Search

The Tropospheric Ozone Lidar Network (TOLNet) was used to validate retrievals of ozone (O3) profiles in the troposphere from the TROPOspheric Monitoring Instrument (TROPOMI) ultraviolet (UV), Cross-track Infrared Sounder (CrIS) infrared (IR), and a combined UV + IR wavelength retrieval from TROPOMI/CrIS. Observations from six separate ground-based lidar systems and various locations of ozonesondes distributed throughout North America and in the Netherlands were used to quantify systematic bias and random errors for each satellite retrieval. Furthermore, TOLNet data were used to intercompare idealized UV, IR, and UV + IR convolved lidar profiles of O3 in the troposphere during case studies representative of high-O3 events. This study shows that the improved sensitivity and vertical resolution in UV + IR retrievals in the middle- and upper-troposphere resulted in tropospheric degree of freedom (DOF) values ∼ 33 % higher compared to UV- and IR-only retrievals. The increased DOFs in the UV + IR retrievals allowed for improved reproduction of mid- and upper-tropospheric O3 enhancements and, to a lesser degree, near-surface pollution enhancements compared to single-wavelength satellite products. The validation of O3 profiles in the troposphere retrieved with the UV-only, IR-only, and UV + IR Tikhonov regularised Ozone Profile retrievAl with SCIATRAN (TOPAS) algorithm developed at the Institute for Environmental Physics, University of Bremen, demonstrated the utility of using TOLNet as a satellite evaluation data set. TOPAS UV-only, IR-only, and UV + IR wavelength retrievals had systematic biases, quantified with normalized mean bias, throughout the troposphere of 11.2 ppb (22.1 %), −1.7 ppb (−0.3 %), and 3.5 ppb (7.8 %), respectively, which meet the tropospheric systematic bias requirements defined by the science teams for the TROPOMI and CrIS sensors. The primary drivers of systematic bias were determined to be solar zenith angle, surface albedo, and cloud fraction. Random errors, representative of uncertainty in the retrievals and quantified by root mean squared errors (RMSEs), were large for all three retrievals, with UV-only, IR-only, and UV + IR wavelength retrievals having RMSEs throughout the troposphere of 17.4 ppb (19.8 % of mean tropospheric column values), 10.5 ppb (12.6 % of mean tropospheric column values), and 14.0 ppb (14.6 % of mean tropospheric column values), respectively. TOPAS UV-only profiles did not meet the uncertainty requirements defined for TROPOMI for the troposphere; however, CrIS IR-only retrievals did meet the uncertainty requirements defined by this mission. The larger random errors reflect the challenge of retrieving daily O3 profiles due to the limited sensitivity and vertical resolution of these retrievals in the troposphere. Tropospheric systematic biases and random error were lower in IR-only and combined UV + IR retrievals compared to UV-only products due to the increased sensitivity in the troposphere allowing the retrievals to deviate further from the a priori profiles. Observations from TOLNet demonstrated that the performance of the three satellite products varied by season and altitude in the troposphere. TOLNet was shown to result in similar validation statistics compared to ozonesonde data, which are a commonly used satellite evaluation data source, demonstrating that TOLNet is a sufficient source of satellite O3 profile validation data in the troposphere, which is critical as this data source is the primary product identified for the tropospheric O3 validation of the recently launched Tropospheric Emissions: Monitoring of Pollution (TEMPO) mission.

Vertical profiles of aerosols, NO2, and SO2 were retrieved from Multi-Axis Differential Optical Absorption Spectroscopy (MAX-DOAS) measurements at a field site in northern Alberta, Canada, during August and September 2013. The site is approximately 16 km north of two mining operations that are major sources of industrial pollution in the Athabasca oil sands region. Pollution conditions during the study ranged from atmospheric background conditions to heavily polluted with elevated plumes, according to the meteorology. This study aimed to evaluate the performance of the aerosol and trace gas retrievals through comparison with data from a suite of other instruments. Comparisons of aerosol optical depths (AODs) from MAX-DOAS aerosol retrievals, lidar vertical profiles of aerosol extinction, and the AERONET sun photometer indicate good performance by the MAX-DOAS retrievals. These comparisons and modelling of the lidar S ratio highlight the need for accurate knowledge of the temporal variation in the S ratio when comparing MAX-DOAS and lidar data. Comparisons of MAX-DOAS NO2 and SO2 retrievals to Pandora spectral sun photometer vertical column densities (VCDs) and active DOAS mixing ratios indicate good performance of the retrievals, except when vertical profiles of pollutants within the boundary layer varied rapidly, temporally, and spatially. Near-surface retrievals tended to overestimate active DOAS mixing ratios. The MAX-DOAS observed elevated pollution plumes not observed by the active DOAS, highlighting one of the instrument's main advantages. Aircraft measurements of SO2 were used to validate retrieved vertical profiles of SO2. Advantages of the MAX-DOAS instrument include increasing sensitivity towards the surface and the ability to simultaneously retrieve vertical profiles of aerosols and trace gases without requiring additional parameters, such as the S ratio. This complex dataset provided a rare opportunity to evaluate the performance of the MAX-DOAS retrievals under varying atmospheric conditions.

A short, but severe, wildfire smoke episode in July 2015, with an aerosol optical depth (AOD) approaching 9, is shown to strongly impact radiation budgets across four distinct land-use types (forest, field, urban and wetland). At three of the sites, impacts on the energy balance are also apparent, while the event also appears to elicit an ecosystem response with respect to carbon fluxes at the wetland and a forested site. Greatest impacts on radiation and energy budgets were observed at the forested site where the role of canopy architecture and the complex physiological responses to an increase in diffuse radiation were most important. At the forest site, the arrival of smoke reduced both sensible and latent heat flux substantially but also lowered sensible heat flux more than the latent heat flux. With widespread standing water, and little physiological control on evapotranspiration, the impacts on the partitioning of turbulent fluxes were modest at the wetland compared to the physiologically dominated fluxes at the forested site. Despite the short duration and singular nature of the event, there was some evidence of a diffuse radiation fertilization effect when AOD was near or below 2. With lighter smoke, both the wetland and forested site appeared to show enhanced photosynthetic activity (a greater sink for carbon dioxide). However, with dense smoke, the forested site was a strong carbon source. Given the extensive forest cover in the Pacific Northwest and the growing importance of forest fires in the region, these results suggest that wildfire aerosol during the growing season potentially plays an important role in the regional ecosystem response to smoke and ultimately the carbon budget of the region.

Lidar technology has been rapidly advancing over the past several decades. It can be used to measure a variety of atmospheric constituents at very high temporal and spatial resolutions. While the number of lidars continues to increase worldwide, there is generally a dependency on an operator, particularly for high-powered lidar systems. Environment and Climate Change Canada (ECCC) has recently developed a fully autonomous, mobile lidar system called AMOLITE (Autonomous Mobile Ozone Lidar Instrument for Tropospheric Experiments) to simultaneously measure the vertical profile of tropospheric ozone, aerosol and water vapor (nighttime only) from near the ground to altitudes reaching 10 to 15 km. This current system uses a dual-laser, dual-lidar design housed in a single climate-controlled trailer. Ozone profiles are measured by the differential absorption lidar (DIAL) technique using a single 1 m Raman cell filled with CO2. The DIAL wavelengths of 287 and 299 nm are generated as the second and third Stokes lines resulting from stimulated Raman scattering of the cell pumped using the fourth harmonic of a Nd:YAG laser (266 nm). The aerosol lidar transmits three wavelengths simultaneously (355, 532 and 1064 nm) employing a detector designed to measure the three backscatter channels, two nitrogen Raman channels (387 and 607 nm) and one cross-polarization channel at 355 nm. In addition, we added a water vapor channel arising from the Raman-shifted 355 nm output (407 nm) to provide nighttime water vapor profiles. AMOLITE participated in a validation experiment alongside four other ozone DIAL systems before being deployed to the ECCC Oski-ôtin ground site in the Alberta oil sands region in November 2016. Ozone was found to increase throughout the troposphere by as much as a factor of 2 from stratospheric intrusions. The dry stratospheric air within the intrusion was measured to be less than 0.2 g kg−1. A biomass burning event that impacted the region over an 8-day period produced lidar ratios of 35 to 65 sr at 355 nm and 40 to 100 sr at 532. Over the same period the Ångström exponent decreased from 1.56±0.2 to 1.35±0.2 in the 2–4 km smoke region.

The North America-based Tropospheric Ozone Lidar Network (TOLNet) was recently established to provide high spatiotemporal vertical profiles of ozone, to better understand physical processes driving tropospheric ozone variability and to validate the tropospheric ozone measurements of upcoming spaceborne missions such as Tropospheric Emissions: Monitoring Pollution (TEMPO). The network currently comprises six tropospheric ozone lidars, four of which are mobile instruments deploying to the field a few times per year, based on campaign and science needs. In August 2016, all four mobile TOLNet lidars were brought to the fixed TOLNet site of JPL Table Mountain Facility for the 1-week-long Southern California Ozone Observation Project (SCOOP). This intercomparison campaign, which included 400 h of lidar measurements and 18 ozonesonde launches, allowed for the unprecedented simultaneous validation of five of the six TOLNet lidars. For measurements between 3 and 10 km a.s.l., a mean difference of 0.7 ppbv (1.7 %), with a root-mean-square deviation of 1.6 ppbv or 2.4 %, was found between the lidars and ozonesondes, which is well within the combined uncertainties of the two measurement techniques. The few minor differences identified were typically associated with the known limitations of the lidars at the profile altitude extremes (i.e., first 1 km above ground and at the instruments' highest retrievable altitude). As part of a large homogenization and quality control effort within the network, many aspects of the TOLNet in-house data processing algorithms were also standardized and validated. This thorough validation of both the measurements and retrievals builds confidence as to the high quality and reliability of the TOLNet ozone lidar profiles for many years to come, making TOLNet a valuable ground-based reference network for tropospheric ozone profiling.

Biomass burning emissions emit a significant amount of trace gases and aerosols and can affect atmospheric chemistry and radiative forcing for hundreds or thousands of kilometres downwind. They can also contribute to exceedances of air quality standards and have negative impacts on human health. We present a case study of an intense wildfire plume from Siberia that affected the air quality across the Pacific Northwest on 6–10 July 2012. Using satellite measurements (MODIS True Colour RGB imagery and MODIS AOD), we track the wildfire smoke plume from its origin in Siberia to the Pacific Northwest where subsidence ahead of a subtropical Pacific High made the plume settle over the region. The normalized enhancement ratios of O3 and PM1 relative to CO of 0.26 and 0.08 are consistent with a plume aged 6–10 days. The aerosol mass in the plume was mainly submicron in diameter (PM1 ∕ PM2.5 = 0.96) and the part of the plume sampled at the Whistler High Elevation Monitoring Site (2182 m a.s.l.) was 88 % organic material. Stable atmospheric conditions along the coast limited the initial entrainment of the plume and caused local anthropogenic emissions to build up. A synthesis of air quality from the regional surface monitoring networks describes changes in ambient O3 and PM2.5 during the event and contrasts them to baseline air quality estimates from the AURAMS chemical transport model without wildfire emissions. Overall, the smoke plume contributed significantly to the exceedances in O3 and PM2.5 air quality standards and objectives that occurred at several communities in the region during the event. Peak enhancements in 8 h O3 of 34–44 ppbv and 24 h PM2.5 of 10–32 µg m−3 were attributed to the effects of the smoke plume across the Interior of British Columbia and at the Whistler Peak High Elevation Site. Lesser enhancements of 10–12 ppbv for 8 h O3 and of 4–9 µg m−3 for 24 h PM2.5 occurred across coastal British Columbia and Washington State. The findings suggest that the large air quality impacts seen during this event were a combination of the efficient transport of the plume across the Pacific, favourable entrainment conditions across the BC interior, and the large scale of the Siberian wildfire emissions. A warming climate increases the risk of increased wildfire activity and events of this scale reoccurring under appropriate meteorological conditions.

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.

We describe the design and execution of the BORTAS (Quantifying the impact of BOReal forest fires on Tropospheric oxidants over the Atlantic using Aircraft and Satellites) experiment, which has the overarching objective of understanding the chemical aging of air masses that contain the emission products from seasonal boreal wildfires and how these air masses subsequently impact downwind atmospheric composition. The central focus of the experiment was a two-week deployment of the UK BAe-146-301 Atmospheric Research Aircraft (ARA) over eastern Canada, based out of Halifax, Nova Scotia. Atmospheric ground-based and sonde measurements over Canada and the Azores associated with the planned July 2010 deployment of the ARA, which was postponed by 12 months due to UK-based flights related to the dispersal of material emitted by the Eyjafjallajökull volcano, went ahead and constituted phase A of the experiment. Phase B of BORTAS in July 2011 involved the same atmospheric measurements, but included the ARA, special satellite observations and a more comprehensive ground-based measurement suite. The high-frequency aircraft data provided a comprehensive chemical snapshot of pyrogenic plumes from wildfires, corresponding to photochemical (and physical) ages ranging from < 1 day to ~<45 sr 10 days, largely by virtue of widespread fires over Northwestern Ontario. Airborne measurements reported a large number of emitted gases including semi-volatile species, some of which have not been been previously reported in pyrogenic plumes, with the corresponding emission ratios agreeing with previous work for common gases. Analysis of the NOy data shows evidence of net ozone production in pyrogenic plumes, controlled by aerosol abundance, which increases as a function of photochemical age. The coordinated ground-based and sonde data provided detailed but spatially limited information that put the aircraft data into context of the longer burning season in the boundary layer. Ground-based measurements of particulate matter smaller than 2.5 μm (PM2.5) over Halifax show that forest fires can on an episodic basis represent a substantial contribution to total surface PM2.5.

Lidar has the ability to detect the complex vertical structure of the atmosphere and can therefore identify the existence and extent of aerosols with high spatial and temporal resolution, making it well suited for understanding atmospheric dynamics and transport processes. Environment Canada has developed a portable, autonomous lidar system that can be monitored remotely and operated continuously except during precipitation events. The lidar, housed in a small trailer, simultaneously emits two wavelengths of laser light (1064 nm and 532 nm) at energies of approximately 150 mJ/pulse/wavelength and detects the backscatter signal at 1064 nm and both polarizations at 532 nm. For laser energies of this magnitude, the challenge resides in designing a system that meets the airspace safety requirements for autonomous operations. Through the combination of radar technology, beam divergence, laser cavity interlocks and using computer log files, this risk was mitigated. A Continuum Inlite small footprint laser is the backbone of the system because of three design criteria: requiring infrequent flash lamp changes compared to previous Nd : YAG Q-switch lasers, complete software control capability and a built-in laser energy monitoring system. A computer-controlled interface was designed to monitor the health of the system, adjust operational parameters and maintain a climate-controlled environment. Through an Internet connection, it also transmitted the vital performance indicators and data stream to allow the lidar profile data for multiple instruments from near ground to 15 km, every 10 s, to be viewed, in near real-time via a website. The details of the system design and calibration will be discussed and the success of the instrument as tested within the framework of a national lidar network dubbed CORALNet (Canadian Operational Research Aerosol Lidar Network). In addition, the transport of a forest fire plume across the country will be shown as evidenced by the lidar network, HYSPLIT back trajectories, MODIS imagery and CALIPSO overpasses.

A large fraction of submicron aerosol mass throughout the continental boundary layer consists of secondary organic aerosol (SOA) mass. As such, the ability of chemical transport models to accurately predict continental boundary layer aerosol greatly depends on their ability to predict SOA. Although there has been much recent effort to better describe SOA formation mechanisms in models, little attention has been paid to the effects of model spatial resolution on SOA predictions. The Whistler Aerosol and Cloud Study (WACS 2010), held between 22 June and 28 July 2010 and conducted at Whistler, BC, Canada provides a unique data set for testing simulated SOA predictions. The study consisted of intensive measurements of atmospheric trace gases and particles at several locations strongly influenced by biogenic sources in the region. We test the ability of the global chemical transport model GEOS-Chem to predict the aerosol concentrations during this event and throughout the campaign. Simulations were performed using three different resolutions of the model: 4° × 5° , 2° × 2.5° and 0.5° × 0.667°. Predictions of organic aerosol concentrations at Whistler were greatly dependent on the resolution; the 4° × 5° version of the model significantly under predicts organic aerosol, while the 2° × 2.5° and 0.5° × 0.667° versions are much more closely correlated with measurements. In addition, we performed a comparison between the 3 versions of the model across North America. Comparison simulations were run for both a summer case (July) and Winter case (January). For the summer case, 0.5° × 0.667° simulations predicted on average 19% more SOA than 2° × 2.5° and 32% more than 4° × 5° . For the winter case, the 0.5° × 0.667° simulations predicted 8% more SOA than the 2° × 2.5° and 23% more than the 4° × 5°. This increase in SOA with resolution is largely due to sub-grid variability of organic aerosol (OA) that leads to an increase in the partitioning of secondary organic matter to the aerosol phase at higher resolutions. SOA concentrations were further increased because the shift of secondary organic gases to SOA at higher resolutions increased the lifetime of secondary organic matter (secondary organic gases have a shorter deposition lifetime than SOA in the model). SOA precursor emissions also have smaller, but non-negligible, changes with resolution due to non-linear inputs to the MEGAN biogenic emissions scheme. These results suggest that a portion of the traditional under-prediction of SOA by global models may be due to the effects of coarse grid resolution.

Observations from the 2007 Border Air Quality and Meteorology Study (BAQS-Met 2007) in Southern Ontario, Canada, were used to evaluate predictions of primary organic aerosol (POA) and two other carbonaceous species, black carbon (BC) and carbon monoxide (CO), made for this summertime period by Environment Canada's AURAMS regional chemical transport model. Particle component-based factor analysis was applied to aerosol mass spectrometer measurements made at one urban site (Windsor, ON) and two rural sites (Harrow and Bear Creek, ON) to derive hydrocarbon-like organic aerosol (HOA) factors. A novel diagnostic model evaluation was performed by investigating model POA bias as a function of HOA mass concentration and indicator ratios (e.g. BC/HOA). Eight case studies were selected based on factor analysis and back trajectories to help classify model bias for certain POA source types. By considering model POA bias in relation to co-located BC and CO biases, a plausible story is developed that explains the model biases for all three species. At the rural sites, daytime mean PM1 POA mass concentrations were under-predicted compared to observed HOA concentrations. POA under-predictions were accentuated when the transport arriving at the rural sites was from the Detroit/Windsor urban complex and for short-term periods of biomass burning influence. Interestingly, the daytime CO concentrations were only slightly under-predicted at both rural sites, whereas CO was over-predicted at the urban Windsor site with a normalized mean bias of 134%, while good agreement was observed at Windsor for the comparison of daytime PM1 POA and HOA mean values, 1.1 μg m−3 and 1.2 μg m−3, respectively. Biases in model POA predictions also trended from positive to negative with increasing HOA values. Periods of POA over-prediction were most evident at the urban site on calm nights due to an overly-stable model surface layer. This model behaviour can be explained by a combination of model under-estimation of vertical mixing at the urban location, under-representation of PM emissions for on-road traffic exhaust along major urban roads and highways, and a more structured allocation of area POA sources such as food cooking and dust emissions to urban locations. A downward trend in POA bias was also observed at the urban site as a function of the BC/HOA indicator ratio, suggesting a possible association of POA under-prediction with under-representation of diesel combustion sources. An investigation of the emission inventories for the province of Ontario and the nearby US state of Indiana also suggested that the top POA area emission sources (food cooking, organic-bound to dust, waste disposal burning) dominated over mobile and point sources, again consistent with a mobile under-estimation. We conclude that more effort should be placed at reducing uncertainties in the treatment of several large POA emission sources, in particular food cooking, fugitive dust, waste disposal burning, and on-road traffic sources, and especially their spatial surrogates and temporal profiles. This includes using higher spatial resolution model grids to better resolve the urban road network and urban food cooking locations. We also recommend that additional sources of urban-scale vertical mixing in the model, such as a stronger urban heat island effect and vehicle-induced turbulence, would help model predictions at urban locations, especially at night time.

The Whistler Aerosol and Cloud Study (WACS 2010), included intensive measurements of trace gases and particles at two sites on Whistler Mountain. Between 6–11 July 2010 there was a sustained high-pressure system over the region with cloud-free conditions and the highest temperatures of the study. During this period, the organic aerosol concentrations rose from −3 to ∼6 μg m−3. Precursor gas and aerosol composition measurements show that these organics were almost entirely of secondary biogenic nature. Throughout 6–11 July, the anthropogenic influence was minimal with sulfate concentrations −3 and SO2 mixing ratios &approx; 0.05–0.1 ppbv. Thus, this case provides excellent conditions to probe the role of biogenic secondary organic aerosol in aerosol microphysics. Although SO2 mixing ratios were relatively low, box-model simulations show that nucleation and growth may be modeled accurately if Jnuc = 3 × 10−7[H2SO4] and the organics are treated as effectively non-volatile. Due to the low condensation sink and the fast condensation rate of organics, the nucleated particles grew rapidly (2–5 nm h−1) with a 10–25% probability of growing to CCN sizes (100 nm) in the first two days as opposed to being scavenged by coagulation with larger particles. The nucleated particles were observed to grow to ∼200 nm after three days. Comparisons of size-distribution with CCN data show that particle hygroscopicity (κ) was ∼0.1 for particles larger 150 nm, but for smaller particles near 100 nm the κ value decreased near midway through the period from 0.17 to less than 0.06. In this environment of little anthropogenic influence and low SO2, the rapid growth rates of the regionally nucleated particles – due to condensation of biogenic SOA – results in an unusually high efficiency of conversion of the nucleated particles to CCN. Consequently, despite the low SO2, nucleation/growth appear to be the dominant source of particle number.

The validation of ozone profiles retrieved by satellite instruments through comparison with data from ground-based instruments is important to monitor the evolution of the satellite instrument, to assist algorithm development and to allow multi-mission trend analyses. In this study we compare ozone profiles derived from GOMOS night-time observations with measurements from lidar, microwave radiometer and balloon sonde. Collocated pairs are analysed for dependence on several geophysical and instrument observational parameters. Validation results are presented for the operational ESA level 2 data (GOMOS version 5.00) obtained during nearly seven years of observations and a comparison using a smaller dataset from the previous processor (version 4.02) is also included. The profiles obtained from dark limb measurements (solar zenith angle >107°) when the provided processing flag is properly considered match the ground-based measurements within ±2 percent over the altitude range 20 to 40 km. Outside this range, the pairs start to deviate more and there is a latitudinal dependence: in the polar region where there is a higher amount of straylight contamination, differences start to occur lower in the mesosphere than in the tropics, whereas for the lower part of the stratosphere the opposite happens: the profiles in the tropics reach less far down as the signal reduces faster because of the higher altitude at which the maximum ozone concentration is found compared to the mid and polar latitudes. Also the bias is shifting from mostly negative in the polar region to more positive in the tropics Profiles measured under "twilight" conditions are often matching the ground-based measurements very well, but care has to be taken in all cases when dealing with "straylight" contaminated profiles. For the selection criteria applied here (data within 800 km, 3 degrees in equivalent latitude, 20 h (5 h above 50 km) and a relative ozone error in the GOMOS data of 20% or less), no dependence was found on stellar magnitude, star temperature, nor the azimuth angle of the line of sight. No evidence of a temporal trend was seen either in the bias or frequency of outliers, but a comparison applying less strict data selection criteria might show differently.

This paper presents extensive {bias determination} analyses of ozone observations from the Atmospheric Chemistry Experiment (ACE) satellite instruments: the ACE Fourier Transform Spectrometer (ACE-FTS) and the Measurement of Aerosol Extinction in the Stratosphere and Troposphere Retrieved by Occultation (ACE-MAESTRO) instrument. Here we compare the latest ozone data products from ACE-FTS and ACE-MAESTRO with coincident observations from nearly 20 satellite-borne, airborne, balloon-borne and ground-based instruments, by analysing volume mixing ratio profiles and partial column densities. The ACE-FTS version 2.2 Ozone Update product reports more ozone than most correlative measurements from the upper troposphere to the lower mesosphere. At altitude levels from 16 to 44 km, the average values of the mean relative differences are nearly all within +1 to +8%. At higher altitudes (45–60 km), the ACE-FTS ozone amounts are significantly larger than those of the comparison instruments, with mean relative differences of up to +40% (about +20% on average). For the ACE-MAESTRO version 1.2 ozone data product, mean relative differences are within ±10% (average values within ±6%) between 18 and 40 km for both the sunrise and sunset measurements. At higher altitudes (~35–55 km), systematic biases of opposite sign are found between the ACE-MAESTRO sunrise and sunset observations. While ozone amounts derived from the ACE-MAESTRO sunrise occultation data are often smaller than the coincident observations (with mean relative differences down to −10%), the sunset occultation profiles for ACE-MAESTRO show results that are qualitatively similar to ACE-FTS, indicating a large positive bias (mean relative differences within +10 to +30%) in the 45–55 km altitude range. In contrast, there is no significant systematic difference in bias found for the ACE-FTS sunrise and sunset measurements.

The first three Arctic winters of the ACE mission represented two extremes of winter variability: Stratospheric sudden warmings (SSWs) in 2004 and 2006 were among the strongest, most prolonged on record; 2005 was a record cold winter. Canadian Arctic Atmospheric Chemistry Experiment (ACE) Validation Campaigns were conducted at Eureka (80° N, 86° W) during each of these winters. New satellite measurements from ACE-Fourier Transform Spectrometer (ACE-FTS), Sounding of the Atmosphere using Broadband Emission Radiometry (SABER), and Aura Microwave Limb Sounder (MLS), along with meteorological analyses and Eureka lidar temperatures, are used to detail the meteorology in these winters, to demonstrate its influence on transport, and to provide a context for interpretation of ACE-FTS and validation campaign observations. During the 2004 and 2006 SSWs, the vortex broke down throughout the stratosphere, reformed quickly in the upper stratosphere, and remained weak in the middle and lower stratosphere. The stratopause reformed at very high altitude, near 75 km. ACE measurements covered both vortex and extra-vortex conditions in each winter, except in late-February through mid-March 2004 and 2006, when the strong, pole-centered vortex that reformed after the SSWs resulted in ACE sampling only inside the vortex in the middle through upper stratosphere. The 2004 and 2006 Eureka campaigns were during the recovery from the SSWs, with the redeveloping vortex over Eureka. 2005 was the coldest winter on record in the lower stratosphere, but with an early final warming in mid-March. The vortex was over Eureka at the start of the 2005 campaign, but moved away as it broke up. Disparate temperature profile structure and vortex evolution resulted in much lower (higher) temperatures in the upper (lower) stratosphere in 2004 and 2006 than in 2005. Satellite temperatures agree well with lidar data up to 50–60 km, and ACE-FTS, MLS and SABER show good agreement in high-latitude temperatures throughout the winters. Consistent with a strong, cold upper stratospheric vortex and enhanced radiative cooling after the SSWs, MLS and ACE-FTS trace gas measurements show strongly enhanced descent in the upper stratospheric vortex in late January through March 2006 compared to that in 2005.

An ensemble of space-borne and ground-based instruments has been used to evaluate the quality of the version 2.2 temperature retrievals from the Atmospheric Chemistry Experiment Fourier Transform Spectrometer (ACE-FTS). The agreement of ACE-FTS temperatures with other sensors is typically better than 2 K in the stratosphere and upper troposphere and 5 K in the lower mesosphere. There is evidence of a systematic high bias (roughly 3–6 K) in the ACE-FTS temperatures in the mesosphere, and a possible systematic low bias (roughly 2 K) in ACE-FTS temperatures near 23 km. Some ACE-FTS temperature profiles exhibit unphysical oscillations, a problem fixed in preliminary comparisons with temperatures derived using the next version of the ACE-FTS retrieval software. Though these relatively large oscillations in temperature can be on the order of 10 K in the mesosphere, retrieved volume mixing ratio profiles typically vary by less than a percent or so. Statistical comparisons suggest these oscillations occur in about 10% of the retrieved profiles. Analysis from a set of coincident lidar measurements suggests that the random error in ACE-FTS version 2.2 temperatures has a lower limit of about ±2 K.