Global age of air spectrum from the earth surface to the upper troposphere and tropopause: a model study

Author(s):  
Aurelien Podglajen ◽  
Edward Charlesworth ◽  
Felix Ploeger

<p>Transport of air masses from the surface into the atmosphere occurs via a variety of processes (including clear-air turbulence, atmospheric convection and large-scale circulations), which entails a multitude of transport time scales. This complexity can be characterized in an atmospheric transport model by calculating the age of air spectrum (transit time distribution from the surface). Up to now, mainly the slow time scales of stratospheric and interhemispheric transport (>10 days) have thus been studied. Vertical transport through the troposphere, for which convection is the major player, has only been evaluated using a handful of measured compounds (Radon, CO2 and SF6). However, a wealth of chemically relevant species are affected by the detailed structure of the age spectrum. Recent work (Luo et al., 2018) have used this sensitivity in order to gain observational insights into the tropospheric age spectrum, calling for a comparison with models.</p><p>To that end, we derive upper tropospheric and tropopause age spectra in the EMAC (ECHAM/MESSy Atmospheric Chemistry) model using the Boundary Impulse Response (BIR) method. Because of the large range of time scales involved in tropospheric transport, which extend from tens of minutes (convective transport) to years (stratospheric intrusions), we rely on a suite of pulses with variable durations providing hourly resolution for short time scales (< 12 hours) and monthly for long ones (> 1 month). We first describe the age spectra obtained and their diurnal and seasonal variability. Then, we examine the transport properties from a few specific surface regions to the upper troposphere and stratosphere, with an emphasis on fast pathways from the tropical Western Pacific and on interhemispheric transport. Finally, we investigate the sensitivity of different transport pathways to changes in some of the available model parameterizations (convection) and to different set-ups (using nudging or not).</p>

2008 ◽  
Vol 8 (12) ◽  
pp. 3231-3246 ◽  
Author(s):  
B. Barret ◽  
P. Ricaud ◽  
C. Mari ◽  
J.-L. Attié ◽  
N. Bousserez ◽  
...  

Abstract. The transport pathways of carbon monoxide (CO) in the African Upper Troposphere (UT) during the West African Monsoon (WAM) is investigated through the assimilation of CO observations by the Aura Microwave Limb Sounder (MLS) in the MOCAGE Chemistry Transport Model (CTM). The assimilation setup, based on a 3-D First Guess at Assimilation Time (3-D-FGAT) variational method is described. Comparisons between the assimilated CO fields and in situ airborne observations from the MOZAIC program between Europe and both Southern Africa and Southeast Asia show an overall good agreement around the lowermost pressure level sampled by MLS (~215 hPa). The 4-D assimilated fields averaged over the month of July 2006 have been used to determine the main dynamical processes responsible for the transport of CO in the African UT. The studied period corresponds to the second AMMA (African Monsoon Multidisciplinary Analyses) aircraft campaign. At 220 hPa, the CO distribution is characterized by a latitudinal maximum around 5° N mostly driven by convective uplift of air masses impacted by biomass burning from Southern Africa, uplifted within the WAM region and vented predominantly southward by the upper branch of the winter hemisphere Hadley cell. Above 150 hPa, the African CO distribution is characterized by a broad maximum over northern Africa. This maximum is mostly controlled by the large scale UT circulation driven by the Asian Summer Monsoon (ASM) and characterized by the Asian Monsoon Anticyclone (AMA) centered at 30° N and the Tropical Easterly Jet (TEJ) on the southern flank of the anticyclone. Asian pollution uplifted to the UT over large region of Southeast Asia is trapped within the AMA and transported by the anticyclonic circulation over Northeast Africa. South of the AMA, the TEJ is responsible for the tranport of CO-enriched air masses from India and Southeast Asia over Africa. Using the high time resolution provided by the 4-D assimilated fields, we give evidence that the variability of the African CO distribution above 150 hPa and north of the WAM region is mainly driven by the synoptic dynamical variability of both the AMA and the TEJ.


2008 ◽  
Vol 8 (1) ◽  
pp. 2863-2902 ◽  
Author(s):  
B. Barret ◽  
P. Ricaud ◽  
C. Mari ◽  
J.-L. Attié ◽  
N. Bousserez ◽  
...  

Abstract. The transport pathways of carbon monoxide (CO) in the African Upper Troposphere (UT) during the West African Monsoon (WAM) is investigated through the assimilation of CO observations by the Aura Microwave Limb Sounder (MLS) in the MOCAGE Chemistry Transport Model (CTM). The assimilation setup, based on a 3-D First Guess at Assimilation Time (3-D-FGAT) variational method is described. Comparisons between the assimilated CO fields and in situ airborne observations from the MOZAIC program between Europe and both Southern Africa and Southeast Asia show an overall good agreement around the lowermost pressure level sampled by MLS (~215 hPa). The 4-D assimilated fields averaged over the month of July 2006 have been used to determine the main dynamical processes responsible for the transport of CO in the African UT. The studied period corresponds to the second AMMA (African Monsoon Multidisciplinary Analyses) aircraft campaign. At 220 hPa, the CO distribution is characterized by a latitudinal maximum around 5° N mostly driven by convective uplift of air masses impacted by biomass burning from Southern Africa, uplifted within the WAM region and vented predominantly southward by the upper branch of the winter hemisphere Hadley cell. Above 150 hPa, the African CO distribution is characterized by a broad maximum over northern Africa. This maximum is mostly controlled by the large scale UT circulation driven by the Asian Summer Monsoon (ASM) and characterized by the Asian Monsoon Anticyclone (AMA) centered at 30° N and the Tropical Easterly Jet (TEJ) on the southern flank of the anticyclone. Asian pollution uplifted to the UT over large region of Southeast Asia is trapped within the AMA and transported by the anticyclonic circulation over Northeast Africa. South of the AMA, the TEJ is responsible for the tranport of CO-enriched air masses from India and Southeast Asia over Africa. Using the high time resolution provided by the 4-D assimilated fields, we give evidence that the variability of the African CO distribution above 150 hPa and north of the WAM region is mainly driven by the synoptic dynamical variability of both the AMA and the TEJ.


2009 ◽  
Vol 9 (3) ◽  
pp. 10883-10912 ◽  
Author(s):  
Q. Li ◽  
P. I. Palmer ◽  
H. C. Pumphrey ◽  
P. Bernath ◽  
E. Mahieu

Abstract. We use the GEOS-Chem global 3-D chemistry transport model to investigate the relative importance of chemical and physical processes that determine observed variability of hydrogen cyanide (HCN) in the troposphere and lower stratosphere. Consequently, we reconcile ground-based FTIR column measurements of HCN, which show annual and semi-annual variations, with recent space-borne measurements of HCN mixing ratio in the tropical lower stratosphere, which show a large two-year variation. We find that the observed column variability over the ground-based stations is determined by a superposition of HCN from several regional burning sources, with GEOS-Chem reproducing these column data with a positive bias of 5%. GEOS-Chem reproduces the observed tropical HCN variability from the Microwave Limb Sounder and the Atmospheric Chemistry Experiment satellite instruments with a negative bias of 7%. We show the tropical biomass burning emissions explain mostly the observed HCN variations in the upper troposphere and lower stratosphere (UTLS), with the remainder due to atmospheric transport and HCN chemistry. In the mid and upper stratosphere, atmospheric dynamics progressively exerts more influences on HCN variations. The extent of temporal overlap between African and other continental burning seasons is key in establishing the apparent bienniel cycle in the UTLS. Similar analysis of other, shorter-lived trace gases have not observed the transition between annual and bienniel cycles in the UTLS probably because the signal of inter-annual variations from surface emission has vanished before arriving at the lower stratosphere (LS), due to shorter atmospheric lifetimes.


2008 ◽  
Vol 8 (20) ◽  
pp. 6037-6050 ◽  
Author(s):  
M. G. Lawrence ◽  
M. Salzmann

Abstract. Global chemistry-transport models (CTMs) and chemistry-GCMs (CGCMs) generally simulate vertical tracer transport by deep convection separately from the advective transport by the mean winds, even though a component of the mean transport, for instance in the Hadley and Walker cells, occurs in deep convective updrafts. This split treatment of vertical transport has various implications for CTM simulations. In particular, it has led to a misinterpretation of several sensitivity simulations in previous studies in which the parameterized convective transport of one or more tracers is neglected. We describe this issue in terms of simulated fluxes and fractions of these fluxes representing various physical and non-physical processes. We then show that there is a significant overlap between the convective and large-scale mean advective vertical air mass fluxes in the CTM MATCH, and discuss the implications which this has for interpreting previous and future sensitivity simulations, as well as briefly noting other related implications such as numerical diffusion.


2017 ◽  
Vol 56 (7) ◽  
pp. 2035-2052 ◽  
Author(s):  
Thomas Garot ◽  
Hélène Brogniez ◽  
Renaud Fallourd ◽  
Nicolas Viltard

AbstractThe spatial and temporal distribution of upper-tropospheric humidity (UTH) observed by the Sounder for Atmospheric Profiling of Humidity in the Intertropics by Radiometry (SAPHIR)/Megha-Tropiques radiometer is analyzed over two subregions of the Indian Ocean during October–December over 2011–14. The properties of the distribution of UTH were studied with regard to the phase of the Madden–Julian oscillation (active or suppressed) and large-scale advection versus local production of moisture. To address these topics, first, a Lagrangian back-trajectory transport model was used to assess the role of the large-scale transport of air masses in the intraseasonal variability of UTH. Second, the temporal evolution of the distribution of UTH is analyzed using the computation of the higher moments of its probability distribution function (PDF) defined for each time step over the domain. The results highlight significant differences in the PDF of UTH depending on the phase of the MJO. The modeled trajectories ending in the considered domain originate from an area that strongly varies depending on the phases of the MJO: during the active phases, the air masses are spatially constrained within the tropical Indian Ocean domain, whereas a distinct upper-tropospheric (200–150 hPa) westerly flow guides the intraseasonal variability of UTH during the suppressed phases. Statistical relationships between the cloud fractions and the UTH PDF moments of are found to be very similar regardless of the convective activity. However, the occurrence of thin cirrus clouds is associated with a drying of the upper troposphere (enhanced during suppressed phases), whereas the occurrence of thick cirrus anvil clouds appears to be significantly related to a moistening of the upper troposphere.


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.


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.


2014 ◽  
Vol 14 (2) ◽  
pp. 609-627 ◽  
Author(s):  
C. A. Klich ◽  
H. E. Fuelberg

Abstract. We use the Weather Research and Forecasting with Chemistry (WRF-Chem) online chemical transport model to simulate a middle latitude cyclone in East Asia at three different horizontal resolutions (45, 15, and 5 km grid spacing). The cyclone contains a typical warm conveyor belt (WCB) with an embedded squall line that passes through an area having large surface concentrations (> 400 ppbv) of carbon monoxide (CO). Model output from WRF-Chem is used to compare differences between the large-scale CO vertical transport by the WCB (the 45 km simulation) with the smaller-scale transport due to its convection (the 5 km simulation). Forward trajectories are calculated from WRF-Chem output using the Hybrid Single Particle Lagrangian Integrated Trajectory (HYSPLIT) model. At 45 km grid spacing, the WCB exhibits gradual ascent, lofting surface CO to 6–7 km. Upon reaching the warm front, the WCB and associated CO ascend more rapidly and later turn eastward over the Pacific Ocean. Convective transport at 5 km resolution with explicitly resolved convection occurs much more rapidly, with surface CO lofted to altitudes greater than 10 km in 1 h or less. We also compute CO vertical mass fluxes over specified areas and times to compare differences in transport due to the different grid spacings. Upward CO flux exceeds 110 000 t h−1 in the domain with explicit convection when the squall line is at peak intensity, while fluxes from the two coarser resolutions are an order of magnitude smaller. Specific areas of interest within the 5 km domain are defined to compare the magnitude of convective transport to that within the entire 5 km region. Although convection encompasses only a small portion of the 5 km domain, it is responsible for ~40% of the upward CO transport. We also examine the vertical transport due to a short wave trough and its associated area of convection, not related to the cyclone, that lofts CO to the upper troposphere. Results indicate that fine-scale resolution with explicitly resolved convection is important when assessing the vertical transport of surface emissions in areas of deep convection.


2018 ◽  
Vol 18 (24) ◽  
pp. 17895-17907 ◽  
Author(s):  
Oscar B. Dimdore-Miles ◽  
Paul I. Palmer ◽  
Lori P. Bruhwiler

Abstract. We consider the utility of the annual inter-polar difference (IPD) as a metric for changes in Arctic emissions of methane (CH4). The IPD has been previously defined as the difference between weighted annual means of CH4 mole fraction data collected at stations from the two polar regions (defined as latitudes poleward of 53∘ N and 53∘ S, respectively). This subtraction approach (IPD) implicitly assumes that extra-polar CH4 emissions arrive within the same calendar year at both poles. We show using a continuous version of the IPD that the metric includes not only changes in Arctic emissions but also terms that represent atmospheric transport of air masses from lower latitudes to the polar regions. We show the importance of these atmospheric transport terms in understanding the IPD using idealized numerical experiments with the TM5 global 3-D atmospheric chemistry transport model that is run from 1980 to 2010. A northern mid-latitude pulse in January 1990, which increases prior emission distributions, arrives at the Arctic with a higher mole fraction and ≃12 months earlier than at the Antarctic. The perturbation at the poles subsequently decays with an e-folding lifetime of ≃4 years. A similarly timed pulse emitted from the tropics arrives with a higher value at the Antarctic ≃11 months earlier than at the Arctic. This perturbation decays with an e-folding lifetime of ≃7 years. These simulations demonstrate that the assumption of symmetric transport of extra-polar emissions to the poles is not realistic, resulting in considerable IPD variations due to variations in emissions and atmospheric transport. We assess how well the annual IPD can detect a constant annual growth rate of Arctic emissions for three scenarios, 0.5 %, 1 %, and 2 %, superimposed on signals from lower latitudes, including random noise. We find that it can take up to 16 years to detect the smallest prescribed trend in Arctic emissions at the 95 % confidence level. Scenarios with higher, but likely unrealistic, growth in Arctic emissions are detected in less than a decade. We argue that a more reliable measurement-driven approach would require data collected from all latitudes, emphasizing the importance of maintaining a global monitoring network to observe decadal changes in atmospheric greenhouse gases.


2016 ◽  
Author(s):  
B. Barret ◽  
B. Sauvage ◽  
Y. Bennouna ◽  
E. Le Flochmoen

Abstract. During the Asian Summer Monsoon, the circulation in the Upper Troposphere-Lower Stratosphere (UTLS) is dominated by the Asian Monsoon Anticyclone (AMA). Pollutants convectively uplifted to the upper troposphere are trapped within this anticyclonic circulation that extends from the Pacific Ocean to the eastern Mediterranean basin. Among the uplifted pollutants are ozone (O3) and its precursors, such as carbon monoxide (CO) and nitrogen oxides (NOx). Many studies based on global modelisation and satellite data have documented the source regions and transport pathways of primary pollutants (CO, HCN) into the AMA. Here, we aim to quantify the O3 budget by taking into consideration anthropogenic and natural sources. We first use CO and O3 data from the Metop-A/IASI sensor to document their tropospheric distributions over Asia, taking advantage of the useful information they provide on the vertical dimension. These satellite data are used together with MOZAIC/IAGOS tropospheric profiles recorded in India to validate the distributions simulated by the global GEOS-Chem chemistry transport model. Over the Asian region, UTLS monthly CO and O3 distributions from IASI and GEOS-Chem display the same large-scale features. UTLS CO columns from GEOS-Chem are in agreement with IASI, with a low bias of 11 ± 9% and a correlation coefficient of 0.70. For O3, the model underestimates IASI UTLS columns over Asia by 14 ± 26% but the correlation between both is high (0.94). GEOS-Chem is further used to quantify the CO and O3 budget through sensitivity simulations. For CO, these simulations confirm that South-Asian anthropogenic emissions have a more important impact on enhanced concentrations within the AMA (∼25 ppbv) than East-Asian emissions (∼10 ppbv). The correlation between enhanced emissions over the Indo–gangetic–Plain and monsoon deep convection is responsible for this larger impact. Consistently, South-Asian anthropogenic NOx emissions also play a larger role in producing O3 within the AMA (∼8 ppbv) than East-Asian emissions (∼5 ppbv) but Asian lightning produced NOx are responsible for the largest O3 production (10–14 ppbv). Stratosphere to Troposphere Exchanges (STE) are also important in transporting O3 in the upper part of the AMA.


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