Measurements of hydrogen cyanide (HCN) and acetylene (C2H2) from the Infrared Atmospheric Sounding Interferometer (IASI)

Hydrogen cyanide (HCN) and acetylene (C2H2) are ubiquitous atmospheric trace gases with medium lifetime, which are frequently used as indicators of combustion sources and as tracers for atmospheric transport and chemistry. Because of their weak infrared absorption, overlapped by the CO2 Q branch near 720 cm−1, nadir sounders have up to now failed to measure these gases routinely. Taking into account CO2 line mixing, we provide for the first time extensive measurements of HCN and C2H2 total columns at Reunion Island (21° S, 55° E) and Jungfraujoch (46° N, 8° E) in 2009–2010 using observations from the Infrared Atmospheric Sounding Interferometer (IASI). A first order comparison with local ground-based Fourier transform InfraRed (FTIR) measurements has been carried out allowing tests of seasonal consistency which is reasonably captured, except for HCN at Jungfraujoch. The IASI data shows a greater tendency to high C2H2 values. We also examine a nonspecific biomass burning plume over austral Africa and show that the emission ratios with respect to CO agree with previously reported values

The evaluation of SCIAMACHY CO and CH_4 scientific data products, using ground-based FTIR measurements

In the framework of the European EVERGREEN project, three scientific algorithms, namely WFM-DOAS, IMAPDOAS and IMLM, have been developed to retrieve the total column amounts of key atmospheric trace gases including CO and CH_4 from SCIAMACHY nadir observations in its near-infrared channels. These channels offer the capability to detect trace gases in the planetary boundary layer, potentially making the associated retrieval products suited for regional source-sink studies. The retrieval products of these three algorithms, in their present status of development, have been compared to independent data from a ground-based quasi-global network of Fourier-transform infrared (FTIR) spectrometers, for the year 2003. Comparisons have been made for individual data, as well as for monthly averages. To maximize the number of coincidences that satisfy the temporal and spatial collocation criteria, the individual SCIAMACHY data points have been compared with a 3rd order polynomial interpolation of the ground-based data with time. Particular attention has been paid to the question whether the products reproduce correctly the seasonal and latitudinal variabilities of the target species. We present an overall assessment of the data quality of the currently available latest versions of the CO and CH4 total column products from the three scientific retrieval algorithms

The Greenhouse Gas Climate Change Initiative (GHG-CCI): comparative validation of GHG-CCI SCIAMACHY/ENVISAT and TANSO-FTS/GOSAT CO₂ and CH₄ retrieval algorithm products with measurements from the TCCON

Column-averaged dry-air mole fractions of carbon dioxide and methane have been retrieved from spectra acquired by the TANSO-FTS (Thermal And Near-infrared Sensor for carbon Observations-Fourier Transform Spectrometer) and SCIAMACHY (Scanning Imaging Absorption Spectrometer for Atmospheric Cartography) instruments on board GOSAT (Greenhouse gases Observing SATellite) and ENVISAT (ENVIronmental SATellite), respectively, using a range of European retrieval algorithms. These retrievals have been compared with data from ground-based high-resolution Fourier transform spectrometers (FTSs) from the Total Carbon Column Observing Network (TCCON). The participating algorithms are the weighting function modified differential optical absorption spectroscopy (DOAS) algorithm (WFMD, University of Bremen), the Bremen optimal estimation DOAS algorithm (BESD, University of Bremen), the iterative maximum a posteriori DOAS (IMAP, Jet Propulsion Laboratory (JPL) and Netherlands Institute for Space Research algorithm (SRON)), the proxy and full-physics versions of SRON's RemoTeC algorithm (SRPR and SRFP, respectively) and the proxy and full-physics versions of the University of Leicester's adaptation of the OCO (Orbiting Carbon Observatory) algorithm (OCPR and OCFP, respectively). The goal of this algorithm inter-comparison was to identify strengths and weaknesses of the various so-called round- robin data sets generated with the various algorithms so as to determine which of the competing algorithms would proceed to the next round of the European Space Agency's (ESA) Greenhouse Gas Climate Change Initiative (GHG-CCI) project, which is the generation of the so-called Climate Research Data Package (CRDP), which is the first version of the Essential Climate Variable (ECV) "greenhouse gases" (GHGs). For XCO₂, all algorithms reach the precision requirements for inverse modelling (< 8 ppm), with only WFMD having a lower precision (4.7 ppm) than the other algorithm products (2.4–2.5 ppm). When looking at the seasonal relative accuracy (SRA, variability of the bias in space and time), none of the algorithms have reached the demanding < 0.5 ppm threshold. For XCH₄, the precision for both SCIAMACHY products (50.2 ppb for IMAP and 76.4 ppb for WFMD) fails to meet the < 34 ppb threshold for inverse modelling, but note that this work focusses on the period after the 2005 SCIAMACHY detector degradation. The GOSAT XCH₄ precision ranges between 18.1 and 14.0 ppb. Looking at the SRA, all GOSAT algorithm products reach the < 10 ppm threshold (values ranging between 5.4 and 6.2 ppb). For SCIAMACHY, IMAP and WFMD have a SRA of 17.2 and 10.5 ppb, respectively

Retrieval of stratospheric and tropospheric BrO profiles and columns using ground-based zenith-sky DOAS observations at Harestua, 60° N

A profiling algorithm based on the optimal estimation method is applied to ground-based zenith-sky UV-visible measurements from Harestua, Southern Norway (60&deg; N, 11&deg; E) in order to retrieve BrO vertical profiles. The sensitivity of the zenith-sky observations to the tropospheric BrO detection is increased by using for the spectral analysis a fixed reference spectrum corresponding to clear-sky noon summer conditions. The information content and retrieval errors are characterized and it is shown that the retrieved stratospheric profiles and total columns are consistent with correlative balloon and satellite observations, respectively. Tropospheric BrO columns are derived from profiles retrieved at 80&deg; solar zenith angle during sunrise and sunset for the 2000&ndash;2006 period. They show a marked seasonality with mean column value ranging from 1.52&plusmn;0.62&times;10¹³ molec/cm² in late winter/early spring to 0.92&plusmn;0.38&times;10¹³ molec/cm² in summer, which corresponds to 1.0&plusmn;0.4 and 0.6&plusmn;0.2 pptv, respectively, if we assume that BrO is uniformly mixed in the troposphere. These column values are also consistent with previous estimates made from balloon, satellite, and other ground-based observations. Daytime (10:30 LT) tropospheric BrO columns are compared to the <i>p</i>-TOMCAT 3-D tropospheric chemical transport model (CTM) for the 2002&ndash;2003 period. <i>p</i>-TOMCAT shows a good agreement with the retrieved columns except in late winter/early spring where an underestimation by the model is obtained. This finding could be explained by the non-inclusion of sea-ice bromine sources in the current version of <i>p</i>-TOMCAT. Therefore the model cannot reproduce the possible transport of air-masses with enhanced BrO concentration due to bromine explosion events from the polar region to Harestua. The daytime stratospheric BrO columns are compared to the SLIMCAT stratospheric 3-D-CTM. The model run used in this study, which assumes 21.2 pptv for the Br_y loading (15 pptv for long-lived bromine species and additional 6 pptv for very short-lived species (VSLS) added by a scaling of CH₃Br), significantly underestimates the retrieved BrO columns. A sensitivity study shows that a good agreement can only be obtained if 6 to 8 pptv accounting for VSLS are added directly (and not by a scaling of CH₃Br) to the SLIMCAT long-lived bromine species profile. This contribution of the VSLS to the total bromine loading is also consistent with recently published studies

Retrieval of nitrogen dioxide stratospheric profiles from ground-based zenith-sky UV-visible observations: validation of the technique through correlative comparisons

A retrieval algorithm based on the Optimal Estimation Method (OEM) has been developed in order to provide vertical distributions of NO₂ in the stratosphere from ground-based (GB) zenith-sky UV-visible observations. It has been applied to observational data sets from the NDSC (Network for Detection of Stratospheric Change) stations of Harestua (60&deg; N, 10&deg; E) and And&#248;ya (69&deg; N, 16&deg; E) in Norway. The information content and retrieval errors have been analyzed following a formalism used for characterizing ozone profiles retrieved from solar infrared absorption spectra. In order to validate the technique, the retrieved NO₂ vertical profiles and columns have been compared to correlative balloon and satellite observations. Such extensive validation of the profile and column retrievals was not reported in previously published work on the profiling from GB UV-visible measurements. A good agreement - generally better than 25% - has been found with the SAOZ (Syst&#232;me d'Analyse par Observations Z&#233;nithales) and DOAS (Differential Optical Absorption Spectroscopy) balloons. A similar agreement has been reached with correlative satellite data from the HALogen Occultation Experiment (HALOE) and Polar Ozone and Aerosol Measurement (POAM) III instruments above 25km of altitude. Below 25km, a systematic underestimation - by up to 40% in some cases - of both HALOE and POAM III profiles by our GB profile retrievals has been observed, pointing out more likely a limitation of both satellite instruments at these altitudes. We have concluded that our study strengthens our confidence in the reliability of the retrieval of vertical distribution information from GB UV-visible observations and offers new perspectives in the use of GB UV-visible network data for validation purposes

Ozone seasonal evolution and photochemical production regime in the polluted troposphere in eastern China derived from high-resolution Fourier transform spectrometry (FTS) observations

The seasonal evolution of O3 and its photochemical production regime in a polluted region of eastern China between 2014 and 2017 has been investigated using observations. We used tropospheric ozone (O3), carbon monoxide (CO), and formaldehyde (HCHO, a marker of VOCs (volatile organic compounds)) partial columns derived from high-resolution Fourier transform spectrometry (FTS); tropospheric nitrogen dioxide (NO2, a marker of NOx (nitrogen oxides)) partial column deduced from the Ozone Monitoring Instrument (OMI); surface meteorological data; and a back trajectory cluster analysis technique. A broad O3 maximum during both spring and summer (MAM/JJA) is observed; the day-to-day variations in MAM/JJA are generally larger than those in autumn and winter (SON/DJF). Tropospheric O3 columns in June are 1.55x1018moleculescm-2 (56DU (Dobson units)), and in December they are 1.05x1018moleculescm-2 (39 DU). Tropospheric O3 columns in June were ∼ 50% higher than those in December. Compared with the SON/DJF season, the observed tropospheric O3 levels in MAM/JJA are more influenced by the transport of air masses from densely populated and industrialized areas, and the high O3 level and variability in MAM/JJA is determined by the photochemical O3 production. The tropospheric-column HCHO/NO2 ratio is used as a proxy to investigate the photochemical O3 production rate (PO3). The results show that the PO3 is mainly nitrogen oxide (NOx) limited in MAM/JJA, while it is mainly VOC or mixed VOC-NOx limited in SON/DJF. Statistics show that NOx-limited, mixed VOC-NOx-limited, and VOC-limited PO3 accounts for 60.1%, 28.7%, and 11% of days, respectively. Considering most of PO3 is NOx limited or mixed VOC-NOx limited, reductions in NOx would reduce O3 pollution in eastern China

Acetylene (C2H2) and hydrogen cyanide (HCN) from IASI satellite observations: Global distributions, validation, and comparison with model

We present global distributions of C$_{2}$H$_{2}$ and hydrogen cyanide (HCN) total columns derived from the Infrared Atmospheric Sounding Interferometer (IASI) for the years 2008–2010. These distributions are obtained with a fast method allowing to retrieve C$_{2}$H$_{2}$ abundance globally with a 5% precision and HCN abundance in the tropical (subtropical) belt with a 10% (25 %) precision. IASI data are compared for validation purposes with ground-based Fourier transform infrared (FTIR) spectrometer measurements at four selected stations.We show that there is an overall agreement between the ground-based and space measurements with correlation coefficients for daily mean measurements ranging from 0.28 to 0.81, depending on the site. Global C$_{2}$H$_{2}$ and subtropical HCN abundances retrieved from IASI spectra show the expected seasonality linked to variations in the anthropogenic emissions and seasonal biomass burning activity, as well as exceptional events, and are in good agreement with previous spaceborne studies. Total columns simulated by the Model for Ozone and Related Chemical Tracers, version 4 (MOZART-4) are compared to the ground-based FTIR measurements at the four selected stations. The model is able to capture the seasonality in the two species in most of the cases, with correlation coefficients for daily mean measurements ranging from 0.50 to 0.86, depending on the site. IASI measurements are also compared to the distributions from MOZART-4. Seasonal cycles observed from satellite data are reasonably well reproduced by the model with correlation coefficients ranging from -0.31 to 0.93 for C$_{2}$H$_{2}$ daily means, and from 0.09 to 0.86 for HCN daily means, depending on the considered region. However, the anthropogenic (biomass burning) emissions used in the model seem to be overestimated (underestimated), and a negative global mean bias of 1% (16 %) of the model relative to the satellite observations was found for C$_{2}$H$_{2}$ (HCN)

Validation and data characteristics of methane and nitrous oxide profiles observed by MIPAS and processed with Version 4.61 algorithm

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