scholarly journals Midlatitude stratosphere – troposphere exchange as diagnosed by MLS O<sub>3</sub> and MOPITT CO assimilated fields

2009 ◽  
Vol 9 (5) ◽  
pp. 20677-20720
Author(s):  
L. El Amraoui ◽  
J.-L. Attié ◽  
N. Semane ◽  
M. Claeyman ◽  
V.-H. Peuch ◽  
...  

Abstract. This paper presents a complete characterization of a very deep stratospheric intrusion which occurred over the British Isles on 15 August 2007. The signature of this event is diagnosed using ozonesonde measurements over Lerwick, UK (60.14° N, 1.19° W) and is also well characterized using meteorological analyses from the global operational weather prediction model of Météo-France, ARPEGE. Modelled as well as assimilated fields of both ozone (O3) and carbon monoxide (CO) have been used in order to better document this event. The paper also presents a demonstration of the capability of O3 and CO assimilated fields to better describe a stratosphere-troposphere exchange (STE) event in comparison with the free run modelled O3 and CO fields. O3 and CO from Aura/MLS and Terra/MOPITT instruments, respectively, are assimilated into the three-dimensional chemical transport model MOCAGE of Météo-France using a variational 3-D-FGAT (First Guess at Appropriate Time) method within the MOCAGE-PALM assimilation system. The usefulness of assimilated MOPITT CO data in a STE study is demonstrated in this novel result. The study shows that the use of the model MOCAGE gives consistent 3-D fields capable of describing the synoptic evolution of the event. However, modelled O3 and CO vertical distributions do not provide a quantitative evaluation of the intrusion. Although the assimilation of MLS data improves the distribution of O3 above the tropopause compared to the free model run, it is not sufficient to reproduce the stratospheric intrusion event well. Conversely, assimilated MOPITT CO allows a better description of the stratospheric intrusion event. Indeed, the horizontal distribution of the CO assimilated field is consistent with meteorological analyses. Moreover, the vertical distribution of the CO assimilated field is in accordance with the potential vorticity distribution and reveals a deeper intrusion from the lower stratosphere downward to the mid-troposphere compared to the O3 assimilated field. This study clearly demonstrates the capability of the assimilation of MOPITT CO to improve the CO distribution in the upper troposphere and lower stratosphere region. In addition, the behaviour of CO assimilated field is consistent with the synoptic evolution of the meteorological conditions. Therefore, the results of this study open the perspectives for using MOPITT CO in the STE studies.

2010 ◽  
Vol 10 (5) ◽  
pp. 2175-2194 ◽  
Author(s):  
L. El Amraoui ◽  
J.-L. Attié ◽  
N. Semane ◽  
M. Claeyman ◽  
V.-H. Peuch ◽  
...  

Abstract. This paper presents a comprehensive characterization of a very deep stratospheric intrusion which occurred over the British Isles on 15 August 2007. The signature of this event is diagnosed using ozonesonde measurements over Lerwick, UK (60.14° N, 1.19° W) and is also well characterized using meteorological analyses from the global operational weather prediction model of Météo-France, ARPEGE. Modelled as well as assimilated fields of both ozone (O3) and carbon monoxide (CO) have been used in order to better document this event. O3 and CO from Aura/MLS and Terra/MOPITT instruments, respectively, are assimilated into the three-dimensional chemical transport model MOCAGE of Météo-France using a variational 3-D-FGAT (First Guess at Appropriate Time) method. The validation of O3 and CO assimilated fields is done using self-consistency diagnostics and by comparison with independent observations such as MOZAIC (O3 and CO), AIRS (CO) and OMI (O3). It particularly shows in the upper troposphere and lower stratosphere region that the assimilated fields are closer to MOZAIC than the free model run. The O3 bias between MOZAIC and the analyses is −11.5 ppbv with a RMS of 22.4 ppbv and a correlation coefficient of 0.93, whereas between MOZAIC and the free model run, the corresponding values are 33 ppbv, 38.5 ppbv and 0.83, respectively. In the same way, for CO, the bias, RMS and correlation coefficient between MOZAIC and the analyses are −3.16 ppbv, 13 ppbv and 0.79, respectively, whereas between MOZAIC and the free model they are 6.3 ppbv, 16.6 ppbv and 0.71, respectively. The paper also presents a demonstration of the capability of O3 and CO assimilated fields to better describe a stratosphere-troposphere exchange (STE) event in comparison with the free run modelled O3 and CO fields. Although the assimilation of MLS data improves the distribution of O3 above the tropopause compared to the free model run, it is not sufficient to reproduce the STE event well. Assimilated MOPITT CO allows a better qualitative description of the stratospheric intrusion event. The MOPITT CO analyses appear more promising than the MLS O3 analyses in terms of their ability to capture a deep STE event. Therefore, the results of this study open the perspectives for using MOPITT CO in the STE studies.


2009 ◽  
Vol 9 (5) ◽  
pp. 18511-18543 ◽  
Author(s):  
J. Aschmann ◽  
B. M. Sinnhuber ◽  
E. L. Atlas ◽  
S. M. Schauffler

Abstract. The transport of very short-lived substances into the tropical upper troposphere and lower stratosphere is investigated by a three-dimensional chemical transport model using archived convective updraft mass fluxes (or detrainment rates) from the European Centre for Medium-Range Weather Forecast's ERA-Interim reanalysis. Large-scale vertical velocities are calculated from diabatic heating rates. With this approach we explicitly model the large scale subsidence in the tropical troposphere with convection taking place in fast and isolated updraft events. The model calculations agree generally well with observations of bromoform and methyl iodide from aircraft campaigns and with ozone and water vapor from sonde and satellite observations. Using a simplified treatment of dehydration and bromine product gas washout we give a range of 1.6 to 3 ppt for the contribution of bromoform to stratospheric bromine, assuming a uniform source in the boundary layer of 1 ppt. We show that the most effective region for VSLS transport into the stratosphere is the West Pacific, accounting for about 55% of the bromine from bromoform transported into the stratosphere under the supposition of a uniformly distributed source.


2003 ◽  
Vol 3 (1) ◽  
pp. 1081-1107 ◽  
Author(s):  
M. P. Chipperfield

Abstract. We have used a 3D off-line chemical transport model (CTM) to study the causes of the observed changes in ozone in the mid-high latitude lower stratosphere from 1979–1998. The model was forced by European Centre for Medium Range Weather Forecasts (ECMWF) analyses and contains a detailed chemistry scheme. A series of model runs were performed at a horizontal resolution of 7.5°×7.5° and covered the domain from about 12 km to 30 km. The basic model performs well in reproducing the decadal evolution of the springtime depletion in the northern hemisphere (NH) and southern hemisphere (SH) high latitudes in the 1980s and early 1990s. After about 1994 the modelled interannual variability does not match the observations as well, which is probably due in part to changes in the operational ECMWF analyses – which places limits on using this dataset to diagnose dynamical trends. For mid-latitudes (35°–60°) the basic model reproduces the observed column ozone decreases from 1980 until the early 1990s. Model experiments show that the halogen trends appear to dominate this modelled decrease and of this around 30–50% is due to high-latitude processing on polar stratospheric clouds (PSCs). Dynamically induced ozone variations in the model correlate with observations over the timescale of a few years. Large discrepancies between the modelled and observed variations in the mid 1980s and mid 1990s can be largely resolved by assuming that the 11-year solar cycle (not explicitly included in the 3D model) causes a 2% (min-max) change in mid-latitude column ozone.


2018 ◽  
Vol 18 (2) ◽  
pp. 833-844 ◽  
Author(s):  
Sakae Toyoda ◽  
Naohiro Yoshida ◽  
Shinji Morimoto ◽  
Shuji Aoki ◽  
Takakiyo Nakazawa ◽  
...  

Abstract. Vertical profiles of nitrous oxide (N2O) and its isotopocules, isotopically substituted molecules, were obtained over the Equator at altitudes of 16–30 km. Whole air samples were collected using newly developed balloon-borne compact cryogenic samplers over the eastern equatorial Pacific in 2012 and Biak Island, Indonesia, in 2015. They were examined in the laboratory using gas chromatography and mass spectrometry. The mixing ratio and isotopocule ratios of N2O in the equatorial stratosphere showed a weaker vertical gradient than the previously reported profiles in the subtropical and mid-latitude and high-latitude stratosphere. From the relation between the mixing ratio and isotopocule ratios, further distinct characteristics were found over the Equator: (1) observed isotopocule fractionations (ε values) in the middle stratosphere (25–30 km or [N2O] < ca. 260 nmol mol−1) are almost equal to ε values reported from broadband photolysis experiments conducted in the laboratory; (2) ε values in the lower stratosphere (< ca. 25 km or [N2O] > ca. 260 nmol mol−1) are about half of the experimentally obtained values, being slightly larger than those observed in the mid-latitude and high-latitude lower stratosphere ([N2O] > ca. 170 nmol mol−1). These results from the deep tropics suggest the following. (i) The timescale for quasi-horizontal mixing between tropical and mid-latitude air in the tropical middle stratosphere is sufficiently slow relative to the tropical upwelling rate that isotope fractionation approaches the Rayleigh limit for N2O photolysis. (ii) The air in the tropical lower stratosphere is exchanged with extratropical air on a timescale that is shorter than that of photochemical decomposition of N2O. Previously observed ε values, which are invariably smaller than those of photolysis, can be explained qualitatively using a three-dimensional chemical transport model and using a simple model that assumes mixing of “aged” tropical air and extratropical air during residual circulation. Results show that isotopocule ratios are useful to examine the stratospheric transport scheme deduced from tracer–tracer relations.


2018 ◽  
Author(s):  
Dmitry Belikov ◽  
Satoshi Sugawara ◽  
Shigeyuki Ishidoya ◽  
Fumio Hasebe ◽  
Shamil Maksyutov ◽  
...  

Abstract. A three-dimensional simulation of gravitational separation, defined as the process of atmospheric molecule separation under gravity according to their molar masses, is performed for the first time in the upper troposphere and lower stratosphere. We analyze distributions of two isotopes with a small difference in molecular mass (13C16O2 (Mi = 45) and 12C16O2 (Mi = 44)) simulated by the National Institute for Environmental Studies (NIES) chemical transport model with a parameterization of molecular diffusion. The NIES model employs global reanalysis and an isentropic vertical coordinate and uses optimized CO2 fluxes. This study includes a comparison with measurements recorded by cryogenic balloon-borne samplers in the lower stratosphere and two-dimensional model simulations. The benefits of the NIES TM simulations are discussed. We investigate the processes affecting gravitational separation by a detailed estimation of terms in the molecular diffusion equation. At the same time, we study the age of air derived from the tracer distributions. We find a strong relationship between age of air and gravitational separation for the main climatic zones. The advantages and limitations of using age of air and gravitational separation as indicators of the variability in the stratosphere circulation are discussed.


2012 ◽  
Vol 5 (2) ◽  
pp. 1561-1626 ◽  
Author(s):  
O. A. Søvde ◽  
M. J. Prather ◽  
I. S. A. Isaksen ◽  
T. K. Berntsen ◽  
F. Stordal ◽  
...  

Abstract. We present here the global chemical transport model Oslo CTM3, an update of the Oslo CTM2. The update comprises a faster transport scheme, an improved wet scavenging scheme for large scale rain, updated photolysis rates and a new lightning parameterization. Oslo CTM3 is better parallelized and allows for stable, large time steps for advection, enabling more complex or high resolution simulations. Thorough comparisons between the Oslo CTM3, Oslo CTM2 and measurements are performed, and in general the Oslo CTM3 is found to reproduce measurements well. Inclusion of tropospheric sulfur chemistry and nitrate aerosols in CTM3 is shown to be important to reproduce tropospheric O3, OH and the CH4 lifetime well. Using the same meteorology to drive the two models, shows that some features related to transport are better resolved by the CTM3, such as polar cap transport, while features like transport close to the vortex edge are resolved better in the Oslo CTM2 due to its required shorter transport time step. The longer transport time steps in CTM3 result in larger errors e.g. near the jets, and when necessary, this can be remedied by using a shorter time step. An additional, more accurate and time consuming, treatment of polar cap transport is presented, however, both perform acceptably. A new treatment of the horizontal distribution of lightning is presented and found to compare well with measurements. Vertical distributions of lighting are updated, and tested against the old vertical distribution. The new profiles are found to produce more NOx in the tropical middle troposphere, and less at the surface and at high altitudes.


2019 ◽  
Vol 19 (8) ◽  
pp. 5349-5361 ◽  
Author(s):  
Dmitry Belikov ◽  
Satoshi Sugawara ◽  
Shigeyuki Ishidoya ◽  
Fumio Hasebe ◽  
Shamil Maksyutov ◽  
...  

Abstract. A three-dimensional simulation of gravitational separation, defined as the process of atmospheric molecule separation under gravity according to their molar masses, is performed for the first time in the upper troposphere and lower stratosphere. We analyze distributions of two isotopes with a small difference in molecular mass (13C16O2 (Mi=45) and 12C16O2 (Mi=44)) simulated by the National Institute for Environmental Studies (NIES) chemical transport model (TM) with a parameterization of molecular diffusion. The NIES model employs global reanalysis and an isentropic vertical coordinate and uses optimized CO2 fluxes. The applicability of the NIES TM to the modeling of gravitational separation is demonstrated by a comparison with measurements recorded by high-precision cryogenic balloon-borne samplers in the lower stratosphere. We investigate the processes affecting the seasonality of gravitational separation and examine the age of air derived from the tracer distributions modeled by the NIES TM. We find a strong relationship between age of air and gravitational separation for the main climatic zones. The advantages and limitations of using age of air and gravitational separation as indicators of the variability in the stratosphere circulation are discussed.


2003 ◽  
Vol 3 (4) ◽  
pp. 1253-1265 ◽  
Author(s):  
M. P. Chipperfield

Abstract. We have used a 3D off-line chemical transport model (CTM) to study the causes of the observed changes in ozone in the mid-high latitude lower stratosphere from 1979-1998. The model was forced by European Centre for Medium Range Weather Forecasts (ECMWF) analyses and contains a detailed chemistry scheme. A series of model runs were performed at a horizontal resolution of 7.5°x7.5° and covered the domain from about 12 km to 30 km. The basic model performs well in reproducing the decadal evolution of the springtime depletion of ozone in the northern hemisphere (NH) and southern hemisphere (SH) high latitudes in the 1980s and early 1990s. After about 1994 the modelled interannual variability does not match the observations as well, which is probably due in part to changes in the operational ECMWF analyses - which places limits on using this dataset to diagnose dynamical trends. For mid-latitudes (35°-60°) the basic model reproduces the observed column ozone decreases from 1980 until the early 1990s. Model experiments show that the halogen trends appear to dominate this modelled decrease and of this around 30-50% is due to high-latitude processing on polar stratospheric clouds (PSCs). Dynamically induced ozone variations in the model correlate with observations over the timescale of a few years. Large discrepancies between the modelled and observed variations in the mid 1980s and mid 1990s can be largely resolved by assuming that the 11-year solar cycle (not explicitly included in the 3D model) causes a 2% (min-max) change in mid-latitude column ozone.


2011 ◽  
Vol 11 (1) ◽  
pp. 121-162 ◽  
Author(s):  
J. Aschmann ◽  
B.-M. Sinnhuber ◽  
M. P. Chipperfield ◽  
R. Hossaini

Abstract. Stratospheric bromine loading due to very short-lived substances is investigated with a three-dimensional chemical transport model over a period of 21 years using meteorological input data from the European Centre for Medium-Range Weather Forecasts ERA-Interim reanalysis from 1989 to the end of 2009. Within this framework we analyze the impact of dehydration and deep convection on the amount of stratospheric bromine using an idealized and a detailed full chemistry approach. We model the two most important brominated short-lived substances, bromoform (CHBr3) and dibromomethane (CH2Br2), assuming a uniform detrainment mixing ratio of 1 part per trillion by volume (pptv) for both species. The contribution of very short-lived substances to stratospheric bromine varies drastically with the applied dehydration mechanism and the associated scavenging of soluble species ranging from 3.4 pptv in the idealized setup up to 5 pptv using the full chemistry scheme. In the latter case virtually the entire amount of bromine originating from very short-lived source gases is able to reach the stratosphere thus rendering the impact of dehydration and scavenging on inorganic bromine in the tropopause insignificant. Furthermore, our long-term calculations show that the mixing ratios of very short-lived substances are strongly correlated to convective activity, i.e. intensified convection leads to higher amounts of very short-lived substances in the upper troposphere/lower stratosphere especially under extreme conditions like El Niño seasons. However, this does not apply to the inorganic brominated product gases whose concentrations are anti-correlated to convective activity mainly due to convective dilution and possible scavenging, depending on the applied approach.


2011 ◽  
Vol 11 (6) ◽  
pp. 2671-2687 ◽  
Author(s):  
J. Aschmann ◽  
B.-M. Sinnhuber ◽  
M. P. Chipperfield ◽  
R. Hossaini

Abstract. Stratospheric bromine loading due to very short-lived substances is investigated with a three-dimensional chemical transport model over a period of 21 years using meteorological input data from the European Centre for Medium-Range Weather Forecasts ERA-Interim reanalysis from 1989 to the end of 2009. Within this framework we analyze the impact of dehydration and deep convection on the amount of stratospheric bromine using an idealized and a detailed full chemistry approach. We model the two most important brominated short-lived substances, bromoform (CHBr3) and dibromomethane (CH2Br2), assuming a uniform convective detrainment mixing ratio of 1 part per trillion by volume (pptv) for both species. The contribution of very short-lived substances to stratospheric bromine varies drastically with the applied dehydration mechanism and the associated scavenging of soluble species ranging from 3.4 pptv in the idealized setup up to 5 pptv using the full chemistry scheme. In the latter case virtually the entire amount of bromine originating from very short-lived source gases is able to reach the stratosphere thus rendering the impact of dehydration and scavenging on inorganic bromine in the tropopause insignificant. Furthermore, our long-term calculations show that the mixing ratios of very short-lived substances are strongly correlated to convective activity, i.e. intensified convection leads to higher amounts of very short-lived substances in the upper troposphere/lower stratosphere especially under extreme conditions like El Niño seasons. However, this does not apply to the inorganic brominated product gases whose concentrations are anti-correlated to convective activity mainly due to convective dilution and possible scavenging, depending on the applied approach.


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