References of "Mahieu, Emmanuel"
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See detailObserved and simulated atmospheric inorganic fluorine: short term and long term trends related to circulation changes
Prignon, Maxime ULiege; Bernath, P. F.; Chabrillat, S. et al

Conference (2020, October 15)

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See detailTrends of atmospheric water vapour in Switzerland from ground-based radiometry, FTIR and GNSS data
Bernet, L.; Brockmann, E.; von Clarmann, T. et al

in Atmospheric Chemistry and Physics (2020), 20(19), 11223--11244

Vertically integrated water vapour (IWV) is expected to increase globally in a warming climate. To determine whether IWV increases as expected on a regional scale, we present IWV trends in Switzerland ... [more ▼]

Vertically integrated water vapour (IWV) is expected to increase globally in a warming climate. To determine whether IWV increases as expected on a regional scale, we present IWV trends in Switzerland from ground-based remote sensing techniques and reanalysis models, considering data for the time period 1995 to 2018. We estimate IWV trends from a ground-based microwave radiometer in Bern, from a Fourier transform infrared (FTIR) spectrometer at Jungfraujoch, from reanalysis data (ERA5 and MERRA-2) and from Swiss ground-based Global Navigation Satellite System (GNSS) stations. Using a straightforward trend method, we account for jumps in the GNSS data, which are highly sensitive to instrumental changes. We found that IWV generally increased by 2 % per decade to 5 % per decade,with deviating trends at some GNSS stations. Trends were significantly positive at 17 % of all GNSS stations, which of-ten lie at higher altitudes (between 850 and 1650 m above sea level). Our results further show that IWV in Bern scales to air temperature as expected (except in winter), but the IWV–temperature relation based on reanalysis data in the whole of Switzerland is not clear everywhere. In addition to our positive IWV trends, we found that the radiometer in Bern agrees within 5 % with GNSS and reanalyses. At the Jungfraujoch high-altitude station, we found a mean difference of 0.26 mm (15 %) between the FTIR and coincident GNSS data, improving to 4 % after an antenna update in 2016. In general,we showed that ground-based GNSS data are highly valuable for climate monitoring, given that the data have been homogeneously reprocessed and that instrumental changes are accounted for. We found a response of IWV to rising temperature in Switzerland, which is relevant for projected changes in local cloud and precipitation processes [less ▲]

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See detailObserved Hemispheric Asymmetry in Stratospheric Transport Trends From 1994 to 2018
Strahan, Susan E.; Smale, Dan; Douglass, Anne R. et al

in Geophysical Research Letters (2020), 47(17), 2020088567

Abstract Total columns of the trace gases nitric acid (HNO3) and hydrogen chloride (HCl) are sensitive to variations in the lower stratospheric age of air, a quantity that describes transport time scales ... [more ▼]

Abstract Total columns of the trace gases nitric acid (HNO3) and hydrogen chloride (HCl) are sensitive to variations in the lower stratospheric age of air, a quantity that describes transport time scales in the stratosphere. Analyses of HNO3 and HCl columns from the Network for the Detection of Atmospheric Composition Change panning 77°S to 79°N have detected changes in the extratropical stratospheric transport circulation from 1994 to 2018. The HNO3 and HCl analyses combined with the age of air from a simulation using the MERRA2 reanalysis show that the Southern Hemisphere lower stratosphere has become 1 month/decade younger relative to the Northern Hemisphere, largely driven by the Southern Hemisphere transport circulation. The analyses reveal multiyear anomalies with a 5- to 7-year period driven by interactions between the circulation and the quasi-biennial oscillation in tropical winds. This hitherto unrecognized variability is large relative to hemispheric transport trends and may bias ozone trend regressions. [less ▲]

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See detailA statistical analysis of time trends in atmospheric ethane
Friedrich, Marina; Beutner, Eric; Reuvers, Hanno et al

in Climatic Change (2020)

Ethane is the most abundant non-methane hydrocarbon in the Earth’s atmosphere and an important precursor of tropospheric ozone through various chemical pathways. Ethane is also an indirect greenhouse gas ... [more ▼]

Ethane is the most abundant non-methane hydrocarbon in the Earth’s atmosphere and an important precursor of tropospheric ozone through various chemical pathways. Ethane is also an indirect greenhouse gas (global warming potential), influencing the atmospheric lifetime of methane through the consumption of the hydroxyl radical (OH). Understanding the development of trends and identifying trend reversals in atmospheric ethane is thereforecrucial. Our dataset consists of four series of daily ethane columns. As with many otherdecadal time series, our data are characterized by autocorrelation, heteroskedasticity, and seasonal effects. Additionally, missing observations due to instrument failure or unfavorable measurement conditions are common in such series. The goal of this paper is therefore to analyze trends in atmospheric ethane with statistical tools that correctly address these data features. We present selected methods designed for the analysis of time trends and trend reversals. We consider bootstrap inference on broken linear trends and smoothly varying nonlinear trends. In particular, for the broken trend model, we propose a bootstrap method for inference on the break location and the corresponding changes in slope. For the smooth trend model, we construct simultaneous confidence bands around the non parametrically estimated trend. Our autoregressive wild bootstrap approach, combined with a seasonal filter, is able to handle all issues mentioned above (we provide R code for all proposed methods on https://www.stephansmeekes.nl/code.). [less ▲]

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See detailTROPOMI--Sentinel-5 Precursor formaldehyde validation using an extensive network of ground-based Fourier-transform infrared stations
Vigouroux, C.; Langerock, B.; Bauer Aquino, C. A. et al

in Atmospheric Measurement Techniques (2020), 13(7), 3751--3767

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See detailFourier transform infrared time series of tropospheric HCN in eastern China: seasonality interannual variability, and source attribution
Sun, Y.; Liu, C.; Zhang, L. et al

in Atmospheric Chemistry and Physics (2020), 20(9), 5437--5456

We analyzed seasonality and interannual variability of tropospheric hydrogen cyanide (HCN) columns in densely populated eastern China for the first time. The results were derived from solar absorption ... [more ▼]

We analyzed seasonality and interannual variability of tropospheric hydrogen cyanide (HCN) columns in densely populated eastern China for the first time. The results were derived from solar absorption spectra recorded with a ground-based high-spectral-resolution Fourier transform infrared (FTIR) spectrometer in Hefei (31°54′ N, 117°10′ E) between 2015 and 2018. The tropospheric HCN columns over Hefei, China, showed significant seasonal variations with three monthly mean peaks throughout the year. The magnitude of the tropospheric HCN column peaked in May, September, and December. The tropospheric HCN column reached a maximum monthly mean of (9.8±0.78)E15 molecules cm−2 in May and a minimum monthly mean of (7.16±0.75)E15 molecules cm−2 in November. In most cases, the tropospheric HCN columns in Hefei (32°N) are higher than the FTIR observations in Ny-Ålesund (79°N), Kiruna (68°N), Bremen (53°N), Jungfraujoch (47°N), Toronto (44°N), Rikubetsu (43°N), Izana (28°N), Mauna Loa (20°N), La Reunion Maido (21°S), Lauder (45°S), and Arrival Heights (78°S) that are affiliated with the Network for Detection of Atmospheric Composition Change (NDACC). Enhancements of tropospheric HCN column were observed between September 2015 and July 2016 compared to the same period of measurements in other years. The magnitude of the enhancement ranges from 5 % to 46 % with an average of 22 %. Enhancement of tropospheric HCN (ΔHCN) is correlated with the concurrent enhancement of tropospheric CO (ΔCO), indicating that enhancements of tropospheric CO and HCN were due to the same sources. The GEOS-Chem tagged CO simulation, the global fire maps, and the potential source contribution function (PSCF) values calculated using back trajectories revealed that the seasonal maxima in May are largely due to the influence of biomass burning in Southeast Asia (SEAS) (41±13.1 %), Europe and boreal Asia (EUBA) (21±9.3 %), and Africa (AF) (22±4.7 %). The seasonal maxima in September are largely due to the influence of biomass burnings in EUBA (38±11.3 %), AF (26±6.7 %), SEAS (14±3.3 %), and North America (NA) (13.8±8.4 %). For the seasonal maxima in December, dominant contributions are from AF (36±7.1 %), EUBA (21±5.2 %), and NA (18.7±5.2 %). The tropospheric HCN enhancement between September 2015 and July 2016 at Hefei (32°N) was attributed to an elevated influence of biomass burnings in SEAS, EUBA, and Oceania (OCE) in this period. In particular, an elevated number of fires in OCE in the second half of 2015 dominated the tropospheric HCN enhancement between September and December 2015. An elevated number of fires in SEAS in the first half of 2016 dominated the tropospheric HCN enhancement between January and July 2016. [less ▲]

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See detailN2O-based climatology of the Brewer Dobson Circulation in WACCM, a chemical reanalysis and a CTM driven by four dynamical reanalyses
Minganti, Daniele ULiege; Chabrillat, Simon; Christophe, Yves et al

Conference (2020, May 05)

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See detailDOAS measurements of NO2 and H2CO at Kinshasa and Comparisons with Satellites Observations
Yombo Phaka, Rodriguez ULiege; Merlaud, Alexis; Pinardi, Gaia et al

Poster (2020, April 04)

Africa experiences a fast urban inhabitants growth, caused by the largest population boom in the world, combined with rural exodus. Many cities are heavily affected by air pollution. It is therefore ... [more ▼]

Africa experiences a fast urban inhabitants growth, caused by the largest population boom in the world, combined with rural exodus. Many cities are heavily affected by air pollution. It is therefore essential to monitor the concentrations of the various polluting species such as NO2, HCHO, O3 and aerosols, which have a direct impact on the population health. The sources of pollutant in Africa are different from those found in Europe. For example, forest fires and household cooking largely contribute to the NO2 and HCHO burdens in Central Africa. However, many large African cities, such as the City of Kinshasa, capital of the Democratic Republic of Congo, do not have atmospheric measurement instruments. In order to tackle the lack of measurements in Kinshasa, the Royal Belgian Institute of Space Aeronomy (BIRA-IASB) has, in collaboration with the University of Kinshasa (UniKin), installed an optical remote sensing instrument on the UniKin site (-4.42°S, 15.31°E). Installed in May 2017, the instrument has been in operation until today and provides data to measure the column amounts of several polluting species in the atmosphere of Kinshasa. The instrument is based on a compact AVANTES spectrometer covering the spectral range 290 - 450 nm with 0.7 nm resolution. The spectrometer is a Czerny-Turner type with an entry slit of 50 μm wide, and an array of 1200 l/mm. A 10 m long and 600 μm diameter optical fiber is connected to the spectrometer to receive the incident light beam from the sky. Measurements were mainly made by looking in a fixed direction until November 2019. Since then, a Multi-Axis geometry (MAX-DOAS) has been implemented. The measurements provided by this DOAS instrument allowed us to start studying the atmosphere of Kinshasa using the QDOAS software, which allows us to find the oblique columns of different observed species. This poster will present the instrument, the database and the procedure used to convert these oblique columns into vertical columns, using the air mass factors calculated with the radiative transfer model. We also present our first MAX-DOAS results, analyzed using the retrieval tools of the ESA FRM4DOAS project. The study of current results clearly shows the signature of polluting species such as NO2, HCHO in the atmosphere of Kinshasa. We also use simulations by the GEOS-Chem chemistry transport model to evaluate the magnitude of the emissions needed to explain the observed column amounts. These observations made in Kinshasa could contribute to the validation of satellite products and the refinement of models. We present a first comparison of Kinshasa's ground-based observations with those of the OMI and TROPOMI satellites [less ▲]

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See detailSpaceborne Measurements of Formic and Acetic Acid: A Global View of the Regional Sources
Franco, B; Clarisse, L; Stavrakou, T et al

in Geophysical Research Letters (2020), 47

Formic (HCOOH) and acetic acid (CH3COOH) are the most abundant carboxylic acids in the Earth’s atmosphere and key compounds to aqueous-phase chemistry. Here we present the first distributions of CH3COOH ... [more ▼]

Formic (HCOOH) and acetic acid (CH3COOH) are the most abundant carboxylic acids in the Earth’s atmosphere and key compounds to aqueous-phase chemistry. Here we present the first distributions of CH3COOH retrieved from the 2007–2018 satellite observations of the nadir-looking Infrared Atmospheric Sounding Interferometer (IASI), using a neural network-based retrieval approach. A joint analysis with the IASI HCOOH product reveals that the two species exhibit similar distributions, seasonality and atmospheric burden, pointing to major common sources. We show that their abundance is highly correlated to isoprene and monoterpenes emissions, as well as to biomass burning. Over Africa, evidence is provided that residual smoldering combustion might be a major driver of the HCOOH and CH3COOH seasonality. Earlier seasonal enhancement of HCOOH at Northern Hemisphere middle and high latitudes, and late seasonal secondary peaks of CH3COOH in the tropics, suggest that sources and production pathways specific to each species are also at play. [less ▲]

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See detailQuantification of Stratospheric Ozone Recovery Due to Anthropogenic Halogens
Salawitch, R. J.; Tribett, W.; Wales, P. et al

Conference (2020, January 14)

Human release of CFCs and other ozone depleting substances (ODS) has led to a slow, steady erosion of the thickness of the global ozone layer over the past several decades. The ozone layer has begun to ... [more ▼]

Human release of CFCs and other ozone depleting substances (ODS) has led to a slow, steady erosion of the thickness of the global ozone layer over the past several decades. The ozone layer has begun to recover due to actions taken under the Montreal Protocol, which has led to a decrease in the atmospheric abundance of ozone depleting substances. Yet, unreported emissions of CFC-11 have led to a slower than expected decline, and there has been a rise in the atmospheric abundance of chlorinated very short lived (VSL) compounds not regulated under the Montreal Protocol. In this presentation, we examine time series of ozone and halogens from a variety of observational platforms to quantify the attribution of the change in stratospheric ozone that is due to halogens. Our focus is on the extra-polar region: i.e., the state of the ozone layer between 55S and 55N where the vast majority of the world’s population resides. We will quantify the effect of continued release of CFC-11 and the presence of chlorinated VSL species on the recovery of the ozone layer. Additionally, we will use atmospheric observations to evaluate several proposed formulations for defining the quantity known as “Equivalent Effective Stratospheric Chlorine” (EESC) and assess the impact of these formulations on the projected recovery of the ozone layer. [less ▲]

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See detailInfrared remote sensing of atmospheric composition at the Jungfraujoch station, Swiss Alps, since 1950
Mahieu, Emmanuel ULiege

Scientific conference (2019, December 13)

It is in the early 1950s that researchers from the University of Liège have recorded the first atmospheric infrared solar spectra at the Jungfraujoch scientific station, in the Swiss Alps, at a time when ... [more ▼]

It is in the early 1950s that researchers from the University of Liège have recorded the first atmospheric infrared solar spectra at the Jungfraujoch scientific station, in the Swiss Alps, at a time when climate change was not a matter of worry. These pioneering observations have allowed to confirm that methane and carbon monoxide were ubiquitous constituents of the Earth’s atmosphere. The recording of atmospheric spectra resumed in the mid-1970s, stimulated by rising concerns related to possible stratospheric ozone depletion. Since then, this monitoring activity has been conducted at that site without interruption, allowing to gather high-quality data crucial for the characterization of the Earth’s atmosphere and of the changes affecting it, resulting from anthropogenic activities or natural causes. In this talk, we present some recent results relevant for the verification of international environmental treaties such as the Montreal Protocol on substances that deplete ozone, and the Kyoto Protocol for the limitation of greenhouse gases emissions. We further illustrate contributions of our monitoring program relevant to study air quality and precursors of tropospheric ozone. Finally, we evoke a new DFG project involving University of Leeds, Universität Bremen (lead) and the University of Liège that will digitize and exploit the early spectra for in-depth investigation of atmospheric composition in the early 1950s. [less ▲]

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See detailN2O-based climatology of the Brewer-Dobson Circulation in WACCM, a chemical renalysis and a CTM driven by four dynamical reanalyses
Minganti, Daniele ULiege; Chabrillat, Simon; Christophe, Yves et al

Poster (2019, December 11)

The Brewer-Dobson Circulation (BDC) plays a major role in the stratospheric dynamics in terms of tracer transport through the mean residual meridional advection and the isentropic two-way mixing. The ... [more ▼]

The Brewer-Dobson Circulation (BDC) plays a major role in the stratospheric dynamics in terms of tracer transport through the mean residual meridional advection and the isentropic two-way mixing. The climatological BDC in the Whole Atmosphere Community Climate Model (WACCM) is separated in those components and evaluated through a comparison with a chemical reanalysis of Aura MLS (BRAM2) and with a chemistry-transport model driven by four modern reanalyses (ERA-Interim, JRA-55, MERRA and MERRA2), using the Transformed Eulerian Mean (TEM) analysis of the long-lived tracer N2O and focusing on the vertical residual advection and the horizontal two-way mixing terms. In the wintertime Southern polar region the horizontal mixing term in WACCM shows near-zero values, while all the reanalyses show strong negative contributions. This disagreement is likely due to the different representation of the polar transport barrier, that affects the mixing inside the polar vortex. In this region the reanalyses are characterized by large uncertainties of the TEM analysis, i.e. the residual term of the budget is quite large (the N2O TEM budget is not fully closed). In the wintertime Northern polar latitudes WACCM shows smaller values of the horizontal mixing term compared to the reanalyses, which show lower uncertainties of the TEM budget. The agreement is improved in the middle and low latitudes, especially in the Northern Hemisphere: the differences are smaller and the residual term is lower compared to the polar latitudes. The inter-annual variability of the horizontal mixing term is large in the Southern polar latitudes during austral fall and in the Northern polar latitudes during boreal winter. [less ▲]

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See detailBiomass Burning Unlikely to Account for Missing Source of Carbonyl Sulfide
Stinecipher, James R.; Cameron-Smith, Philip J.; Blake, Nicola J. et al

in Geophysical Research Letters (2019), 46(24), 14912--14920

Carbonyl sulfide (OCS) provides a proxy for measuring photosynthesis and is the primary background source of stratospheric aerosols. OCS emissions due to biomass burning are a variable and substantial ... [more ▼]

Carbonyl sulfide (OCS) provides a proxy for measuring photosynthesis and is the primary background source of stratospheric aerosols. OCS emissions due to biomass burning are a variable and substantial (over 10%) part of the current OCS budget. OCS emission ratios from open burning fires, coupled with 1997–2016 data from the Global Fire Emissions Database (GFED4), yield OCS biomass burning emissions with a global average annual flux of 60 ± 37 Gg(S)/year. A global box model suggests these emissions are more consistent with observations from global atmospheric composition monitoring networks than fluxes derived from previous synthesis papers. Even after considering the uncertainty in emission factor observations for each category of emissions and the interannual variation in total burned dry matter, the total OCS emissions from open burning are insufficient to account for the large imbalance between current estimates of global OCS sources and sinks. [less ▲]

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See detailDetection and Attribution of Wildfire Pollution in the Arctic and Northern Mid-latitudes using a Network of FTIR Spectrometers and GEOS-Chem
Lutsch, Erik; Strong, Kimberly; Jones, Dylan B. A. et al

E-print/Working paper (2019)

We present a multi-year time series of column abundances of carbon monoxide (CO), hydrogen cyanide (HCN), and ethane (C2H6) measured using Fourier transform infrared (FTIR) spectrometers at ten sites ... [more ▼]

We present a multi-year time series of column abundances of carbon monoxide (CO), hydrogen cyanide (HCN), and ethane (C2H6) measured using Fourier transform infrared (FTIR) spectrometers at ten sites affiliated with the Network for Detection of Atmospheric Composition Change (NDACC). Six are high-latitude sites: Eureka, Ny-Alesund, Thule, Kiruna, Poker Flat, and St. Petersburg , and four are mid-latitude sites: Zugspitze, Jungfraujoch, Toronto, and Rikubetsu. For each site, the inter-annual trends and seasonal variabilities of the CO time series are accounted for, allowing ambient concentrations to be determined. Enhancements above ambient levels were used to identify possible wildfire pollution events. Since the abundance of each trace gas emitted in a wildfire event is specific to the type of vegetation burned and the burning phase, correlations of CO to the long-lived wildfire tracers HCN and C2H6 allow for further confirmation of the detection of wildfire pollution, while complementary measurements of aerosol optical depth from nearby AERONET sites confirm the presence of wildfire smoke. A GEOS-Chem tagged CO simulation with Global Fire Assimilation System (GFAS) biomass burning emissions was used to determine the source attribution of CO concentrations at each site from 2003–2018. The influence of the various wildfire sources is found to differ between sites while North American and Asian boreal wildfires fires were found to be the greatest contributors to episodic CO enhancements in the summertime at all sites. [less ▲]

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See detailFTIR measurements at Jungfraujoch
Mahieu, Emmanuel ULiege

Scientific conference (2019, November 06)

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See detailSurveillance à long terme de l’atmosphère terrestre à la station du Jungfraujoch
Mahieu, Emmanuel ULiege; Flock, Olivier ULiege; Notholt, Justus et al

in Bulletin de la Société Royale des Sciences de Liège (2019, November), 88

It is in the early 1950s that researchers from the University of Liège have recorded the first atmospheric solar spectra at the Jungfraujoch scientific station, in the Swiss Alps, at a time when climate ... [more ▼]

It is in the early 1950s that researchers from the University of Liège have recorded the first atmospheric solar spectra at the Jungfraujoch scientific station, in the Swiss Alps, at a time when climate change was not a matter of worry. These pioneering observations have allowed to confirm that methane and carbon monoxide were ubiquitous constituents of the Earth’s atmosphere. The recording of atmospheric spectra resumed in the mid-1970s, stimulated by rising concerns related to possible stratospheric ozone depletion. Since then, this monitoring activity has been conducted at that site without interruption, allowing to gather high-quality data crucial for the characterization of the Earth’s atmosphere and of the changes affecting it, resulting from anthropogenic activities or natural causes. In this paper, we present some recent results relevant for the verification of international environmental treaties. [less ▲]

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See detailImproved FTIR retrieval strategy for HCFC-22 (CHClF2), comparisons with in situ and satellite datasets with the support of models, and determination of its long-term trend above Jungfraujoch
Prignon, Maxime ULiege; Chabrillat, Simon; Minganti, Daniele ULiege et al

in Atmospheric Chemistry and Physics (2019), 19(19), 1230912324

Hydrochlorofluorocarbons (HCFCs) are the first, but temporary, substitution products for the strong ozone-depleting chlorofluorocarbons (CFCs). In this work, we present and validate an improved method to ... [more ▼]

Hydrochlorofluorocarbons (HCFCs) are the first, but temporary, substitution products for the strong ozone-depleting chlorofluorocarbons (CFCs). In this work, we present and validate an improved method to retrieve the most abundant HCFC in the atmosphere, allowing its evolution to be monitored independently in the troposphere and stratosphere. These kinds of contributions are fundamental for scrutinizing the fulfilment of the Montreal Protocol on Substances that Deplete the Ozone Layer. [less ▲]

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See detailImpacts of H2O variability on accuracy of CH4 observations from MIPAS satellite over tropics
Yirdaw Berhe, T.; Mengistu Tsidu, G.; Blumenstock, T. et al

E-print/Working paper (2019)

Uncertainties of tropical methane concentrations, retrieved from spectra recorded by the Michelson Interferometer for Passive Atmospheric Sounding (MIPAS), MIPAS version V5R_CH4_220 are large. We explore ... [more ▼]

Uncertainties of tropical methane concentrations, retrieved from spectra recorded by the Michelson Interferometer for Passive Atmospheric Sounding (MIPAS), MIPAS version V5R_CH4_220 are large. We explore the relation of these uncertainties with water vapour variability. We further show that these uncertainties have been reduced in MIPAS version V5R_CH4_224. Coincident measurements of CH4 by MIPAS, ground based FTIR and CH4 derived from EOS MLS coincident measurements of atmospheric water vapour (H2O), carbon monoxide (CO) and nitrous oxide (N2O) are used to estimate the standard uncertainty of MIPAS CH4 220, MIPAS CH4 224 and natural variability of H2O. Different methods such as bias evaluation, differential method and correlation coefficient are employed to explore the latitudinal variations of standard uncertainty of MIPAS CH4 220 and natural variability of water vapour as well as its reduction on MIPAS CH4 224. The averaged bias between MIPAS CH4 220 and ground-based FTIR measurements are −12.3 %, 8.4 % and 1.2 % for tropics, mid-latitudes and high latitudes, respectively. The standard deviations of the differences for these latitudinal bands are 5.9 %, 4.8 % and 4.7 %. More-over, the correlation coefficient between MIPAS CH4 220 and MIPAS V5R_N2O_220 is 0.32 in the upper troposphere and lower stratosphere over tropics and larger than the mod-est value 0.5 in mid and high latitudes. The poor correlation between MIPAS CH4 220 and MIPAS N2O 220 over tropics can indicate the large uncertainty of MIPAS CH4 220 over tropics that is related to water variability. Similarly, mean relative difference between MIPAS CH4 224 and ground-based FTIR measurements are 3.9 %, −2.6 % and −2.7 % in altitude 15–21 km and the average estimated uncertainty of MIPAS CH4 224 methane were obtained 2.4 %, 1.4 % and 5.1 % in altitude ranges of 15 to 27 km for tropics, mid and high latitudes, respectively. The estimated measurement uncertainty of MIPAS CH4 224 is different for the three latitude bands in the northern hemisphere, reflecting the latitudinal variation of uncertainties of MIPAS methane. However, the large reduction of uncertainty in MIPAS CH4 224 as compared to MIPAS CH4 220 has been confirmed for the tropical measurements. The correlation coefficients between the uncertainty of MIPAS CH4 220 and the variability of water vapour in lower stratosphere are strong (0.88) on monthly temporal scales. Similar methods were used for MIPAS CH4 224. It was found that the uncertainty in methane due to the variability of water vapor has been reduced. [less ▲]

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See detailPost-peak trend of upper stratospheric hydrogen chloride derived from ground-based FTIR solar spectra and model simulations
Mahieu, Emmanuel ULiege; Prignon, Maxime ULiege; Servais, Christian ULiege et al

Conference (2019, May 23)

After several decades of sustained increase, hydrogen chloride (HCl, the main reservoir for stratospheric chlorine) showed a maximum abundance around 1997. Since then, its decrease has been documented ... [more ▼]

After several decades of sustained increase, hydrogen chloride (HCl, the main reservoir for stratospheric chlorine) showed a maximum abundance around 1997. Since then, its decrease has been documented, characterized by short-term variability which was attributed to atmospheric circulation changes, affecting mainly the lower stratosphere (Mahieu et al., 2014). This notably led to a temporary increase of HCl over 2007-2011, complicating the determination of the long-term HCl trend and the accurate verification of the success of the Montreal Protocol for the protection of the stratospheric ozone layer. Studies have used other long-lived tracers to remove the effects of dynamical variability in the lower stratosphere (e.g., Stolarski et al., 2018), while other investigations have suggested that trends in the upper stratosphere were potentially more appropriate for the long-term characterization of the HCl decrease (e.g., Froidevaux et al., 2015; Bernath and Fernando, 2018), especially when dealing with satellite height-resolved data. In this contribution, we use FTIR (Fourier Transform InfraRed) data from the Jungfraujoch station (Swiss Alps, 3580 m a.s.l.), a site of the NDACC network (http://www.ndacc.org), to study the evolution of HCl in some detail. The SFIT-4 retrieval algorithm implementing the Optimal Estimation Method of Rodgers (2000) is employed, providing HCl columns with good sensitivity from the tropopause up to about 40 km altitude. Moreover, the vertical resolution is sufficient to determine independent partial columns for the lower and upper stratosphere. With the support of model simulations performed with the 3D-Chemistry Transport Model of the Belgian Assimilation System for Chemical ObsErvations (BASCOE; Chabrillat et al., 2018), driven by the ERA-Interim meteorological reanalysis, we investigate the post-peak trend of HCl in the lower and upper stratosphere. We also determine the magnitude of the uncertainties affecting the various trends, using bootstrap tools which are specifically developed to take into account the auto-correlation present in our geophysical data sets. [less ▲]

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