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 ◽  
...  

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.

2011 ◽  
Vol 11 (11) ◽  
pp. 5321-5333 ◽  
Author(s):  
A. Jones ◽  
J. Urban ◽  
D. P. Murtagh ◽  
C. Sanchez ◽  
K. A. Walker ◽  
...  

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.


2015 ◽  
Vol 15 (8) ◽  
pp. 4215-4224 ◽  
Author(s):  
G. E. Nedoluha ◽  
D. E. Siskind ◽  
A. Lambert ◽  
C. Boone

Abstract. While global stratospheric O3 has begun to recover, there are localized regions where O3 has decreased since 1991. Specifically, we use measurements from the Halogen Occultation Experiment (HALOE) for the period 1991–2005 and the NASA Aura Microwave Limb Sounder (MLS) for the period 2004–2013 to demonstrate a significant decrease in O3 near ~ 10 hPa in the tropics. O3 in this region is very sensitive to variations in NOy, and the observed decrease can be understood as a spatially localized, yet long-term increase in NOy. In turn, using data from MLS and from the Atmospheric Chemistry Experiment (ACE), we show that the NOy variations are caused by decreases in N2O which are likely linked to long-term variations in dynamics. To illustrate how variations in dynamics can affect N2O and O3, we show that by decreasing the upwelling in the tropics, more of the N2O can photodissociate with a concomitant increase in NOy production (via N2O + O(1D) → 2NO) at 10 hPa. Ultimately, this can cause an O3 decrease of the observed magnitude.


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).


2015 ◽  
Vol 15 (1) ◽  
pp. 453-480 ◽  
Author(s):  
G. E. Nedoluha ◽  
D. E. Siskind ◽  
A. Lambert ◽  
C. Boone

Abstract. While global stratospheric O3 has begun to recover, there are localized regions where O3 has decreased since 1991. Specifically, we use measurements from the Halogen Occultation Experiment (HALOE) for the period 1991–2005 and the NASA/Aura Microwave Limb Sounder (MLS) for the period 2004–2013 to demonstrate a significant decrease in O3 near ~10 hPa in the tropics. O3 in this region is very sensitive to variations in NOy, and the observed decrease can be understood as a spatially localized, yet long term increase in NOy. In turn, using data from MLS and from the Atmospheric Chemistry Experiment (ACE), we show that the NOy variations are caused by decreases in N2O which are likely linked to long term variations in dynamics. To illustrate how variations in dynamics can affect N2O and O3, we show that by decreasing the upwelling in the tropics, more of the N2O can photodissociate with a concomitant increase in NOy production (via N2O+O(1D → 2 NO) at 10 hPa. Ultimately, this can cause an O3 decrease of the observed magnitude.


2009 ◽  
Vol 9 (16) ◽  
pp. 6055-6075 ◽  
Author(s):  
A. Jones ◽  
J. Urban ◽  
D. P. Murtagh ◽  
P. Eriksson ◽  
S. Brohede ◽  
...  

Abstract. The long term evolution of stratospheric ozone and water vapour has been investigated by extending satellite time series to April 2008. For ozone, we examine monthly average ozone values from various satellite data sets for nine latitude and altitude bins covering 60° S to 60° N and 20–45 km and covering the time period of 1979–2008. Data are from the Stratospheric Aerosol and Gas Experiment (SAGE I+II), the HALogen Occultation Experiment (HALOE), the Solar BackscatterUltraViolet-2 (SBUV/2) instrument, the Sub-Millimetre Radiometer (SMR), the Optical Spectrograph InfraRed Imager System (OSIRIS), and the SCanning Imaging Absorption spectroMeter for Atmospheric CHartograpY (SCIAMACHY). Monthly ozone anomalies are calculated by utilising a linear regression model, which also models the solar, quasi-biennial oscillation (QBO), and seasonal cycle contributions. Individual instrument ozone anomalies are combined producing an all instrument average. Assuming a turning point of 1997 and that the all instrument average is represented by good instrumental long term stability, the largest statistically significant ozone declines (at two sigma) from 1979–1997 are seen at the mid-latitudes between 35 and 45 km, namely −7.2%±0.9%/decade in the Northern Hemisphere and −7.1%±0.9%/in the Southern Hemisphere. Furthermore, for the period 1997 to 2008 we find that the same locations show the largest ozone recovery (+1.4% and +0.8%/decade respectively) compared to other global regions, although the estimated trend model errors indicate that the trend estimates are not significantly different from a zero trend at the 2 sigma level. An all instrument average is also constructed from water vapour anomalies during 1991–2008, using the SAGE II, HALOE, SMR, and the Microwave Limb Sounder (Aura/MLS) measurements. We report that the decrease in water vapour values after 2001 slows down around 2004–2005 in the lower tropical stratosphere (20–25 km) and has even shown signs of increasing until present. We show that a similar correlation is also seen with the temperature measured at 100 hPa during this same period.


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).


2013 ◽  
Vol 13 (9) ◽  
pp. 23491-23548 ◽  
Author(s):  
A. T. Brown ◽  
M. P. Chipperfield ◽  
S. Dhomse ◽  
C. Boone ◽  
P. F. Bernath

Abstract. We present chlorine budgets calculated between 2004 and 2009 for four latitude bands (70° N–30° N, 30° N–0° N, 0° N–30° S, and 30° S–70° S). The budgets were calculated using ACE-FTS version 3.0 retrievals of the volume mixing ratios (VMRs) of 9 chlorine-containing species: CCl4, CFC-12 (CCl2F2), CFC-11 (CCl3F), COCl2, COClF, HCFC-22 (CHF2Cl), CH3Cl, HCl and ClONO2. These data were supplemented with calculated VMRs from the SLIMCAT 3-D chemical transport model (CFC-113, CFC-114, CFC-115, H-1211, H-1301, HCFC-141b, HCFC-142b, ClO and HOCl). The total chlorine profiles are dominated by chlorofluorocarbons (CFCs) and halons up to 24 km in the tropics and 19 km in the extra-tropics. In this altitude range CFCs and halons account for 58% of the total chlorine VMR. Above this altitude HCl increasingly dominates the total chlorine profile, reaching a maximum of 95% of total chlorine at 54 km. All total chlorine profiles exhibit a positive slope with altitude, suggesting that the total chlorine VMR is now decreasing with time. This conclusion is supported by the time series of the mean stratospheric total chlorine budgets which show mean decreases in total stratospheric chlorine of 0.38 ± 0.03% per year in the Northern Hemisphere extra-tropics, 0.35 ± 0.07% per year in the Northern Hemisphere tropical stratosphere, 0.54 ± 0.16% per year in the Southern Hemisphere tropics and 0.53 ± 0.12% per year in the Southern Hemisphere extra-tropical stratosphere for 2004–2009. Globally stratospheric chlorine is decreasing by 0.46 ± 0.02% per year. Both global warming potential-weighted chlorine and ozone depletion potential-weighted chlorine are decreasing at all latitudes. These results show that the Montreal Protocol has had a significant effect in reducing emissions of both ozone-depleting substances and greenhouse gases.


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.


2019 ◽  
Author(s):  
David D. Parrish ◽  
Richard G. Derwent ◽  
Simon O'Doherty ◽  
Peter G. Simmonds

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.


2016 ◽  
Author(s):  
Andreas Ostler ◽  
Ralf Sussmann ◽  
Prabir K. Patra ◽  
Sander Houweling ◽  
Marko De Bruine ◽  
...  

Abstract. The distribution of methane (CH4) in the stratosphere can be a major driver of spatial variability in the dry-air column-averaged CH4 mixing ratio (XCH4), which is being measured increasingly for the assessment of CH4 surface emissions. Chemistry-transport models (CTMs) therefore need to simulate the tropospheric and stratospheric fractional columns of XCH4 accurately for estimating surface emissions from XCH4. Simulations from three CTMs are tested against XCH4 observations from the Total Carbon Column Network (TCCON). We analyze how the model-TCCON agreement in XCH4 depends on the model representation of stratospheric CH4 distributions. Model equivalents of TCCON XCH4 are computed with stratospheric CH4 fields from both the model simulations and from satellite-based CH4 distributions from MIPAS (Michelson Interferometer for Passive Atmospheric Sounding) and MIPAS CH4 fields adjusted to ACE-FTS (Atmospheric Chemistry Experiment Fourier Transform Spectrometer) observations. In comparison to simulated model fields we find an improved model-TCCON XCH4 agreement for all models with MIPAS-based stratospheric CH4 fields. For the Atmospheric Chemistry Transport Model (ACTM) the average XCH4 bias is significantly reduced from 38.1 ppb to 13.7 ppb, whereas small improvements are found for the models TM5 (Transport Model, version 5; from 8.7 ppb to 4.3 ppb), and LMDz (Laboratoire de Météorologie Dynamique model with Zooming capability; from 6.8 ppb to 4.3 ppb), respectively. MIPAS stratospheric CH4 fields adjusted to ACE-FTS reduce the average XCH4 bias for ACTM (3.3 ppb), but increase the average XCH4 bias for TM5 (10.8 ppb) and LMDz (20.0 ppb). These findings imply that the range of satellite-based stratospheric CH4 is insufficient to resolve a possible stratospheric contribution to differences in total column CH4 between TCCON and TM5 or LMDz. Applying transport diagnostics to the models indicates that model-to-model differences in the simulation of stratospheric transport, notably the age of stratospheric air, can largely explain the inter-model spread in stratospheric CH4 and, hence, its contribution to XCH4. This implies that there is a need to better understand the impact of individual model transport components (e.g., physical parameterization, meteorological data sets, model horizontal/vertical resolution) on modeled stratospheric CH4.


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