scholarly journals Transport of short-lived halocarbons to the stratosphere over the Pacific Ocean

2018 ◽  
Author(s):  
Michal T. Filus ◽  
Elliot L. Atlas ◽  
Maria A. Navarro ◽  
Elena Meneguz ◽  
David Thomson ◽  
...  

Abstract. The effectiveness of transport of short-lived halocarbons to the upper troposphere and lower stratosphere remains an important unknown in quantifying the supply of ozone-depleting substances to the stratosphere. In early 2014, a major field campaign in Guam in the West Pacific, involving UK and US research aircraft, sampled the tropical troposphere and lower stratosphere. The resulting measurements of CH3I, CHBr3 and CH2Br2 are compared here with calculations from a Lagrangian model. This methodology benefits from an updated convection scheme which improves simulation of the effect of deep convective motions on particle distribution within the tropical troposphere. We find that the observed CH3I, CHBr3 and CH2Br2 mixing ratios in the Tropical Tropopause Layer (TTL) are consistent with those in the boundary layer when the new convection scheme is used to account for convective transport. Particularly, comparisons between modelled estimates and observations of shortest-lived CH3I indicates that the NAME convection scheme is realistic up to the lower TTL but less good at reproducing the small number of extreme convective events in the upper TTL. This study consolidates our understanding of the transport of short-lived halocarbons to the upper troposphere and lower stratosphere by using improved model calculations to confirm consistency between observations in the boundary layer, observations in the TTL, and atmospheric transport processes. Our results support recent estimates of the contribution of short-lived bromocarbons to the stratospheric bromine budget.

2020 ◽  
Vol 20 (2) ◽  
pp. 1163-1181
Author(s):  
Michal T. Filus ◽  
Elliot L. Atlas ◽  
Maria A. Navarro ◽  
Elena Meneguz ◽  
David Thomson ◽  
...  

Abstract. The effectiveness of transport of short-lived halocarbons to the upper troposphere and lower stratosphere remains an important uncertainty in quantifying the supply of ozone-depleting substances to the stratosphere. In early 2014, a major field campaign in Guam in the western Pacific, involving UK and US research aircraft, sampled the tropical troposphere and lower stratosphere. The resulting measurements of CH3I, CHBr3 and CH2Br2 are compared here with calculations from a Lagrangian model. This methodology benefits from an updated convection scheme that improves simulation of the effect of deep convective motions on particle distribution within the tropical troposphere. We find that the observed CH3I, CHBr3 and CH2Br2 mixing ratios in the tropical tropopause layer (TTL) are consistent with those in the boundary layer when the new convection scheme is used to account for convective transport. More specifically, comparisons between modelled estimates and observations of short-lived CH3I indicate that the updated convection scheme is realistic up to the lower TTL but is less good at reproducing the small number of extreme convective events in the upper TTL. This study consolidates our understanding of the transport of short-lived halocarbons to the upper troposphere and lower stratosphere by using improved model calculations to confirm consistency between observations in the boundary layer, observations in the TTL and atmospheric transport processes. Our results support recent estimates of the contribution of short-lived bromocarbons to the stratospheric bromine budget.


2018 ◽  
Vol 18 (3) ◽  
pp. 1819-1833 ◽  
Author(s):  
Satoshi Sugawara ◽  
Shigeyuki Ishidoya ◽  
Shuji Aoki ◽  
Shinji Morimoto ◽  
Takakiyo Nakazawa ◽  
...  

Abstract. The gravitational separation of major atmospheric components, in addition to the age of air, would provide additional useful information about stratospheric circulation. However, observations of the age of air and gravitational separation are still geographically sparse, especially in the tropics. In order to address this issue, air samples were collected over Biak, Indonesia in February 2015 using four large plastic balloons, each loaded with two compact cryogenic samplers. With a vertical resolution of better than 2 km, air samples from seven different altitudes were analyzed for CO2 and SF6 mole fractions, δ15N of N2, δ18O of O2, and δ(Ar∕N2) to examine the vertically dependent age and gravitational separation of air in the tropical tropopause layer (TTL) and the equatorial stratosphere. By comparing their measured mole fractions with aircraft observations in the upper tropical troposphere, we have found that CO2 and SF6 ages increase gradually with increasing altitude from the TTL to 22 km, and then rapidly from there up to 29 km. The CO2 and SF6 ages agree well with each other in the TTL and in the lower stratosphere, but show a significant difference above 24 km. The average values of δ15N of N2, δ18O of O2, and δ(Ar∕N2) all show a small but distinct upward decrease due to the gravitational separation effect. Simulations with a two-dimensional atmospheric transport model indicate that the gravitational separation effect decreases as tropical upwelling is enhanced. From the model calculations with enhanced eddy mixing, it is also found that the upward increase in air age is magnified by horizontal mixing. These model simulations also show that the gravitational separation effect remains relatively constant in the lower stratosphere. The results of this study strongly suggest that the gravitational separation, combined with the age of air, can be used to diagnose air transport processes in the stratosphere.


2021 ◽  
Vol 13 (9) ◽  
pp. 1677
Author(s):  
Dmitry A. Belikov ◽  
Naoko Saitoh ◽  
Prabir K. Patra ◽  
Naveen Chandra

We examined methane (CH4) variability over different regions of India and the surrounding oceans derived from thermal infrared (TIR) band observations (TIR CH4) by the Thermal and Near-infrared Sensor for carbon Observation—Fourier Transform Spectrometer (TANSO-FTS) onboard the Greenhouse gases Observation SATellite (GOSAT) for the period 2009–2014. This study attempts to understand the sensitivity of the vertical profile retrievals at different layers of the troposphere and lower stratosphere, on the basis of the averaging kernel (AK) functions and a priori assumptions, as applied to the simulated concentrations by the MIROC4.0-based Atmospheric Chemistry-Transport Model (MIROC4-ACTM). We stress that this is of particular importance when the satellite-derived products are analyzed using different ACTMs other than those used as retrieved a priori. A comparison of modeled and retrieved CH4 vertical profiles shows that the GOSAT/TANSO-FTS TIR instrument has sufficient sensitivity to provide critical information about the transport of CH4 from the top of the boundary layer to the upper troposphere. The mean mismatch between TIR CH4 and model is within 50 ppb, except for the altitude range above 150 hPa, where the sensitivity of TIR CH4 observations becomes very low. Convolved model profiles with TIR CH4 AK reduces the mismatch to less than the retrieval uncertainty. Distinct seasonal variations of CH4 have been observed near the atmospheric boundary layer (800 hPa), free troposphere (500 hPa), and upper troposphere (300 hPa) over the northern and southern regions of India, corresponding to the southwest monsoon (July–September) and post-monsoon (October–December) seasons. Analysis of the transport and emission contributions to CH4 suggests that the CH4 seasonal cycle over the Indian subcontinent is governed by both the heterogeneous distributions of surface emissions and the influence of the global monsoon divergent wind circulations. The major contrast between monsoon, and pre- and post-monsoon profiles of CH4 over Indian regions are noticed near the boundary layer heights, which is mainly caused by seasonal change in local emission strength with a peak during summer due to increased emissions from the paddy fields and wetlands. A strong difference between seasons in the middle and upper troposphere is caused by convective transport of the emission signals from the surface and redistribution in the monsoon anticyclone of upper troposphere. TIR CH4 observations provide additional information on CH4 in the region compared to what is known from in situ data and total-column (XCH4) measurements. Based on two emission sensitivity simulations compared to TIR CH4 observations, we suggest that the emissions of CH4 from the India region were 51.2 ± 4.6 Tg year−1 during the period 2009–2014. Our results suggest that improvements in the a priori profile shape in the upper troposphere and lower stratosphere (UT/LS) region would help better interpretation of CH4 cycling in the earth’s environment.


2010 ◽  
Vol 10 (8) ◽  
pp. 20355-20404 ◽  
Author(s):  
C. R. Hoyle ◽  
V. Marécal ◽  
M. R. Russo ◽  
J. Arteta ◽  
C. Chemel ◽  
...  

Abstract. The tropical transport processes of 14 different models or model versions were compared, within the framework of the SCOUT-O3 (Stratospheric-Climate Links with Emphasis on the Upper Troposphere and Lower Stratosphere) project. The tested models range from the regional to the global scale, and include numerical weather prediction (NWP), chemistry transport, and climate chemistry models. Idealised tracers were used in order to prevent the model's chemistry schemes from influencing the results substantially, so that the effects of modelled transport could be isolated. We find large differences in the vertical transport of very short lived tracers (with a lifetime of 6 hours) within the tropical troposphere. Peak convective outflow altitudes range from around 300 hPa to almost 100 hPa among the different models, and the upper tropospheric tracer mixing ratios differ by up to an order of magnitude. The timing of convective events is found to differ between the models, even among those which source their forcing data from the same NWP model (ECMWF). The differences are less pronounced for longer lived tracers, however they could have implications for the modelling of the halogen burden of the lowermost stratosphere through species such as bromoform, or for the transport of short lived hydrocarbons into the lowermost stratosphere. The modelled tracer profiles are found to be strongly influenced by the convective transport parameterisations, and boundary layer mixing parameterisations of the models. The location of rapid transport into the upper troposphere is similar among the models, and is mostly concentrated over the western Pacific, the Maritime Continent and the Indian Ocean. In contrast, none of the models indicates significant enhancement in upward transport over western Africa. The mean mixing ratios of an idealised CO like tracer in the upper tropical troposphere are found to be sensitive to the surface CO mixing ratios in the regions with the most active convection, revealing the importance of correctly modelling both the location of convective transport and the geographical pollutant emission patterns.


2017 ◽  
Author(s):  
Satoshi Sugawara ◽  
Shigeyuki Ishidoya ◽  
Shuji Aoki ◽  
Shinji Morimoto ◽  
Takakiyo Nakazawa ◽  
...  

Abstract. Stratospheric air samples were collected over Biak, Indonesia in February 2015 using four large plastic balloons, each loaded with two compact cryogenic samplers. With a vertical resolution of better than 2 km, air samples from seven different altitudes were analyzed for CO2 and SF6 mole fractions, δ15N of N2, δ18O of O2, and δ(Ar/N2), to examine vertically dependent age and gravitational separation of air in the Tropical Tropopause Layer (TTL) and the equatorial stratosphere. By comparing their measured mole fractions with aircraft observation in the upper tropical troposphere, we have found that CO2 and SF6 age increases gradually with increasing altitude from the TTL to 22 km, and then rapidly from there up to 25 km. The CO2 and SF6 age agrees well with each other in the TTL and in the lower stratosphere, but shows a significant difference above 24 km. The average values of δ15N of N2, δ18O of O2, and δ(Ar/N2) all show small but distinct upward decrease due to the gravitational separation effect. Simulations with a two-dimensional atmospheric transport model indicate that the gravitational separation effect decreases as tropical upwelling is enhanced. From the model calculations with enhanced eddy mixing, it is also found that the upward increase in air age is magnified by horizontal mixing. These model simulations also show that the gravitational separation effect remains relatively constant in the lower stratosphere. The results of this study strongly suggest that the gravitational separation, combined with the age of air, can be used to diagnose air transport processes in the stratosphere.


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.


2015 ◽  
Vol 15 (11) ◽  
pp. 6467-6486 ◽  
Author(s):  
W. Frey ◽  
R. Schofield ◽  
P. Hoor ◽  
D. Kunkel ◽  
F. Ravegnani ◽  
...  

Abstract. In this study we examine the simulated downward transport and mixing of stratospheric air into the upper tropical troposphere as observed on a research flight during the SCOUT-O3 campaign in connection with a deep convective system. We use the Advanced Research Weather and Research Forecasting (WRF-ARW) model with a horizontal resolution of 333 m to examine this downward transport. The simulation reproduces the deep convective system, its timing and overshooting altitudes reasonably well compared to radar and aircraft observations. Passive tracers initialised at pre-storm times indicate the downward transport of air from the stratosphere to the upper troposphere as well as upward transport from the boundary layer into the cloud anvils and overshooting tops. For example, a passive ozone tracer (i.e. a tracer not undergoing chemical processing) shows an enhancement in the upper troposphere of up to about 30 ppbv locally in the cloud, while the in situ measurements show an increase of 50 ppbv. However, the passive carbon monoxide tracer exhibits an increase, while the observations show a decrease of about 10 ppbv, indicative of an erroneous model representation of the transport processes in the tropical tropopause layer. Furthermore, it could point to insufficient entrainment and detrainment in the model. The simulation shows a general moistening of air in the lower stratosphere, but it also exhibits local dehydration features. Here we use the model to explain the processes causing the transport and also expose areas of inconsistencies between the model and observations.


2009 ◽  
Vol 137 (8) ◽  
pp. 2493-2514 ◽  
Author(s):  
Charles Chemel ◽  
Maria R. Russo ◽  
John A. Pyle ◽  
Ranjeet S. Sokhi ◽  
Cornelius Schiller

Abstract The development of a severe Hector thunderstorm that formed over the Tiwi Islands, north of Australia, during the Aerosol and Chemical Transport in Tropical Convection/Stratospheric-Climate Links with Emphasis on the Upper Troposphere and Lower Stratosphere (ACTIVE/SCOUT-O3) field campaign in late 2005, is simulated by the Advanced Research Weather Research and Forecasting (ARW) model and the Met Office Unified Model (UM). The general aim of this paper is to investigate the role of isolated deep convection over the tropics in regulating the water content in the upper troposphere/lower stratosphere (UT/LS). Using a horizontal resolution as fine as 1 km, the numerical simulations reproduce the timing, structure, and strength of Hector fairly well when compared with field campaign observations. The sensitivity of results from ARW to horizontal resolution is investigated by running the model in a large-eddy simulation mode with a horizontal resolution of 250 m. While refining the horizontal resolution to 250 m leads to a better representation of convection with respect to rainfall, the characteristics of the Hector thunderstorm are basically similar in space and time to those obtained in the 1-km-horizontal-resolution simulations. Several overshooting updrafts penetrating the tropopause are produced in the simulations during the mature stage of Hector. The penetration of rising towering cumulus clouds into the LS maintains the entrainment of air at the interface between the UT and the LS. Vertical exchanges resulting from this entrainment process have a significant impact on the redistribution of atmospheric constituents within the UT/LS region at the scale of the islands. In particular, a large amount of water is injected in the LS. The fate of the ice particles as Hector develops drives the water vapor mixing ratio to saturation by sublimation of the injected ice particles, moistening the air in the LS. The moistening was found to be fairly significant above 380 K and averaged about 0.06 ppmv in the range 380–420 K for ARW. As for UM, the moistening was found to be much larger (about 2.24 ppmv in the range of 380–420 K) than for ARW. This result confirms that convective transport can play an important role in regulating the water vapor mixing ratio in the LS.


2017 ◽  
Author(s):  
Martine Collaud Coen ◽  
Elisabeth Andrews ◽  
Diego Aliaga ◽  
Marcos Andrade ◽  
Hristo Angelov ◽  
...  

Abstract. High altitude stations are often emphasized as free tropospheric measuring sites but they remain influenced by atmospheric boundary layer (ABL) air masses due to convective transport processes. The local and meso-scale topographical features around the station are involved in the convective boundary layer development and in the formation of thermally induced winds leading to ABL air lifting. The station altitude is not a sufficient parameter to characterize the ABL influence. Topography data from the global digital elevation model GTopo30 were used to calculate 5 parameters for 46 high altitude stations situated in five continents. The geometric mean of these 5 parameters determines a topography based index called ABL-TopoIndex which can be used to rank the high altitude stations as a function of the ABL influence. To construct the ABL-TopoIndex, we rely on the criteria that the ABL influence will be low if the station is one of the highest points in the mountainous massif, if there is a large altitude difference between the station and the valleys or plateaus, if the slopes around the station are steep, and finally if the drainage basin for air convection is small. All stations on volcanic islands exhibit a low ABL-TopoIndex whereas stations in the Himalaya and the Tibetan Plateau have high ABL-TopoIndex values. Spearman's rank correlation between aerosol optical properties and number concentration from 28 stations and the ABL-TopoIndex, the altitude and the latitude are used to validate this topographical approach. Statistically significant (s.s.) correlations are found between the 5 and 50 percentiles of all aerosol parameters and the ABL-TopoIndex whereas no s.s. correlation is found with the station altitude. The diurnal cycles of aerosol parameters seem to be best explained by the station latitude although a s.s. correlation is found between the amplitude of the diurnal cycles of the absorption coefficient and the ABL-TopoIndex. Finally, the main flow paths for air convection were calculated for various ABL heights.


2018 ◽  
Author(s):  
Paul Konopka ◽  
Mengchu Tao ◽  
Felix Ploeger ◽  
Mohamadou Diallo ◽  
Martin Riese

Abstract. Inaccurate representation of mixing in chemistry transport model, mainly suffering from an excessive numerical diffusion, strongly influences the quantitative estimates of the stratosphere-troposphere exchange (STE). The Lagrangian view of transport offers an alternative to exploit the numerical diffusion for parametrization of the physical mixing. Here, we follow this concept and discuss how to extend the representation of tropospheric transport in the Chemical Lagrangian Model of the Stratosphere (CLaMS). Although the current transport scheme in CLaMS shows good ability of representing transport of tracers in the stably stratified stratosphere (Pommrich et al., (2014) and the references therein), there are deficiencies in representation of the effects of convective uplift and mixing due to weak vertical stability in the troposphere. We show how the CLaMS transport scheme was modified by including additional tropospheric mixing and vertical transport due to unresolved convection by parametrizing these processes in terms of the dry and moist Brunt-Vaisala frequency, respectively. The regions with enhanced vertical transport in the novel CLaMS simulation covering the 2005-08 period coincide with regions of enhanced convection as diagnosed from the satellite observations of the Outgoing Longwave Radiation (OLR). We analyze how well this approach improves the CLaMS representation of CO2 in the upper troposphere and lower stratosphere, in particular the propagation of the CO2 seasonal cycle from the Planetary Boundary Layer (PBL) into the lower stratosphere. The CO2 values in the PBL are specified by the CarbonTracker data set (version CT2013B) and the Comprehensive Observation Network for TRace gases by AIrLiner (CONTRAIL) observations are used to validate the model. The proposed extension of tropospheric transport increases the tropospheric influence in the middle and upper troposphere and at the same time influences the STE. The effect on mean age away from the troposphere in the deep stratosphere is weak.


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