rate in the lower latitudes lower stratosphere was about 6 to 7 pptv yr−1 in the period 2005–2012. The obtained profiles were compared with ACE-FTS satellite data v3.5, as well as with MkIV balloon profiles and in situ 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. Obtained MIPAS HCFC-22 time series below 10 km altitude are shown to agree mostly well to corresponding time series of near-surface abundances from NOAA/ESRL and AGAGE networks, although a more pronounced seasonal cycle is obvious in the satellite data, probably due 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. In the middle stratosphere between 20 and 30 km, the observed trend is not consistent with the age of stratospheric air-corrected trend at ground, but stronger positive at the Southern Hemisphere and less strong increasing in the Northern Hemisphere, hinting towards changes in the stratospheric circulation over the observation period.


2013 ◽  
Vol 13 (9) ◽  
pp. 4563-4575 ◽  
Author(s):  
T. Flury ◽  
D. L. Wu ◽  
W. G. Read

Abstract. We use Aura/MLS stratospheric water vapour (H2O) measurements as tracer for dynamics and infer interannual variations in the speed of the Brewer–Dobson circulation (BDC) from 2004 to 2011. We correlate one-year time series of H2O in the lower stratosphere at two subsequent pressure levels (68 hPa, ~18.8 km and 56 hPa, ~19.9 km at the Equator) and determine the time lag for best correlation. The same calculation is made on the horizontal on the 100 hPa (~16.6 km) level by correlating the H2O time series at the Equator with the ones at 40° N and 40° S. From these lag coefficients we derive the vertical and horizontal speeds of the BDC in the tropics and extra-tropics, respectively. We observe a clear interannual variability of the vertical and horizontal branch. The variability reflects signatures of the Quasi Biennial Oscillation (QBO). Our measurements confirm the QBO meridional circulation anomalies and show that the speed variations in the two branches of the BDC are out of phase and fairly well anti-correlated. Maximum ascent rates are found during the QBO easterly phase. We also find that transport of H2O towards the Northern Hemisphere (NH) is on the average two times faster than to the Southern Hemisphere (SH) with a mean speed of 1.15 m s−1 at 100 hPa. Furthermore, the speed towards the NH shows much more interannual variability with an amplitude of about 21% whilst the speed towards the SH varies by only 10%. An amplitude of 21% is also observed in the variability of the ascent rate at the Equator which is on the average 0.2 mm s−1.


2016 ◽  
Vol 8 (1) ◽  
pp. 61-78 ◽  
Author(s):  
S. Tegtmeier ◽  
M. I. Hegglin ◽  
J. Anderson ◽  
B. Funke ◽  
J. Gille ◽  
...  

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).


2013 ◽  
Vol 13 (20) ◽  
pp. 10405-10423 ◽  
Author(s):  
M. Höpfner ◽  
N. Glatthor ◽  
U. Grabowski ◽  
S. Kellmann ◽  
M. Kiefer ◽  
...  

Abstract. We present a climatology of monthly and 10° zonal mean profiles of sulfur dioxide (SO2) volume mixing ratios (vmr) derived from MIPAS/Envisat measurements in the altitude range 15–45 km from July 2002 until April 2012. The vertical resolution varies from 3.5–4 km in the lower stratosphere up to 6–10 km at the upper end of the profiles, with estimated total errors of 5–20 pptv for single profiles of SO2. Comparisons with the few available observations of SO2 up to high altitudes from ATMOS for a volcanically perturbed situation from ACE-FTS and, at the lowest altitudes, with stratospheric in situ observations reveal general consistency of the datasets. The observations are the first empirical confirmation of features of the stratospheric SO2 distribution, which have only been shown by models up to now: (1) the local maximum of SO2 at around 25–30 km altitude, which is explained by the conversion of carbonyl sulfide (COS) as the precursor of the Junge layer; and (2) the downwelling of SO2-rich air to altitudes of 25–30 km at high latitudes during winter and its subsequent depletion on availability of sunlight. This has been proposed as the reason for the sudden appearance of enhanced concentrations of condensation nuclei during Arctic and Antarctic spring. Further, the strong increase of SO2 to values of 80–100 pptv in the upper stratosphere through photolysis of H2SO4 has been confirmed. Lower stratospheric variability of SO2 could mainly be explained by volcanic activity, and no hints of a strong anthropogenic influence have been found. Regression analysis revealed a QBO (quasi-biennial oscillation) signal of the SO2 time series in the tropics at about 30–35 km, an SAO (semi-annual oscillation) signal at tropical and subtropical latitudes above 32 km and annual periodics predominantly at high latitudes. Further, the analysis indicates a correlation with the solar cycle in the tropics and southern subtropics above 30 km. Significant negative linear trends are found in the tropical lower stratosphere, probably due to reduced tropical volcanic activity and at southern mid-latitudes above 35 km. A positive trend is visible in the lower and middle stratosphere at polar to subtropical southern latitudes.


2018 ◽  
Vol 36 (2) ◽  
pp. 381-404 ◽  
Author(s):  
Abdoulwahab Mohamed Toihir ◽  
Thierry Portafaix ◽  
Venkataraman Sivakumar ◽  
Hassan Bencherif ◽  
Andréa Pazmiño ◽  
...  

Abstract. Long-term variability in ozone trends was assessed over eight Southern Hemisphere tropical and subtropical sites (Natal, Nairobi, Ascension Island, Java, Samoa, Fiji, Reunion and Irene), using total column ozone data (TCO) and vertical ozone profiles (altitude range 15–30 km) recorded during the period January 1998–December 2012. The TCO datasets were constructed by combination of satellite data (OMI and TOMS) and ground-based observations recorded using Dobson and SAOZ spectrometers. Vertical ozone profiles were obtained from balloon-sonde experiments which were operated within the framework of the SHADOZ network. The analysis in this study was performed using the Trend-Run model. This is a multivariate regression model based on the principle of separating the variations of ozone time series into a sum of several forcings (annual and semi-annual oscillations, QBO (Quasi-Biennial Oscillation), ENSO, 11-year solar cycle) that account for most of its variability. The trend value is calculated based on the slope of a normalized linear function which is one of the forcing parameters included in the model. Three regions were defined as follows: equatorial (0–10∘ S), tropical (10–20∘ S) and subtropical (20–30∘ S). Results obtained indicate that ozone variability is dominated by seasonal and quasi-biennial oscillations. The ENSO contribution is observed to be significant in the tropical lower stratosphere and especially over the Pacific sites (Samoa and Java). The annual cycle of ozone is observed to be the most dominant mode of variability for all the sites and presents a meridional signature with a maximum over the subtropics, while semi-annual and quasi-biannual ozone modes are more apparent over the equatorial region, and their magnitude decreases southward. The ozone variation mode linked to the QBO signal is observed between altitudes of 20 and 28 km. Over the equatorial zone there is a strong signal at ∼26 km, where 58 % ±2 % of total ozone variability is explained by the effect of QBO. Annual ozone oscillations are more apparent at two different altitude ranges (below 24 km and in the 27–30 km altitude band) over the tropical and subtropical regions, while the semi-annual oscillations are more significant over the 27–30 km altitude range in the tropical and equatorial regions. The estimated trend in TCO is positive and not significant and corresponds to a variation of ∼1.34±0.50 % decade−1 (averaged over the three regions). The trend estimated within the equatorial region (0–15∘ S) is less than 1 % per decade, while it is assessed at more than 1.5 % decade−1 for all the sites located southward of 17∘ S. With regard to the vertical distribution of trend estimates, a positive trend in ozone concentration is obtained in the 22–30 km altitude range, while a delay in ozone improvement is apparent in the UT–LS (upper troposphere–lower stratosphere) below 22 km. This is especially noticeable at approximately 19 km, where a negative value is observed in the tropical regions.


2012 ◽  
Vol 12 (8) ◽  
pp. 21291-21320 ◽  
Author(s):  
T. Flury ◽  
D. L. Wu ◽  
W. G. Read

Abstract. We use Aura/MLS stratospheric water vapor measurements to infer interannual variations in the speed of the Brewer-Dobson circulation (BDC) from 2004 to 2011. Stratospheric water vapor (H2O) is utilized as a tracer for dynamics and we follow its path along the vertical and meridional branch of the BDC from the tropics to mid-latitudes. We correlate one year time series of H2O in the lower stratosphere at two subsequent altitude levels (68 hPa, ~18.8 km and 56 hPa, ~19.9 km at the Equator) and determine the time lag for best correlation. The same calculation is made on the horizontal on the 100 hPa (~16.6 km) level by correlating the H2O time series at the Equator with the ones at 40° N and 40° S. From these lag coefficients we derive the vertical and horizontal speeds of the BDC in the tropics and extra-tropics respectively. We observe a clear interannual variability of the vertical and horizontal branch. The variability reflects signatures of the Quasi Biennial Oscillation (QBO). Our measurements confirm the QBO meridional circulation anomalies and show that the speed variations in the two branches of the BDC are out of phase and fairly well anti-correlated. Maximum ascent rates are found during the QBO easterly phase. We also find that the transport towards the Northern Hemisphere (NH) is on the average two times faster than to the Southern Hemisphere (SH) with a mean speed of 1.15 m s−1 at 100 hPa. Furthermore, the speed towards the NH shows much more variability with an amplitude of about 21% whilst the speed towards the SH varies by only 10%. An amplitude of 21% is also observed in the variability of the ascent rate at the Equator which is on the average 0.2 mm s−1 and hence about 5000 times slower than the meridional branch.


2013 ◽  
Vol 13 (5) ◽  
pp. 12389-12436 ◽  
Author(s):  
M. Höpfner ◽  
N. Glatthor ◽  
U. Grabowski ◽  
S. Kellmann ◽  
M. Kiefer ◽  
...  

Abstract. We present a climatology of monthly and 10° zonal mean profiles of sulfur dioxide (SO2) volume mixing ratios (vmr) derived from MIPAS/Envisat measurements in the altitude range 15–45 km from July 2002 until April 2012. The vertical resolution varies from 3.5–4 km in the lower stratosphere up to 6–10 km at the upper end of the profiles with estimated total errors of 5–20 pptv for single profiles of SO2. Comparisons with few available observations of SO2 up to high altitudes from ATMOS, for a volcanically perturbed situations from ACE-FTS and, at the lowest altitudes, with stratospheric in-situ observations reveal general consistency of the datasets. The observations are the first empirical confirmation of features of the stratospheric SO2 distribution which have only been shown by models up to now: (1) the local maximum of SO2 at around 25–30 km altitude which is explained by the conversion of carbonyl sulfide (COS) as the precursor of the Junge layer, and (2) the downwelling of SO2 rich air to altitudes of 25–30 km at high latitudes during winter and its subsequent depletion on availability of sunlight. This has been proposed as the reason for the sudden appearance of enhanced concentrations of condensation nuclei during Arctic and Antarctic spring. Further, the strong increase of SO2 to values of 80–100 pptv in the upper stratosphere through photolysis of H2SO4 has been confirmed. Lower stratospheric variability of SO2 could mainly be explained by volcanic activity and no hint for a strong anthropogenic influence has been found. Regression analysis revealed a QBO (quasi-biennial oscillation) signal of the SO2 time series in the tropics at about 30–35 km, a SAO (semi-annual oscillation) signal at tropical and subtropical latitudes above 32 km and annual periodics predominantly at high latitudes. Further, the analysis indicates a correlation with the solar cycle in the tropics and southern subtropics above 30 km. Significant negative linear trends are found in the tropical lower stratosphere, probably due to reduced tropical volcanic activity and at southern mid-latitudes above 35 km. A positive trend is visible in the lower and middle stratosphere at polar to subtropical southern latitudes.


2015 ◽  
Vol 8 (2) ◽  
pp. 759-808
Author(s):  
S. Tegtmeier ◽  
M. I. Hegglin ◽  
J. Anderson ◽  
B. Funke ◽  
J. Gille ◽  
...  

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 inter-comparison. 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 inter-comparisons 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 1-sigma 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 center and through PANGAEA (doi:10.1594/PANGAEA.849223).


2014 ◽  
Vol 7 (10) ◽  
pp. 3337-3354 ◽  
Author(s):  
M. Pastel ◽  
J.-P. Pommereau ◽  
F. Goutail ◽  
A. Richter ◽  
A. Pazmiño ◽  
...  

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.


2014 ◽  
Vol 7 (4) ◽  
pp. 5087-5139 ◽  
Author(s):  
R. Pommrich ◽  
R. Müller ◽  
J.-U. Grooß ◽  
P. Konopka ◽  
F. Ploeger ◽  
...  

Abstract. Variations in the mixing ratio of trace gases of tropospheric origin entering the stratosphere in the tropics are of interest for assessing both troposphere to stratosphere transport fluxes in the tropics and the impact of these transport fluxes on the composition of the tropical lower stratosphere. Anomaly patterns of carbon monoxide (CO) and long-lived tracers in the lower tropical stratosphere allow conclusions about the rate and the variability of tropical upwelling to be drawn. Here, we present a simplified chemistry scheme for the Chemical Lagrangian Model of the Stratosphere (CLaMS) for the simulation, at comparatively low numerical cost, of CO, ozone, and long-lived trace substances (CH4, N2O, CCl3F (CFC-11), CCl2F2 (CFC-12), and CO2) in the lower tropical stratosphere. For the long-lived trace substances, the boundary conditions at the surface are prescribed based on ground-based measurements in the lowest model level. The boundary condition for CO in the free troposphere is deduced from MOPITT measurements (at ≈ 700–200 hPa). Due to the lack of a specific representation of mixing and convective uplift in the troposphere in this model version, enhanced CO values, in particular those resulting from convective outflow are underestimated. However, in the tropical tropopause layer and the lower tropical stratosphere, there is relatively good agreement of simulated CO with in-situ measurements (with the exception of the TROCCINOX campaign, where CO in the simulation is biased low ≈ 10–20 ppbv). Further, the model results are of sufficient quality to describe large scale anomaly patterns of CO in the lower stratosphere. In particular, the zonally averaged tropical CO anomaly patterns (the so called "tape recorder" patterns) simulated by this model version of CLaMS are in good agreement with observations. The simulations show a too rapid upwelling compared to observations as a consequence of the overestimated vertical velocities in the ERA-interim reanalysis data set. Moreover, the simulated tropical anomaly patterns of N2O are in good agreement with observations. In the simulations, anomaly patterns for CH4 and CFC-11 were found to be consistent with those of N2O; for all long-lived tracers, positive anomalies are simulated because of the enhanced tropical upwelling in the easterly phase of the quasi-biennial oscillation.


Sign in / Sign up

Export Citation Format

Share Document