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

2007 ◽  
Vol 7 (5) ◽  
pp. 13839-13860 ◽  
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 tropopause level inside the anticyclone.

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 Observations of peroxyacetyl nitrate (PAN) in the upper troposphere by the Atmospheric Chemistry Experiment Fourier Transform Spectrometer (ACE-FTS)

2013 ◽  
Vol 13 (1) ◽  
pp. 1575-1607 ◽  
Author(s):  
K. A. Tereszchuk ◽  
D. P. Moore ◽  
J. J. Harrison ◽  
C. D. Boone ◽  
M. Park ◽  
...  
Keyword(s):  
Fourier Transform ◽  
Biomass Burning ◽  
Atmospheric Chemistry ◽  
Lower Stratosphere ◽  
Fourier Transform Spectrometer ◽  
Data Set ◽  
Upper Troposphere ◽  
Volatile Organic ◽  
The Impact ◽  
Chemistry Experiment

Abstract. Peroxyacetyl nitrate (CH3CO·O2NO2, abbreviated as PAN) is a trace molecular species present in the troposphere and lower stratosphere due primarily to pollution from fuel combustion and the pyrogenic outflows from biomass burning. In the lower troposphere, PAN has a relatively short life-time and is principally destroyed within a few hours through thermolysis, but it can act as a reservoir and carrier of NOx in the colder temperatures of the upper troposphere where UV photolysis becomes the dominant loss mechanism. Pyroconvective updrafts from large biomass burning events can inject PAN into the upper troposphere and lower stratosphere (UTLS), providing a means for the long-range transport of NOx. Given the extended lifetimes at these higher altitudes, PAN is readily detectable via satellite remote sensing. A new PAN data product is now available for the Atmospheric Chemistry Experiment Fourier Transform Spectrometer (ACE-FTS) Version 3.0 data set. We report measurements of PAN in Boreal biomass burning plumes recorded during the Quantifying the impact of BOReal forest fires on Tropospheric oxidants over the Atlantic using Aircraft and Satellites (BORTAS) campaign. The retrieval method employed and errors analysis are described in full detail. The retrieved volume mixing ratio (VMR) profiles are compared to coincident measurements made by the Michelson Interferometer for Passive Atmospheric Sounding (MIPAS) instrument on the European Space Agency (ESA) ENVIronmental SATellite (ENVISAT). Three ACE-FTS occultations containing measurements of Boreal biomass burning outflows, recorded during BORTAS, were identified as having coincident measurements with MIPAS. In each case, the MIPAS measurements demonstrated good agreement with the ACE-FTS VMR profiles for PAN. The ACE-FTS PAN data set is used to obtain zonal mean distributions of seasonal averages from ~5 to 20 km. A strong seasonality is clearly observed for PAN concentrations in the global UTLS. Since the principal source of PAN in the UTLS is due to lofted biomass burning emissions from the pyroconvective updrafts created by large fires, the observed seasonality in enhanced PAN coincides with fire activity in different geographical regions throughout the year. This work is part of an in-depth investigation that is being conducted in an effort to study the aging and chemical evolution of biomass burning emissions in the UTLS by remote, space-borne measurements made by ACE-FTS to further our understanding of the impact of pyrogenic emissions on atmospheric chemistry. Included in this study will be the addition of new, pyrogenic, volatile organic hydrocarbons (VOCs) and oxygenated volatile organic compounds (OVOCs) to expand upon the already extensive suite of molecules retrieved by ACE-FTS to aid in elucidating biomass burning plume chemistry in the free troposphere.

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 Trajectory model simulations of ozone (O<sub>3</sub>) and carbon monoxide (CO) in the lower stratosphere

2014 ◽  
Vol 14 (14) ◽  
pp. 7135-7147 ◽  
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 lower stratosphere. 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 lower stratosphere.

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

2008 ◽  
Vol 8 (9) ◽  
pp. 2421-2435 ◽  
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 Observations of peroxyacetyl nitrate (PAN) in the upper troposphere by the Atmospheric Chemistry Experiment-Fourier Transform Spectrometer (ACE-FTS)

2013 ◽  
Vol 13 (11) ◽  
pp. 5601-5613 ◽  
Author(s):  
K. A. Tereszchuk ◽  
D. P. Moore ◽  
J. J. Harrison ◽  
C. D. Boone ◽  
M. Park ◽  
...  
Keyword(s):  
Fourier Transform ◽  
Biomass Burning ◽  
Atmospheric Chemistry ◽  
Lower Stratosphere ◽  
Full Detail ◽  
Fourier Transform Spectrometer ◽  
Peroxyacetyl Nitrate ◽  
Data Set ◽  
Upper Troposphere ◽  
Chemistry Experiment

Abstract. Peroxyacetyl nitrate (CH3CO·O2NO2, abbreviated as PAN) is a trace molecular species present in the troposphere and lower stratosphere due primarily to pollution from fuel combustion and the pyrogenic outflows from biomass burning. In the lower troposphere, PAN has a relatively short lifetime and is principally destroyed within a few hours through thermolysis, but it can act as a reservoir and carrier of NOx in the colder temperatures of the upper troposphere, where UV photolysis becomes the dominant loss mechanism. Pyroconvective updrafts from large biomass burning events can inject PAN into the upper troposphere and lower stratosphere (UTLS), providing a means for the long-range transport of NOx. Given the extended lifetimes at these higher altitudes, PAN is readily detectable via satellite remote sensing. A new PAN data product is now available for the Atmospheric Chemistry Experiment Fourier Transform Spectrometer (ACE-FTS) version 3.0 data set. We report observations of PAN in boreal biomass burning plumes recorded during the BORTAS (quantifying the impact of BOReal forest fires on Tropospheric oxidants over the Atlantic using Aircraft and Satellites) campaign (12 July to 3 August 2011). The retrieval method employed by incorporating laboratory-recorded absorption cross sections into version 3.0 of the ACE-FTS forward model and retrieval software is described in full detail. The estimated detection limit for ACE-FTS PAN is 5 pptv, and the total systematic error contribution to the ACE-FTS PAN retrieval is ~ 16%. The retrieved volume mixing ratio (VMR) profiles are compared to coincident measurements made by the Michelson Interferometer for Passive Atmospheric Sounding (MIPAS) instrument on the European Space Agency (ESA) Environmental Satellite (ENVISAT). The MIPAS measurements demonstrated good agreement with the ACE-FTS VMR profiles for PAN, where the measured VMR values are well within the associated measurement errors for both instruments and comparative measurements differ no more than 70 pptv. The ACE-FTS PAN data set is used to obtain zonal mean distributions of seasonal averages from ~ 5–20 km. A strong seasonality is clearly observed for PAN concentrations in the global UTLS. Since the principal source of PAN in the UTLS is due to lofted biomass burning emissions from the pyroconvective updrafts created by large fires, the observed seasonality in enhanced PAN coincides with fire activity in different geographical regions throughout the year.

scholarly journals The high Arctic in extreme winters: vortex, temperature, and MLS and ACE-FTS trace gas evolution

2008 ◽  
Vol 8 (3) ◽  
pp. 505-522 ◽  
Author(s):  
G. L. Manney ◽  
W. H. Daffer ◽  
K. B. Strawbridge ◽  
K. A. Walker ◽  
C. D. Boone ◽  
...  
Keyword(s):  
Atmospheric Chemistry ◽  
Lower Stratosphere ◽  
High Arctic ◽  
Trace Gas ◽  
Satellite Measurements ◽  
Broadband Emission ◽  
Gas Measurements ◽  
Chemistry Experiment ◽  
Very High ◽  
Good Agreement

Abstract. The first three Arctic winters of the ACE mission represented two extremes of winter variability: Stratospheric sudden warmings (SSWs) in 2004 and 2006 were among the strongest, most prolonged on record; 2005 was a record cold winter. Canadian Arctic Atmospheric Chemistry Experiment (ACE) Validation Campaigns were conducted at Eureka (80° N, 86° W) during each of these winters. New satellite measurements from ACE-Fourier Transform Spectrometer (ACE-FTS), Sounding of the Atmosphere using Broadband Emission Radiometry (SABER), and Aura Microwave Limb Sounder (MLS), along with meteorological analyses and Eureka lidar temperatures, are used to detail the meteorology in these winters, to demonstrate its influence on transport, and to provide a context for interpretation of ACE-FTS and validation campaign observations. During the 2004 and 2006 SSWs, the vortex broke down throughout the stratosphere, reformed quickly in the upper stratosphere, and remained weak in the middle and lower stratosphere. The stratopause reformed at very high altitude, near 75 km. ACE measurements covered both vortex and extra-vortex conditions in each winter, except in late-February through mid-March 2004 and 2006, when the strong, pole-centered vortex that reformed after the SSWs resulted in ACE sampling only inside the vortex in the middle through upper stratosphere. The 2004 and 2006 Eureka campaigns were during the recovery from the SSWs, with the redeveloping vortex over Eureka. 2005 was the coldest winter on record in the lower stratosphere, but with an early final warming in mid-March. The vortex was over Eureka at the start of the 2005 campaign, but moved away as it broke up. Disparate temperature profile structure and vortex evolution resulted in much lower (higher) temperatures in the upper (lower) stratosphere in 2004 and 2006 than in 2005. Satellite temperatures agree well with lidar data up to 50–60 km, and ACE-FTS, MLS and SABER show good agreement in high-latitude temperatures throughout the winters. Consistent with a strong, cold upper stratospheric vortex and enhanced radiative cooling after the SSWs, MLS and ACE-FTS trace gas measurements show strongly enhanced descent in the upper stratospheric vortex in late January through March 2006 compared to that in 2005.

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