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See detailRemote sensing of the atmospheric composition in the infrared spectral region within the Network for the Detection of Atmospheric Composition Change (NDACC) and the Total Carbon Column Observing Network (TCCON)
Notholt, J; Blumenstock, T; Deutscher, N et al

Conference (2015, May 12)

Remote sensing has been established as a powerful tool in atmospheric research. Throughout the last decades satellite and ground-based remote sensing instruments and methods have been developed to sample ... [more ▼]

Remote sensing has been established as a powerful tool in atmospheric research. Throughout the last decades satellite and ground-based remote sensing instruments and methods have been developed to sample the atmosphere from the microwave to the UV/Vis. The international ground based networks NDACC-IR and TCCON are based on solar absorption spectrometry in the infrared. Both networks consist of more than 30 observations sites around the globe, from the high Arctic through mid-latitudes and the tropics to the southern hemisphere and Antarctica. NDACC concentrates on stratospheric observations in relation to ozone chemistry, in many instances, information on the vertical distribution of the target species is determined. Measured trace gases include O3, HCl, HF, HNO3, ClONO2 and many others. In addition, the tropospheric composition is studied by measuring anthropogenic and biogenic species including HCN, OCS, H2O, CO, CH2O, C2H6, and C2H2. The aim of TCCON is to acquire accurate and precise column-averaged abundances of CO2, CH4, N2O, i.e. atmospheric trace gases which have a very small natural variability. TCCON measurements are linked to WMO calibration scales by comparisons with co-incident in situ profiles measured from aircraft or balloon. Results from both networks have been used in many studies in relation to stratospheric ozone chemistry, air-pollution, and with regard to the carbon-cycle. Long-term series are necessary for trend analysis, gaining insight into annual and longer term variability and placing into context shorter term process studies. Due to the similar observation geometry, the ground-based observations are optimally suitable for satellite and model validation and form an essential part of many satellite projects. They also play an important role in the validation of the Copernicus Atmospheric Monitoring Service. In our contribution we will give an overview on the current status of both networks, ongoing efforts to improve network coverage, precision and accuracy, and several examples of scientific highlights. [less ▲]

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See detailValidation of SCIAMACHY HDO/H2O measurements using the TCCON and NDACC-MUSICA networks
Scheepmaker, R. A.; Frankenberg, C.; Deutscher, N. M. et al

in Atmospheric Measurement Techniques (2015), 8(4), 1799-1818

Measurements of the atmospheric HDO/H2O ratio help us to better understand the hydrological cycle and improve models to correctly simulate tropospheric humidity and therefore climate change. We present an ... [more ▼]

Measurements of the atmospheric HDO/H2O ratio help us to better understand the hydrological cycle and improve models to correctly simulate tropospheric humidity and therefore climate change. We present an updated version of the column-averaged HDO/H2O ratio data set from the SCanning Imaging Absorption spectroMeter for Atmospheric CHartographY (SCIAMACHY). The data set is extended with 2 additional years, now covering 2003–2007, and is validated against co-located ground-based total column δD measurements from Fourier transform spectrometers (FTS) of the Total Carbon Column Observing Network (TCCON) and the Network for the Detection of Atmospheric Composition Change (NDACC, produced within the framework of the MUSICA project). Even though the time overlap among the available data is not yet ideal, we determined a mean negative bias in SCIAMACHY δD of −35 ± 30‰ compared to TCCON and −69 ± 15‰ compared to MUSICA (the uncertainty indicating the station-to-station standard deviation). The bias shows a latitudinal dependency, being largest (∼ −60 to −80‰) at the highest latitudes and smallest (∼ −20 to −30‰) at the lowest latitudes. We have tested the impact of an offset correction to the SCIAMACHY HDO and H2O columns. This correction leads to a humidity- and latitude-dependent shift in δD and an improvement of the bias by 27‰, although it does not lead to an improved correlation with the FTS measurements nor to a strong reduction of the latitudinal dependency of the bias. The correction might be an improvement for dry, high-altitude areas, such as the Tibetan Plateau and the Andes region. For these areas, however, validation is currently impossible due to a lack of ground stations. The mean standard deviation of single-sounding SCIAMACHY–FTS differences is ∼ 115‰, which is reduced by a factor ∼ 2 when we consider monthly means. When we relax the strict matching of individual measurements and focus on the mean seasonalities using all available FTS data, we find that the correlation coefficients between SCIAMACHY and the FTS networks improve from 0.2 to 0.7–0.8. Certain ground stations show a clear asymmetry in δD during the transition from the dry to the wet season and back, which is also detected by SCIAMACHY. This asymmetry points to a transition in the source region temperature or location of the water vapour and shows the added information that HDO/H2O measurements provide when used in combination with variations in humidity. [less ▲]

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See detailRetrieval of ammonia from ground-based FTIR measurements and its use for validation of satellite observations by IASI
Dammers, E; Palm, M; Warneke, T et al

in Geophysical Research Abstracts (2015, April 13), 17

Atmospheric Ammonia (NH3) has a major impact on human health and ecosystem services and plays a major role in the formation of aerosols [Erisman et al.,2013; Paulot and Jacob 2014]. NH3 concentrations are ... [more ▼]

Atmospheric Ammonia (NH3) has a major impact on human health and ecosystem services and plays a major role in the formation of aerosols [Erisman et al.,2013; Paulot and Jacob 2014]. NH3 concentrations are highly variable in space and time with overall short lifetime due to deposition and aerosol formation. The global atmospheric budget of nitrogen and in turn NH3 is still uncertain which asks for more ground-based and satellite observations around the world. Recent papers have described the possibility to measure NH3 with satellite infrared sounders which open up the way for calculations of global and regional nitrogen budgets [Clarisse et al 2009,Van Damme et al 2014a]. Validation of the satellite observations is essential to determine the uncertainty in the signal and its potential use. So far available surface layer observations of atmospheric NH3 concentrations have been used for comparisons with total columns retrieved from satellite observations [Van Damme 2014b]. We developed a retrieval for NH3 column density concentrations (molecules NH3/cm2) by fitting a set of spectral windows to ground-based solar absorption Fourier transform infrared (FTIR) measurements with the spectral fitting program SFIT4 [Hase et al., 2004]. The retrieval is then applied to FTIR measurements from a set of spectrometer sites from the Network for detection of Atmospheric Composition Change (NDACC) to retrieve NH3 columns for the sites located in Bremen, Germany; Lauder, New Zealand; Jungfraujoch, Switzerland; and the island of Reunion, France. Using eight years (2005-2013) of retrieved NH3 columns clear seasonal cycles are observed for each of the stations. Maximum concentrations can be related to NH3 emission sources, specific for the regions. A comparison between the retrieved NH3 columns and observations from the recent IASI- NH3 product [Van Damme et al, 2014a] using strict spatial and temporal criteria for the selection of observations showed a good correlation (R=0.82; slope=0.63). The IASI- NH3 columns for the Bremen and Lauder area show similar temporal cycles when compared to the FTIR observations. [less ▲]

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See detailUsing XCO2 retrievals for assessing the long-term consistency of NDACC/FTIR data sets
Barthlott, S; Schneider, M; Hase, F et al

in Atmospheric Measurement Techniques (2015), 8

Within the NDACC (Network for the Detection of Atmospheric Composition Change), more than 20 FTIR (Fourier-transform infrared) spectrometers, spread worldwide, provide long-term data records of many ... [more ▼]

Within the NDACC (Network for the Detection of Atmospheric Composition Change), more than 20 FTIR (Fourier-transform infrared) spectrometers, spread worldwide, provide long-term data records of many atmospheric trace gases. We present a method that uses measured and modelled XCO2 for assessing the consistency of these NDACC data records. Our XCO2 retrieval setup is kept simple so that it can easily be adopted for any NDACC/FTIR-like measurement made since the late 1950s. By a comparison to coincident TCCON (Total Carbon Column Observing Network) measurements, we empirically demonstrate the useful quality of this suggested NDACC XCO2 product (empirically obtained scatter between TCCON and NDACC is about 4‰ for daily mean as well as monthly mean comparisons, and the bias is 25 ‰). Our XCO2 model is a simple regression model fitted to CarbonTracker results and the Mauna Loa CO2 in situ records. A comparison to TCCON data suggests an uncertainty of the model for monthly mean data of below 3 ‰. We apply the method to the NDACC/FTIR spectra that are used within the project MUSICA (multi-platform remote sensing of isotopologues for investigating the cycle of atmospheric water) and demonstrate that there is a good consistency for these globally representative set of spectra measured since 1996: the scatter between the modelled and measured XCO2 on a yearly time scale is only 3 ‰. [less ▲]

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See detailTrends of ozone total columns and vertical distribution from FTIR observations at eight NDACC stations around the globe
Vigouroux, C; Blumenstock, T; Coffey, M et al

in Atmospheric Chemistry and Physics (2015), 15

Ground-based Fourier transform infrared (FTIR) measurements of solar absorption spectra can provide ozone total columns with a precision of 2 % but also independent partial column amounts in about four ... [more ▼]

Ground-based Fourier transform infrared (FTIR) measurements of solar absorption spectra can provide ozone total columns with a precision of 2 % but also independent partial column amounts in about four vertical layers, one in the troposphere and three in the stratosphere up to about 45 km, with a precision of 5–6 %. We use eight of the Network for the Detection of Atmospheric Composition Change (NDACC) stations having a long-term time series of FTIR ozone measurements to study the total and vertical ozone trends and variability, namely, Ny-Ålesund (79ºN), Thule (77ºN), Kiruna (68ºN), Harestua (60ºN), Jungfraujoch (47ºN), Izaña (28ºN), Wollongong (34ºS) and Lauder (45ºS). The length of the FTIR time series varies by station but is typically from about 1995 to present. We applied to the monthly means of the ozone total and four partial columns a stepwise multiple regression model including the following proxies: solar cycle, quasi-biennial oscillation (QBO), El Niño–Southern Oscillation (ENSO), Arctic and Antarctic Oscillation (AO/AAO), tropopause pressure (TP), equivalent latitude (EL), Eliassen–Palm flux (EPF), and volume of polar stratospheric clouds (VPSC). At the Arctic stations, the trends are found mostly negative in the troposphere and lower stratosphere, very mixed in the middle stratosphere, positive in the upper stratosphere due to a large increase in the 1995–2003 period, and non-significant when considering the total columns. The trends for mid-latitude and subtropical stations are all non-significant, except at Lauder in the troposphere and upper stratosphere and at Wollongong for the total columns and the lower and middle stratospheric columns where they are found positive. At Jungfraujoch, the upper stratospheric trend is close to significance (+0.9 ± 1.0 %/decade). Therefore, some signs of the onset of ozone mid-latitude recovery are observed only in the Southern Hemisphere, while a few more years seem to be needed to observe it at the northern mid-latitude station. [less ▲]

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See detailRecent Northern Hemisphere stratospheric HCl increase due to atmospheric circulation changes
Mahieu, Emmanuel ULg; Chipperfield, M. P.; Notholt, J. et al

in Nature (2014), 515(7525), 104--107

The abundance of chlorine in the Earth’s atmosphere increased considerably during the 1970s to 1990s, following large emissions of anthropogenic long-lived chlorine-containing source gases, notably the ... [more ▼]

The abundance of chlorine in the Earth’s atmosphere increased considerably during the 1970s to 1990s, following large emissions of anthropogenic long-lived chlorine-containing source gases, notably the chlorofluorocarbons. The chemical inertness of chlorofluorocarbons allows their transport and mixing throughout the troposphere on a global scale[1], before they reach the stratosphere where they release chlorine atoms that cause ozone depletion[2]. The large ozone loss over Antarctica[3] was the key observation that stimulated the definition and signing in 1987 of the Montreal Protocol, an international treaty establishing a schedule to reduce the production of the major chlorine- and bromine-containing halocarbons. Owing to its implementation, the near-surface total chlorine concentration showed a maximum in 1993, followed by a decrease of half a per cent to one per cent per year[4], in line with expectations. Remote-sensing data have revealed a peak in stratospheric chlorine after 1996[5], then a decrease of close to one per cent per year[6,7], in agreement with the surface observations of the chlorine source gases and model calculations[7]. Here we present ground-based and satellite data that show a recent and significant increase, at the 2σ level, in hydrogen chloride (HCl), the main stratospheric chlorine reservoir, starting around 2007 in the lower stratosphere of the Northern Hemisphere, in contrast with the ongoing monotonic decrease of near-surface source gases. Using model simulations, we attribute this trend anomaly to a slowdown in the Northern Hemisphere atmospheric circulation, occurring over several consecutive years, transporting more aged air to the lower stratosphere, and characterized by a larger relative conversion of source gases to HCl. This short-term dynamical variability will also affect other stratospheric tracers and needs to be accounted for when studying the evolution of the stratospheric ozone layer. [less ▲]

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See detailIncrease in northern hemisphere stratospheric hydrogen chloride over recent years
Mahieu, Emmanuel ULg; Chipperfield, MP; Notholt, J et al

Poster (2014, October 07)

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See detailRecent increases in Stratospheric HCl: Stratospheric Dynamics versus the Montreal Protocol
Chipperfield, M.P.; Mahieu, Emmanuel ULg; Notholt, J. et al

in Geophysical Research Abstracts (2014), 16

Long-lived chlorine-containing source gases, such as chlorofluorocarbons (CFCs), are transported into the stratosphere where they decompose and cause ozone depletion. Increases in chlorine during the ... [more ▼]

Long-lived chlorine-containing source gases, such as chlorofluorocarbons (CFCs), are transported into the stratosphere where they decompose and cause ozone depletion. Increases in chlorine during the 1970s-1990s resulted in long-term ozone decreases, especially in the polar regions. Following the implementation of the Montreal Protocol, the near-surface chlorine loading was observed to peak in 1993 and, since then, to decrease in line with expectations. After release from source gases in the stratosphere, chlorine mainly forms the reservoir HCl, providing an alternative method for monitoring the progress of the Montreal Protocol. A maximum in stratospheric HCl was observed around 1996, followed by decay at a rate close to 1%/year, consistent with the tropospheric chlorine peak and known transport timescales. However, we will present total column observations from ground-based FTIR instruments which show an unexpected and significant upturn in stratospheric HCl around 2007 in the northern hemisphere. Height-resolved observations from satellite instruments (HALOE, MLS, ACE) confirm this increase and show that it occurs in the lower stratosphere. These observations contrast with the ongoing monotonic decrease of near-surface chlorine source gases. Using 3-D model simulations (TOMCAT/SLIMCAT and KASIMA) we attribute this trend anomaly to a slowdown in the NH atmospheric circulation, causing air in the lower stratosphere to become more aged with a larger relative conversion of source gases to HCl. An important conclusion is that the Montreal Protocol is still on track and will still lead to long-term decreases in stratospheric chlorine. This dynamical variability could also significantly affect the evolution of stratospheric ozone and must be accounted for when searching for signs of ozone recovery. [less ▲]

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See detailGround-based remote sensing of tropospheric water vapour isotopologues within the project MUSICA
Schneider, M.; Barthlott, S.; Hase, F. et al

in Atmospheric Measurement Techniques (2012), 5(2012), 3007-3027

Within the project MUSICA (MUlti-platform remote Sensing of Isotopologues for investigating the Cycle of Atmospheric water), long-term tropospheric water vapour isotopologue data records are provided for ... [more ▼]

Within the project MUSICA (MUlti-platform remote Sensing of Isotopologues for investigating the Cycle of Atmospheric water), long-term tropospheric water vapour isotopologue data records are provided for ten globally distributed ground-based mid-infrared remote sensing stations of the NDACC (Network for the Detection of Atmospheric Composition Change). We present a new method allowing for an extensive and straightforward characterisation of the complex nature of such isotopologue remote sensing datasets. We demonstrate that the MUSICA humidity profiles are representative for most of the troposphere with a vertical resolution ranging from about 2 km (in the lower troposphere) to 8 km (in the upper troposphere) and with an estimated precision of better than 10%. We find that the sensitivity with respect to the isotopologue composition is limited to the lower and middle troposphere, whereby we estimate a precision of about 30‰ for the ratio between the two isotopologues HD16O and H216O. The measurement noise, the applied atmospheric temperature profiles, the uncertainty in the spectral baseline, and the cross-dependence on humidity are the leading error sources. We introduce an a posteriori correction method of the cross-dependence on humidity, and we recommend applying it to isotopologue ratio remote sensing datasets in general. In addition, we present mid-infrared CO2 retrievals and use them for demonstrating the MUSICA network-wide data consistency. In order to indicate the potential of long-term isotopologue remote sensing data if provided with a well-documented quality, we present a climatology and compare it to simulations of an isotope incorporated AGCM (Atmospheric General Circulation Model). We identify differences in the multi-year mean and seasonal cycles that significantly exceed the estimated errors, thereby indicating deficits in the modeled atmospheric water cycle. [less ▲]

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See detailValidation of IASI FORLI carbon monoxide retrievals using FTIR data from NDACC
Kerzenmacher, T; Dils, B; Kumps, N et al

in Atmospheric Measurement Techniques (2012), 5

Carbon monoxide (CO) is retrieved daily and globally from space-borne IASI radiance spectra using the Fast Optimal Retrievals on Layers for IASI (FORLI) software developed at the Université Libre de ... [more ▼]

Carbon monoxide (CO) is retrieved daily and globally from space-borne IASI radiance spectra using the Fast Optimal Retrievals on Layers for IASI (FORLI) software developed at the Université Libre de Bruxelles (ULB). The IASI CO total column product for 2008 from the most recent FORLI retrieval version (20100815) is evaluated using correlative CO profile products retrieved from groundbased solar absorption Fourier transform infrared (FTIR) observations at the following FTIR spectrometer sites from the Network for the Detection of Atmospheric Composition Change (NDACC): Ny-Alesund, Kiruna, Bremen, Jungfraujoch, Izana and Wollongong. In order to have good statistics for the comparisons, we included all IASI data from the same day, within a 100 km radius around the ground-based stations. The individual ground-based data were adjusted to the lowest altitude of the co-located IASI CO profiles. To account for the different vertical resolutions and sensitivities of the ground-based and satellite measurements, the averaging kernels associated with the various retrieved products have been used to properly smooth coincident data products. It has been found that the IASI CO total column products compare well on average with the co-located ground-based FTIR total columns at the selected NDACC sites and that there is no significant bias for the mean values at all stations. [less ▲]

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See detailObserved and simulated time evolution of HCl, ClONO2, and HF total column abundances
Kohlhepp, R; Ruhnke, R; Chipperfield, M P et al

in Atmospheric Chemistry and Physics (2012), 12(7), 3527--3556

Time series of total column abundances of hydrogen chloride (HCl), chlorine nitrate (ClONO2), and hydrogen fluoride (HF) were determined from ground-based Fourier transform infrared (FTIR) spectra ... [more ▼]

Time series of total column abundances of hydrogen chloride (HCl), chlorine nitrate (ClONO2), and hydrogen fluoride (HF) were determined from ground-based Fourier transform infrared (FTIR) spectra recorded at 17 sites belonging to the Network for the Detection of Atmospheric Composition Change (NDACC) and located between 80.05°N and 77.82°S. By providing such a near-global overview on ground-based measurements of the two major stratospheric chlorine reservoir species, HCl and ClONO2, the present study is able to confirm the decrease of the atmospheric inorganic chlorine abundance during the last few years. This decrease is expected following the 1987 Montreal Protocol and its amendments and adjustments, where restrictions and a subsequent phase-out of the prominent anthropogenic chlorine source gases (solvents, chlorofluorocarbons) were agreed upon to enable a stabilisation and recovery of the stratospheric ozone layer. The atmospheric fluorine content is expected to be influenced by the Montreal Protocol, too, because most of the banned anthropogenic gases also represent important fluorine sources. But many of the substitutes to the banned gases also contain fluorine so that the HF total column abundance is expected to have continued to increase during the last few years. The measurements are compared with calculations from five different models: the two-dimensional Bremen model, the two chemistry-transport models KASIMA and SLIMCAT, and the two chemistry-climate models EMAC and SOCOL. Thereby, the ability of the models to reproduce the absolute total column amounts, the seasonal cycles, and the temporal evolution found in the FTIR measurements is investigated and inter-compared. This is especially interesting because the models have different architectures. The overall agreement between the measurements and models for the total column abundances and the seasonal cycles is good. Linear trends of HCl, ClONO2, and HF are calculated from both measurement and model time series data, with a focus on the time range 2000–2009. This period is chosen because from most of the measurement sites taking part in this study, data are available during these years. The precision of the trends is estimated with the bootstrap resampling method. The sensitivity of the trend results with respect to the fitting function, the time of year chosen and time series length is investigated, as well as a bias due to the irregular sampling of the measurements. The measurements and model results investigated here agree qualitatively on a decrease of the chlorine species by around 1%yr-1. The models simulate an increase of HF of around 1%yr-1. This also agrees well with most of the measurements, but some of the FTIR series in the Northern Hemisphere show a stabilisation or even a decrease in the last few years. In general, for all three gases, the measured trends vary more strongly with latitude and hemisphere than the modelled trends. Relative to the FTIR measurements, the models tend to underestimate the decreasing chlorine trends and to overestimate the fluorine increase in the Northern Hemisphere. At most sites, the models simulate a stronger decrease of ClONO2 than of HCl. In the FTIR measurements, this difference between the trends of HCl and ClONO2 depends strongly on latitude, especially in the Northern Hemisphere. [less ▲]

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See detailProcess-evaluation of tropospheric humidity simulated by general circulation models using water vapor isotopologues: 1. Comparison between models and observations
Risi, C; Noone, D; Worden, J et al

in Journal of Geophysical Research (2012), 117(D5), 05303

N2 - The goal of this study is to determine how H2O and HDO measurements in water vapor can be used to detect and diagnose biases in the representation of processes controlling tropospheric humidity in ... [more ▼]

N2 - The goal of this study is to determine how H2O and HDO measurements in water vapor can be used to detect and diagnose biases in the representation of processes controlling tropospheric humidity in atmospheric general circulation models (GCMs). We analyze a large number of isotopic data sets (four satellite, sixteen ground-based remote-sensing, five surface in situ and three aircraft data sets) that are sensitive to different altitudes throughout the free troposphere. Despite significant differences between data sets, we identify some observed HDO/H2O characteristics that are robust across data sets and that can be used to evaluate models. We evaluate the isotopic GCM LMDZ, accounting for the effects of spatiotemporal sampling and instrument sensitivity. We find that LMDZ reproduces the spatial patterns in the lower and mid troposphere remarkably well. However, it underestimates the amplitude of seasonal variations in isotopic composition at all levels in the subtropics and in midlatitudes, and this bias is consistent across all data sets. LMDZ also underestimates the observed meridional isotopic gradient and the contrast between dry and convective tropical regions compared to satellite data sets. Comparison with six other isotope-enabled GCMs from the SWING2 project shows that biases exhibited by LMDZ are common to all models. The SWING2 GCMs show a very large spread in isotopic behavior that is not obviously related to that of humidity, suggesting water vapor isotopic measurements could be used to expose model shortcomings. In a companion paper, the isotopic differences between models are interpreted in terms of biases in the representation of processes controlling humidity. [less ▲]

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See detailCO2 total column retrieval by mid-IR FT Spectroscopy
Buschmann, M; Dohe, S; Mahieu, Emmanuel ULg et al

in Geophysical Research Abstracts (2012), 14

Over the last decade ground-based remote sensing measurements of CO2 have been established as an important component in the global observing system for greenhouse gases. Since 2004 the Total Carbon Column ... [more ▼]

Over the last decade ground-based remote sensing measurements of CO2 have been established as an important component in the global observing system for greenhouse gases. Since 2004 the Total Carbon Column Observing Network (TCCON) sites have provided CO2 retrievals in the near-IR region. CO2 can also be retrieved in the mid-IR spectral region and it would be of great benefit to use these spectra to produce CO2-data of sufficient precision. With this, 20 years of additional observations obtained in the mid-IR at a suite of FT-IR sites of the Network Detection of Atmospheric Composition Change (NDACC) will be accessible. We investigated a series of different CO2 microwindows in the mid-IR spectral region and present results from the most promising candidates for a showcase FT-IR site (Ny Alesund). Limitations of the approach are outlined and the feasibility of a future Mid-IR CO2-product of sufficient precision is discussed. [less ▲]

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See detailCarbon monoxide (CO) and ethane (C2H6) trends from ground-based solar FTIR measurements at six European stations, comparison and sensitivity analysis with the EMEP model
Angelbratt, J.; Mellqvist, J.; Simpson, D. et al

in Atmospheric Chemistry and Physics (2011), 11(17), 9253--9269

Trends in the CO and C2H6 partial columns ~0–15 km) have been estimated from four European ground-based solar FTIR (Fourier Transform InfraRed) stations for the 1996–2006 time period. The CO trends from ... [more ▼]

Trends in the CO and C2H6 partial columns ~0–15 km) have been estimated from four European ground-based solar FTIR (Fourier Transform InfraRed) stations for the 1996–2006 time period. The CO trends from the four stations Jungfraujoch, Zugspitze, Harestua and Kiruna have been estimated to −0.45 ± 0.16% yr−1, −1.00 ± 0.24% yr−1, −0.62 ± 0.19 % yr−1 and −0.61 ± 0.16% yr−1, respectively. The corresponding trends for C2H6 are −1.51 ± 0.23% yr−1, −2.11 ± 0.30% yr−1, −1.09 ± 0.25% yr−1 and −1.14 ± 0.18% yr−1. All trends are presented with their 2-σ confidence intervals. To find possible reasons for the CO trends, the global-scale EMEP MSC-W chemical transport model has been used in a series of sensitivity scenarios. It is shown that the trends are consistent with the combination of a 20% decrease in the anthropogenic CO emissions seen in Europe and North America during the 1996–2006 period and a 20% increase in the anthropogenic CO emissions in East Asia, during the same time period. The possible impacts of CH4 and biogenic volatile organic compounds (BVOCs) are also considered. The European and global-scale EMEP models have been evaluated against the measured CO and C2H6 partial columns from Jungfraujoch, Zugspitze, Bremen, Harestua, Kiruna and Ny-Ålesund. The European model reproduces, on average the measurements at the different sites fairly well and within 10–22% deviation for CO and 14–31% deviation for C2H6. Their seasonal amplitude is captured within 6–35% and 9–124% for CO and C2H6, respectively. However, 61–98% of the CO and C2H6 partial columns in the European model are shown to arise from the boundary conditions, making the global-scale model a more suitable alternative when modeling these two species. In the evaluation of the global model the average partial columns for 2006 are shown to be within 1–9% and 37–50% of the measurements for CO and C2H6, respectively. The global model sensitivity for assumptions made in this paper is also analyzed. [less ▲]

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See detailValidation of five years (2003–2007) of SCIAMACHY CO total column measurements using ground-based spectrometer observations
de Laat, A. T. J.; Gloudemans, A. M. S.; Schrijver, H. et al

in Atmospheric Measurement Techniques (2010), 3(5), 1457--1471

This paper presents a validation study of SCanning Imaging Absorption spectroMeter for Atmospheric CHartographY (SCIAMACHY) carbon monoxide (CO) total column measurements from the Iterative Maximum ... [more ▼]

This paper presents a validation study of SCanning Imaging Absorption spectroMeter for Atmospheric CHartographY (SCIAMACHY) carbon monoxide (CO) total column measurements from the Iterative Maximum Likelihood Method (IMLM) algorithm using ground-based spectrometer observations from twenty surface stations for the five year time period of 2003–2007. Overall we find a good agreement between SCIAMACHY and ground-based observations for both mean values as well as seasonal variations. For high-latitude Northern Hemisphere stations absolute differences between SCIAMACHY and ground-based measurements are close to or fall within the SCIAMACHY CO 2σ precision of 0.2 × 1018 molecules/cm2 (~10%) indicating that SCIAMACHY can observe CO accurately at high Northern Hemisphere latitudes. For Northern Hemisphere mid-latitude stations the validation is complicated due to the vicinity of emission sources for almost all stations, leading to higher ground-based measurements compared to SCIAMACHY CO within its typical sampling area of 8° × 8°. Comparisons with Northern Hemisphere mountain stations are hampered by elevation effects. After accounting for these effects, the validation provides satisfactory results. At Southern Hemisphere mid- to high latitudes SCIAMACHY is systematically lower than the ground-based measurements for 2003 and 2004, but for 2005 and later years the differences between SCIAMACHY and ground-based measurements fall within the SCIAMACHY precision. The 2003–2004 bias is consistent with previously reported results although its origin remains under investigation. No other systematic spatial or temporal biases could be identified based on the validation presented in this paper. Validation results are robust with regard to the choices of the instrument-noise error filter, sampling area, and time averaging required for the validation of SCIAMACHY CO total column measurements. Finally, our results show that the spatial coverage of the ground-based measurements available for the validation of the 2003–2007 SCIAMACHY CO columns is sub-optimal for validation purposes, and that the recent and ongoing expansion of the ground-based network by carefully selecting new locations may be very beneficial for SCIAMACHY CO and other satellite trace gas measurements validation efforts. [less ▲]

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See detailValidation of version-4.61 methane and nitrous oxide observed by MIPAS
Payan, S.; Camy-Peyret, C.; Oelhaf, H. et al

in Atmospheric Chemistry and Physics (2009), 9(2), 413-442

The ENVISAT validation programme for the atmospheric instruments MIPAS, SCIAMACHY and GOMOS is based on a number of balloon-borne, aircraft, satellite and ground-based correlative measurements. In ... [more ▼]

The ENVISAT validation programme for the atmospheric instruments MIPAS, SCIAMACHY and GOMOS is based on a number of balloon-borne, aircraft, satellite and ground-based correlative measurements. In particular the activities of validation scientists were coordinated by ESA within the ENVISAT Stratospheric Aircraft and Balloon Campaign or ESABC. As part of a series of similar papers on other species [this issue] and in parallel to the contribution of the individual validation teams, the present paper provides a synthesis of comparisons performed between MIPAS CH4 and N2O profiles produced by the current ESA operational software (Instrument Processing Facility version 4.61 or IPF v4.61, full resolution MIPAS data covering the period 9 July 2002 to 26 March 2004) and correlative measurements obtained from balloon and aircraft experiments as well as from satellite sensors or from ground-based instruments. In the middle stratosphere, no significant bias is observed between MIPAS and correlative measurements, and MIPAS is providing a very consistent and global picture of the distribution of CH4 and N2O in this region. In average, the MIPAS CH4 values show a small positive bias in the lower stratosphere of about 5%. A similar situation is observed for N2O with a positive bias of 4%. In the lower stratosphere/upper troposphere (UT/LS) the individual used MIPAS data version 4.61 still exhibits some unphysical oscillations in individual CH4 and N2O profiles caused by the processing algorithm (with almost no regularization). Taking these problems into account, the MIPAS CH4 and N2O profiles are behaving as expected from the internal error estimation of IPF v4.61 and the estimated errors of the correlative measurements. [less ▲]

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See detailEvaluation of tropospheric and stratospheric ozone trends over Western Europe from ground-based FTIR network observations.
Vigouroux, C.; De Mazière, M.; Demoulin, Philippe ULg et al

in Atmospheric Chemistry and Physics (2008), 362(8), 6865-6886

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See detailPrecursor Gas Measurements (Chapter 2)
Notholt, J.; Bingemer, H.; Berresheim, H. et al

in Thomason, Larry W.; Peter, Thomas (Eds.) Assessment of Stratospheric Aerosol Properties (2006)

Assessments of stratospheric ozone have been conducted for nearly two decades and have evolved from describing ozone morphology to estimating ozone trends, and then to attribution of those trends ... [more ▼]

Assessments of stratospheric ozone have been conducted for nearly two decades and have evolved from describing ozone morphology to estimating ozone trends, and then to attribution of those trends. Stratospheric aerosol has only been integrated in assessments in the context of their effects on ozone chemistry and has not been critically evaluated itself. As a result, the Assessment of Stratospheric Aerosol Properties (ASAP) has been carried out by the WCRP project on Stratospheric Process and their Role in Climate (SPARC). The objective of this report is to present a systematic analysis of the state of knowledge of stratospheric aerosols including their precursors. It includes an examination of precursor concentrations and trends, measurements of stratospheric aerosol properties, trends in those properties, and modeling of aerosol formation, transport, and distribution in both background and volcanic conditions. The scope of this report is extensive; however, some aspects of stratospheric aerosol science have been deliberately excluded. For instance, we have not attempted to include an examination of polar stratospheric clouds (PSCs) or other clouds (such as cirrus clouds) occurring at or above the tropopause except in as much as they influence aerosol observations. Polar stratospheric clouds are the subject of a separate SPARC activity. We have produced a gap-free aerosol data base for use beyond this report. This required some new analysis that has not previously appeared in the technical literature. Similarly, the trend analysis required the development of a new analysis technique that is the subject of an article published in the Journal of Geophysical Research. New work is clearly identified in the present report. [less ▲]

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See detailInterannual variations of the carbon monoxide tropospheric burden between 30ºN and 90ºN in 1996-2003: ground-based and satellite measurements, estimate of biomass burning emissions
Yurganov, L. N.; Edwards, D. P.; Grechko, E. I. et al

in Geophysical Research Abstracts (2005), 7(EGU05-A-03850),

Carbon monoxide total column amounts in the atmosphere were measured in the High Northern Hemisphere (30º-90º N, HNH) between January 1996 and December 2003 using Fourier Transform Infrared high ... [more ▼]

Carbon monoxide total column amounts in the atmosphere were measured in the High Northern Hemisphere (30º-90º N, HNH) between January 1996 and December 2003 using Fourier Transform Infrared high resolution spectrometers installed at the NDSC (Network for Detection of Stratospheric Change) sites. A grating spectrometer of moderate resolution was employed for the same purpose at the Zvenigorod Research Station of the Institute of Atmospheric Physics near Moscow. CO mixing ratios were measured in the air samples obtained at the ground-level stations of the CMDL (Climate Modeling and Diagnostic Laboratory, NOAA) network. Total column CO amounts were measured from space by the Terra/MOPITT instrument between March, 2000, and December, 2003 (Edwards et al., 2004). Anomalies of monthly mean CO densities (related to a quiet period of 2000 - 2001) for different sites in the HNH were in agreement. This fact confirmed a good mixing of CO in the Northern Hemisphere on the montly basis that may be expected from a 1.5-2-month-long CO life-time. The data were integrated over the HNH reservoir (0-10 km in altitude and 30º-90º N in latitude) and the CO burden anomalies (in Tg) were analysed using a box model. Two CO sinks were taken into account: i) internal chemical removal in the reaction between CO and OH, and ii) transport of CO into the southertn part of the Northern hemisphere, where CO concentrations are usually lower. OH concentarations were taken from Spivakovsky et al. (2000). The air exchange through the 30º N boundary of the reservoir was estimated using the GEOS-CHEM model with a real meteorology of 1998 (Yurganov et al., 2004). The interannual variations of the sinks were neglected; a corresponding uncertainty in the retrieved source anomaly was estimated to be 20-30%. Since 1996 four years have been found to experience high CO emission of similar magnitude (1996, 1998, 2002, and 2003). During four years (1997, 1999, 2000, and 2001) the emissions were relatively low. Seasonal patterns of the emissions in active years were similar, maxima occured in July-August. However, in 2003 emissions in June-July were higher than in August. These semi-hemisphere averaged emission rates correlate with Siberian forest fire counts detected at night time by the ATSR radiometer of the ERS-2 satellite (R2 =0.51). The early peak of 2003 may be attributed to forest fires in Baikal region, Siberia. An inclusion of fire counts for other areas (Europe, North America) only worsen the correlation; this implies a decisive role of the Siberian fires for polluting the Northern Hemisphere troposphere (cf., Kasischke et al., 2005). It was estimated that the boreal forest fires during active years emit 30-60 Tg CO per month in July-August and 150-200 Tg annually. These emissions may be compared to industrial and transport pollution in the Northern Hemisphere estimated by Kasischke et al. (2005) as 290 Tg CO annually (i.e., 25 Tg monthly). [less ▲]

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See detailComparisons between SCIAMACHY Scientific Products and Ground-Based FTIR Data for Total Columns of CO, CH4 and N2O
De Mazière, M.; Barret, B.; Blumenstock, T. et al

Scientific conference (2004, May)

Total column amounts of CO, CH4 and N2O retrieved from SCIAMACHY nadir observations in its near-infrared channels have been compared to data from a ground-based network of Fourier-transform infrared (FTIR ... [more ▼]

Total column amounts of CO, CH4 and N2O retrieved from SCIAMACHY nadir observations in its near-infrared channels have been compared to data from a ground-based network of Fourier-transform infrared (FTIR) spectrometers as well as to data obtained with an FTIR instrument during a ship cruise in January-February 2003, along the African West Coast. The SCIAMACHY data considered here have been produced by two different scientific retrieval algorithms, wfm-doas (version 4.0) and IMLM (version 5.1), and cover different time periods, making the number of reliable coincidences that satisfy the temporal and spatial collocation criteria rather limited and different for both. Also the quality of the SCIAMACHY Level 1 data, and thus of the Level 2 data for the different time periods is very different. Still the comparisons demonstrate the capability of SCIAMACHY, using one of both algorithms, to deliver geophysically valuable products for the target species under consideration, on a global scale. [less ▲]

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