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The Observatoire de Haute Provence (OHP) weekly Electrochemical Concentration Cell (ECC) ozonesonde data have been homogenized for the time period 1991–2020 according to the recommendations of the Ozonesonde Data Quality Assessment (O3S-DQA) panel. The assessment of the ECC homogenization benefit has been carried out using comparisons with ground based instruments also measuring ozone at the same station (lidar, surface measurements) and with collocated satellite observations of the O3 vertical profile by Microwave Limb Sounder (MLS). The major differences between uncorrected and homogenized ECC are related to a change of ozonesonde type in 1997, removal of the pressure dependency of the ECC background current and correction of internal ozonesonde temperature. The 3–4 ppbv positive bias between ECC and lidar in the troposphere is corrected with the homogenization. The ECC 30-years trends of the seasonally adjusted ozone concentrations are also significantly improved both in the troposphere and the stratosphere when the ECC concentrations are homogenized, as shown by the ECC/lidar or ECC/surface ozone trend comparisons. A −0.29 % per year negative trend of the normalization factor (NT) calculated using independent measurements of the total ozone column (TOC) at OHP disappears after homogenization of the ECC. There is however a remaining −5 % negative bias in the TOC which is likely related to an underestimate of the ECC concentrations in the stratosphere above 50 hPa as shown by direct comparison with the OHP lidar and MLS. The reason for this bias is still unclear, but a possible explanation might be related to freezing or evaporation of the sonde solution in the stratosphere. Both the comparisons with lidar and satellite observations suggest that homogenization increases the negative bias of the ECC up to 10 % above 28 km.

The Observatoire de Haute Provence (OHP) weekly electrochemical concentration cell (ECC) ozonesonde data have been homogenized for the period 1991–2021 according to the recommendations of the Ozonesonde Data Quality Assessment (O3S-DQA) panel. The assessment of the ECC homogenization benefit has been carried out using comparisons with other ozone-measuring ground-based instruments at the same station (lidar, surface measurements) and with colocated satellite observations of the O3 vertical profile by Microwave Limb Sounder (MLS). The major differences between uncorrected and homogenized ECC data are related to a change of ozonesonde type in 1997, removal of the pressure dependency of the ECC background current and correction of internal pump temperature. The original 3–4 ppbv positive bias between ECC and lidar in the troposphere is corrected with the homogenization. The ECC 30-year trends of the seasonally adjusted ozone concentrations are also significantly improved in both the troposphere and the stratosphere after the ECC homogenization, as shown by the ECC/lidar or ECC/surface ozone trend comparisons. A −0.19 % yr−1 negative trend of the normalization factor (NT) calculated using independent measurements of the total ozone column (TOC) at OHP disappears after homogenization of the ECC data. There is, however, a remaining −3.7 % negative bias in the TOC which is likely related to an underestimate of the ECC concentrations in the stratosphere above 50 hPa. Differences between TOC measured by homogenized ECC and satellite observations show a smaller bias of −1 %. Comparisons between homogenized ECC and OHP stratospheric lidar and MLS observations below 26 km are slightly negative (−2 %) or positive (+2 %), respectively. The comparisons with both lidar and satellite observations suggest that homogenization increases the negative bias of the ECC to values lower than −6 % above 28 km. The reason for this bias is still unclear, but a possible explanation might be related to freezing or evaporation of the sonde solution in the stratosphere.

Between December 2005 and 2013, the In-service Aircraft for a Global Observing System (IAGOS) program produced almost daily in situ measurements of CO and O3 between Europe and southern Africa. IAGOS data combined with measurements from the IASI instrument onboard the Metop-A satellite (2008–2013) are used to characterize meridional distributions and seasonality of CO and O3 in the African upper troposphere (UT). The FLEXPART particle dispersion model and the SOFT-IO model which combines the FLEXPART model with CO emission inventories are used to explore the sources and origins of the observed transects of CO and O3. We focus our analysis on two main seasons: December to March (DJFM) and June to October (JJASO). These seasons have been defined according to the position of Intertropical Convergence Zone (ITCZ), determined using in situ measurements from IAGOS. During both seasons, the UT CO meridional transects are characterized by maximum mixing ratios located 10° from the position of the ITCZ above the dry regions inside the hemisphere of the strongest Hadley cell (132 to 165 ppb at 0–5° N in DJFM and 128 to 149 ppb at 3–7° S in JJASO), and decreasing values south- and north-ward. The O3 meridional transects are characterized by mixing ratio minima of ~ 42–54 ppb at the ITCZ (10–16° S in DJFM and 5–8° N in JJASO) framed by local maxima (~ 53–71 ppb) coincident with the wind shear zones North and South of the ITCZ. O3 gradients are strongest in the hemisphere of the strongest Hadley cell. IASI UT O3 distributions in DJFM have revealed that the maxima are a part of a crescent-shaped O3 plume above the Atlantic Ocean around the Gulf of Guinea. CO emitted at the surface is transported towards the ITCZ by the trade winds and then convectively uplifted. Once in the upper troposphere, CO enriched air masses are transported away from the ITCZ by the upper branches of the Hadley cells and accumulate within the zonal wind shear zones where the maximum CO mixing ratios are found. Anthropogenic and fires both contribute, by the same order of magnitude, to the CO budget of the African upper troposphere. Local fires have the highest contribution, drive the location of the observed UT CO maxima, and are related to the following transport pathway: CO emitted at the surface is transported towards the ITCZ by the trade winds and further convectively uplifted. Then UT CO enriched air masses are transported away from the ITCZ by the upper branches of the Hadley cells and accumulate within the zonal wind shear zones where the maxima are located. Anthropogenic CO contribution is mostly from Africa during the entire year, with a low seasonal variability, and is related to similar transport circulation than fire air masses. There is also a large contribution from Asia in JJASO related to the fast convective uplift of polluted air masses in the Asian monsoon region which are further westward transported by the tropical easterly jet (TEJ) and the Asian monsoon anticyclone (AMA). O3 minima correspond to air masses that were recently uplifted from the surface where mixing ratios are low at the ITCZ. The O3 maxima correspond to old high altitude air masses uplifted from either local or long distance area of high O3 precursor emissions (Africa and South America during all the year, South Asia mainly in JJASO), and must be created during transport by photochemistry. This analysis of meridional transects contribute to a better understanding of distributions of CO and O3 in the intertropical African upper troposphere and the processes which drive these distributions. Therefore, it provides a solid basis for comparison and improvement of models and satellite products in order to get the good O3 for the good reasons.

We review the current state of knowledge of ozonesonde uncertainty and bias, with reference to recent developments in laboratory and field experiments. In the past 20 years ozonesonde precision has improved by a factor of 2, primarily through the adoption of strict standard operating procedures. The uncertainty budget for the ozone partial pressure reading has contributions from stoichiometry, cell background current, pump efficiency and temperature, sensing solution type, and volume. Corrections to historical data for known issues may reduce biases but simultaneously introduce additional uncertainties. This paper describes a systematic approach to quantifying these uncertainties by considering the physical and chemical processes involved and attempts to place our estimates on a firm theoretical or empirical footing. New equations or tables for ozone/iodine conversion efficiency, humidity and temperature corrections to pump flow rate, and altitude‐dependent pump flow corrections are presented, as well as detailed discussion of stoichiometry and conversion efficiencies. The nature of the so‐called “background current” is considered in detail. Two other factors particularly affecting past measurements, uncertainties and biases in the pressure measurement, and the comparison of sonde profiles to spectrophotometric measurements of total column ozone, are also discussed. Several quality assurance issues remain, but are tractable problems that can be addressed with further research. This will be required if the present goal of better than 5% overall uncertainty throughout the global ozonesonde network is to be achieved.

Reprocessed ozonesonde data from eight SHADOZ (Southern Hemisphere ADditional OZonesondes) sites have been used to derive the first analysis of uncertainty estimates for both profile and total column ozone (TCO). The ozone uncertainty is a composite of the uncertainties of the individual terms in the ozone partial pressure (PO3) equation, those being the ozone sensor current, background current, internal pump temperature, pump efficiency factors, conversion efficiency, and flow rate. Overall, PO3 uncertainties (ΔPO3) are within 15% and peak around the tropopause (15 ± 3 km) where ozone is a minimum and ΔPO3 approaches the measured signal. The uncertainty in the background and sensor currents dominates the overall ΔPO3 in the troposphere including the tropopause region, while the uncertainties in the conversion efficiency and flow rate dominate in the stratosphere. Seasonally, ΔPO3 is generally a maximum in the March–May, with the exception of SHADOZ sites in Asia, for which the highest ΔPO3 occurs in September–February. As a first approach, we calculate sonde TCO uncertainty (ΔTCO) by integrating the profile ΔPO3 and adding the ozone residual uncertainty, derived from the McPeters and Labow (2012, doi:10.1029/2011JD017006) 1σ ozone mixing ratios. Overall, ΔTCO are within ±15 Dobson units (DU), representing ~5–6% of the TCO. Total Ozone Mapping Spectrometer and Ozone Monitoring Instrument (TOMS and OMI) satellite overpasses are generally within the sonde ΔTCO. However, there is a discontinuity between TOMS v8.6 (1998 to September 2004) and OMI (October 2004–2016) TCO on the order of 10 DU that accounts for the significant 16 DU overall difference observed between sonde and TOMS. By comparison, the sonde‐OMI absolute difference for the eight stations is only ~4 DU.

The ozonesonde is a small balloon-borne instrument that is attached to a standard radiosonde to measure profiles of ozone from the surface to 35 km with ∼100-m vertical resolution. Ozonesonde data constitute a mainstay of satellite calibration and are used for climatologies and analysis of trends, especially in the lower stratosphere where satellites are most uncertain. The electrochemical concentration cell (ECC) ozonesonde has been deployed at ∼100 stations worldwide since the 1960s, with changes over time in manufacture and procedures, including details of the cell chemical solution and data processing. As a consequence, there are biases among different stations and discontinuities in profile time series from individual site records. For 22 years the Jülich (Germany) Ozonesonde Intercomparison Experiment (JOSIE) has periodically tested ozonesondes in a simulation chamber designated the World Calibration Centre for Ozonesondes (WCCOS) by WMO. During October–November 2017 a JOSIE campaign evaluated the sondes and procedures used in Southern Hemisphere Additional Ozonesondes (SHADOZ), a 14-station sonde network operating in the tropics and subtropics. A distinctive feature of the 2017 JOSIE was that the tests were conducted by operators from eight SHADOZ stations. Experimental protocols for the SHADOZ sonde configurations, which represent most of those in use today, are described, along with preliminary results. SHADOZ stations that follow WMO-recommended protocols record total ozone within 3% of the JOSIE reference instrument. These results and prior JOSIEs demonstrate that regular testing is essential to maintain best practices in ozonesonde operations and to ensure high-quality data for the satellite and ozone assessment communities.

An international effort to improve ozonesonde data quality and to reevaluate historical records has made significant improvements in the accuracy of global network data. However, between 2014 and 2016, ozonesonde total column ozone (TCO; O3) at 14 of 37 regularly reporting stations exhibited a sudden dropoff relative to satellite measurements. The ozonesonde TCO drop is 3–7% compared to satellite and ground‐based TCO, and 5–10% or more compared to satellite stratospheric O3 profiles, compromising the use of recent data for trends, although they remain reliable for other uses. Hardware changes in the ozonesonde instrument are likely a major factor in the O3 dropoff, but no single property of the ozonesonde explains the findings. The bias remains in recent data. Research to understand the dropoff is in progress; this letter is intended as a caution to users of the data. Our findings underscore the importance of regular ozonesonde data evaluation.

The Electrochemical Concentration Cell (ECC) ozonesonde has been the main instrument for in situ profiling of ozone worldwide; yet, some details of its operation, which contribute to the ozone uncertainty budget, are not well understood. Here, we investigate the time response of the chemical reactions inside the ECC and how corrections can be used to remove some systematic biases. The analysis is based on the understanding that two reaction pathways involving ozone occur inside the ECC that generate electrical currents on two very different time scales. A slow reaction pathway involving the buffer with a time constant of about 25 min can be interpreted as what has conventionally been considered the “background current”. This contribution can be calculated and removed from the measured current instead of the “background current”. The remaining fast reaction pathway with a time constant of about 20 s is due the conversion of iodide to molecular iodine and the generation of two free electrons per ozone molecule. Here we provide an algorithm to calculate and remove the contribution of the slow reaction pathway and to correct for the time lag of the faster reaction pathway. This processing algorithm has been applied to ozonesonde profiles at Costa Rica and during the Central Equatorial Pacific Experiment (CEPEX) and to laboratory experiments evaluating the performance of ECC ozonesondes. At Costa Rica, where a 1 % KI, 1/10th buffer solution is used, there is no change in the derived total ozone column; however, in the upper troposphere and lower stratosphere, average reported ozone concentrations increase by up to 7 % and above 30 km decrease by up to 7 %. During CEPEX, where a 1 % KI, full buffer solution was used, ozone concentrations are increased mostly in the upper troposphere with no change near to the top of the profile. In the laboratory measurements, the processing algorithms have been applied to measurements using all current sensing solutions and using only the stronger pump efficiency correction reported by Johnson et al. (2002), which improves the time response of the ECCs and removes some biases relative to the reference instruments. In the surface layer, the correction algorithm shows that ECC ozonesonde measurements are influenced by the operational procedures prior to launch and that typical gradients above the surface layer may be steeper than originally reported.

An international effort to improve ozonesonde data quality and to reevaluate historical records has made significant improvements in the accuracy of global network data. However, between 2014 and 2...

The electrochemical concentration cell (ECC) ozonesonde has been the main instrument for in situ profiling of ozone worldwide; yet, some details of its operation, which contribute to the ozone uncertainty budget, are not well understood. Here, we investigate the time response of the chemical reactions inside the ECC and how corrections can be used to remove some systematic biases. The analysis is based on the understanding that two reaction pathways involving ozone occur inside the ECC that generate electrical currents on two very different timescales. The main fast-reaction pathway with a time constant of about 20 s is due the conversion of iodide to molecular iodine and the generation of two free electrons per ozone molecule. A secondary slow-reaction pathway involving the buffer generates an excess current of about 2 %–10 % with a time constant of about 25 min. This excess current can be interpreted as what has conventionally been considered the “background current”. This contribution can be calculated and removed from the measured current instead of the background current. Here we provide an algorithm to calculate and remove the contribution of the slow-reaction pathway and to correct for the time lag of the fast-reaction pathway. This processing algorithm has been applied to ozonesonde profiles at Costa Rica and during the Central Equatorial Pacific Experiment (CEPEX) as well as to laboratory experiments evaluating the performance of ECC ozonesondes. At Costa Rica, where a 1 % KI, 1/10th buffer solution is used, there is no change in the derived total ozone column; however, in the upper troposphere and lower stratosphere, average reported ozone concentrations increase by up to 7 % and above 30 km decrease by up to 7 %. During CEPEX, where a 1 % KI, full-buffer solution was used, ozone concentrations are increased mostly in the upper troposphere, with no change near the top of the profile. In the laboratory measurements, the processing algorithms have been applied to measurements using the majority of current sensing solutions and using only the stronger pump efficiency correction reported by Johnson et al. (2002). This improves the accuracy of the ECC sonde ozone profiles, especially for low ozone concentrations or large ozone gradients and removes systematic biases relative to the reference instruments. In the surface layer, operational procedures prior to launch, in particular the use of filters, influence how typical gradients above the surface are detected. The correction algorithm may report gradients that are steeper than originally reported, but their uncertainty is strongly influenced by the prelaunch procedures.

The vertical distribution and seasonal variation of water vapour volume mixing ratio (H2O VMR), of relative humidity with respect to ice (RHice) and particularly of regions with ice-supersaturated air masses (ISSRs) in the extratropical upper troposphere and lowermost stratosphere are investigated at northern mid-latitudes over the eastern North American, North Atlantic and European regions for the period 1995 to 2010. Observation data originate from regular and continuous long-term measurements on board instrumented passenger aircraft in the framework of the European research programme MOZAIC (1994–2010), which continues as the European research infrastructure IAGOS (from 2011). Data used in our study result from collocated observations of O3 VMR, RHice and temperature, as well as H2O VMR deduced from RHice and temperature data. The in situ observations of H2O VMR and RHice with a vertical resolution of 30 hPa (< 750 m at the extratropical tropopause level) and a horizontal resolution of 1 km resolve detailed features of the distribution of water vapour and ice-supersaturated air relative to the thermal tropopause, including their seasonal and regional variability and chemical signatures at various distances from the tropopause layer. Annual cycles of the investigated properties document the highest H2O VMR and temperatures above the thermal tropopause in the summer months, whereas RHice above the thermal tropopause remains almost constant in the course of the year. Over all investigated regions, upper tropospheric air masses close to the tropopause level are nearly saturated with respect to ice and contain a significant fraction of ISSRs with a distinct seasonal cycle of minimum values in summer (30 % over the ocean, 20 %–25 % over land) and maximum values in late winter (35 %–40 % over both land and ocean). Above the thermal tropopause, ISSRs are occasionally observed with an occurrence probability of 1.5 ± 1.1 %, whereas above the dynamical tropopause at 2 PVU (PVU: potential vorticity unit), the occurrence probability increases 4-fold to 8.4 ± 4.4 %. In both coordinate systems related to tropopause height (TPH), the ISSR occurrence probabilities drop to values below 1 % for the next higher air mass layer with pressure levels p < pTPH−15 hPa. For both tropopause definitions, the tropospheric nature or fingerprint, based on O3 VMR, indicates the continuing tropospheric influence on ISSRs inside and above the respective tropopause layer. For the non-ISSRs, however, the stratospheric nature is clearly visible above the thermal tropopause, whereas above the dynamical tropopause the air masses show a still substantial tropospheric influence. For all three regions, seasonal deviations from the long-term annual cycle of ISSR occurrence show no significant trends over the observation period of 15 years, whereas a statistically significant correlation between the North Atlantic Oscillation (NAO) index and the deviation of ISSR occurrence from the long-term average is observed for the North Atlantic region but not for the eastern North American and European regions.

Electrochemical concentration cell ozonesonde measurements are an important source of highly resolved vertical profiles of ozone with long-term data records for deriving ozone trends, model development, satellite validation, and air quality studies. Ozonesonde stations employ a range of operational and data processing procedures, metadata reporting, and instrument changes that have resulted in inhomogeneities within individual station data records. A major milestone is the first reprocessing of seven Southern Hemisphere ADditional OZonesondes (SHADOZ) station ozonesonde records to account for errors and biases in operating/processing procedures. Ascension Island, Hanoi, Irene, Kuala Lumpur, La Reunion, Natal, and Watukosek station records all show an overall increase in ozone after reprocessing. Watukosek shows the largest increase of 9.0 plus or minus 2.1 Dobson Units (DU) in total column ozone; Irene and Hanoi show a 5.5 plus or minus 2.5 DU increase, while remaining sites show statistically insignificant enhancements. Negligible to modest ozone enhancements are observed after reprocessing in the troposphere (up to 8%) and stratosphere (up to 6%), except at La Reunion for which the application of background currents reduces tropospheric ozone (2.1 plus or minus1.3 DU). Inhomogeneities due to ozonesonde/solution-type changes at Ascension, Natal, and La Reunion are resolved with the application of transfer functions. Comparisons with EP-TOMS, Aura's Ozone Monitoring Instrument and Microwave Limb Sounder (MLS) satellite ozone overpasses show an overall improvement in agreement after reprocessing. Most reprocessed data sets show a significant reduction in biases with MLS at the ozone maximum region (50-10 hPa). Changes in radiosonde/ozonesonde system and nonstandard solution types can account for remaining discrepancies observed at several sites when compared to satellites.

This study is based on the analysis of the measurement of ozone and water vapor by airbus in-service aircraft (MOZAIC) data of vertical ozone (O3) and carbon monoxide (CO) over Hyderabad during November 2005–March 2009. Measurements in the upper troposphere show highest values of O3 (53–75 ppbv) and CO (80–110 ppbv) during the pre-monsoon and post-monsoon seasons, respectively. The episodes of strong wind shears (>20 ms−1) were frequent during the monsoon/post-monsoon months, while weak shear conditions (

The ozonesonde stations at Uccle (Belgium) and De Bilt (the Netherlands) are separated by only 175 km but use different ozonesonde types (or different manufacturers for the same electrochemical concentration cell (ECC) type), operating procedures, and correction strategies. As such, these stations form a unique test bed for the Ozonesonde Data Quality Assessment (O3S-DQA) activity, which aims at providing a revised, homogeneous, consistent dataset with an altitude-dependent estimated uncertainty for each revised profile. For the ECC ozonesondes at Uccle mean relative uncertainties in the 4–6 % range are obtained. To study the impact of the corrections on the ozone profiles and trends, we compared the Uccle and De Bilt average ozone profiles and vertical ozone trends, calculated from the operational corrections at both stations and the O3S-DQA corrected profiles. In the common ECC 1997–2014 period, the O3S-DQA corrections effectively reduce the differences between the Uccle and De Bilt ozone partial pressure values with respect to the operational corrections only for the stratospheric layers below the ozone maximum. The upper-stratospheric ozone measurements at both sites are substantially different, regardless of the correction methodology used. The origin of this difference is not clear. The discrepancies in the tropospheric ozone concentrations between both sites can be ascribed to the problematic background measurement and correction at De Bilt, especially in the period before November 1998. The Uccle operational correction method, applicable to both ozonesonde types used, diminishes the relative stratospheric ozone differences of the Brewer–Mast sondes in the 1993–1996 period with De Bilt to less than 5 % and to less than 6 % in the free troposphere for the De Bilt operational corrections. Despite their large impact on the average ozone profiles, the different (sensible) correction strategies do not change the ozone trends significantly, usually only within their statistical uncertainty due to atmospheric noise. The O3S-DQA corrections bring the Uccle and De Bilt ozone trend estimates for 1997–2014 closer to each other in the lower stratosphere and lower troposphere. Throughout the whole vertical profile, these trend estimates are, however, not significantly different from each other, and only in the troposphere significantly positive. For the entire Uccle observation period (1969–2014), the operational corrections lead to height-independent and consistent ozone trends for both the troposphere and the stratosphere, with rates of +2 to +3 % decade−1 and −1 to −2 % decade−1, respectively.

This paper investigates in an innovative way the climatological vertical stratification of relative humidity (RH) and ozone (O3) and carbon monoxide (CO) mixing ratios within the planetary boundary layer (PBL) and at the interface with the free troposphere (FT). The climatology includes all vertical profiles available at northern mid-latitudes over the period 1994–2016 in both IAGOS (In-service Aircraft for a Global Observing System) and WOUDC (World Ozone and Ultraviolet Radiation Data Centre) databases, which represents more than 90,000 vertical profiles. For all individual profiles, apart from the specific case of surface-based temperature inversions (SBIs), the PBL height is estimated following the elevated temperature inversion (EI) method. Several features of both SBIs and EIs are analysed, including their diurnal and seasonal variations. Based on these PBL height estimates (denoted h), the original approach introduced in this paper consists in building a so-called PBL-referenced vertical distribution of O3, CO and RH by averaging all individual profiles beforehand expressed as a function of z/h rather than z (with z the altitude). Using this vertical coordinate system allows to highlight the features existing at the PBL-FT interface that would have been smoothed otherwise. Results demonstrate that the frequently assumed well-mixed PBL remains an exception for both chemical species. Within the PBL, CO profiles are characterized by a mean vertical stratification (here defined as the standard deviation of the CO profile between the surface and the PBL top, normalized by the mean) of 11 %, with moderate seasonal and diurnal variations. A higher vertical stratification is observed for O3 mixing ratios (18 %), with stronger seasonal and diurnal variability (from ~ 10 % in spring/summer midday/afternoon to ~ 25 % in winter/fall night). This vertical stratification is distributed heterogeneously in the PBL with stronger vertical gradients observed at both the surface (due to dry deposition and titration by NO for O3; and due to surface emissions for CO) and the PBL-FT interface. These gradients vary with the season from lowest values in summer to highest ones in winter. Contrary to CO, the O3 vertical stratification was found to vary with the surface potential temperature following an interesting bell shape with weakest stratification for both lowest (typically negative) and highest temperatures, which could be due to a much lower O3 dry deposition under the presence of snow. Therefore, results demonstrate that EIs act as a geophysical interface separating air masses of distinct chemical composition and/or chemical regime. This is further supported by the analysis of the correlation of O3 and CO mixing ratios between the different altitude levels in the PBL and FT (the so-called vertical autocorrelation). Results indeed highlight lower correlations apart from the PBL-FT interface and higher correlations within each of the two atmospheric compartments (PBL and FT).

As part of the DENCHAR (Development and Evaluation of Novel Compact Hygrometer for Airborne Research) inter-comparison campaign in North-Germany in 2011, a commercial cavity ring-down spectroscopy (CRDS) based gas analyzer (G2401-m, Picarro Inc., US) was installed on a Learjet to measure atmospheric water vapor, CO2, CH4 and CO. The CRDS components were identical to those chosen for integration aboard commercial airliners within the IAGOS (In-service Aircraft for a Global Observing System) project. Thus, the campaign allowed for an initial assessment validation of the long-term IAGOS water vapor measurements by CRDS against reference instruments with a long performance record (Fast In-situ Stratospheric Hygrometer (FISH), CR-2 frost point hygrometer (Buck Research Instruments L.L.C., US), both operated by research centre Juelich). The inlet system, a 50 cm long 1/8" FEP-tube connected to a Rosemount TAT housing (model 102BX, deiced) installed on a window plate of the aircraft, was designed to eliminate sampling of larger aerosols, ice particles, and water droplets, and provided additional ram-pressure. In combination with a low sample flow of 100 sccm, corresponding to a 4 second response time, this ensured a fully controlled pressure in the sample cell of 186.65 hPa (140 Torr) throughout the aircraft altitude operating range up to 12.5 km without the need of an upstream sampling pump. This setup ensures full compatibility with the deployment of the analyzer within IAGOS. For the initial water calibration of the instrument it was compared against a dew point mirror (Dewmet TDH, Michell instruments Ltd., UK) in the range from 0.7 to 2.5 % water vapor mole fraction. During the inter-comparison campaign the analyzer was compared on ground against a dew point hygrometer, which is used for calibrating the reference instrument FISH, in the range from 2 to 600 ppm. Furthermore, a new independent calibration method, based on the dilution effect of water vapor on CO2, was tested. Comparison of the in-flight data against the reference instruments showed that the analyzer is reliable and has a good long-term stability. The flight data suggest a conservative precision estimate for measurements made at 0.4 Hz (2.5 seconds measurement interval) of 4 ppm or 5 % (relative) (whichever is greater) for H2O &lt 100 ppm, and 5 % (relative) or 30 ppm (whichever is smaller) for H2O &gt 100 ppm. Accuracy of the CRDS instrument was estimated, based on laboratory calibrations, as 1 % (relative) for the water vapor range from 2.5 % down to 0.7 %, than increasing to 5 % (relative) at 50 ppm water vapor. Accuracy at water vapor mole fractions below 50 ppm was difficult to assess, as the reference systems suffered from lack of data availability.

NOAA’s program of long term monitoring of the vertical distribution of ozone with Electrochemical Concentration Cell (ECC) ozonesondes has undergone a number of changes over the 50 year record. In order to produce a homogenous data set, these changes must be documented and where necessary, appropriate corrections applied. This is the first comprehensive and consistent reprocessing of NOAA’s ozonesonde data records that corrects for these changes using the rawest form of the data (cell current and pump temperature) in native resolution as well as a point by point uncertainty calculation that is unique to each sounding. The reprocessing is carried out uniformly at all eight ozonesonde sites in NOAA’s network with differences in sensing solution and ozonesonde types accounted for in the same way at all sites. The corrections used to homogenize the NOAA ozonesonde data records greatly improve the ozonesonde measurements with an average one sigma uncertainty of ±4–6 % in the stratosphere and ±5–20 % in the troposphere. A comparison of the integrated column ozone from the ozonesonde profile with co-located Dobson spectrophotometers total column ozone measurements shows agreement within ±5 % for > 70 % of the profiles. Very good agreement is also found in the stratosphere between ozonesonde profiles and profiles retrieved from the Solar Backscatter Ultraviolet Instruments (SBUV).

Airborne trace gas, microphysical, and radiation measurements were performed during the AIRcraft TOwed Sensor Shuttle - Inhomogeneous Cirrus Experiment over northern Germany in 2013. Based on high-precision nitrous oxide (N2O) and carbon monoxide (CO) in situ data, stratospheric air could be identified, which contained cirrus cloud particles. Consistent with the stratospheric N2O data, backward trajectories indicate that the sampled air masses crossed the dynamical tropopause in the last 3 h before the measurement. These air masses contained cirrus particles, which were formed during slow ascent in the troposphere and subsequently mixed with stratospheric air. From the CO-N2O correlation the irreversibility of this transport is deduced. To our knowledge, this is the first in situ detection of cirrus particles mixed with stratospheric air in the midlatitudes.

In situ observational data on the relative humidity (RH) in the upper troposphere and lowermost stratosphere (UT/LS), or tropopause region, collected aboard civil passenger aircraft in the MOZAIC (Measurements of OZone, water vapour, carbon monoxide and nitrogen oxides by in-service AIrbus airCraft) programme were reanalysed for the period 2000 to 2009. Previous analyses of probability distribution functions (PDFs) of upper troposphere humidity (UTH) data from MOZAIC observations from year 2000 and later indicated a bias of UTH data towards higher RH values compared to data of the period 1994 to 1999. As a result, the PDF of UTH data show a substantial fraction of observations above 100% relative humidity with respect to liquid water. Such supersaturations, however, do not occur in the atmosphere because there is always a sufficient number of condensation nuclei available, that trigger condensation as soon as liquid saturation is slightly exceeded. An in-depth reanalysis of the data set identified a coding error in the calibration procedure from year 2000 on. The error did not affect earlier data from 1994 to 1999. The full data set for 2000–2009 was reanalysed applying the corrected calibration procedure. Applied correction schemes and a revised error analysis are presented along with the reanalysed PDF of relative humidity with respect to liquid water (RHliquid) and ice (RHice).

Despite several studies on temperature trends in the tropopause region, a comprehensive understanding of the evolution of temperatures in this climate-sensitive region of the atmosphere remains elusive. Here we present a unique global-scale, long-term data set of high-resolution in-situ temperature data measured aboard passenger aircraft within the European Research Infrastructure IAGOS (In-service Aircraft for a Global Observing System, www.iagos.org). This data set is used to investigate temperature trends within the global upper troposphere and lowermost stratosphere (UTLS) for the period 1995 to 2012 in different geographical regions and vertical layers of the UTLS. The largest amount of observations is available over the North Atlantic. Here, a neutral temperature trend is found within the lowermost stratosphere. This contradicts the temperature trend in the European Centre for Medium Range Weather Forecast (ECMWF) ERA-Interim reanalysis, where a significant (95 % confidence) temperature increase of +0.56 K/decade is obtained. Differences between trends derived from observations and reanalysis data can be traced back to changes in the temperature bias between observation and model data over the studied period. This study demonstrates the value of the IAGOS temperature observations as anchor point for the evaluation of reanalyses and its suitability for independent trend analyses.

From the mid 1990s to the late 2000s the consistency of electrochemical cell ozonesonde long term records has been compromised by differences in manufacturers, Science Pump and ENSCI, and differences in recommended sensor solution concentrations, 1.0 % potassium iodide (KI) and the one half dilution 0.5 %. To investigate these differences a number of organizations independently undertook comparisons of the various ozonesonde types and solution concentrations, resulting in 197 ozonesonde comparison profiles. The goal is to derive transfer functions to allow measurements outside of standard recommendations, for sensor composition and ozonesonde type, to be converted to a standard measurement and thus homogenize the data to the expected accuracy of 5 % (10 %) in the stratosphere (troposphere). Subsets of these data have been analyzed previously and intermediate transfer functions derived. Here all the comparison data are analyzed to compare: 1) differences in sensor solution composition for a single ozonesonde type, 2) differences in ozonesonde type for a single sensor solution composition and 3) the manufacturer’s recommendations of 1.0 % KI solution for Science Pump and 0.5 % KI for ENSCI. From the recommendations it is clear that ENSCI ozonesondes and 1.0 % KI solution result in higher amounts of ozone sensed. The results indicate that differences in solution composition and in ozonesonde type display little pressure dependence at pressures ≥ 30 hPa and thus the transfer function can be characterized as a simple ratio of the less sensitive to the more sensitive method. This ratio is 0.96 for both solution concentration and ozonesonde type. The ratios differ at pressures

IAGOS (In-service Aircraft for a Global Observing System) performs long-term routinein situobservations of atmospheric chemical composition (O3, CO, NOx, NOy, CO2, CH4), water vapour, aerosols, clouds, and temperature on a global scale by operating compact instruments on board of passenger aircraft. The unique characteristics of the IAGOS data set originate from the global scale sampling on air traffic routes with similar instrumentation such that the observations are truly comparable and well suited for atmospheric research on a statistical basis. Here, we present the analysis of 15 months of simultaneous observations of relative humidity with respect to ice (RHice) and ice crystal number concentration in cirrus (Nice) from July 2014 to October 2015. The joint data set of 360 hours of RHice–Niceobservations in the global upper troposphere and tropopause region is analysed with respect to the in-cloud distribution of RHiceand related cirrus properties. The majority of the observed cirrus is thin withNice< 0.1 cm−3. The respective fractions of all cloud observations range from 90% over the mid-latitude North Atlantic Ocean and the Eurasian Continent to 67% over the subtropical and tropical Pacific Ocean. The in-cloud RHicedistributions do not depend on the geographical region of sampling. Types of cirrus origin (in situorigin, liquid origin) are inferred for differentNiceregimes and geographical regions. Most importantly, we found that in-cloud RHiceshows a strong correlation toNicewith slightly supersaturated dynamic equilibrium RHiceassociated with higherNicevalues in stronger updrafts.

[1] The Measurement of Ozone and Water Vapor by Airbus In-Service Aircraft (MOZAIC) profiles of O3 and CO were analyzed to study their variation in the troposphere over Bangkok. Mixing ratios of O3 and CO were enhanced in planetary boundary layer (PBL) being highest in winter followed by summer and wet seasons. The daytime profiles of O3 show higher values compared to nighttime observations in PBL region, but little differences were observed in the free troposphere. The decreasing mixing ratios of O3 in the lower and upper troposphere were associated with shallow and deep convections, respectively. Back trajectory and fire count data indicate that the seasonal variations in trace gases were caused mainly by the regional shift in long-range transport and biomass-burning patterns. In wet season, flow of oceanic air and negligible presence of local biomass burning resulted in lowest O3 and CO, while their high levels in dry season were due to extensive biomass burning and transport of continental air masses. The Model for Ozone and Related Chemical Tracers (MOZART) underestimated both O3 and CO in the PBL region but overestimated these in the free troposphere. Simulations of O3 and CO also show the daytime/nighttime differences but do not capture several key features observed in the vertical distributions. The observed and simulated values of O3 and CO during September–November 2006 were significantly higher than the same period of 2005. The year-to-year differences were mainly due to El Nino-led extensive fires in Indonesia during 2006 but normal condition during 2005.

Peak stratospheric chlorofluorocarbon (CFC) and other ozone depleting substance (ODS) concentrations were reached in the mid- to late 1990s. Detection and attribution of the expected recovery of the stratospheric ozone layer in an atmosphere with reduced ODSs as well as efforts to understand the evolution of stratospheric ozone in the presence of increasing greenhouse gases are key current research topics. These require a critical examination of the ozone changes with an accurate knowledge of the spatial (geographical and vertical) and temporal ozone response. For such an examination, it is vital that the quality of the measurements used be as high as possible and measurement uncertainties well quantified. In preparation for the 2014 United Nations Environment Programme (UNEP)/World Meteorological Organization (WMO) Scientific Assessment of Ozone Depletion, the SPARC/IO3C/IGACO-O3/NDACC (SI2N) Initiative was designed to study and document changes in the global ozone profile distribution. This requires assessing long-term ozone profile data sets in regards to measurement stability and uncertainty characteristics. The ultimate goal is to establish suitability for estimating long-term ozone trends to contribute to ozone recovery studies. Some of the data sets have been improved as part of this initiative with updated versions now available. This summary presents an overview of stratospheric ozone profile measurement data sets (ground and satellite based) available for ozone recovery studies. Here we document measurement techniques, spatial and temporal coverage, vertical resolution, native units and measurement uncertainties. In addition, the latest data versions are briefly described (including data version updates as well as detailing multiple retrievals when available for a given satellite instrument). Archive location information for each data set is also given.

The ozone profile records of a large number of limb and occultation satellite instruments are widely used to address several key questions in ozone research. Further progress in some domains depends on a more detailed understanding of these data sets, especially of their long-term stability and their mutual consistency. To this end, we made a systematic assessment of 14 limb and occultation sounders that, together, provide more than three decades of global ozone profile measurements. In particular, we considered the latest operational Level-2 records by SAGE II, SAGE III, HALOE, UARS MLS, Aura MLS, POAM II, POAM III, OSIRIS, SMR, GOMOS, MIPAS, SCIAMACHY, ACE-FTS and MAESTRO. Central to our work is a consistent and robust analysis of the comparisons against the ground-based ozonesonde and stratospheric ozone lidar networks. It allowed us to investigate, from the troposphere up to the stratopause, the following main aspects of satellite data quality: long-term stability, overall bias and short-term variability, together with their dependence on geophysical parameters and profile representation. In addition, it permitted us to quantify the overall consistency between the ozone profilers. Generally, we found that between 20 and 40 km the satellite ozone measurement biases are smaller than ±5 %, the short-term variabilities are less than 5–12 % and the drifts are at most ±5 % decade−1 (or even ±3 % decade−1 for a few records). The agreement with ground-based data degrades somewhat towards the stratopause and especially towards the tropopause where natural variability and low ozone abundances impede a more precise analysis. In part of the stratosphere a few records deviate from the preceding general conclusions; we identified biases of 10 % and more (POAM II and SCIAMACHY), markedly higher single-profile variability (SMR and SCIAMACHY) and significant long-term drifts (SCIAMACHY, OSIRIS, HALOE and possibly GOMOS and SMR as well). Furthermore, we reflected on the repercussions of our findings for the construction, analysis and interpretation of merged data records. Most notably, the discrepancies between several recent ozone profile trend assessments can be mostly explained by instrumental drift. This clearly demonstrates the need for systematic comprehensive multi-instrument comparison analyses.

Accuracy, precision, repeatability and long-term stability, are the most important requirements to enable reliable airborne humidity measurements, which are needed for climate models or to validate e.g. remote sensing instrumentation like satellites. However, various hygrometer artifacts which depend on the individual sensor principle and the application profile frequently cause problems and significantly complicate the hygrometer choice. Sensor intercomparisons are one way of providing the information for an optimal choice. In this paper we present the first part of a blind, static, laboratory-based intercomparison of a new, calibration-free, 1.4 μm diode laser-based, optical hygrometer (SEALDH) with the two most important measurement principles for airborne hygrometry (frost-point hygrometers, FPH, and Lyman-alpha fluorescence hygrometers, LAFH). During three days of measurement, the TDL-hygrometer achieved a H2O resolution of up to 0.5 ppmv (Δt=2 sec) at tropospheric pressure and H2O concentration levels (100–800 hPa, 10 to 8000 ppmv H2O). Its absolute accuracy was investigated via blind intercomparison with two reference FPHs and a LAFH. Without any calibration of SEALDH, i.e. without a comparison to a water vapor standard, we achieve an excellent agreement with the reference sensors, with an average systematic offset (over all three days) of −3.9 %±1.5 %, which is fully consistent with the sensor’s uncertainty bounds. Further we also reevaluated the SEALDH data of day 2 and 3 in a calibrated mode using an independent set of FPH data from the first day and found an 8-fold accuracy improvement, yielding an excellent overall relative deviation of only 0.52 %±1.5 % with respect to a LAFH and a D/FH sensor.

Ozone soundings are used to integrate models, satellite, aircraft and ground-based measurements for better interpretation of ozone variability, including atmospheric losses (predominantly in the stratosphere) and pollution (troposphere). A well-designed network of ozonesonde stations gives information with high vertical and horizontal resolution on a number of dynamical and chemical processes, allowing us to answer questions not possible with aircraft campaigns or current satellite technology. Strategic ozonesonde networks are discussed for high, mid- and low latitude studies. The Match sounding network was designed specifically to follow ozone depletion within the polar vortex; the standard sites are at middle to high northern hemisphere latitudes and typically operate from December through mid-March. Three mid-latitude strategic networks (the IONS series) operated over North America in July-August 2004, March-May and August 2006, and April and June-July-2008. These were designed to address questions about tropospheric ozone budgets and sources, including stratosphere-troposphere transport, and to validate satellite instruments and models. A global network focusing on processes in the equatorial zone, SHADOZ (Southern Hemisphere Additional Ozonesondes), has operated since 1998 in partnership with NOAA, NASA and the Meteorological Services of host countries. Examples of important findings from these networks are described

Global positioning system (GPS) radio occultation (RO) observations aboard low earth orbiting (LEO) satellites provide a powerful tool for global atmospheric sounding. Almost continuously activated since mid-2001, the challenging minisatellite payload (CHAMP) GPS RO experiment provides up to 200 vertical atmospheric profiles per day. In this paper, we intercompare CHAMP RO humidity results and analyses from the European Centre for Medium-Range Weather Forecasts (ECMWF) with coinciding measurement of ozone and water vapor by airbus in-service aircraft (MOZAIC) data collected during aircraft ascents and descents. About 320 coinciding profiles with CHAMP were found from 2001 to 2006 (coincidence radius: 3 h, 300 km). Between about 650 and 300 hPa, the CHAMP-MOZAIC humidity bias is smaller than the ECMWF-MOZAIC bias. On the other hand, the standard deviation between MOZAIC and CHAMP humidity is slightly higher than that between MOZAIC and ECMWF through the entire altitude range. Apart from the water vapor validation (ascent and descent data), we also compare MOZAIC cruise data at an altitude of typically 10-11 km with CHAMP refractivity and temperature results (dry retrieval), and corresponding ECMWF analysis data. Whereas refractivity data from MOZAIC, CHAMP, and ECMWF show excellent agreement, the CHAMP temperature exhibits a cold bias of about 0.9 K in comparison to MOZAIC and ECMWF.

A new in-flight calibration (IFC) method is described for the humidity sensor flown routinely since 1994 on the Measurement of Ozone and Water Vapor by Airbus In-Service Aircraft (MOZAIC) program’s aircraft. The IFC method corrects the potential drift of the sensor offset at zero relative humidity, which is the critical parameter in determining the uncertainty of the measurements. The sensor offset is determined from the measurements themselves as obtained during periods when the aircraft is flying in the lower stratosphere at or above the hygropause, where the H2O mixing ratio reaches well-defined minimum values of about 5 ppmv and the contribution of atmospheric H2O to the sensor signal is minimal. The selection of stratospheric data is achieved with the help of potential temperature, which can be calculated in situ from measured temperature and pressure. The IFC method is capable of providing humidity measurements in near–real time with an uncertainty of ±8% RH at the surface and ±7% RH in the upper troposphere. For validation, the IFC method was applied to 5 yr of archived raw signals from the MOZAIC aircraft. The resulting humidity data are in good agreement (within 2% RH) with the original MOZAIC data that used monthly pre- and postflight calibrations of the sensor. The standard deviation of the differences varies with altitude between ±4% and ±6% RH, which is comparable to the accuracy of the MOZAIC laboratory calibrations. Compared to MOZAIC operation based on monthly calibrations in the laboratory, the use of IFC will substantially reduce the efforts for maintenance and thus will enable operation of the sensor on a large fleet of in-service aircraft for near-real-time measurements of humidity in the troposphere. Because the IFC method will not work on aircraft that never enter the lower stratosphere, for example, aircraft that fly exclusively regional routes or in the tropics, regular offline calibrations will remain important for such aircraft.

In a recent publication (Part I), the authors introduced a data source—Measurement of Ozone and Water Vapor by Airbus In-Service Aircraft (MOZAIC)—for monitoring and studying upper-tropospheric water vapor (UTWV) and analyzed 10 yr (1994–2004) of MOZAIC measurements of tropical UTWV in its climatology, variability, transport, and relation to deep convection. In this study (Part II), MOZAIC is used to assess the ECMWF humidity analysis over the tropics, taking advantage of the unique nature of the MOZAIC data, namely, the long data record, near-global coverage, and high accuracy. In parallel to Part I, the ECMWF UTWV analysis is assessed against MOZAIC in the following five aspects: 1) annual cycle, 2) vertical structure, 3) probability density functions (PDFs), 4) moisture flux divergence, and 5) interannual variability. The annual cycle of the ECMWF UTWV shows a similar pattern as MOZAIC but has an overall dry bias of about 10%–30% relative humidity with respect to ice (RHi). The dry biases are larger in the deep tropics than the subtropics and larger over the Asian monsoon region than the tropical Atlantic region. The increase in RH with height (from about 300 to 200 hPa) as observed by MOZAIC is largely missing in the ECMWF analysis, which has a roughly constant RH profile. The bimodal distribution of tropical UTWV is well established in MOZAIC, but for ECMWF, the moist mode is abruptly cut off at 100% RHi due to the lack of ice supersaturation (ISS) in the forecast model. Lack of ISS capability is, however, not the only cause for the dry bias in the ECMWF; it also has more occurrences of lower humidity compared to MOZAIC. There is also evidence that ECMWF underestimates the range of upper-tropospheric humidity (UTH) variation. A comparison of moisture flux divergence is conducted to assess the ability of ECMWF to capture the divergent transport of water vapor. It is shown that the ECMWF can represent the distribution of this quantity fairly well, although the dry bias leads to some underestimate of the magnitude. Finally, the authors show a comparison of the ECMWF and MOZAIC depictions of the interannual variation of UTWV during the 1997/98 ENSO event as an illustration that UTWV variations are more difficult to capture than those of the UT temperature.

Using nine years (1995--2003) of MOZAIC temperature and humidity data, we analyse the statistics of instantaneous fluctuations of temperature, relative and absolute humidity with various spatial resolutions. We determine the probability density functions (p.d.f.s), their low order moments up to kurtosis, and study how these quantities vary with spatial resolution and with the background mean relative humidity. Seasonal and geographical variations are considered. Bivariate distributions of joint fluctuations of temperature and relative humidity are presented as well. These investigations are thought to provide an observational basis for the validation of statistical cloud schemes for large--scale models. For instance, we can show that temperature fluctuations cannot be neglected in such a scheme and that the bivariate distributions of simultaneous fluctuations of temperature and humidity have to be taken into account.

Ten years (1994–2004) of measurements of tropical upper-tropospheric water vapor (UTWV) by the Measurement of Ozone and Water Vapor by Airbus In-Service Aircraft (MOZAIC) are investigated over three regions—the tropical Atlantic, tropical Africa, and the Asian monsoon region—to determine the UTWV climatology and variability on multiple scales and to understand them in relation to moisture transport and deep convection. The seasonal migration of upper-tropospheric humidity (UTH) keeps pace with that of the ITCZ, indicating the convective influence on UTH distribution. Some significant regional differences are identified with the tropical Africa and the Asian monsoon regions being moister than the tropical Atlantic. UTH generally increases with height by 10%–20% relative humidity with respect to ice (RHi) from about 300 to 200 hPa, and the differences are larger in the deep Tropics than in the subtropics. The probability density functions of tropical UTH are often bimodal. The two modes stay rather constant; differences in the mean value are largely due to the variations in the proportion of the two modes as opposed to changes in the modes themselves. In the deep Tropics, the moisture level frequently reaches ice supersaturation, the most notable case being the near-equatorial Asian monsoon region during the wet season when ice supersaturation is observed 46% of the time. Interannual variations are observed in association with the 1997–98 ENSO event. A warming of about 1–2 K is observed for all three regions equatorward of roughly 15°. Specific humidity also increases somewhat for the tropical Atlantic and tropical Africa, but the increase in temperature outweighs the increase in specific humidity such that RH decreases by 5%–15% RHi. In addition to the ENSO-related variation, MOZAIC also sees increases in both RH and specific humidity over tropical Africa from 2000 onward. Moisture fluxes are computed from MOZAIC data and decomposed into contributions from the mean circulation and from eddies. The flux divergence, which represents the moisture source/sink from horizontal transport, is also estimated. Finally, the MOZAIC climatology and variability are revisited in relation to deep convection obtained from the International Satellite Cloud Climatology Project (ISCCP).

In Canada routine ozone soundings have been carried at Resolute Bay since 1966, making this record the longest in the world. Similar measurements started in the 1970s at three other sites, and the network was expanded in stages to 10 sites by 2003. This important record for understanding long-term changes in tropospheric and stratospheric ozone has been re-evaluated as part of the SPARC/IO3C/IGACO-O3/NDACC (SI2N) initiative. The Brewer–Mast sonde, used in the Canadian network until 1980, is different in construction from the ECC sonde, and the ECC sonde itself has also undergone a variety of minor design changes over the period 1980–2013. Corrections have been made for the estimated effects of these changes, to produce a more homogeneous dataset. The effect of the corrections is generally modest, and so should not invalidate past analyses that have used Canadian network data. However, the overall result is entirely positive: the comparison with co-located total ozone spectrometers is improved, in terms of both bias and SD, and trends in the bias have been reduced or eliminated. An uncertainty analysis (including the additional uncertainty from the corrections, where appropriate) has also been conducted, and the altitude-dependent estimated uncertainty is included with each revised profile. The resulting time series show negative trends in the lower stratosphere of up to 5% decade−1 for the period 1966–2013. Most of this decline occurred before 1997, and linear trends for the more recent period are generally not significant. The time series also show large variations from year to year. Some of these anomalies can be related to cold winters (in the Arctic stratosphere), or changes in the Brewer–Dobson circulation, which may thereby be influencing trends. In the troposphere trends for the 48 year period are small, and for the most part not significant. This suggests that ozone levels in the free troposphere over Canada have not changed significantly in nearly 50 years.

This paper describes a tunable diode laser-based dual-channel photoacoustic (PA) humidity measuring system primarily designed for aircraft-based environment research. It is calibrated for total pressure and water vapor (WV) volume mixing ratios (VMRs) possible during airborne applications. WV VMR is calculated by using pressure-dependent calibration curves and a cubic spline interpolation method. Coverage of the entire atmospheric humidity concentration range that might be encountered during airborne measurements is facilitated by applying an automated sensitivity mode switching algorithm. The calibrated PA system was validated through laboratory and airborne intercomparisons, which proved that the repeatability, the estimated accuracy and the response time of the system are 0.5 ppmV or 0.5% of the actual reading (whichever value is the greater), 5% of the actual reading within the VMR range of 1–12 000 ppmV and 2 s, respectively. The upper detection limit of the system is theoretically about 85 000 ppmV, limited only by condensation of water vapor on the walls of the 318 K heated PA cells and inlet lines, and was experimentally verified up to 20 000 ppmV. The unique advantage of the presented system is its applicability for simultaneous water vapor and total water volume mixing ratio measurements.

The MOZAIC Capacitive Hygrometer (MCH) is usually operated aboard passenger aircraft in the framework of MOZAIC (Measurement of Ozone by Airbus In-Service Aircraft) for measuring atmospheric relative humidity (RH). In order to evaluate the performance of the MCH, the instrument was operated aboard a Learjet 35A research aircraft as part of the CIRRUS-III field study together with a closed-cell Lyman-α fluorescence hygrometer (Fast in situ Stratospheric Hygrometer, or FISH) and an open-path tunable diode laser system (Open-path Jülich Stratospheric TDL ExpeRiment, or OJSTER) for water vapour measurement. After reducing the CIRRUS-III data set to data corresponding to MOZAIC aircraft operation conditions, the 1 Hz RH data cross correlation between the MCH and reference instruments FISH (clear sky) and OJSTER (in-cirrus) yielded a remarkably good agreement of R2 = 0.92 and slope m = 1.02 and provided a MCH uncertainty of 5% RH. Probability distribution functions of RH deduced from the MCH and reference instruments agreed well between 10 and 70% RH with respect to liquid water in the ambient temperature range of ca. −70 to −40 °C. The use of MCH data is limited to sensor temperatures above the calibration limit of Tsensor = −40 °C (corresponds to ambient temperature of Tambient = −70 °C at typical cruising speed of long-haul passenger aircraft). Good performance of the MCH for clear sky as well as for in-cirrus conditions demonstrated the sensor robustness also for operation inside ice clouds.

This study is based on the analysis of Measurement of Ozone and Water Vapor by Airbus In-Service Aircraft (MOZAIC) data measured over Hyderabad, India during the years 2006-2008. Tropospheric profiles of O3 show clear seasonality with high and low values during the premonsoon and monsoon seasons, respectively. Analysis of back trajectory and fire count data indicates major roles for long-range transport and biomass burning in the seasonal variation of O3. Typically, lower levels of O3 in the monsoon season were due to the flow of marine air and negligible regional biomass burning, while higher levels in other seasons were due to transport of continental air. In the upper troposphere, relatively low levels of O3 during the monsoon and postmonsoon seasons were associated with deep convection. In the free troposphere, levels of O3 also show year-to-year variability as the values in the premonsoon of 2006 were higher by about 30 ppbv compared to 2008. The year-to-year variations were mainly due to transition from El Ni�o (2006) to La Ni�a (2008). The higher and lower levels of O 3 were associated with strong and weak wind shears, respectively. Typically, vertical variations of O3 were anticorrelated with the lapse rate profile. The lower O3 levels were observed in the stable layers, but higher values in the midtroposphere were caused by long-range transport. In the PBL region, the mixing ratio of O3 shows strong dependencies on meteorological parameters. The Chemistry Climate Model (CCM2) reasonably reproduced the observed profiles of O3 except for the premonsoon season. � 2014. American Geophysical Union. All Rights Reserved.

The methodology and validation of upper tropospheric humidity (UTH) measurements by the Microwave Limb Sounder (MLS) on the Upper Atmosphere Research Satellite (UARS) are described. The MLS instrument was not specifically designed to measure UTH, but its measurement is achieved by modeling the radiance signal from a window channel as the instrument field of view is scanned through the troposphere. UTH is retrieved as a piecewise-linear function in relative humidity with respect to ice (% RHi) with breakpoints at 147, 215, 316, and 464 hPa. MLS version 4.9 is believed to be the most accurate version to date; its estimated global-averaged accuracy (precision) is 23(21), 22(10), 22(8), and 50(19) %RHi at 147, 215, 316, and 464, hPa respectively. The validation of UTH is established by its consistency with (1) climatological fields, (2) coincident comparisons with in situ Vaisala RS80 balloon sondes, frostpoint hygrometers and Measurement of Ozone and Water Vapor by Airbus In-Service Aircraft measurements, (3) cirrus observations, and (4) meteorological dynamics and assimilation fields. MLS climatological UTH is morphologically consistent with Stratospheric Aerosol and Gas Experiment II and Vaisala zonal climatologies. Comparisons with coincident in situ data show a wide range of agreement. Relative to the other in situ instruments, V4.9 MLS humidities agree on average within 11% at 147 hPa, 3–36% dry at 215 hPa, and 14–39% dry at 316 and 464 hPa. The standard deviation of the individual comparisons about the mean between MLS UTH and the other techniques is approximately 25%RHi at all heights. Humidity measurements in cirrus are compared with UARS Cryogenic Limb Array Etalon Spectrometer (CLAES) extinction measurements and an MLS cirrus detection algorithm. CLAES extinction measurements from 316 to 147 hPa which indicate the presence of cirrus correspond well with MLS UTH measurements greater than ∼100 %RHi. Global MLS UTH distributions appear consistent with those expected from upper tropospheric dynamics and with the Goddard Data Assimilation Office humidity fields.

Ozone (O 3 ) and relative humidity (RH) profiles over the Indian Ocean, obtained during the 1999 Indian Ocean Experiment, were analyzed. Upper-tropospheric O 3 mixing ratios were generally very high (varying from 100 ppbv up to 150 ppbv at the (upper) tropopause). Maxima were observed as laminae (between 14-16 km) and as O 3 -rich layers between the chemopause in O 3 and the tropopause (between 15-18 km), resembling a transition zone between tropospheric and stratospheric O 3 mixing ratios. Very dry, high O 3 air is observed in the midtroposphere (between 5-8 km). The 1999 laminae are similar to those observed in 1998 in a pre-INDOEX campaign, although they appear older. This complicates the attribution of an origin but there are indications, i.e., by back trajectory analyses, that the air in all these O 3 maxima originates in the subtropical jet stream (STJ). This is a favored region for stratosphere-troposphere exchange (STE). A new feature is that the transition zone is supplied with air from both the northern and the southern STJ. A pair of anticyclones located over the western Pacific/Australia directs this interhemispheric transport (IHT). IHT also occurs in the midtroposphere where a flow channel along the east coast of Africa connects the upper troposphere of both hemispheres. Although our analysis, involving the ozone profiles, trajectories, and ECMWF model data, supports the idea that all O 3 maxima have sources similar to 1998, the upper-tropospheric flow is anomalously easterly in 1999. This is probably associated with the La Nina phase of the tropospheric quasi-biennial oscillation as opposed to the 1998 El Nino. Thus, although climatological conditions are very different, the tropospheric O 3 budget over the Indian Ocean during the winter monsoon is still largely influenced by stratospheric intrusions.

This study investigates the distribution and the sources of ozone (O3) observed in the uppermost troposphere and lowermost stratosphere within the framework of the Measurement of Ozone and Water Vapor by Airbus InService Aircraft (MOZAIC) program. The O3 measurement data taken aboard five commercial aircraft during a 1-year period are combined with 8-day three-dimensional back trajectories ending at the aircraft positions. Potential vorticity along the trajectories is used to form subsets of the data taken in the troposphere, in the stratosphere, and in stratosphere-troposphere exchange flows. A measured O3 value is then attributed to the entire path of the corresponding trajectory. A statistical analysis of this data set extends previous global MOZAIC O3 climatologies which are restricted to the major flight corridors. Furthermore, it allows source region identification of the measured O3. It is found that the North American and Eurasian continental boundary layers are the major sources of upper tropospheric O3 in spring and summer, while the African boundary layer is the greatest Os source in fall and winter. The seasonal O3 variation is strongest in air masses exported from central Asia, followed by North America. The central Asian O3 maximum is higher and occurs earlier in the year than the North American maximum, which possibly indicates a great influence from biomass burning emissions in Asia. In the lowermost stratosphere the dominant structures in the O3 distribution are a strong north-south gradient and a wave-like pattern with O3 maxima over North America and eastern Asia. O3 concentrations in stratosphere-troposphere exchange flows are higher than in tropospheric air throughout the year and thus provide an important O3 source for the troposphere. However, our analysis suggests that photochemical O3 formation is more important than stratosphere-troposphere exchange during most of the year.