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The ACE-FTS (Atmospheric Chemistry Experiment-Fourier Transform Spectrometer) instrument on the Canadian SCISAT satellite, which has been in operation for over 12 years, has the capability of deriving stratospheric profiles of many of the NO (N+NO+NO+NO+2×NO+HNO+HNO+ClONO+BrONO) species. Version 2.2 of ACE-FTS NO, NO, HNO, NO, and ClONO has previously been validated, and this study compares the most recent version (v3.5) of these five ACE-FTS products to spatially and temporally coincident measurements from other satellite instruments-GOMOS, HALOE, MAESTRO, MIPAS, MLS, OSIRIS, POAM III, SAGE III, SCIAMACHY, SMILES, and SMR. For each ACE-FTS measurement, a photochemical box model was used to simulate the diurnal variations of the NOy species and the ACE-FTS measurements were scaled to the local times of the coincident measurements. The comparisons for all five species show good agreement with correlative satellite measurements. For NO in the altitude range of 25-50 km, ACE-FTS typically agrees with correlative data to within .10 %. Instrumentaveraged mean relative differences are approximately.10% at 30-40 km for NO, within-7% at 8-30 km for HNO, better than.7% at 21-34 km for local morning NO, and better than.8% at 21-34 km for ClONO. Where possible, the variations in the mean differences due to changes in the comparison local time and latitude are also discussed.©2016 Author(s)., The Atmospheric Chemistry Experiment is a Canadian-led mission mainly supported by the CSA. Odin is a Swedish-led satellite project funded jointly by Sweden (Swedish National Space Board), Canada (CSA), France (Centre National d'Etudes Spatiales), and Finland (Tekes), with support by the third-party mission programme of the European Space Agency (ESA). Coauthor CER was funded by NASA grant NNX14AH54G. The University of Bremen team was funded in parts by the DLR Space Agency (Germany) and by the University and State of Bremen.

Stratospheric transport in global circulation models and chemistry–climate models is an important component in simulating the recovery of the ozone layer as well as changes in the climate system. The Brewer–Dobson circulation is not well constrained by observations and further investigation is required to resolve uncertainties related to the mechanisms driving the circulation. This study has assessed the specified dynamics mode of the Canadian Middle Atmosphere Model (CMAM30) by comparing to the Atmospheric Chemistry Experiment Fourier transform spectrometer (ACE-FTS) profile measurements of CFC-11 (CCl3F), CFC-12 (CCl2F2), and N2O. In the CMAM30 specified dynamics simulation, the meteorological fields are nudged using the ERA-Interim reanalysis and a specified tracer was employed for each species, with hemispherically defined surface measurements used as the boundary condition. A comprehensive sampling technique along the line of sight of the ACE-FTS measurements has been utilized to allow for direct comparisons between the simulated and measured tracer concentrations. The model consistently overpredicts tracer concentrations of CFC-11, CFC-12, and N2O in the lower stratosphere, particularly in the northern hemispheric winter and spring seasons. The three mixing barriers investigated, including the polar vortex, the extratropical tropopause, and the tropical pipe, show that there are significant inconsistencies between the measurements and the simulations. In particular, the CMAM30 simulation underpredicts mixing efficiency in the tropical lower stratosphere during the June–July–August season.

The long-term evolution of the vertical column abundance of carbon tetrafluoride (CF4) above the high-altitude Jungfraujoch station (Swiss Alps, 46.5° N, 8.0° E, 3580 m a.s.l.) has been derived from the spectrometric analysis of Fourier transform infrared solar spectra recorded at that site between 1989 and 2012. The investigation is based on a multi-microwindow approach, two encompassing pairs of absorption lines belonging to the R-branch of the strong ν3 band of CF4 centered at 1283 cm−1, and two additional ones to optimally account for weak but overlapping HNO3 interferences. The analysis reveals a steady accumulation of the very long-lived CF4 above the Jungfraujoch at mean rates of (1.38 ± 0.11) × 1013 molec cm−2 yr−1 from 1989 to 1997, and (0.98 ± 0.02) × 1013 molec cm−2 yr−1 from 1998 to 2012, which correspond to linear growth rates of 1.71 ± 0.14 and 1.04 ± 0.02% yr−1 respectively referenced to 1989 and 1998. Related global CF4 anthropogenic emissions required to sustain these mean increases correspond to 15.8 ± 1.3 and 11.1 ± 0.2 Gg yr−1 over the above specified time intervals. Findings reported here are compared and discussed with respect to relevant northern mid-latitude results obtained remotely from space and balloons as well as in situ at the ground, including new gas chromatography mass spectrometry measurements performed at the Jungfraujoch since 2010.

International audience

We investigate the spatial and temporal distribution of hydrogen cyanide (HCN) in the upper troposphere through numerical simulations and comparison with observations from a space-based instrument. To perform the simulations, we used the Global Environmental Multiscale Air Quality model (GEM-AQ), which is based on the three-dimensional global multiscale model developed by the Meteorological Service of Canada for operational weather forecasting. The model was run for the period 2004–2006 on a 1.5°×1.5° global grid with 28 hybrid vertical levels from the surface up to 10 hPa. Objective analysis data from the Canadian Meteorological Centre were used to update the meteorological fields every 24 h. Fire emission fluxes of gas species were generated by using year-specific inventories of carbon emissions with 8-day temporal resolution from the Global Fire Emission Database (GFED) version 2. The model output is compared with HCN profiles measured by the Atmospheric Chemistry Experiment Fourier Transform Spectrometer (ACE-FTS) instrument onboard the Canadian SCISAT-1 satellite. High values of up to a few ppbv are observed in the tropics in the Southern Hemisphere; the enhancement in HCN volume mixing ratios in the upper troposphere is most prominent in October. Low upper-tropospheric mixing ratios of less than 100 pptv are mostly recorded at middle and high latitudes in the Southern Hemisphere in May–July. Mixing ratios in Northern Hemisphere peak in the boreal summer. The amplitude of the seasonal variation is less pronounced than in the Southern Hemisphere. The comparison with the satellite data shows that in the upper troposphere GEM-AQ performs well globally for all seasons, except at northern high and middle latitudes in summer, where the model has a large negative bias, and in the tropics in winter and spring, where it exhibits large positive bias. This may reflect inaccurate emissions or possible inaccuracies in the emission profile. The model is able to explain most of the observed variability in the upper troposphere HCN field, including the interannual variations in the observed mixing ratio. A complementary comparison with daily total columns of HCN from two middle latitude ground-based stations in Northern Japan for the same simulation period shows that the model captures the observed seasonal variation and also points to an underestimation of model emissions in the Northern Hemisphere in the summer. The estimated average global emission equals 1.3 Tg N yr−1. The average atmospheric burden is 0.53 Tg N, and the corresponding lifetime is 4.9 months.

Low-resolution atmospheric thermal emission spectra collected by balloon-borne radiometers over the time span of 1990–2002 are used to retrieve vertical profiles of HNO3, CFC-11 and CFC-12 volume mixing ratios between approximately 10 and 35 km altitude. All of the data analyzed have been collected from launches from a Northern Hemisphere mid-latitude site, during late summer, when stratospheric dynamic variability is at a minimum. The retrieval technique incorporates detailed forward modeling of the instrument and the radiative properties of the atmosphere, and obtains a best fit between modeled and measured spectra through a combination of onion-peeling and optimization steps. The retrieved HNO3 profiles are consistent over the 12-year period, and are consistent with recent measurements by the Atmospheric Chemistry Experiment-Fourier transform spectrometer satellite instrument. We therefore find no evidence of long-term changes in the HNO3 summer mid-latitude profile, although the uncertainty of our measurements precludes a conclusive trend analysis.

Recommendations of an IUPAC Task Group, formed in 2011 on “Intensities and line shapes in high-resolution spectra of water isotopologues from experiment and theory”(Project No. 2011-022-2-100), on line profiles of isolated high-resolution rotational-vibrational transitions perturbed by neutral gas-phase molecules are presented. The well-documented inadequacies of the Voigt profile, used almost universally by databases and radiative-transfer codes to represent pressure effects and Doppler broadening in isolated vibrational-rotational and pure rotational transitions of the water molecule, have resulted in the development of a variety of alternative line profile models. These models capture more of the physics of the influence of pressure on line shapes but, in general, at the price of greater complexity. The Task Group recommends that the partially-Correlated quadratic-Speed-Dependent Hard-Collision profile should be adopted as the appropriate model for high-resolution spectroscopy. For simplicity this should be called the Hartmann–Tran profile (HTP). This profile is sophisticated enough to capture the various collisional contributions to the isolated line shape, can be computed in a straightforward and rapid manner, and reduces to simpler profiles, including the Voigt profile, under certain simplifying assumptions. For further details see: J. Tennyson et al, Pure Appl. Chem., 2014, in press.

We present the results of extensive validation program of Version V5R_O3_220 of ozone vertical profiles retrieved with IMK/IAA MIPAS scientific level 2 processor from version 5 of spectral Level 1 files provided by ESA. The time period covered corresponds to Reduced Resolution period of MIPAS instrument, i.e. January 2005-present. The comparison with satellite instruments includes ACE-FTS, MLS, GOMOS, SCIAMACHY, OSIRIS, HALOE and POAM. The comparison with ground-based instruments includes 5 stations from SHADOZ Network and LIDAR from NDACC network. Also, the comparison with Mark IV balloon measurements is presented. For each reference dataset, bias determination and precision validation are performed.

The 2006 Canadian Arctic ACE (Atmospheric Chemistry Experiment) Validation Campaign collected measurements at the Polar Environment Atmospheric Research Laboratory (PEARL, 80.05° N, 86.42° W, 610 m above sea level) at Eureka, Canada from 17 February to 31 March 2006. Two of the ten instruments involved in the campaign, both Fourier transform spectrometers (FTSs), were operated simultaneously, recording atmospheric solar absorption spectra. The first instrument was an ABB Bomem DA8 high-resolution infrared FTS. The second instrument was the Portable Atmospheric Research Interferometric Spectrometer for the Infrared (PARIS-IR), the ground-based version of the satellite-borne FTS on the ACE satellite (ACE-FTS). From the measurements collected by these two ground-based instruments, total column densities of seven stratospheric trace gases (O3, HNO3, NO2, HCl, HF, NO, and ClONO2 were retrieved using the optimal estimation method and these results were compared. Since the two instruments sampled the same portions of atmosphere by synchronizing observations during the campaign, the biases in retrieved columns from the two spectrometers represent the instrumental differences. These differences were consistent with those seen in previous FTS intercomparison studies. Partial column results from the ground-based spectrometers were also compared with partial columns derived from ACE-FTS version 2.2 (including updates for O3, HDO and N2O5 profiles and the differences found were consistent with the other validation comparison studies for the ACE-FTS version 2.2 data products. Column densities of O3, HCl, ClONO2, and HNO3 from the three FTSs were normalized with respect to HF and used to probe the time evolution of the chemical constituents in the atmosphere over Eureka during spring 2006.

International audience; The Atmospheric Chemistry Experiment (ACE) mission was launched in August 2003 to sound the atmosphere by solar occultation. Water vapour (H2O), one of the most important molecules for climate and atmospheric chemistry, is one of the key species provided by the two principal instruments, the infrared Fourier Transform Spectrometer (ACE-FTS) and the MAESTRO UV-Visible spectrometer (ACE-MAESTRO). The first instrument performs measurements on several lines in the 1362?2137 cm?1 range, from which vertically resolved H2O concentration profiles are retrieved, from 7 to 90 km altitude. ACE-MAESTRO measures profiles using the water absorption band in the near infrared part of the spectrum at 926.0?969.7 nm. This paper presents a comprehensive validation of the ACE-FTS profiles. We have compared the H2O volume mixing ratio profiles with space-borne (SAGE II, HALOE, POAM III, MIPAS, SMR) observations and measurements from balloon-borne frostpoint hygrometers and a ground based lidar. We show that the ACE-FTS measurements provide H2O profiles with small retrieval uncertainties in the stratosphere (better than 5% from 15 to 70 km, gradually increasing above). The situation is unclear in the upper troposphere, due mainly to the high variability of the water vapour volume mixing ratio in this region. A new water vapour data product from the ACE-MAESTRO (Measurement of Aerosol Extinction in the Stratosphere and Troposphere Retrieved by Occultation) is also presented and initial comparisons with ACE-FTS are discussed.

Vertical profiles of NO2 and NO have been obtained from solar occultation measurements by the Atmospheric Chemistry Experiment (ACE), using an infrared Fourier Transform Spectrometer (ACE-FTS) and (for NO2) an ultraviolet-visible-near-infrared spectrometer, MAESTRO (Measurement of Aerosol Extinction in the Stratosphere and Troposphere Retrieved by Occultation). In this paper, the quality of the ACE-FTS version 2.2 NO2 and NO and the MAESTRO version 1.2 NO2 data are assessed using other solar occultation measurements (HALOE, SAGE II, SAGE III, POAM III, SCIAMACHY), stellar occultation measurements (GOMOS), limb measurements (MIPAS, OSIRIS), nadir measurements (SCIAMACHY), balloon-borne measurements (SPIRALE, SAOZ) and ground-based measurements (UV-VIS, FTIR). Time differences between the comparison measurements were reduced using either a tight coincidence criterion, or where possible, chemical box models. ACE-FTS NO2 and NO and the MAESTRO NO2 are generally consistent with the correlative data. The ACE-FTS and MAESTRO NO2 volume mixing ratio (VMR) profiles agree with the profiles from other satellite data sets to within about 20% between 25 and 40 km, with the exception of MIPAS ESA (for ACE-FTS) and SAGE II (for ACE-FTS (sunrise) and MAESTRO) and suggest a negative bias between 23 and 40 km of about 10%. MAESTRO reports larger VMR values than the ACE-FTS. In comparisons with HALOE, ACE-FTS NO VMRs typically (on average) agree to ±8% from 22 to 64 km and to +10% from 93 to 105 km, with maxima of 21% and 36%, respectively. Partial column comparisons for NO2 show that there is quite good agreement between the ACE instruments and the FTIRs, with a mean difference of +7.3% for ACE-FTS and +12.8% for MAESTRO.

International audience; The Atmospheric Chemistry Experiment (ACE) satellite was launched on 12 August 2003. Its two instruments measure vertical profiles of over 30 atmospheric trace gases by analyzing solar occultation spectra in the ultraviolet/visible and infrared wavelength regions. The reservoir gases HNO3, ClONO2, and N2O5 are three of the key species provided by the primary instrument, the ACE Fourier Transform Spectrometer (ACE-FTS). This paper describes the ACE-FTS version 2.2 data products, including the N2O5 update, for the three species and presents validation comparisons with available observations. We have compared volume mixing ratio (VMR) profiles of HNO3, ClONO2, and N2O5 with measurements by other satellite instruments (SMR, MLS, MIPAS), aircraft measurements (ASUR), and single balloon-flights (SPIRALE, FIRS-2). Partial columns of HNO3 and ClONO2 were also compared with measurements by ground-based Fourier Transform Infrared (FTIR) spectrometers. Overall the quality of the ACE-FTS v2.2 HNO3 VMR profiles is good from 18 to 35 km. For the statistical satellite comparisons, the mean absolute differences are generally within ±1 ppbv (±20%) from 18 to 35 km. For MIPAS and MLS comparisons only, mean relative differences lie within ±10% between 10 and 36 km. ACE-FTS HNO3 partial columns (~15–30 km) show a slight negative bias of -1.3% relative to the ground-based FTIRs at latitudes ranging from 77.8° S–76.5° N. Good agreement between ACE-FTS ClONO2 and MIPAS, using the Institut für Meteorologie und Klimaforschung and Instituto de Astrofisica de Andalucia (IMK-IAA) data processor is seen. Mean absolute differences are typically within ±0.01 ppbv between 16 and 27 km and less than +0.09 ppbv between 27 and 34 km. The ClONO2 partial column comparisons show varying degrees of agreement, depending on the location and the quality of the FTIR measurements. Good agreement was found for the comparisons with the midlatitude Jungfraujoch partial columns for which the mean relative difference is 4.7%. ACE-FTS N2O5 has a low bias relative to MIPAS IMK-IAA, reaching -0.25 ppbv at the altitude of the N2O5 maximum (around 30 km). Mean absolute differences at lower altitudes (16–27 km) are typically -0.05 ppbv for MIPAS nighttime and ±0.02 ppbv for MIPAS daytime measurements.

Mechanisms for transporting and dehydrating air across the tropical tropopause layer (TTL) are investigated with a conceptual two dimensional (2-D) model. The 2-D TTL model combines the Holton and Gettelman cold trap dehydration mechanism (Holton and Gettelman, 2001) with the two column convection model of Folkins and Martin (2005). We investigate 3 possible transport scenarios through the TTL: 1) slow uniform ascent across the level of zero radiative heating without direct convective mixing, 2) convective mixing of H2O vapor at 100% relative humidity with respect to ice (RHi) with no ice retention, and 3) convective mixing of extremely subsaturated air (100% RHi following the moist adiabatic temperature above the level of neutral buoyancy) with sufficient ice retention such that total H2O is 100%RHi. The three mechanisms produce similar seasonal cycles for H2O that are in good quantitative agreement with the Aura Microwave Limb Sounder (MLS) measurements. We use Aura MLS measurement of CO and Atmospheric Chemistry Experiment-Fourier Transform Spectrometer measurement of HDO to distinguish among the transport mechanisms. Model comparisons with the observations support the view that H2O is predominantly controlled by regions having the lowest cold point tropopause temperature but the trace species CO and HDO support the convective mixing of dry air and lofted ice. The model provides some insight into the processes affecting the long term trends observed in stratospheric H2O.

The UV-visible Global Ozone Monitoring by Occultation of Stars (GOMOS) instrument onboard Envisat performs nighttime measurements of ozone, NO2, NO3 and of the aerosol extinction, using the stellar occultation method. We have conducted a validation exercise using various balloon-borne instruments in different geophysical conditions from 2002 to 2006, using GOMOS measurements performed with stars of different magnitudes. GOMOS and balloon-borne vertical columns in the middle stratosphere are in excellent agreement for ozone and NO2. Some discrepancies can appear between GOMOS and balloon-borne vertical profiles for the altitude and the amplitude of the concentration maximum. These discrepancies are randomly distributed, and no bias is detected. The accuracy of individual profiles in the middle stratosphere is 10 % for ozone and 25 % for NO2. On the other hand, the GOMOS NO3 retrieval is difficult and no direct validation can be conducted. The GOMOS aerosol content is also well estimated, but the wavelength dependence can be better estimated if the aerosol retrieval is performed only in the visible domain. We can conclude that the GOMOS operational retrieval algorithm works well and that GOMOS has fully respected its primary objective for the study of the trends of species in the middle stratosphere, using the profiles in a statistical manner. Some individual profiles can be partly inaccurate, in particular in the lower stratosphere. Improvements could be obtained by reprocessing some GOMOS transmissions in case of specific studies in the middle and lower stratosphere when using the individual profiles.

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.

International audience; In the course of our study of the upper tropospheric composition with the infrared Atmospheric Chemistry Experiment – Fourier Transform Spectrometer (ACE–FTS), we found an occultation sequence that on 8 October 2005, sampled a remarkable plume near the east coast of Tanzania. Model simulations of the CO distribution in the Southern hemisphere are performed for this period and they suggest that the emissions for this event likely originated from a nearby forest fire, after which the plume was transported from the source region to the upper troposphere. Taking advantage of the very high signal-to-noise ratio of the ACE–FTS spectra over a wide wavenumber range (750–4400 cm-1), we present in-depth analyses of the chemical composition of this plume in the middle and upper troposphere, focusing on the measurements of weakly absorbing pollutants. For this specific biomass burning event, we report simultaneous observations of an unprecedented number of organic species. Measurements of C2H4 (ethene), C3H4 (propyne), H2CO (formaldehyde), C3H6O (acetone) and CH3COO2NO2 (peroxyacetylnitrate, abbreviated as PAN) are the first reported detections using infrared occultation spectroscopy from satellites. Based on the lifetime of the emitted species, we discuss the photochemical age of the plume and also report, whenever possible, the enhancement ratios relative to CO.

International audience; The purpose of this study is to perform a global search of the upper troposphere (z?10 km) for enhancements of nitrogen dioxide and determine their sources. This is the first application of satellite-based limb scattering to study upper tropospheric NO2. We have searched two years (May 2003?May 2005) of OSIRIS (Optical Spectrograph and Infrared Imager System) operational NO2 concentrations (version 2.3/2.4) to find large enhancements in the observations by comparing with photochemical box model calculations and by identifying local maxima in NO2 volume mixing ratio. We find that lightning is the main production mechanism responsible for the large enhancements in OSIRIS NO2 observations as expected. Similar patterns in the abundances and spatial distribution of the NO2 enhancements are obtained by perturbing the lightning within the GEOS-Chem 3-dimensional chemical transport model. In most cases, the presence of lightning is confirmed with coincident imagery from LIS (Lightning Imaging Sensor) and the spatial extent of the NO2 enhancement is mapped using nadir observations of tropospheric NO2 at high spatial resolution from SCIAMACHY (Scanning Imaging Absorption Spectrometer for Atmospheric Chartography) and OMI (Ozone Monitoring Instrument). The combination of the lightning and chemical sensors allows us to investigate globally the role of lightning to the abundance of NO2 in the upper troposphere (UT). Lightning contributes 60% of the tropical upper tropospheric NO2 in GEOS-Chem simulations. The spatial and temporal distribution of NO2 enhancements from lightning (May 2003?May 2005) is investigated. The enhancements generally occur at 12 to 13 km more frequently than at 10 to 11 km. This is consistent with the notion that most of the NO2 is forming and persisting near the cloud top altitude in the tropical upper troposphere. The latitudinal distribution is mostly as expected. In general, the thunderstorms exhibiting weaker vertical development (e.g. 11?z?13 km) extend latitudinally as far poleward as 45° but the thunderstorms with stronger vertical development (z?14 km) tend to be located within 33° of the equator. There is also the expected hemispheric asymmetry in the frequency of the NO2 enhancements, as most were observed in the northern hemisphere for the period analyzed.

International audience; The Michelson Interferometer for Passive Atmospheric Sounding (MIPAS) onboard the ENVISAT satellite provides profiles of temperature and various trace-gases from limb-viewing mid-infrared emission measurements. The stratospheric nitric acid (HNO3) from September 2002 to March 2004 was retrieved from the MIPAS observations using the science-oriented data processor developed at the Institut für Meteorologie und Klimaforschung (IMK), which is complemented by the component of non-local thermodynamic equilibrium (non-LTE) treatment from the Instituto de Astrofísica de Andalucía (IAA). The IMK-IAA research product, different from the ESA operational product, is validated in this paper by comparison with a number of reference data sets. Individual HNO3 profiles of the IMK-IAA MIPAS show good agreement with those of the balloon-borne version of MIPAS (MIPAS-B) and the infrared spectrometer MkIV, with small differences of less than 0.5 ppbv throughout the entire altitude range up to about 38 km, and below 0.2 ppbv above 30 km. However, the degree of consistency is largely affected by their temporal and spatial coincidence, and differences of 1 to 2 ppbv may be observed between 22 and 26 km at high latitudes near the vortex boundary, due to large horizontal inhomogeneity of HNO3. Statistical comparisons of MIPAS IMK-IAA HNO3 VMRs with respect to those of satellite measurements of Odin/SMR, ILAS-II, ACE-FTS, as well as the MIPAS ESA product show good consistency. The mean differences are generally ±0.5 ppbv and standard deviations of the differences are of 0.5 to 1.5 ppbv. The maximum differences are 2.0 ppbv around 20 to 25 km. This gives confidence in the general reliability of MIPAS HNO3 VMR data and the other three satellite data sets.

International audience; First measurements from space of upper tropospheric and lower stratospheric methanol profiles within aged fire plumes are reported. Elevated levels of methanol at 0–45° S from 30 September to 3 November 2004 have been measured by the high resolution infrared spectrometer ACE-FTS onboard the SCISAT satellite. Methanol volume mixing ratios higher than 4000 pptv are detected and are strongly correlated with other fire products such as CO, C2H6, and HCN. A sensitivity study of the methanol retrieval, accounting for random and systematic contributions, shows that the retrieved methanol profile is reliable from 8.5 to 16.5 km, with an accuracy of about 20% for measurements inside polluted air masses. The upper tropospheric enhancement ratio of methanol with respect to CO is estimated from the correlation plot between methanol and CO for aged tropical biomass burning plumes. This ratio is in good agreement with the ratio measured in the free troposphere (up to 12 km) by recent aircraft studies and does not suggest any secondary production of methanol by oxidation in aged biomass burning plumes.