scholarly journals Global upper-tropospheric formaldehyde: seasonal cycles observed by the ACE-FTS satellite instrument

2009 ◽  
Vol 9 (1) ◽  
pp. 1051-1095 ◽  
Author(s):  
G. Dufour ◽  
S. Szopa ◽  
M. P. Barkley ◽  
C. D. Boone ◽  
A. Perrin ◽  
...  
Keyword(s):  
Southern Hemisphere ◽  
Northern Hemisphere ◽  
Biomass Burning ◽  
Growing Season ◽  
Global Scale ◽  
Tropospheric Chemistry ◽  
Data Set ◽  
Mixing Ratios ◽  
Good Reproduction ◽  
Summer Maximum

Abstract. Seasonally-resolved upper tropospheric profiles of formaldehyde (HCHO) observed by the ACE Fourier transform spectrometer (ACE-FTS) on a near-global scale are presented for the time period from March 2004 to November 2006. Large upper tropospheric HCHO mixing ratios (>150 pptv) are observed during the growing season of the terrestrial biosphere in the Northern Hemisphere and during the biomass burning season in the Southern Hemisphere. The total errors estimated for the retrieved mixing ratios range from 30 to 40% in the upper troposphere and increase in the lower stratosphere. The sampled HCHO concentrations are in satisfactory agreement with previous aircraft and satellite observations with a negative bias (<25%) within observation errors. An overview of the seasonal cycle of the upper tropospheric HCHO is given for different latitudes. A maximum is observed during summer, i.e. during the growing season, in the northern mid- and high latitudes. The influence of biomass burning is visible in HCHO upper tropospheric concentrations during the September-to-October period in the southern tropics and subtropics. Comparisons with two state-of-the-art models (GEOS-Chem and LMDz-INCA) show that the models fail to reproduce the seasonal variations observed in the southern tropics and subtropics but they capture well the variations observed in the Northern Hemisphere (correlation >0.9). Both models underestimate the summer maximum over Europe and Russia and differences in the emissions used for North America result in a good reproduction of the summer maximum by GEOS-Chem but in an underestimate by LMDz-INCA. Globally, GEOS-Chem reproduces well the observations on average over one year but has some difficulties in reproducing the spatial variability of the observations. LMDz-INCA shows significant bias in the Southern Hemisphere, likely related to an underestimation of methane, but better reproduces the temporal and spatial variations. The differences between the models underline the large uncertainties that remain in the emissions of HCHO precursors. Observations of the HCHO upper tropospheric profile provided by the ACE-FTS represent a unique data set for investigating and improving our current understanding of the formaldehyde budget and upper tropospheric chemistry.

scholarly journals Global upper-tropospheric formaldehyde: seasonal cycles observed by the ACE-FTS satellite instrument

2009 ◽  
Vol 9 (12) ◽  
pp. 3893-3910 ◽  
Author(s):  
G. Dufour ◽  
S. Szopa ◽  
M. P. Barkley ◽  
C. D. Boone ◽  
A. Perrin ◽  
...  
Keyword(s):  
Southern Hemisphere ◽  
Northern Hemisphere ◽  
Biomass Burning ◽  
Growing Season ◽  
Global Scale ◽  
High Latitudes ◽  
Mixing Ratios ◽  
Good Reproduction ◽  
Summer Maximum ◽  
One Year

Abstract. Seasonally-resolved upper tropospheric profiles of formaldehyde (HCHO) observed by the ACE Fourier transform spectrometer (ACE-FTS) on a near-global scale are presented for the time period from March 2004 to November 2006. Large upper tropospheric HCHO mixing ratios (>150 pptv) are observed during the growing season of the terrestrial biosphere in the Northern Hemisphere and during the biomass burning season in the Southern Hemisphere. The total errors estimated for the retrieved mixing ratios range from 30 to 40% in the upper troposphere and increase in the lower stratosphere. The sampled HCHO concentrations are in satisfactory agreement with previous aircraft and satellite observations with a negative bias (<25%) within observation errors. An overview of the seasonal cycle of the upper tropospheric HCHO is given for different latitudes, with a particular focus on mid-to-high latitudes that are well sampled by the observations. A maximum is observed during summer, i.e. during the growing season, in the northern mid- and high latitudes. The influence of biomass burning is visible in HCHO upper tropospheric concentrations during the September-to-October period in the southern tropics and subtropics. Comparisons with two state-of-the-art models (GEOS-Chem and LMDz-INCA) show that the models capture well the seasonal variations observed in the Northern Hemisphere (correlation >0.9). Both models underestimate the summer maximum over Europe and Russia and differences in the emissions used for North America result in a good reproduction of the summer maximum by GEOS-Chem but in an underestimate by LMDz-INCA. Globally, GEOS-Chem reproduces well the observations on average over one year but has some difficulties in reproducing the spatial variability of the observations. LMDz-INCA shows significant bias in the Southern Hemisphere, perhaps related to an underestimation of methane, but better reproduces the temporal and spatial variations. The differences between the models underline the large uncertainties that remain in the emissions of HCHO precursors.

scholarly journals The influence of biogenic emissions on upper-tropospheric methanol as revealed from space

2007 ◽  
Vol 7 (24) ◽  
pp. 6119-6129 ◽  
Author(s):  
G. Dufour ◽  
S. Szopa ◽  
D. A. Hauglustaine ◽  
C. D. Boone ◽  
C. P. Rinsland ◽  
...  
Keyword(s):  
Northern Hemisphere ◽  
Biomass Burning ◽  
Transport Model ◽  
Tropospheric Chemistry ◽  
Biogenic Emissions ◽  
Chemistry Transport Model ◽  
Mixing Ratios ◽  
Oxygenated Compounds ◽  
Global Space ◽  
The Impact

Abstract. The distribution and budget of oxygenated organic compounds in the atmosphere and their impact on tropospheric chemistry are still poorly constrained. Near-global space-borne measurements of seasonally resolved upper tropospheric profiles of methanol (CH3OH) by the ACE Fourier transform spectrometer provide a unique opportunity to evaluate our understanding of this important oxygenated organic species. ACE-FTS observations from March 2004 to August 2005 period are presented. These observations reveal the pervasive imprint of surface sources on upper tropospheric methanol: mixing ratios observed in the mid and high latitudes of the Northern Hemisphere reflect the seasonal cycle of the biogenic emissions whereas the methanol cycle observed in the southern tropics is highly influenced by biomass burning emissions. The comparison with distributions simulated by the state-of-the-art global chemistry transport model, LMDz-INCA, suggests that: (i) the background methanol (high southern latitudes) is correctly represented by the model considering the measurement uncertainties; (ii) the current emissions from the continental biosphere are underestimated during spring and summer in the Northern Hemisphere leading to an underestimation of modelled upper tropospheric methanol; (iii) the seasonal variation of upper tropospheric methanol is shifted to the fall in the model suggesting either an insufficient destruction of CH3OH (due to too weak chemistry and/or deposition) in fall and winter months or an unfaithful representation of transport; (iv) the impact of tropical biomass burning emissions on upper tropospheric methanol is rather well reproduced by the model. This study illustrates the potential of these first global profile observations of oxygenated compounds in the upper troposphere to improve our understanding of their global distribution, fate and budget.

scholarly journals Ship-borne FTIR measurements of CO and O<sub>3</sub> in the Western Pacific from 43° N to 35° S: an evaluation of the sources

2012 ◽  
Vol 12 (2) ◽  
pp. 815-828 ◽  
Author(s):  
T. Ridder ◽  
C. Gerbig ◽  
J. Notholt ◽  
M. Rex ◽  
O. Schrems ◽  
...  
Keyword(s):  
Fourier Transform ◽  
Southern Hemisphere ◽  
Northern Hemisphere ◽  
Biomass Burning ◽  
Fossil Fuel ◽  
Fuel Combustion ◽  
Western Pacific ◽  
Fossil Fuel Combustion ◽  
Source Regions ◽  
The Western Pacific

Abstract. Carbon monoxide (CO) and ozone (O3) have been measured in the Western Pacific (43° N to 35° S) during a ship campaign with Research Vessel Sonne in fall 2009. Observations have been performed using ship-based solar absorption Fourier Transform infrared spectrometry, flask sampling, balloon sounding, and in-situ Fourier Transform infrared analysis. The results obtained are compared to the GEOS-Chem global 3-D chemistry transport model for atmospheric composition. In general, a very good agreement is found between the GEOS-Chem model and all instruments. The CO and O3 distributions show a comparable variability suggesting an impact from the same source regions. Tagged-CO simulations implemented in the GEOS-Chem model make it possible to differentiate between different source processes and source regions. The source regions are verified with HYSPLIT backward trajectory calculations. In the Northern Hemisphere fossil fuel combustion in Asia is the dominant source. European and North American fossil fuel combustion also contribute to Northern Hemispheric CO pollution. In the Southern Hemisphere contributions from biomass burning and fossil fuel combustion are dominant; African biomass burning has a significant impact on Western Pacific CO pollution. Furthermore, in the tropical Western Pacific enhanced upper tropospheric CO within the tropical tropopause layer mainly originates from Indonesian fossil fuel combustion and can be transported into the stratosphere. The source regions of the measured O3 pollution are simulated with a tagged-O3 simulation implemented in the GEOS-Chem model. Similar source regions compared to the tagged-CO simulations are identified by the model. In the Northern Hemisphere contributions from Asia, Europe, and North America are significant. In the Southern Hemisphere emissions from South America, south-east Africa, and Oceania significantly contribute to the measured O3 pollution.

scholarly journals Nighttime O(<sup>1</sup>D) distributions in the mesopause region derived from SABER data

2020 ◽  
Vol 38 (4) ◽  
pp. 815-822 ◽  
Author(s):  
Mikhail Yu. Kulikov ◽  
Mikhail V. Belikovich
Keyword(s):  
Southern Hemisphere ◽  
Northern Hemisphere ◽  
Data Set ◽  
Mesopause Region

Abstract. In this study, the new source of O(1D) in the mesopause region due to the process OH(ν≥5)+O(3P)→OH(0≤ν′≤ν-5)+O(1D) is applied to SABER data to estimate the nighttime O(1D) distributions for the years 2003–2005. It is found that O(1D) evolutions in these years are very similar to each other. Depending on the month, monthly averaged O(1D) distributions show two to four maxima with values up to 340 cm−3 which are localized in height (at ∼92–96 km) and latitude (at ∼20–40 and ∼60–80∘ S, N). Annually averaged distributions in 2003–2005 have one weak maximum at ∼93 km and ∼65∘ S with values of 150–160 cm−3 and three pronounced maxima (with values up to 230 cm−3) at ∼95 km and ∼35∘ S, at ∼94 km and ∼40∘ N and at ∼93 km and ∼65–75∘ N, correspondingly. In general, there is slightly more O(1D) in the Northern Hemisphere than in the Southern Hemisphere. The obtained results are a useful data set for subsequent estimation of nighttime O(1D) influence on the chemistry of the mesopause region.

scholarly journals Reactive nitrogen, ozone and ozone production in the Arctic troposphere and the impact of stratosphere-troposphere exchange

2011 ◽  
Vol 11 (4) ◽  
pp. 10721-10767 ◽  
Author(s):  
Q. Liang ◽  
J. M. Rodriguez ◽  
A. R. Douglass ◽  
J. H. Crawford ◽  
E. Apel ◽  
...  
Keyword(s):  
Biomass Burning ◽  
Arctic Region ◽  
Tropospheric Chemistry ◽  
Ozone Production ◽  
The Arctic ◽  
Source Attribution ◽  
Air Masses ◽  
Upper Troposphere ◽  
Mixing Ratios ◽  
The Impact

Abstract. We analyze the aircraft observations obtained during the Arctic Research of the Composition of the Troposphere from Aircraft and Satellite (ARCTAS) mission together with the GEOS-5 CO simulation to examine O3 and NOy in the Arctic and sub-Arctic region and their source attribution. Using a number of marker tracers and their probability density distributions, we distinguish various air masses from the background troposphere and examine their contribution to NOx, O3, and O3 production in the Arctic troposphere. The background Arctic troposphere has mean O3 of ~60 ppbv and NOx of ~25 pptv throughout spring and summer with CO decreases from ~145 ppbv in spring to ~100 ppbv in summer. These observed CO, NOx and O3 mixing ratios are not notably different from the values measured during the 1988 ABLE-3A and the 2002 TOPSE field campaigns despite the significant changes in the past two decades in processes that could have changed the Arctic tropospheric composition. Air masses associated with stratosphere-troposphere exchange are present throughout the mid and upper troposphere during spring and summer. These air masses with mean O3 concentration of 140–160 ppbv are the most important direct sources of O3 in the Arctic troposphere. In addition, air of stratospheric origin is the only notable driver of net O3 formation in the Arctic due to its sustainable high NOx (75 pptv in spring and 110 pptv in summer) and NOy (~800 pptv in spring and ~1100 pptv in summer) levels. The ARCTAS measurements present observational evidence suggesting significant conversion of nitrogen from HNO3 to NOx and then to PAN (a net formation of ~120 pptv PAN) in summer when air of stratospheric origin is mixed with tropospheric background during stratosphere-to-troposphere transport. These findings imply that an adequate representation of stratospheric O3 and NOy input are essential in accurately simulating O3 and NOx photochemistry as well as the atmospheric budget of PAN in tropospheric chemistry transport models of the Arctic. Anthropogenic and biomass burning pollution plumes observed during ARCTAS show highly elevated hydrocarbons and NOy (mostly in the form of NOx and PAN), but do not contribute significantly to O3 in the Arctic troposphere except in some of the aged biomass burning plumes sampled during spring. Convection and/or lightning influences are negligible sources of O3 in the Arctic troposphere but can have significant impacts in the upper troposphere in the continental sub-Arctic during summer.

scholarly journals Ship-borne FTIR measurements of CO and O<sub>3</sub> in the Western Pacific from 43° N to 35° S: an evaluation of the sources

2011 ◽  
Vol 11 (8) ◽  
pp. 22951-22985 ◽  
Author(s):  
T. Ridder ◽  
C. Gerbig ◽  
J. Notholt ◽  
M. Rex ◽  
O. Schrems ◽  
...  
Keyword(s):  
Fourier Transform ◽  
Southern Hemisphere ◽  
Northern Hemisphere ◽  
Biomass Burning ◽  
Fossil Fuel ◽  
Fuel Combustion ◽  
Western Pacific ◽  
Fossil Fuel Combustion ◽  
Source Regions ◽  
The Western Pacific

Abstract. Carbon monoxide (CO) and ozone (O3) have been measured in the Western Pacific (43° N to 35° S) during a ship campaign with Research Vessel Sonne in fall 2009. Observations have been performed using ship-based solar absorption Fourier Transform infrared spectrometry, flask sampling, balloon sounding, and in-situ Fourier Transform infrared analysis. The obtained results are compared to the GEOS-Chem global 3-D chemistry transport model for atmospheric composition. In general, a very good agreement is found between the GEOS-Chem model and all instruments. The CO and O3 distributions show a comparable variability suggesting an impact from the same source regions. Tagged-CO simulations implemented in the GEOS-Chem model allow to differentiate between different sources and source regions. The sources are verified with HYSPLIT backward trajectory calculations. In the Northern Hemisphere fossil fuel combustion in Asia is the dominant source. European and North American fossil fuel combustion also contribute to Northern Hemispheric CO pollution. In the Southern Hemisphere contributions from biomass burning and fossil fuel combustion are dominant; African biomass burning has a significant impact on Western Pacific CO pollution. Furthermore, in the tropical Western Pacific enhanced upper tropospheric CO within the tropical tropopause layer mainly originates from Indonesian fossil fuel combustion and can be transported into the stratosphere. The sources and source regions of the measured O3 pollution are simulated with a tagged-O3 simulation implemented in the GEOS-Chem model. Similar source regions compared to the tagged-CO simulations are identified by the model. In the Northern Hemisphere contributions from Asia, Europe, and North America are significant. In the Southern Hemisphere the impact of emissions from South America, South-East Africa, and Oceania is important.

scholarly journals Inversion of CO and NO<sub>x</sub> emissions using the adjoint of the IMAGES model

2004 ◽  
Vol 4 (6) ◽  
pp. 7985-8068 ◽  
Author(s):  
J.-F. Müller ◽  
T. Stavrakou
Keyword(s):  
Southern Hemisphere ◽  
Biomass Burning ◽  
A Priori ◽  
Source Parameters ◽  
Anthropogenic Sources ◽  
Anthropogenic Source ◽  
Vertical Column ◽  
Bottom Up ◽  
Tropical Regions ◽  
Mixing Ratios

Abstract. We use ground-based observations of CO mixing ratios and vertical column abundances together with tropospheric NO2 columns from the GOME satellite instrument as constraints for improving the global annual emission estimates of CO and NOx for the year 1997. The agreement between concentrations calculated by the global 3-dimensional CTM IMAGES and the observations is optimized using the adjoint modelling technique, which allows to invert for CO and NOx fluxes simultaneously, taking their chemical interactions into account. Our analysis quantifies a total of 39 flux parameters, comprising anthropogenic and biomass burning sources over large continental regions, soil and lightning emissions of NOx, biogenic emissions of CO and non-methane hydrocarbons, as well as the deposition velocities of both CO and NOx. Comparison between observed, prior and optimized CO mixing ratios at NOAA/CMDL sites shows that the inversion performs well at the northern mid- and high latitudes, and that it is less efficient in the Southern Hemisphere, as expected due to the scarsity of measurements over this part of the globe. The inversion, moreover, brings the model much closer to the measured NO2 columns over all regions. Sensitivity tests show that anthropogenic sources exhibit weak sensitivity to changes of the a priori errors associated to the bottom-up inventory, whereas biomass burning sources are subject to a strong variability. Our best estimate for the 1997 global top-down CO source amounts to 2760 Tg CO. Anthropogenic emissions increase by 28%, in agreement with previous inverse modelling studies, suggesting that the present bottom-up inventories underestimate the anthropogenic CO emissions in the Northern Hemisphere. The magnitude of the optimized NOx global source decreases by 14% with respect to the prior, and amounts to 42.1 Tg N, out of which 22.8 Tg N are due to anthropogenic sources. The NOx emissions increase over Tropical regions, whereas they decrease over Europe and Asia. Our inversion results have been evaluated against independent observations from aircraft campaigns. This comparison shows that the optimization of CO emissions constrained by both CO and NO2 observations leads to a better agreement between modelled and observed values, especially in the Tropics and the Southern Hemisphere, compared to the case where only CO observations are used. A posteriori estimation of errors on the control parameters shows that a significant error reduction is achieved for the majority of the anthropogenic source parameters, whereas biomass burning emissions are still subject to large errors after optimization. Nonetheless, the constraints provided by the GOME measurements allow to reduce the uncertainties on savanna burning emissions of both CO and NOx, suggesting thus that the incorporation of these data in the inversion yields more robust results for carbon monoxide.

scholarly journals MIPAS measurements of upper tropospheric C<sub>2</sub>H<sub>6</sub> and O<sub>3</sub> during the southern hemispheric biomass burning season in 2003

2007 ◽  
Vol 7 (22) ◽  
pp. 5861-5872 ◽  
Author(s):  
T. von Clarmann ◽  
N. Glatthor ◽  
M. E. Koukouli ◽  
G. P. Stiller ◽  
B. Funke ◽  
...  
Keyword(s):  
Southern Hemisphere ◽  
Biomass Burning ◽  
Michelson Interferometer ◽  
Measured Signal ◽  
South American ◽  
African Savanna ◽  
Upper Troposphere ◽  
Mixing Ratios ◽  
Savanna Fires ◽  
Spectrally Resolved

Abstract. Under cloud free conditions, the Michelson Interferometer for Passive Atmospheric Sounding (MIPAS) provides measurements of spectrally resolved limb radiances down to the upper troposphere. These are used to infer global distributions of mixing ratios of atmospheric constituents in the upper troposphere and the stratosphere. From 21 October to 12 November 2003, MIPAS observed enhanced amounts of upper tropospheric C2H6 (up to about 400 pptv) and ozone (up to about 80 ppbv). The absolute values of C2H6, however, may be systematically low by about 30% due to uncertainties of the spectroscopic data used. By means of trajectory calculations, the enhancements observed in the southern hemisphere are, at least partly, attributed to a biomass burning plume, which covers wide parts of the Southern hemisphere, from South America, the Atlantic Ocean, Africa, the Indian Ocean to Australia. The chemical composition of the part of the plume-like pollution belt associated with South American fires, where rainforest burning is predominant appears different from the part of the plume associated with southern African savanna burning. In particular, African savanna fires lead to a larger ozone enhancement than equatorial American fires. In this analysis, MIPAS observations of high ozone were disregarded where low CFC-11 (below 245 pptv) was observed, because this hints at a stratospheric component in the measured signal. Different type of vegetation burning (flaming versus smouldering combustion) has been identified as a candidate explanation for the different plume compositions.

scholarly journals Observations of the mesospheric semi-annual oscillation (MSAO) in water vapour by Odin/SMR

2008 ◽  
Vol 8 (21) ◽  
pp. 6527-6540 ◽  
Author(s):  
S. Lossow ◽  
J. Urban ◽  
J. Gumbel ◽  
P. Eriksson ◽  
D. Murtagh
Keyword(s):  
Water Vapour ◽  
Southern Hemisphere ◽  
Northern Hemisphere ◽  
Annual Variation ◽  
Equatorial Region ◽  
Peak Amplitude ◽  
Altitude Range ◽  
Double Peak Structure ◽  
Latitude Range ◽  
Mixing Ratios

Abstract. Mesospheric water vapour measurements taken by the SMR instrument aboard the Odin satellite between 2002 and 2006 have been analysed with focus on the mesospheric semi-annual circulation in the tropical and subtropical region. This analysis provides the first complete picture of mesospheric SAO in water vapour, covering altitudes above 80 km where previous studies were limited. Our analysis shows a clear semi-annual variation in the water vapour distribution in the entire altitude range between 65 km and 100 km in the equatorial area. Maxima occur near the equinoxes below 75 km and around the solstices above 80 km. The phase reversal occurs in the small layer in-between, consistent with the downward propagation of the mesospheric SAO in the zonal wind in this altitude range. The SAO amplitude exhibits a double peak structure in the equatorial region, with maxima at about 75 km and 81 km. The observed amplitudes show higher values than an earlier analysis based on UARS/HALOE data. The upper peak amplitude remains relatively constant with latitude. The lower peak amplitude decreases towards higher latitudes, but recovers in the Southern Hemisphere subtropics. On the other hand, the annual variation is much more prominent in the Northern Hemisphere subtropics. Furthermore, higher volume mixing ratios during summer and lower values during winter are observed in the Northern Hemisphere subtropics, as compared to the corresponding latitude range in the Southern Hemisphere.

scholarly journals Effects of the interplanetary magnetic field y component on the dayside aurora

2019 ◽  
Vol 6 (1) ◽  
Author(s):  
K. Liou ◽  
E. Mitchell
Keyword(s):  
Magnetic Field ◽  
Interplanetary Magnetic Field ◽  
Southern Hemisphere ◽  
Northern Hemisphere ◽  
Energy Flux ◽  
Mirror Image ◽  
Emission Data ◽  
Data Set ◽  
Total Energy Flux ◽  
The Imf

Abstract A dawn–dusk asymmetry in many high-latitude ionospheric and magnetospheric phenomena, including the aurora, can be linked to the east–west (y) component of the interplanetary magnetic field (IMF). Owing to the scarcity of observations in the Southern Hemisphere, most of the previous findings are associated with the Northern Hemisphere. It has long been suspected that if the IMF By component also produces a dawn–dusk asymmetry and/or a mirror image in the Southern Hemisphere as predicted by some theories. The present study explores the effect of the IMF By component on the dayside aurora from both hemispheres by analyzing the auroral emission data from the Global UltraViolet scanning spectrograph Imager on board the Thermosphere Ionosphere Mesosphere Energetics and Dynamics mission spacecraft from 2002 to 2007. The data set comprises 28,774 partial images of the northern hemispheric oval and 29,742 partial images of the southern hemispheric oval, allowing for a statistical analysis. It is found that even though auroras in different regions of the dayside oval respond differently to the orientation of the IMF By component, their responses are opposite between the two hemispheres. For example, at ~ 1400–1600 MLT in the Northern Hemisphere, where the so-called 1500 MLT auroral hot spots occur, peak auroral energy flux is larger for negative IMF By comparing to positive IMF By. The response is reversed in the Southern Hemisphere. The present study also suggests that the total energy flux does not change with the IMF By orientation change. This result is consistent with a larger (smaller) convection vortex in the postnoon sector for IMF By < 0 (By > 0) resulting from anti-parallel merging.

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