Detection Of Atmospheric Composition Change Research Articles

Technical note: Sensitivity of instrumental line shape monitoring for the ground-based high-resolution FTIR spectrometer with respect to different optical attenuators

Abstract. The TCCON (Total Carbon Column Observing Network) and most NDACC (Network for Detection of Atmospheric Composition Change) sites assume an ideal ILS (instrumental line shape) for analysis of the spectra. In order to adapt the radiant energy received by the detector, an attenuator or different sizes of field stop can be inserted in the light path. These processes may alter the alignment of a high-resolution FTIR (Fourier transform infrared) spectrometer, and may result in bias due to ILS drift. In this paper, we first investigated the sensitivity of the ILS monitoring with respect to application of different kinds of attenuators for ground-based high-resolution FTIR spectrometers within the TCCON and NDACC networks. Both lamp and sun cell measurements were conducted after the insertion of five different attenuators in front of and behind the interferometer. The ILS characteristics derived from lamp and sun spectra are in good agreement. ILSs deduced from all lamp cell measurements were compared. As a result, the disturbances to the ILS of a high-resolution FTIR spectrometer with respect to the insertion of different attenuators at different positions were quantified. A potential strategy to adapt the incident intensity of a detector was finally deduced.

The recent increase of atmospheric methane from 10 years of ground-based NDACC FTIR observations since 2005

Abstract. Changes of atmospheric methane total columns (CH4) since 2005 have been evaluated using Fourier transform infrared (FTIR) solar observations carried out at 10 ground-based sites, affiliated to the Network for Detection of Atmospheric Composition Change (NDACC). From this, we find an increase of atmospheric methane total columns of 0.31 ± 0.03 % year−1 (2σ level of uncertainty) for the 2005–2014 period. Comparisons with in situ methane measurements at both local and global scales show good agreement. We used the GEOS-Chem chemical transport model tagged simulation, which accounts for the contribution of each emission source and one sink in the total methane, simulated over 2005–2012. After regridding according to NDACC vertical layering using a conservative regridding scheme and smoothing by convolving with respective FTIR seasonal averaging kernels, the GEOS-Chem simulation shows an increase of atmospheric methane total columns of 0.35 ± 0.03 % year−1 between 2005 and 2012, which is in agreement with NDACC measurements over the same time period (0.30 ± 0.04 % year−1, averaged over 10 stations). Analysis of the GEOS-Chem-tagged simulation allows us to quantify the contribution of each tracer to the global methane change since 2005. We find that natural sources such as wetlands and biomass burning contribute to the interannual variability of methane. However, anthropogenic emissions, such as coal mining, and gas and oil transport and exploration, which are mainly emitted in the Northern Hemisphere and act as secondary contributors to the global budget of methane, have played a major role in the increase of atmospheric methane observed since 2005. Based on the GEOS-Chem-tagged simulation, we discuss possible cause(s) for the increase of methane since 2005, which is still unexplained.

Variability and evolution of the midlatitude stratospheric aerosol budget from 22 years of ground-based lidar and satellite observations

Abstract. The article presents new high-quality continuous stratospheric aerosol observations spanning 1994–2015 at the French Observatoire de Haute-Provence (OHP, 44° N, 6° E) obtained by two independent, regularly maintained lidar systems operating within the Network for Detection of Atmospheric Composition Change (NDACC). Lidar series are compared with global-coverage observations by Stratospheric Aerosol and Gas Experiment (SAGE II), Global Ozone Monitoring by Occultation of Stars (GOMOS), Optical Spectrograph and InfraRed Imaging System (OSIRIS), Cloud-Aerosol Lidar with Orthogonal Polarization (CALIOP), and Ozone Mapping Profiling Suite (OMPS) satellite instruments, altogether covering the time span of OHP lidar measurements. Local OHP and zonal-mean satellite series of stratospheric aerosol optical depth are in excellent agreement, allowing for accurate characterization of stratospheric aerosol evolution and variability at northern midlatitudes during the last 2 decades. The combination of local and global observations is used for a careful separation between volcanically perturbed and quiescent periods. While the volcanic signatures dominate the stratospheric aerosol record, the background aerosol abundance is found to be modulated remotely by the poleward transport of convectively cleansed air from the deep tropics and aerosol-laden air from the Asian monsoon region. The annual cycle of background aerosol at midlatitudes, featuring a minimum during late spring and a maximum during late summer, correlates with that of water vapor from the Aura Microwave Limb Sounder (MLS). Observations covering two volcanically quiescent periods over the last 2 decades provide an indication of a growth in the nonvolcanic component of stratospheric aerosol. A statistically significant factor of 2 increase in nonvolcanic aerosol since 1998, seasonally restricted to late summer and fall, is associated with the influence of the Asian monsoon and growing pollution therein.

Tropospheric water vapour isotopologue data (H<sub>2</sub><sup>16</sup>O, H<sub>2</sub><sup>18</sup>O, and HD<sup>16</sup>O) as obtained from NDACC/FTIR solar absorption spectra

Abstract. We report on the ground-based FTIR (Fourier transform infrared) tropospheric water vapour isotopologue remote sensing data that have been recently made available via the database of NDACC (Network for the Detection of Atmospheric Composition Change; ftp://ftp.cpc.ncep.noaa.gov/ndacc/MUSICA/) and via doi:10.5281/zenodo.48902. Currently, data are available for 12 globally distributed stations. They have been centrally retrieved and quality-filtered in the framework of the MUSICA project (MUlti-platform remote Sensing of Isotopologues for investigating the Cycle of Atmospheric water). We explain particularities of retrieving the water vapour isotopologue state (vertical distribution of H216O, H218O, and HD16O) and reveal the need for a new metadata template for archiving FTIR isotopologue data. We describe the format of different data components and give recommendations for correct data usage. Data are provided as two data types. The first type is best-suited for tropospheric water vapour distribution studies disregarding different isotopologues (comparison with radiosonde data, analyses of water vapour variability and trends, etc.). The second type is needed for analysing moisture pathways by means of H2O, δD-pair distributions.

Seasonal features of quasi-biennial variations of NO2 stratospheric content derived from ground-based measurements

Seasonal and latitudinal distributions of amplitudes of quasi-biennial variations in total NO2 content (NO2 TC), total ozone content (TOC), and stratospheric temperature are obtained. NO2 TC data from ground-based spectrometric measurements within the Network for the Detection of Atmospheric Composition Change (NDACC), TOC data from satellite measurements, and stratospheric temperature data from ERA-Interim reanalysis are used for the analysis. The differences in the NO2 TC diurnal cycles are identified between the westerly and easterly phases of the quasi-biennial oscillations (QBO) of equatorial stratospheric wind. The QBO effects in the NO2 TC, TOC, and stratospheric temperature in the Northern (NH) and Southern (SH) hemispheres are most significant in the winter–spring periods, with essential differences between the NH and SH. The NO2 TC in the Antarctic is less for the westerly phase of the QBO than that for the easterly phase, and the NO2 TC quasi-biennial variations in the SH mid-latitudes are opposite of the variations in the Antarctic. In the NH, the winter values of the NO2 TC are generally less during the westerly QBO phase than during the easterly phase, whereas in spring, on the contrary, the values for the westerly QBO phase exceed those for the easterly phase. Along with NO2, the features of the quasi-biennial variations of TOC and stratospheric temperature are discussed. Possible mechanisms of the quasi-biennial variations of the analyzed parameters are considered for the different latitudinal zones.

Validation of satellite-based noontime UVI with NDACC ground-based instruments: influence of topography, environment and satellite overpass time

Abstract. Spectral solar UV radiation measurements are performed in France using three spectroradiometers located at very different sites. One is installed in Villeneuve d'Ascq, in the north of France (VDA). It is an urban site in a topographically flat region. Another instrument is installed in Observatoire de Haute-Provence, located in the southern French Alps (OHP). It is a rural mountainous site. The third instrument is installed in Saint-Denis, Réunion Island (SDR). It is a coastal urban site on a small mountainous island in the southern tropics. The three instruments are affiliated with the Network for the Detection of Atmospheric Composition Change (NDACC) and carry out routine measurements to monitor the spectral solar UV radiation and enable derivation of UV index (UVI). The ground-based UVI values observed at solar noon are compared to similar quantities derived from the Ozone Monitoring Instrument (OMI, onboard the Aura satellite) and the second Global Ozone Monitoring Experiment (GOME-2, onboard the Metop-A satellite) measurements for validation of these satellite-based products. The present study concerns the period 2009–September 2012, date of the implementation of a new OMI processing tool. The new version (v1.3) introduces a correction for absorbing aerosols that were not considered in the old version (v1.2). Both versions of the OMI UVI products were available before September 2012 and are used to assess the improvement of the new processing tool. On average, estimates from satellite instruments always overestimate surface UVI at solar noon. Under cloudless conditions, the satellite-derived estimates of UVI compare satisfactorily with ground-based data: the median relative bias is less than 8 % at VDA and 4 % at SDR for both OMI v1.3 and GOME-2, and about 6 % for OMI v1.3 and 2 % for GOME-2 at OHP. The correlation between satellite-based and ground-based data is better at VDA and OHP (about 0.99) than at SDR (0.96) for both space-borne instruments. For all sky conditions, the median relative biases are much larger, with large dispersion for both instruments at all sites (VDA: about 12 %; OHP: 9 %; SDR: 11 %). Correlation between satellite-based and ground-based data is still better at VDA and OHP (about 0.95) than at SDR (about 0.73) for both satellite instruments. These results are explained considering the time of overpass of the two satellites, which is far from solar noon, preventing a good estimation of the cloud cover necessary for a good modelling of the UVI. Site topography and environment are shown to have a non-significant influence. At VDA and OHP, OMI v1.3 shows a significant improvement with respect to v1.2, which did not account for absorbing aerosols.

ARISE project capabilities for hazards monitoring

The ARISE (Atmospheric dynamics InfraStructure in Europe) project funded by the European Union combines the International infrasound monitoring system developed for the CTBT (Comprehensive nuclear-Test-Ban Treaty) verification, the NDACC (Network for the Detection of Atmospheric Composition Changes) lidar network, European observatories at mid latitudes (OHP observatory), tropics (OPAR observatory), high latitudes (ALOMAR), the European infrasound stations and satellites for the study of the dynamics of the atmosphere from ground to thermosphere. The ARISE network is unique by its coverage from equatorial to polar regions and the involved scales both in time (to tens of years) and space (one to thousands of kilometers). One of the major objective of ARISE is the monitoring of extreme events including lightning, earthquakes, tornadoes, and volcanoes. A review of the ARISE results will be presented. Volcano monitoring by the infrasound technology presents a strong interest for aviation safety in case of eru...

First characterization and validation of FORLI-HNO<sub>3</sub> vertical profiles retrieved from IASI/Metop

Abstract. Knowing the spatial and seasonal distributions of nitric acid (HNO3) around the globe is of great interest and allows us to comprehend the processes regulating stratospheric ozone, especially in the polar regions. Due to its unprecedented spatial and temporal sampling, the nadir-viewing Infrared Atmospheric Sounding Interferometer (IASI) is capable of sounding the atmosphere twice a day globally, with good spectral resolution and low noise. With the Fast Optimal Retrievals on Layers for IASI (FORLI) algorithm, we are retrieving, in near real time, columns as well as vertical profiles of several atmospheric species, among which is HNO3. We present in this paper the first characterization of the FORLI-HNO3 profile products, in terms of vertical sensitivity and error budgets. We show that the sensitivity of IASI to HNO3 is highest in the lower stratosphere (10–20 km), where the largest amounts of HNO3 are found, but that the vertical sensitivity of IASI only allows one level of information on the profile (degrees of freedom for signal, DOFS; ∼ 1). The sensitivity near the surface is negligible in most cases, and for this reason, a partial column (5–35 km) is used for the analyses. Both vertical profiles and partial columns are compared to FTIR ground-based measurements from the Network for the Detection of Atmospheric Composition Change (NDACC) to characterize the accuracy and precision of the FORLI-HNO3 product. The profile validation is conducted through the smoothing of the raw FTIR profiles by the IASI averaging kernels and gives good results, with a slight overestimation of IASI measurements in the upper troposphere/lower stratosphere (UTLS) at the six chosen stations (Thule, Kiruna, Jungfraujoch, Izaña, Lauder and Arrival Heights). The validation of the partial columns (5–35 km) is also conclusive with a mean correlation of 0.93 between IASI and the FTIR measurements. An initial survey of the HNO3 spatial and seasonal variabilities obtained from IASI measurements for a 1-year (2011) data set shows that the expected latitudinal gradient of concentrations from low to high latitudes and the large seasonal variability in polar regions (cycle amplitude around 30 % of the seasonal signal, peak to peak) are well represented by IASI data.

The natural oscillations in stratospheric ozone observed by the GROMOS microwave radiometer at the NDACC station Bern

Abstract. A multilinear parametric regression analysis was performed to assess the seasonal and interannual variations of stratospheric ozone profiles from the GROMOS (GROund-based Millimeter-wave Ozone Spectrometer) microwave radiometer at Bern, Switzerland (46.95° N, 7.44° E; 577 m). GROMOS takes part in the Network for the Detection of Atmospheric Composition Change (NDACC). The study covers the stratosphere from 50 to 0.5 hPa (from 21 to 53 km) and extends over the period from January 1997 to January 2015. The natural variability was fitted during the regression analysis through the annual and semi-annual oscillations (AO, SAO), the quasi-biennial oscillation (QBO), the El Niño–Southern Oscillation (ENSO) and the solar activity cycle. Seasonal ozone variations mainly appear as an annual cycle in the middle and upper stratosphere and a semi-annual cycle in the upper stratosphere. Regarding the interannual variations, they are primarily present in the lower and middle stratosphere. In the lower and middle stratosphere, ozone variations are controlled predominantly by transport processes, due to the long lifetime of ozone, whereas in the upper stratosphere its lifetime is relatively short and ozone is controlled mainly by photochemistry. The present study shows agreement in the observed naturally induced ozone signatures with other studies. Further, we present an overview of the possible causes of the effects observed in stratospheric ozone due to natural oscillations at a northern midlatitude station. For instance regarding the SAO, we find that polar winter stratopause warmings contribute to the strength of this oscillation since these temperature enhancements lead to a reduction in upper stratospheric ozone. We have detected a strong peak amplitude of about 5 % for the solar cycle in lower stratospheric ozone for our 1.5 cycles of solar activity. Though the 11-year ozone oscillation above Bern is in phase with the solar cycle, we suppose that the strong amplitude is partly due to meteorological disturbances and associated ozone anomalies in the Northern Hemisphere. Further, our observational study gave the result that ozone above Bern is anti-correlated with the ENSO phenomenon in the lower stratosphere and correlated in the middle stratosphere.

An evaluation of IASI-NH<sub>3</sub> with ground-based Fourier transform infrared spectroscopy measurements

Abstract. Global distributions of atmospheric ammonia (NH3) measured with satellite instruments such as the Infrared Atmospheric Sounding Interferometer (IASI) contain valuable information on NH3 concentrations and variability in regions not yet covered by ground-based instruments. Due to their large spatial coverage and (bi-)daily overpasses, the satellite observations have the potential to increase our knowledge of the distribution of NH3 emissions and associated seasonal cycles. However the observations remain poorly validated, with only a handful of available studies often using only surface measurements without any vertical information. In this study, we present the first validation of the IASI-NH3 product using ground-based Fourier transform infrared spectroscopy (FTIR) observations. Using a recently developed consistent retrieval strategy, NH3 concentration profiles have been retrieved using observations from nine Network for the Detection of Atmospheric Composition Change (NDACC) stations around the world between 2008 and 2015. We demonstrate the importance of strict spatio-temporal collocation criteria for the comparison. Large differences in the regression results are observed for changing intervals of spatial criteria, mostly due to terrain characteristics and the short lifetime of NH3 in the atmosphere. The seasonal variations of both datasets are consistent for most sites. Correlations are found to be high at sites in areas with considerable NH3 levels, whereas correlations are lower at sites with low atmospheric NH3 levels close to the detection limit of the IASI instrument. A combination of the observations from all sites (Nobs = 547) give a mean relative difference of −32.4 ± (56.3) %, a correlation r of 0.8 with a slope of 0.73. These results give an improved estimate of the IASI-NH3 product performance compared to the previous upper-bound estimates (−50 to +100 %).

Accomplishments of the MUSICA project to provide accurate, long-term, global and high-resolution observations of tropospheric {H<sub>2</sub>O,<i>δ</i>D} pairs – a review

Abstract. In the lower/middle troposphere, {H2O,δD} pairs are good proxies for moisture pathways; however, their observation, in particular when using remote sensing techniques, is challenging. The project MUSICA (MUlti-platform remote Sensing of Isotopologues for investigating the Cycle of Atmospheric water) addresses this challenge by integrating the remote sensing with in situ measurement techniques. The aim is to retrieve calibrated tropospheric {H2O,δD} pairs from the middle infrared spectra measured from ground by FTIR (Fourier transform infrared) spectrometers of the NDACC (Network for the Detection of Atmospheric Composition Change) and the thermal nadir spectra measured by IASI (Infrared Atmospheric Sounding Interferometer) aboard the MetOp satellites. In this paper, we present the final MUSICA products, and discuss the characteristics and potential of the NDACC/FTIR and MetOp/IASI {H2O,δD} data pairs. First, we briefly resume the particularities of an {H2O,δD} pair retrieval. Second, we show that the remote sensing data of the final product version are absolutely calibrated with respect to H2O and δD in situ profile references measured in the subtropics, between 0 and 7 km. Third, we reveal that the {H2O,δD} pair distributions obtained from the different remote sensors are consistent and allow distinct lower/middle tropospheric moisture pathways to be identified in agreement with multi-year in situ references. Fourth, we document the possibilities of the NDACC/FTIR instruments for climatological studies (due to long-term monitoring) and of the MetOp/IASI sensors for observing diurnal signals on a quasi-global scale and with high horizontal resolution. Fifth, we discuss the risk of misinterpreting {H2O,δD} pair distributions due to incomplete processing of the remote sensing products.

Rugged optical mirrors for Fourier transform spectrometers operated in harsh environments

Abstract. The Total Carbon Column Observing Network (TCCON) and the Network for the Detection of Atmospheric Composition Change (NDACC) operate a number of Fourier transform spectrometers (FTSs) that measure trace gases in the atmosphere by observing solar spectra. To guide the sunlight into the FTS, a solar tracker has to be placed outside. This device needs high-quality optical mirrors with good reflectance in the near and mid-infrared.More and more FTS stations are operated in remote locations with harsh environments. Optical mirrors are usually made for laboratory conditions and might not last very long there. At the TCCON site on Ascension Island which is operated by the Max Planck Institute for Biogeochemistry (MPI-BGC), several mirrors from different optical manufacturers were destroyed within weeks.To continue operation, the MPI-BGC had to develop rugged mirrors that could sustain the harsh conditions for months or even years. While commercially available mirrors are typically made from a substrate covered with a thin reflective coating, these rugged mirrors were made from stainless steel with no additional coating. Except for their lower reflectance (which can easily be compensated for), their optical properties are comparable to existing mirrors. However, their rugged design makes them mostly immune to corrosion and scratching. Unlike most coated mirrors, they can also be cleaned easily.

Comparison of XCO abundances from the Total Carbon Column Observing Network and the Network for the Detection of Atmospheric Composition Change measured in Karlsruhe

Abstract. We present a comparison of Karlsruhe XCO records (April 2010–December 2014) from the Total Carbon Column Observing Network (TCCON) and from the spectral region covered by the Network for the Detection of Atmospheric Composition Change (NDACC). The Karlsruhe TCCON Fourier transform infrared (FTIR) spectrometer allows us to record spectra in the mid-infrared (MIR) and near-infrared (NIR) spectral region simultaneously, which makes Karlsruhe a favourable FTIR site to directly compare measurements from both spectral regions. We compare XCO retrieved from the fundamental absorption band at 4.7 µm (as used by NDACC) and first overtone absorption band at 2.3 µm (TCCON-style measurements). We observe a bias of (4.47 ± 0.17) ppb between both data sets with a standard deviation of 2.39 ppb in seasonal variation. This corresponds to a relative bias of (4.76 ± 0.18) % and a standard deviation of 2.28 %. We identify different sources which contribute to the observed bias (air-mass-independent correction factor, air-mass-dependent correction factor, isotopic identities, differing a priori volume mixing ratio profiles) and quantify their contributions. We show that the seasonality in the residual of NDACC and TCCON XCO can be largely explained by the smoothing effect caused by differing averaging kernel sensitivities between the MIR and NIR spectral region. This study aims to improve the comparability of NDACC and TCCON XCO validation data sets as desired for potential future satellite missions and model studies.

Evaluation of the inter-annual variability of stratospheric chemical composition in chemistry-climate models using ground-based multi species time series

The variability of stratospheric chemical composition occurs on a broad spectrum of timescales, ranging from day to decades. A large part of the variability appears to be driven by external forcings such as volcanic aerosols, solar activity, halogen loading, levels of greenhouse gases (GHG), and modes of climate variability (quasi-biennial oscillation (QBO), El Niño-Southern Oscillation (ENSO)). We estimate the contributions of different external forcings to the interannual variability of stratospheric chemical composition and evaluate how well 3-D chemistry-climate models (CCMs) can reproduce the observed response-forcing relationships. We carry out multivariate regression analyses on long time series of observed and simulated time series of several traces gases in order to estimate the contributions of individual forcings and unforced variability to their internannual variability. The observations are typically decadal time series of ground-based data from the international Network for the Detection of Atmospheric Composition Change (NDACC) and the CCM simulations are taken from the CCMVal-2 REF-B1 simulations database. The chemical species considered are column O3, HCl, NO2, and N2O. We check the consistency between observations and model simulations in terms of the forced and internal components of the total interannual variability (externally forced variability and internal variability) and identify the driving factors in the interannual variations of stratospheric chemical composition over NDACC measurement sites. Overall, there is a reasonably good agreement between regression results from models and observations regarding the externally forced interannual variability. A much larger fraction of the observed and modelled interannual variability is explained by external forcings in the tropics than in the extratropics, notably in polar regions. CCMs are able to reproduce the amplitudes of responses in chemical composition to specific external forcings. However, CCMs tend to underestimate very substantially the internal variability and hence the total interannual variability for almost all species considered. This lack of internal variability in CCMs might partly originate from the surface forcing of these CCMs by analysed SSTs. The results illustrate the potential of NDACC ground-based observations for evaluating CCMs.

Water Vapour Mixing Ratio Measurements in Potenza in the Frame of the International Network for the Detection of Atmospheric Composition Change - NDACC

In November 2012 the University of BASILicata Raman Lidar system (BASIL ) was approved to enter the International Network for the Detection of Atmospheric Composition Change (NDACC). This network includes more than 70 high-quality, remote-sensing research stations for observing and understanding the physical and chemical state of the upper troposphere and stratosphere and for assessing the impact of stratosphere changes on the underlying troposphere and on global climate. As part of this network, more than thirty groundbased Lidars deployed worldwide are routinely operated to monitor atmospheric ozone, temperature, aerosols, water vapour, and polar stratospheric clouds.In the frame of NDACC, BASIL performs measurements on a routine basis each Thursday, typically from local noon to midnight, covering a large portion of the daily cycle. Measurements from BASIL are included in the NDACC database both in terms of water vapour mixing ratio and temperature. This paper illustrates some measurement examples from BASIL, with a specific focus on water vapour measurements, with the goal to try and characterize the system performances.

Results of a Longer Term NDACC Measurements Comparison Campaign at Mauna Loa Observatory

Between November, 2015 and January, 2015, the Goddard Space Flight Center (GSFC) operated a pair of lidar instruments at the NOAA (National Oceanic and Atmospheric Administration) facility at Mauna Loa on the Big Island of Hawaii (Latitude 19.5 degrees North, Longitude 155.5 degrees West, altitude 3.397 kilometers). Measurements were made during six different four week periods during this time period by both the NASA GSFC Stratospheric Ozone Lidar (STROZ) and the Aerosol and Temperature (ATL) lidar. Also making measurements were the JPL Stratospheric Ozone Lidar and the NOAA Aerosol and Water Vapor Lidar. All instruments participate and archive data with the Network for the Detection of Atmospheric Composition Change (NDACC). Measurement comparisons were made among various instruments in accordance with the standard intercomparison protocols of the NDACC.

Ground-based spectroscopic measurements of atmospheric gas composition near Saint Petersburg (Russia)

Since early 2009, high-resolution solar absorption spectra have been recorded at the Peterhof station (59.88°N, 29.82°E) of Saint Petersburg State University located in the suburbs of St. Petersburg. Measurements are made with the Fourier Transform Infrared (FTIR) system, which consists of Bruker IFS 125HR instrument (with maximum spectral resolution of 0.005cm−1) and self-designed solar tracker. We derived total column (TC) of a dozen of atmospheric gases from recorded spectra and performed the error analysis of these retrievals. Furthermore, we analysed the temporal variability of the important climatically active gases, such as H2O, CH4, O3, CO, and NO2 near St. Petersburg and compared our retrievals with independent ground-based and satellite data, as well as with the results of EMAC model numerical simulations. Currently, the results of our measurements and the measuring system are under validation for entering the international Network for the Detection of Atmospheric Composition Change (NDACC).

Evaluating a new homogeneous total ozone climate data record from GOME/ERS‐2, SCIAMACHY/Envisat, and GOME‐2/MetOp‐A

AbstractThe European Space Agency's Ozone Climate Change Initiative (O3‐CCI) project aims at producing and validating a number of high‐quality ozone data products generated from different satellite sensors. For total ozone, the O3‐CCI approach consists of minimizing sources of bias and systematic uncertainties by applying a common retrieval algorithm to all level 1 data sets, in order to enhance the consistency between the level 2 data sets from individual sensors. Here we present the evaluation of the total ozone products from the European sensors Global Ozone Monitoring Experiment (GOME)/ERS‐2, SCIAMACHY/Envisat, and GOME‐2/MetOp‐A produced with the GOME‐type Direct FITting (GODFIT) algorithm v3. Measurements from the three sensors span more than 16 years, from 1996 to 2012. In this work, we present the latest O3‐CCI total ozone validation results using as reference ground‐based measurements from Brewer and Dobson spectrophotometers archived at the World Ozone and UV Data Centre of the World Meteorological Organization as well as from UV‐visible differential optical absorption spectroscopy (DOAS)/Système D′Analyse par Observations Zénithales (SAOZ) instruments from the Network for the Detection of Atmospheric Composition Change. In particular, we investigate possible dependencies in these new GODFIT v3 total ozone data sets with respect to latitude, season, solar zenith angle, and different cloud parameters, using the most adequate type of ground‐based instrument. We show that these three O3‐CCI total ozone data products behave very similarly and are less sensitive to instrumental degradation, mainly as a result of the new reflectance soft‐calibration scheme. The mean bias to the ground‐based observations is found to be within the 1 ± 1% level for all three sensors while the near‐zero decadal stability of the total ozone columns (TOCs) provided by the three European instruments falls well within the 1–3% requirement of the European Space Agency's Ozone Climate Change Initiative project.

Metrology of ground-based satellite validation: co-location mismatch and smoothing issues of total ozone comparisons

Abstract. Comparisons with ground-based correlative measurements constitute a key component in the validation of satellite data on atmospheric composition. The error budget of these comparisons contains not only the measurement errors but also several terms related to differences in sampling and smoothing of the inhomogeneous and variable atmospheric field. A versatile system for Observing System Simulation Experiments (OSSEs), named OSSSMOSE, is used here to quantify these terms. Based on the application of pragmatic observation operators onto high-resolution atmospheric fields, it allows a simulation of each individual measurement, and consequently, also of the differences to be expected from spatial and temporal field variations between both measurements making up a comparison pair. As a topical case study, the system is used to evaluate the error budget of total ozone column (TOC) comparisons between GOME-type direct fitting (GODFITv3) satellite retrievals from GOME/ERS2, SCIAMACHY/Envisat, and GOME-2/MetOp-A, and ground-based direct-sun and zenith–sky reference measurements such as those from Dobsons, Brewers, and zenith-scattered light (ZSL-)DOAS instruments, respectively. In particular, the focus is placed on the GODFITv3 reprocessed GOME-2A data record vs. the ground-based instruments contributing to the Network for the Detection of Atmospheric Composition Change (NDACC). The simulations are found to reproduce the actual measurements almost to within the measurement uncertainties, confirming that the OSSE approach and its technical implementation are appropriate. This work reveals that many features of the comparison spread and median difference can be understood as due to metrological differences, even when using strict co-location criteria. In particular, sampling difference errors exceed measurement uncertainties regularly at most mid- and high-latitude stations, with values up to 10 % and more in extreme cases. Smoothing difference errors only play a role in the comparisons with ZSL-DOAS instruments at high latitudes, especially in the presence of a polar vortex due to the strong TOC gradient it induces. At tropical latitudes, where TOC variability is lower, both types of errors remain below about 1 % and consequently do not contribute significantly to the comparison error budget. The detailed analysis of the comparison results, including the metrological errors, suggests that the published random measurement uncertainties for GODFITv3 reprocessed satellite data are potentially overestimated, and adjustments are proposed here. This successful application of the OSSSMOSE system to close for the first time the error budget of TOC comparisons, bodes well for potential future applications, which are briefly touched upon.

Trend analysis of the 20-year time series of stratospheric ozone profiles observed by the GROMOS microwave radiometer at Bern

Abstract. The ozone radiometer GROMOS (GROund-based Millimeter-wave Ozone Spectrometer) has been performing continuous observations of stratospheric ozone profiles since 1994 above Bern, Switzerland (46.95° N, 7.44° E, 577 m). GROMOS is part of the Network for the Detection of Atmospheric Composition Change (NDACC). From November 1994 to October 2011, the ozone line spectra were measured by a filter bench (FB). In July 2009, a fast Fourier transform spectrometer (FFTS) was added as a back end to GROMOS. The new FFTS and the original FB measured in parallel for over 2 years. The ozone profiles retrieved separately from the ozone line spectra of FB and FFTS agree within 5 % at pressure levels from 30 to 0.5 hPa, from October 2009 to August 2011. A careful harmonisation of both time series has been carried out by taking the FFTS as the reference instrument for the FB. This enables us to assess the long-term trend derived from stratospheric ozone observations at Bern. The trend analysis was performed by using a robust multilinear parametric trend model which includes a linear term, the solar variability, the El Niño–Southern Oscillation (ENSO) index, the quasi-biennial oscillation (QBO), the annual and semi-annual oscillation and several harmonics with period lengths between 3 and 24 months. Over the last years, some experimental and modelling trend studies have shown that the stratospheric ozone trend is levelling off or even turning positive. With our observed ozone profiles, we are able to support this statement by reporting a statistically significant trend of +3.14 % decade−1 at 4.36 hPa (37.76 km), covering the period from January 1997 to January 2015, above Bern. Additionally, we have estimated a negative trend over this period of −3.94 % decade−1 at 0.2 hPa (59 km).