Network For Detection Of Atmospheric Composition Change Research Articles

Variability of Water Vapor in Central Mexico from Two Remote Sensing Techniques: FTIR Spectroscopy and GPS

Abstract Total column H2O is measured by two remote sensing techniques at the Altzomoni Atmospheric Observatory (19°12′N, 98°65′W, 4000 m above sea level), a high-altitude, tropical background site in central Mexico. A ground-based solar absorption FTIR spectrometer that is part of the Network for Detection of Atmospheric Composition Change (NDACC) is used to retrieve water vapor in three spectral regions (6074–6471, 2925–2941, and 1110–1253 cm−1) and is compared to data obtained from a global positioning system (GPS) receiver that is part of the TLALOCNet GPS-meteorological network. Strong correlations are obtained between the coincident hourly means from the three FTIR products and small relative bias and correction factors could be determined for each when compared to the more consistent GPS data. Retrievals from the 2925–2941 cm−1 spectral region have the highest correlation with GPS [coefficient of determination (R2) = 0.998, standard deviation (STD) = 0.18 cm (78.39%), mean difference = 0.04 cm (8.33%)], although the other products are also highly correlated [R2 ≥ 0.99, STD ≤ 0.20 cm (<90%), mean difference ≤ 0.1 cm (<24%)]. Clear-sky dry bias (CSDB) values are reduced to <10% (<0.20 cm) when coincident hourly means are used in the comparison. The use of GPS and FTIR water vapor products simultaneously leads to a more complete and better description of the diurnal and seasonal cycles of water vapor. We describe the water vapor climatology with both complementary datasets, nevertheless, pointing out the importance of considering the clear-sky dry bias arising from the large diurnal and seasonal variability of water vapor at this high-altitude tropical site.

The Diurnal Variation in Stratospheric Ozone from MACC Reanalysis, ERA-Interim, WACCM, and Earth Observation Data: Characteristics and Intercomparison

In this study, we compare the diurnal variation in stratospheric ozone of the MACC (Monitoring Atmospheric Composition and Climate) reanalysis, ECMWF Reanalysis Interim (ERA-Interim), and the free-running WACCM (Whole Atmosphere Community Climate Model). The diurnal variation of stratospheric ozone results from photochemical and dynamical processes depending on altitude, latitude, and season. MACC reanalysis and WACCM use similar chemistry modules and calculate a similar diurnal cycle in ozone when it is caused by a photochemical variation. The results of the two model systems are confirmed by observations of the Superconducting Submillimeter-Wave Limb-Emission Sounder (SMILES) experiment and three selected sites of the Network for Detection of Atmospheric Composition Change (NDACC) at Mauna Loa, Hawaii (tropics), Bern, Switzerland (midlatitudes), and Ny-Ålesund, Svalbard (high latitudes). On the other hand, the ozone product of ERA-Interim shows considerably less diurnal variation due to photochemical variations. The global maxima of diurnal variation occur at high latitudes in summer, e.g., near the Arctic NDACC site at Ny-Ålesund, Svalbard. The local OZORAM radiometer observes this effect in good agreement with MACC reanalysis and WACCM. The sensed diurnal variation at Ny-Ålesund is up to 8% (0.4 ppmv) due to photochemical variations in summer and negligible during the dynamically dominated winter. However, when dynamics play a major role for the diurnal ozone variation as in the lower stratosphere (100–20 hPa), the reanalysis models ERA-Interim and MACC which assimilate data from radiosondes and satellites outperform the free-running WACCM. Such a domain is the Antarctic polar winter where a surprising novel feature of diurnal variation is indicated by MACC reanalysis and ERA-Interim at the edge of the polar vortex. This effect accounts for up to 8% (0.4 ppmv) in both model systems. In summary, MACC reanalysis provides a global description of the diurnal variation of stratospheric ozone caused by dynamics and photochemical variations. This is of high interest for ozone trend analysis and other research which is based on merged satellite data or measurements at different local time.

Fourier transform infrared time series of tropospheric HCN in eastern China: seasonality, interannual variability, and source attribution

Abstract. We analyzed seasonality and interannual variability of tropospheric hydrogen cyanide (HCN) columns in densely populated eastern China for the first time. The results were derived from solar absorption spectra recorded with a ground-based high-spectral-resolution Fourier transform infrared (FTIR) spectrometer in Hefei (31∘54′ N, 117∘10′ E) between 2015 and 2018. The tropospheric HCN columns over Hefei, China, showed significant seasonal variations with three monthly mean peaks throughout the year. The magnitude of the tropospheric HCN column peaked in May, September, and December. The tropospheric HCN column reached a maximum monthly mean of (9.8±0.78)×1015 molecules cm−2 in May and a minimum monthly mean of (7.16±0.75)×1015 molecules cm−2 in November. In most cases, the tropospheric HCN columns in Hefei (32∘ N) are higher than the FTIR observations in Ny-Ålesund (79∘ N), Kiruna (68∘ N), Bremen (53∘ N), Jungfraujoch (47∘ N), Toronto (44∘ N), Rikubetsu (43∘ N), Izana (28∘ N), Mauna Loa (20∘ N), La Reunion Maido (21∘ S), Lauder (45∘ S), and Arrival Heights (78∘ S) that are affiliated with the Network for Detection of Atmospheric Composition Change (NDACC). Enhancements of tropospheric HCN column were observed between September 2015 and July 2016 compared to the same period of measurements in other years. The magnitude of the enhancement ranges from 5 % to 46 % with an average of 22 %. Enhancement of tropospheric HCN (ΔHCN) is correlated with the concurrent enhancement of tropospheric CO (ΔCO), indicating that enhancements of tropospheric CO and HCN were due to the same sources. The GEOS-Chem tagged CO simulation, the global fire maps, and the potential source contribution function (PSCF) values calculated using back trajectories revealed that the seasonal maxima in May are largely due to the influence of biomass burning in Southeast Asia (SEAS) (41±13.1 %), Europe and boreal Asia (EUBA) (21±9.3 %), and Africa (AF) (22±4.7 %). The seasonal maxima in September are largely due to the influence of biomass burnings in EUBA (38±11.3 %), AF (26±6.7 %), SEAS (14±3.3 %), and North America (NA) (13.8±8.4 %). For the seasonal maxima in December, dominant contributions are from AF (36±7.1 %), EUBA (21±5.2 %), and NA (18.7±5.2 %). The tropospheric HCN enhancement between September 2015 and July 2016 at Hefei (32∘ N) was attributed to an elevated influence of biomass burnings in SEAS, EUBA, and Oceania (OCE) in this period. In particular, an elevated number of fires in OCE in the second half of 2015 dominated the tropospheric HCN enhancement between September and December 2015. An elevated number of fires in SEAS in the first half of 2016 dominated the tropospheric HCN enhancement between January and July 2016.

The influence of instrumental line shape degradation on NDACC gas retrievals: total column and profile

Abstract. We simulated instrumental line shape (ILS) degradations with respect to typical types of misalignment, and compared their influence on each NDACC (Network for Detection of Atmospheric Composition Change) gas. The sensitivities of the total column, the root mean square (rms) of the fitting residual, the total random uncertainty, the total systematic uncertainty, the total uncertainty, degrees of freedom for signal (DOFs), and the profile with respect to different levels of ILS degradation for all current standard NDACC gases, i.e. O3, HNO3, HCl, HF, ClONO2, CH4, CO, N2O, C2H6, and HCN, were investigated. The influence of an imperfect ILS on NDACC gases' retrieval was assessed, and the consistency under different meteorological conditions and solar zenith angles (SZAs) were examined. The study concluded that the influence of ILS degradation can be approximated by the linear sum of individual modulation efficiency (ME) amplitude influence and phase error (PE) influence. The PE influence is of secondary importance compared with the ME amplitude. Generally, the stratospheric gases are more sensitive to ILS degradation than the tropospheric gases, and the positive ME influence is larger than the negative ME. For a typical ILS degradation (10 %), the total columns of stratospheric gases O3, HNO3, HCl, HF, and ClONO2 changed by 1.9, 0.7, 4, 3, and 23 %, respectively, while the columns of tropospheric gases CH4, CO, N2O, C2H6, and HCN changed by 0.04, 2.1, 0.2, 1.1, and 0.75 %, respectively. In order to suppress the fractional difference in the total column for ClONO2 and other NDACC gases within 10 and 1 %, respectively, the maximum positive ME degradations for O3, HNO3, HCl, HF, ClONO2, CO, C2H6, and HCN should be less than 6, 15, 5, 5, 5, 5, 9, and 13 %, respectively; the maximum negative ME degradations for O3, HCl, and HF should be less than 6, 12, and 12 %, respectively; the influence of ILS degradation on CH4 and N2O can be regarded as being negligible.

Intercomparison of Pandora stratospheric NO<sub>2</sub> slant column product with the NDACC-certified M07 spectrometer in Lauder, New Zealand

Abstract. In September 2014, a Pandora multi-spectral photometer operated by the SAGE-III project was sent to Lauder, New Zealand, to operate side-by-side with the National Institute of Water and Atmospheric Research's (NIWA) Network for Detection of Atmospheric Composition Change (NDACC) certified zenith slant column NO2 instrument to allow intercomparison between the two instruments and for evaluation of the Pandora unit as a potential SAGE-III validation tool for stratospheric NO2. This intercomparison spanned a full year, from September 2014 to September 2015. Both datasets were produced using their respective native algorithms using a common reference spectrum (i.e., 12:00 NZDT (UTC + 13) on 26 February 2015). Throughout the entire deployment period both instruments operated in a zenith-only observation configuration. Though conversion from slant column density (SCD) to vertical-column density is routine (by application of an air mass factor), we limit the current analysis to SCD only. This omission is beneficial in that it provides an intercomparison based on similar modes of operation for the two instruments and the retrieval algorithms as opposed to introducing an air mass factor dependence in the intercomparison as well. It was observed that the current hardware configurations and retrieval algorithms are in good agreement (R > 0.95). The detailed results of this investigation are presented herein.

Tropospheric ozone profiles by DIAL at Maïdo Observatory (Reunion Island): system description, instrumental performance and result comparison with ozone external data set

Abstract. In order to recognize the importance of ozone (O3) in the troposphere and lower stratosphere in the tropics, a DIAL (differential absorption lidar) tropospheric O3 lidar system (LIO3TUR) was developed and installed at the Université de la Réunion campus site (close to the sea) on Reunion Island (southern tropics) in 1998. From 1998 to 2010, it acquired 427 O3 profiles from the low to the upper troposphere and has been central to several studies. In 2012, the system was moved up to the new Maïdo Observatory facility (2160 m a.m.s.l. – metres above mean sea level) where it started operation in February 2013. The current system (LIO3T) configuration generates a 266 nm beam obtained with the fourth harmonic of a Nd:YAG laser sent into a Raman cell filled up with deuterium (using helium as buffer gas), generating the 289 and 316 nm beams to enable the use of the DIAL method for O3 profile measurements. The optimal range for the actual system is 6–19 km a.m.s.l., depending on the instrumental and atmospheric conditions. For a 1 h integration time, vertical resolution varies from 0.7 km at 6 km a.m.s.l. to 1.3 km at 19 km a.m.s.l., and mean uncertainty within the 6–19 km range is between 6 and 13 %. Comparisons with eight electrochemical concentration cell (ECC) sondes simultaneously launched from the Maïdo Observatory show good agreement between data sets with a 6.8 % mean absolute relative difference (D) between 6 and 17 km a.m.s.l. (LIO3T lower than ECC). Comparisons with 37 ECC sondes launched from the nearby Gillot site during the daytime in a ±24 h window around lidar shooting result in a 9.4 % D between 6 and 19 km a.m.s.l. (LIO3T lower than ECC). Comparisons with 11 ground-based Network for Detection of Atmospheric Composition Change (NDACC) Fourier transform infrared (FTIR) spectrometer measurements acquired during the daytime in a ±24 h window around lidar shooting show good agreement between data sets with a D of 11.8 % for the 8.5–16 km partial column (LIO3T higher than FTIR), and comparisons with 39 simultaneous Infrared Atmospheric Sounding Interferometer (IASI) observations over Reunion Island show good agreement between data sets with a D of 11.3 % for the 6–16 km partial column (LIO3T higher than IASI). ECC, LIO3TUR and LIO3T O3 monthly climatologies all exhibit the same range of values and patterns. In particular, the Southern Hemisphere biomass burning seasonal enhancement and the ozonopause altitude decrease in late austral winter–spring, as well as the sign of deep convection bringing boundary layer O3-poor air masses up to the middle–upper troposphere in late austral summer, are clearly visible in all data sets.

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.

Diurnal variations of stratospheric ozone measured by ground-based microwave remote sensing at the Mauna Loa NDACC site: measurement validation and GEOSCCM model comparison

Abstract. There is presently renewed interest in diurnal variations of stratospheric and mesospheric ozone for the purpose of supporting homogenization of records of various ozone measurements that are limited by the technique employed to being made at certain times of day. We have made such measurements for 19 years using a passive microwave remote sensing technique at the Mauna Loa Observatory (MLO) in Hawaii, which is a primary station in the Network for Detection of Atmospheric Composition Change (NDACC). We have recently reprocessed these data with hourly time resolution to study diurnal variations. We inspected differences between pairs of the ozone spectra (e.g., day and night) from which the ozone profiles are derived to determine the extent to which they may be contaminated by diurnally varying systematic instrumental or measurement effects. These are small, and we have reduced them further by selecting data that meet certain criteria that we established. We have calculated differences between profiles measured at different times: morning–night, afternoon–night, and morning–afternoon and have intercompared these with like profiles derived from the Aura Microwave Limb Sounder (Aura-MLS), the Upper Atmosphere Research Satellite Microwave Limb Sounder (UARS-MLS), the Superconducting Submillimeter-Wave Limb-Emission Sounder (SMILES), and Solar Backscatter Ultraviolet version 2 (SBUV/2) measurements. Differences between averages of coincident profiles are typically < 1.5% of typical nighttime values over most of the covered altitude range with some exceptions. We calculated averages of ozone values for each hour from the Mauna Loa microwave data, and normalized these to the average for the first hour after midnight for comparison with corresponding values calculated with the Goddard Earth Observing System Chemistry Climate Model (GEOSCCM). We found that the measurements and model output mostly agree to better than 1.5% of the midnight value, with one noteworthy exception: The measured morning–night values are significantly (2–3 %) higher than the modeled ones from 3.2 to 1.8 hPa (~39–43 km), and there is evidence that the measured values are increasing compared to the modeled values before sunrise in this region.

Improved instrumental line shape monitoring for the ground-based, high-resolution FTIR spectrometers of the Network for the Detection of Atmospheric Composition Change

Abstract. We propose an improved monitoring scheme for the instrumental line shape (ILS) of high-resolution, ground-based FTIR (Fourier Transform InfraRed) spectrometers used for chemical monitoring of the atmosphere by the Network for Detection of Atmospheric Composition Change (NDACC). Good ILS knowledge is required for the analysis of the recorded mid-infrared spectra. The new method applies a sequence of measurements using different gas cells instead of a single calibration cell. Three cells are used: cell C1 is a refillable cell offering 200 mm path length and equipped with a pressure gauge (filled with 100 Pa N2O), cells C2 and C3 are sealed cells offering 75 mm path length. C2 is filled with 5 Pa of pure N2O. Cell C3 is filled with 16 Pa N2O in 200 hPa technical air, so provides pressure-broadened N2O lines. We demonstrate that an ILS retrieval using C1 improves significantly the sensitivity of the ILS retrieval over the current calibration cells used in the network, because this cell provides narrow fully saturated N2O lines. The N2O columns derived from C2 and C3 allow the performance of a highly valuable closure experiment: adopting the ILS retrieved from C1, the N2O columns of C2 and C3 are derived. Because N2O is an inert gas, both columns should be constant on long timescales. Apparent changes in the columns would immediately attract attention and indicate either inconsistent ILS results or instrumental problems of other origin. Two different cells are applied for the closure experiment, because the NDACC spectrometers observe both stratospheric and tropospheric gases: C2 mimics signatures of stratospheric gases, whereas C3 mimics signatures of tropospheric gases.

Comparison of ground-based FTIR and Brewer O<sub>3</sub> total column with data from two different IASI algorithms and from OMI and GOME-2 satellite instruments

Abstract. An intercomparison of ozone total column measurements derived from various platforms is presented in this work. Satellite data from Infrared Atmospheric Sounding Interferometer (IASI), Ozone Monitoring Instrument (OMI) and Global Ozone Monitoring Experiment (GOME-2) are compared with data from two ground-based spectrometers (Fourier Transform Infrared spectrometer FTIR and Brewer), located at the Network for Detection of Atmospheric Composition Change (NDACC) super-site of Izaña (Tenerife), measured during a campaign from March to June 2009. These ground-based observing systems have already been demonstrated to perform consistent, precise and accurate ozone total column measurements. An excellent agreement between ground-based and OMI/GOME-2 data is observed. Results from two different algorithms for deriving IASI ozone total column are also compared: the European Organisation for the Exploitation of Meteorological Satellites (EUMETSAT/ESA) operational algorithm and the LISA (Laboratoire Inter-universitaire des Systèmes Atmosphériques) algorithm. A better agreement was found with LISA's analytical approach based on an altitude-dependent Tikhonov-Philips regularization: correlations are 0.94 and 0.89 compared to FTIR and Brewer, respectively; while the operational IASI ozone columns (based on neural network analysis) show correlations of 0.90 and 0.85, respectively, compared to the O3 columns obtained from FTIR and Brewer.

Analysis of global and regional CO burdens measured from space between 2000 and 2009 and validated by ground-based solar tracking spectrometers

Abstract. Interannual variations in AIRS and MOPITT retrieved CO burdens are validated, corrected, and compared with CO emissions from wild fires from the Global Fire Emission Dataset (GFED2) inventory. Validation of daily mean CO total column (TC) retrievals from MOPITT version 3 and AIRS version 5 is performed through comparisons with archived TC data from the Network for Detection of Atmospheric Composition Change (NDACC) ground-based Fourier Transform Spectrometers (FTS) between March 2000 and December 2007. MOPITT V3 retrievals exhibit an increasing temporal bias with a rate of 1.4–1.8% per year; thus far, AIRS retrievals appear to be more stable. For the lowest CO values in the Southern Hemisphere (SH), AIRS TC retrievals overestimate FTS TC by 20%. MOPITT's bias and standard deviation do not depend on CO TC absolute values. Empirical corrections are derived for AIRS and MOPITT retrievals based on the observed annually averaged bias versus the FTS TC. Recently published MOPITT V4 is found to be in a good agreement with MOPITT V3 corrected by us (with exception of 2000–2001 period). With these corrections, CO burdens from AIRS V5 and MOPITT V3 (as well as MOPITT V4) come into good agreement in the mid-latitudes of the Northern Hemisphere (NH) and in the tropical belt. In the SH, agreement between AIRS and MOPITT CO burdens is better for the larger CO TC in austral winter and worse in austral summer when CO TC are smaller. Before July 2008, all variations in retrieved CO burden can be explained by changes in fire emissions. After July 2008, global and tropical CO burdens decreased until October before recovering by the beginning of 2009. The NH CO burden also decreased but reached a minimum in January 2009 before starting to recover. The decrease in tropical CO burdens is explained by lower than usual fire emissions in South America and Indonesia. This decrease in tropical emissions also accounts for most of the change in the global CO burden. However, no such diminution of NH biomass burning is indicated by GFED2. Thus, the CO burden decrease in the NH could result from a combination of lower fossil fuel emissions during the global economic recession and transport of CO-poor air from the tropics. More extensive modeling will be required to fully resolve this issue.

Technical Note: Validation of Odin/SMR limb observations of ozone, comparisons with OSIRIS, POAM III, ground-based and balloon-borne instruments

Abstract. The Odin satellite carries two instruments capable of determining stratospheric ozone profiles by limb sounding: the Sub-Millimetre Radiometer (SMR) and the UV-visible spectrograph of the OSIRIS (Optical Spectrograph and InfraRed Imager System) instrument. A large number of ozone profiles measurements were performed during six years from November 2001 to present. This ozone dataset is here used to make quantitative comparisons with satellite measurements in order to assess the quality of the Odin/SMR ozone measurements. In a first step, we compare Swedish SMR retrievals version 2.1, French SMR ozone retrievals version 222 (both from the 501.8 GHz band), and the OSIRIS retrievals version 3.0, with the operational version 4.0 ozone product from POAM III (Polar Ozone Atmospheric Measurement). In a second step, we refine the Odin/SMR validation by comparisons with ground-based instruments and balloon-borne observations. We use observations carried out within the framework of the Network for Detection of Atmospheric Composition Change (NDACC) and balloon flight missions conducted by the Canadian Space Agency (CSA), the Laboratoire de Physique et de Chimie de l\\'{}Environnement (LPCE, Orléans, France), and the Service d'Aéronomie (SA, Paris, France). Coincidence criteria were 5° in latitude×10° in longitude, and 5 h in time in Odin/POAM III comparisons, 12 h in Odin/NDACC comparisons, and 72 h in Odin/balloons comparisons. An agreement is found with the POAM III experiment (10–60 km) within −0.3±0.2 ppmv (bias±standard deviation) for SMR (v222, v2.1) and within −0.5±0.2 ppmv for OSIRIS (v3.0). Odin ozone mixing ratio products are systematically slightly lower than the POAM III data and show an ozone maximum lower by 1–5 km in altitude. The comparisons with the NDACC data (10–34 km for ozonesonde, 10–50 km for lidar, 10–60 for microwave instruments) yield a good agreement within −0.15±0.3 ppmv for the SMR data and −0.3±0.3 ppmv for the OSIRIS data. Finally the comparisons with instruments on large balloons (10–31 km) show a good agreement, within −0.7±1 ppmv. The official SMR v2.1 dataset is consistent in all altitude ranges with POAM III, NDACC and large balloon-borne instruments measurements. In the SMR v2.1 data, no different systematic error has been found in the 0–35km range in comparison with the 35–60 km range. The same feature has been highlighted in both hemispheres in SMR v2.1/POAM III intercomparisons, and no latitudinal dependence has been revealed in SMR v2.1/NDACC intercomparisons.

Intercomparison of UV-visible measurements of ozone and NO<sub>2</sub> during the Canadian Arctic ACE validation campaigns: 2004–2006

Abstract. The first three Canadian Arctic ACE validation campaigns were held during polar sunrise at Eureka, Nunavut, Canada (80° N, 86° W) from 2004 to 2006 in support of validation of the ACE (Atmospheric Chemistry Experiment) satellite mission. Three or four zenith-sky viewing UV-visible spectrometers have taken part in each of the three campaigns. The differential slant column densities and vertical column densities of ozone and NO2 from these instruments have been compared following the methods of the UV-visible Working Group of the NDACC (Network for Detection of Atmospheric Composition Change). The instruments are found to partially agree within the required accuracies for both species, although both the vertical and slant column densities are more scattered than required. This might be expected given the spatial and temporal variability of the Arctic stratosphere in spring. The vertical column densities are also compared to integrated total columns from ozonesondes and integrated partial columns from the ACE-FTS (ACE-Fourier Transform Spectrometer) and ACE-MAESTRO (ACE-Measurements of Aerosol Extinction in the Stratosphere and Troposphere Retrieved by Occultation) instruments on board ACE. For both species, the columns from the ground-based instruments and the ozonesondes are found to generally agree within their combined error bars. The ACE-FTS ozone partial columns and the ground-based total columns agree within 4.5%, averaged over the three campaigns. The ACE-MAESTRO ozone partial columns are generally smaller than those of the ground-based instruments, by an average of 9.9%, and are smaller than the ACE-FTS columns by an average of 14.4%. The ACE-FTS NO2 partial columns are an average of 13.4% smaller than the total columns from the ground-based instruments, as expected. The ACE-MAESTRO NO2 partial columns are larger than the total columns of the ground-based instruments by an average of 2.5% and are larger than the partial columns of the ACE-FTS by an average of 15.5%.

Ground‐based microwave ozone radiometer measurements compared with Aura‐MLS v2.2 and other instruments at two Network for Detection of Atmospheric Composition Change sites

Ozone measurements made by the Microwave Limb Sounder (MLS) on board the Earth Observing System (EOS) Aura Satellite are compared with measurements made by ground‐based microwave radiometers (MWR) in the Network for Detection of Atmospheric Composition Change (NDACC) stations at Lauder, New Zealand (45°S, 169°E) and Mauna Loa, Hawaii (20°N, 204°E). The latter instruments measure ozone over the pressure range 56 to 0.03 hPa (about 20 to 72 km), allowing validation of ozone to the upper range of the MLS profiles. In addition, because they operate continuously, separate daytime and nighttime comparisons with MLS can be made to account for the large diurnal variations of ozone in the upper stratosphere and mesosphere. MLS‐MWR comparisons show agreement generally within 5% between 24 and 0.04 hPa (about 26 to 70 km) and 5 to 13% elsewhere. To more thoroughly investigate ozone in the stratosphere and mesosphere and establish a consensus between different sets of measurements, comparisons, and analyses with other satellite‐borne instruments, including the Stratospheric Aerosol and Gas Experiment II (SAGE‐II), Halogen Occultation Experiment (HALOE), Global Ozone Monitoring by Occultation of Stars (GOMOS), and Michelson Interferometer for Passive Atmospheric Sounding (MIPAS), are also made, using the ground‐based microwave measurements as a reference. The resulting MLS‐consensus difference profiles remove some of the features present in the MLS‐MWR comparisons and indicate that the overall agreement between MLS and the correlative data, between 56 and 0.04 hPa, is mostly within 5% at both sites.

Comparisons between ground-based FTIR and MIPAS N<sub>2</sub>O and HNO<sub>3</sub> profiles before and after assimilation in BASCOE

Abstract. Within the framework of the Network for Detection of Atmospheric Composition Change (NDACC), regular ground-based Fourier transform infrared (FTIR) measurements of many species are performed at several locations. Inversion schemes provide vertical profile information and characterization of the retrieved products which are therefore relevant for contributing to the validation of MIPAS profiles in the stratosphere and upper troposphere. We have focused on the species HNO3 and N2O at 5 NDACC-sites distributed in both hemispheres, i.e., Jungfraujoch (46.5° N) and Kiruna (68° N) for the northern hemisphere, and Wollongong (34° S), Lauder (45° S) and Arrival Heights (78° S) for the southern hemisphere. These ground-based data have been compared with MIPAS offline profiles (v4.61) for the year 2003, collocated within 1000 km around the stations, in the lower to middle stratosphere. To get around the spatial collocation problem, comparisons have also been made between the same ground-based FTIR data and the corresponding profiles resulting from the stratospheric 4D-VAR data assimilation system BASCOE constrained by MIPAS data. This paper discusses the results of the comparisons and the usefullness of using BASCOE profiles as proxies for MIPAS data. It shows good agreement between MIPAS and FTIR N2O partial columns: the biases are below 5% for all the stations and the standard deviations are below 7% for the three mid-latitude stations, and below 10% for the high latitude ones. The comparisons with BASCOE partial columns give standard deviations below 4% for the mid-latitude stations to less than 8% for the high latitude ones. After making some corrections to take into account the known bias due to the use of different spectroscopic parameters, the comparisons of HNO3 partial columns show biases below 3% and standard deviations below 15% for all the stations except Arrival Heights (bias of 5%, standard deviation of 21%). The results for this species, which has a larger spatial variability, highlight the necessity of defining appropriate collocation criteria and of accounting for the spread of the observed airmasses. BASCOE appears to have more deficiencies in producing proxies of MIPAS HNO3 profiles compared to N2O, but the obtained standard deviation of less than 10% between BASCOE and FTIR is reasonable. Similar results on profiles comparisons are also shown in the paper, in addition to partial column ones.