scholarly journals What drives the observed variability of HCN in the troposphere and lower stratosphere?

2009 ◽  
Vol 9 (3) ◽  
pp. 10883-10912 ◽  
Author(s):  
Q. Li ◽  
P. I. Palmer ◽  
H. C. Pumphrey ◽  
P. Bernath ◽  
E. Mahieu
Keyword(s):  
Atmospheric Chemistry ◽  
Lower Stratosphere ◽  
Transport Model ◽  
Atmospheric Transport ◽  
Chemistry Transport Model ◽  
Upper Troposphere ◽  
Annual Variations ◽  
Surface Emission ◽  
Chemistry Experiment ◽  
Temporal Overlap

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.

scholarly journals What drives the observed variability of HCN in the troposphere and lower stratosphere?

2009 ◽  
Vol 9 (21) ◽  
pp. 8531-8543 ◽  
Author(s):  
Q. Li ◽  
P. I. Palmer ◽  
H. C. Pumphrey ◽  
P. Bernath ◽  
E. Mahieu
Keyword(s):  
Atmospheric Chemistry ◽  
Lower Stratosphere ◽  
Transport Model ◽  
Atmospheric Transport ◽  
Negative Bias ◽  
Mixing Ratio ◽  
Chemistry Transport Model ◽  
Annual Variations ◽  
Surface Emission ◽  
Chemistry Experiment

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 HCN mixing ratio from the Microwave Limb Sounder and the Atmospheric Chemistry Experiment satellite instruments with a mean negative bias of 20%, and the observed HCN variability with a mean negative bias of 7%. We show that tropical biomass burning emissions explain most of 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 influence 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 been diluted before arriving at the lower stratosphere (LS), due to shorter atmospheric lifetimes.

A recent slowdown in the decline of CFC-11 concentrations in the upper troposphere

2020 ◽  
Author(s):  
Patrick Sheese ◽  
Kaley Walker ◽  
Chris Boone ◽  
Laura Saunders ◽  
Sandip Dhomse ◽  
...  
Keyword(s):  
Atmospheric Chemistry ◽  
Transport Model ◽  
Recent Change ◽  
Fourier Transform Spectrometer ◽  
Chemical Transport Model ◽  
Surface Level ◽  
Upper Troposphere ◽  
The Past ◽  
Ozone Depleting Substances ◽  
Chemistry Experiment

<p>Since 2004, the Atmospheric Chemistry Experiment – Fourier Transform Spectrometer (ACE-FTS) instrument has been measuring concentrations of chlorofluorocarbons (CFCs) in the stratosphere and upper troposphere and is currently the only satellite instrument that measures vertically resolved profiles of CFC‑11. Since CFCs are major ozone depleting substances, monitoring their atmospheric abundances is critical for understanding ozone layer recovery. Recent studies based solely on surface-level measurements have shown strong evidence for new CFC‑11 production, leading to an increase in CFC‑11 emissions over the past decade. In this study, the TOMCAT/SLIMCAT 3-D chemical transport model is used in order to bridge the altitude/geolocation gap between ACE-FTS measurements in the UTLS and surface level measurements. Trends in two different time periods over the ACE-FTS mission, 2004-2012 and 2013-2018, are examined to determine if the recent change in surface level CFC-11 trends is influencing UTLS concentrations. The ACE-FTS measurements show that, below ~10 km, the rate of decrease of global CFC-11 concentrations was slower during 2013-2018 (-1.2 pptv/year) than during 2004-2012 (‑2.0 pptv/year). Similar trends are observed in the model data for the same spatial/temporal regions.</p>

scholarly journals Chemical isolation in the Asian monsoon anticyclone observed in Atmospheric Chemistry Experiment (ACE-FTS) data

2008 ◽  
Vol 8 (3) ◽  
pp. 757-764 ◽  
Author(s):  
M. Park ◽  
W. J. Randel ◽  
L. K. Emmons ◽  
P. F. Bernath ◽  
K. A. Walker ◽  
...  
Keyword(s):  
Atmospheric Chemistry ◽  
Asian Monsoon ◽  
Lower Stratosphere ◽  
Chemical Constituents ◽  
Strong Correlations ◽  
Near Surface ◽  
Upper Troposphere ◽  
Relative Age ◽  
Rapid Transport ◽  
Chemistry Experiment

Abstract. Evidence of chemical isolation in the Asian monsoon anticyclone is presented using chemical constituents obtained from the Atmospheric Chemistry Experiment Fourier Transform Spectrometer instrument during summer (June–August) of 2004–2006. Carbon monoxide (CO) shows a broad maximum over the monsoon anticyclone region in the upper troposphere and lower stratosphere (UTLS); these enhanced CO values are associated with air pollution transported upward by convection, and confined by the strong anticyclonic circulation. Profiles inside the anticyclone show enhancement of tropospheric tracers CO, HCN, C2H6, and C2H2 between ~12 to 20 km, with maxima near 13–15 km. Strong correlations are observed among constituents, consistent with sources from near-surface pollution and biomass burning. Stratospheric tracers (O3, HNO3 and HCl) exhibit decreased values inside the anticyclone between ~12–20 km. These observations are further evidence of transport of lower tropospheric air into the UTLS region, and isolation of air within the anticyclone. The relative enhancements of tropospheric species inside the anticyclone are closely related to the photochemical lifetime of the species, with strongest enhancement for shorter lived species. Vertical profiles of the ratio of C2H2/CO (used to measure the relative age of air) suggest relatively rapid transport of fresh emissions up to the tropopause level inside the anticyclone.

scholarly journals Mesosphere-to-stratosphere descent of odd nitrogen in February–March 2009 after sudden stratospheric warming

2011 ◽  
Vol 11 (1) ◽  
pp. 1429-1455 ◽  
Author(s):  
S.-M. Salmi ◽  
P. T. Verronen ◽  
L. Thölix ◽  
E. Kyrölä ◽  
L. Backman ◽  
...  
Keyword(s):  
Atmospheric Chemistry ◽  
Transport Model ◽  
Atmospheric Transport ◽  
Good Opportunity ◽  
Weather Forecasts ◽  
Model Study ◽  
Halogen Chemistry ◽  
Odd Nitrogen ◽  
Chemistry Experiment

Abstract. We use the 3-D FinROSE chemistry transport model (CTM) and ACE-FTS (Atmospheric Chemistry Experiment Fourier Transform Spectrometer) observations to study the connection between atmospheric dynamics and NOx descent during early 2009 in the northern polar region. We force the model NOx at 80 km poleward of 60° N with ACE-FTS observations and then compare the model results with observations at lower altitudes. Low geomagnetic indices indicate absence of local NOx production in early 2009, which gives a good opportunity to study the effects of atmospheric transport on polar NOx. No in-situ production of NOx by energetic particle precipitation is therefore included. This is the first model study using ECMWF (The European Centre for Medium-Range Weather Forecasts) data up to 80 km and simulating the exceptional winter of 2009 with one of the strongest major sudden stratospheric warmings (SSW). The model results show a strong NOx descent in February–March 2009 from the upper mesosphere to the stratosphere after the major SSW. Both observations and model results suggest an increase of NOx to 150–200 ppb (i.e. by factor of 50) at 65 km due to the descent following the SSW. The model, however, underestimates the amount of NOx around 55 km by 40–60 ppb. The results also show that the chemical loss of NOx was insignificant i.e. NOx was mainly controlled by the dynamics. Both ACE-FTS observations and FinROSE show a decrease of ozone of 20–30% at 30–50 km after mid-February to mid-March. However, these changes are not related to the NOx descent, but are due to activation of the halogen chemistry.

scholarly journals Intercomparison and evaluation of satellite peroxyacetyl nitrate observations in the upper troposphere – lower stratosphere

2016 ◽  
Author(s):  
R. J. Pope ◽  
N. A. D. Richards ◽  
M. P. Chipperfield ◽  
D. P. Moore ◽  
S. A. Monks ◽  
...  
Keyword(s):  
Atmospheric Chemistry ◽  
Lower Stratosphere ◽  
Transport Model ◽  
Regional Distribution ◽  
Michelson Interferometer ◽  
Lower Atmosphere ◽  
Chemical Transport Model ◽  
Peroxyacetyl Nitrate ◽  
Subsequent Formation ◽  
Upper Troposphere

Abstract. Peroxyacetyl nitrate (PAN) is an important chemical species in the troposphere as it aids the long-range transport of NOx and subsequent formation of O3 in relatively clean remote regions. Over the past few decades observations from aircraft campaigns and surface sites have been used to better understand the regional distribution of PAN. However, recent measurements made by satellites allow for a global assessment of PAN in the upper troposphere – lower stratosphere (UTLS). In this study, we investigate global PAN distributions from two independent retrieval methodologies, based on measurements from the Michelson Interferometer for Passive Atmospheric Sounding (MIPAS) instrument, on board ENVISAT from the Institute of Meteorology and Climate Research (IMK), Karlsruhe Institute of Technology and the Department of Physics and Astronomy, University of Leicester (UoL). Retrieving PAN from MIPAS is challenging due to the weak signal in the measurements and contamination from other species. Therefore, we compare the two MIPAS datasets with observations from the Atmospheric Chemistry Experiment Fourier Transform Spectrometer (ACE-FTS), insitu aircraft data and the TOMCAT 3-D chemical transport model. MIPAS shows peak UTLS PAN concentrations over the biomass burning regions (e.g. ranging from 150 to > 200 pptv at 150 hPa) and during the summertime Asian monsoon as enhanced convection aids the vertical transport of PAN from the lower atmosphere. At 150 hPa, we find significant differences between the two MIPAS datasets in the tropics, where IMK PAN concentrations are larger by 50–100 pptv. Comparisons between MIPAS and ACE-FTS show better agreement with the UoL MIPAS PAN concentrations at 200 hPa, but with mixed results above this altitude. TOMCAT generally captures the magnitude and structure of climatological aircraft PAN profiles within the observational variability allowing it to be used to investigate the MIPAS PAN differences. TOMCAT-MIPAS comparisons show that the model is both positively (UoL) and negatively (IMK) biased against the satellite products. These results show that satellite PAN observations are able to detect realistic spatial variations in PAN in the UTLS, but further work is needed to resolve differences in existing retrievals to allow quantitative use of the products.

scholarly journals Transport analysis and source attribution of seasonal and interannual variability of CO in the tropical upper troposphere and lower stratosphere

2013 ◽  
Vol 13 (1) ◽  
pp. 129-146 ◽  
Author(s):  
J. Liu ◽  
J. A. Logan ◽  
L. T. Murray ◽  
H. C. Pumphrey ◽  
M. J. Schwartz ◽  
...  
Keyword(s):  
Annual Cycle ◽  
Annual Variation ◽  
Lower Stratosphere ◽  
Transport Model ◽  
Boreal Summer ◽  
Lower Altitude ◽  
Model Simulations ◽  
Upper Troposphere ◽  
Annual Variations ◽  
Upward Transport

Abstract. We used the GEOS-Chem chemistry-transport model to investigate impacts of surface emissions and dynamical processes on the spatial and temporal patterns of CO observed by the Microwave Limb Sounder (MLS) in the upper troposphere (UT) and lower stratosphere (LS). Model simulations driven by GEOS-4 and GEOS-5 assimilated fields present many features of the seasonal and inter-annual variation of CO in the upper troposphere and lower stratosphere. Both model simulations and the MLS data show a transition from semi-annual variations in the UT to annual variations in the LS. Tagged CO simulations indicate that the semi-annual variation of CO in the UT is determined mainly by the temporal overlapping of surface biomass burning from different continents as well as the north-south shifts of deep convection. Both GEOS-4 and GEOS-5 have maximum upward transport in April and May with a minimum in July to September. The CO peaks from the Northern Hemisphere (NH) fires propagate faster to the LS than do those from the Southern Hemisphere (SH) fires. Thus the transition from a semi-annual to an annual cycle around 80 hPa is induced by a combination of the CO signal at the tropopause and the annual cycle of the Brewer-Dobson circulation. In GEOS-5, the shift to an annual cycle occurs at a lower altitude than in MLS CO, a result of inadequate upward transport. We deduce vertical velocities from MLS CO, and use them to evaluate the velocities derived from the archived GEOS meteorological fields. We find that GEOS-4 velocities are similar to those from MLS CO between 215 hPa and 125 hPa, while the velocities in GEOS-5 are too low in spring and summer. The mean tropical vertical velocities from both models are lower than those inferred from MLS CO above 100 hPa, particularly in GEOS-5, with mean downward, rather than upward motion in boreal summer. Thus the models' CO maxima from SH burning are transported less effectively than those in MLS CO above 147 hPa and almost disappear by 100 hPa. The strongest peaks in the CO tape-recorder are in late 2004, 2006, and 2010, with the first two resulting from major fires in Indonesia and the last from severe burning in South America, all associated with intense droughts.

scholarly journals Trajectory model simulations of ozone and carbon monoxide in the Upper Troposphere and Lower Stratosphere (UTLS)

2014 ◽  
Vol 14 (5) ◽  
pp. 5991-6025
Author(s):  
T. Wang ◽  
W. J. Randel ◽  
A. E. Dessler ◽  
M. R. Schoeberl ◽  
D. E. Kinnison
Keyword(s):  
Carbon Monoxide ◽  
Atmospheric Chemistry ◽  
Lower Stratosphere ◽  
Climate Model ◽  
Chemical Production ◽  
Wind Fields ◽  
Upper Troposphere ◽  
Stratospheric Water Vapor ◽  
Trajectory Model ◽  
Chemistry Experiment

Abstract. A domain-filling, forward trajectory model originally developed for simulating stratospheric water vapor is used to simulate ozone (O3) and carbon monoxide (CO) in the upper troposphere and lower stratosphere (UTLS). Trajectories are initialized in the upper troposphere, and the circulation is based on reanalysis wind fields. In addition, chemical production and loss rates along trajectories are included using calculations from the Whole Atmosphere Community Climate Model (WACCM). The trajectory model results show good overall agreement with satellite observations from the Aura Microwave Limb Sounder (MLS) and the Atmospheric Chemistry Experiment Fourier Transform Spectrometer (ACE-FTS) in terms of spatial structure and seasonal variability. The trajectory model results also agree well with the Eulerian WACCM simulations. Analysis of the simulated tracers shows that seasonal variations in tropical upwelling exerts strong influence on O3 and CO in the tropical lower stratosphere, and the coupled seasonal cycles provide a useful test of the transport simulations. Interannual variations in the tracers are also closely coupled to changes in upwelling, and the trajectory model can accurately capture and explain observed changes during 2005–2011. This demonstrates the importance of variability in tropical upwelling in forcing chemical changes in the tropical UTLS.

scholarly journals Validation of ACE-FTS v2.2 methane profiles from the upper troposphere to lower mesosphere

2007 ◽  
Vol 7 (6) ◽  
pp. 17975-18014 ◽  
Author(s):  
M. De Mazière ◽  
C. Vigouroux ◽  
P. F. Bernath ◽  
P. Baron ◽  
T. Blumenstock ◽  
...  
Keyword(s):  
Fourier Transform ◽  
Atmospheric Chemistry ◽  
Lower Stratosphere ◽  
Remote Sensing Data ◽  
Upper Troposphere ◽  
Solar Occultation ◽  
Systematic Uncertainties ◽  
Comparison Results ◽  
Key Species ◽  
Chemistry Experiment

Abstract. The ACE-FTS (Atmospheric Chemistry Experiment – Fourier Transform Spectrometer) solar occultation instrument that was launched onboard the Canadian SCISAT-1 satellite in August 2003 is measuring vertical profiles from the upper troposphere to the lower mesosphere for a large number of atmospheric constituents. Methane is one of the key species. The version v2.2 data of the ACE-FTS CH4 data have been compared to correlative satellite, balloon-borne and ground-based Fourier transform infrared remote sensing data to assess their quality. The comparison results indicate that the accuracy of the data is within 10% in the upper troposphere – lower stratosphere, and within 25% in the middle and higher stratosphere up to the lower mesosphere (<60 km). The observed differences are generally consistent with reported systematic uncertainties. ACE-FTS is also shown to reproduce the variability of methane in the stratosphere and lower mesosphere.

scholarly journals Transport analysis and source attribution of seasonal and interannual variability of CO in the tropical upper troposphere and lower stratosphere

2012 ◽  
Vol 12 (7) ◽  
pp. 17397-17442 ◽  
Author(s):  
Junhua Liu ◽  
J. A. Logan ◽  
L. T. Murray ◽  
H. C. Pumphrey ◽  
M. J. Schwartz ◽  
...  
Keyword(s):  
Annual Cycle ◽  
Annual Variation ◽  
Lower Stratosphere ◽  
Transport Model ◽  
Boreal Summer ◽  
Lower Altitude ◽  
Model Simulations ◽  
Upper Troposphere ◽  
Annual Variations ◽  
Upward Transport

Abstract. We used the GEOS-Chem chemistry-transport model to investigate impacts of surface emissions and dynamical processes on the spatial and temporal patterns of CO observed by the Microwave Limb Sounder (MLS) in the upper troposphere and lower stratosphere (UTLS). Model simulations driven by GEOS-4 and GEOS-5 assimilated fields present many features of the seasonal and inter-annual variation of CO in the UTLS. Both model simulations and the MLS data show a transition from semi-annual variations in the UT to annual variations in the LS. Tagged CO simulations indicate that the semi-annual variation of CO in the UT is determined mainly by the temporal overlapping of surface biomass burning from different continents as well as the north-south shifts of deep convection. Both GEOS-4 and GEOS-5 have maximum upward transport in April and May with a minimum in July to September. The CO peaks from NH fires propagate faster to the LS than do those from SH fires. Thus the transition from a semi-annual to an annual cycle around 80 hPa is induced by a combination of the CO signal at the tropopause and the annual cycle of the Brewer-Dobson circulation. In GEOS-5, the shift to an annual cycle occurs at a lower altitude than in MLS CO, a result of inadequate upward transport. We deduce vertical velocities from MLS CO, and find that those in GEOS-4 agree well with them between 215 hPa and 125 hPa in boreal summer, fall and winter, while the velocities in GEOS-5 are too low in all seasons. The mean tropical vertical velocities from both models are lower than those inferred from MLS CO above 100 hPa in June to November, particularly in GEOS-5, with mean downward, rather than upward motion in boreal summer. Thus the models' CO maxima from SH burning are transported less effectively than those in MLS CO above 147 hPa and almost disappear by 100 hPa. The strongest peaks in the CO tape-recorder are in late 2004, 2006, and 2010, with the first two resulting from major fires in Indonesia and the last from severe burning in South America, all associated with intense droughts.

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

2020 ◽  
Author(s):  
Aurelien Podglajen ◽  
Edward Charlesworth ◽  
Felix Ploeger
Keyword(s):  
Time Scales ◽  
Atmospheric Chemistry ◽  
Large Scale ◽  
Transport Model ◽  
Atmospheric Transport ◽  
Convective Transport ◽  
Transport Pathways ◽  
Upper Troposphere ◽  
Major Player ◽  
Interhemispheric Transport

&lt;p&gt;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 (&gt;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.&lt;/p&gt;&lt;p&gt;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 (&lt; 12 hours) and monthly for long ones (&gt; 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).&lt;/p&gt;

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