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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.

Widespread and persistent summer multi-day episodes of dense wildfire smoke affected western Canada in 2017 and 2018. These events often occurred under otherwise clear-sky, anticyclonic weather conditions and can have significant impacts on surface temperatures, air quality, and surface radiation and energy budgets. Based on upward-pointing lidar observations, vertical temperature soundings and numerical mesoscale modelling for a mountain in south-western British Columbia, Canada, we propose a previously undocumented stability-related impact of wildfire smoke layers on mountain meteorology. This positive feedback (that maintains layer structure and extends the lifetime of layers) appears to suppress mountain “handover processes”. Smoke days are characterized by more stable vertical temperature profiles when compared to clear-sky conditions, and are marked by a lack of diurnal variability in boundary-layer structure in lidar backscatter imagery. We expect the processes described to have general application and propose more detailed aerosol modelling to investigate the physical details of the process.

The goal of the Canadian Arctic Weather Science (CAWS) project is to conduct research into the future operational monitoring and forecasting programs of Environment and Climate Change Canada in the Arctic where increased economic and recreational activities are expected with enhanced transportation and search and rescue requirements. Due to cost, remoteness and vast geographical coverage, the future monitoring concept includes a combination of space-based observations, sparse in situ surface measurements, and advanced reference sites. A prototype reference site has been established at Iqaluit, Nunavut (63°45'N, 68°33'W), that includes a Ka-band radar, water vapor lidars (both in-house and commercial versions), multiple Doppler lidars, ceilometers, radiation flux, and precipitation sensors. The scope of the project includes understanding of the polar processes, evaluating new technologies, validation of satellite products, validation of numerical weather prediction systems, development of warning products, and communication of their risk to a variety of users. This contribution will provide an overview of the CAWS project to show some preliminary results and to encourage collaborations.

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.

Aircraft-based lidar measurements of atmospheric aerosol and ozone were conducted to study air pollution from the oil sands extraction industry in northern Alberta. Significant amounts of aerosol were observed in the polluted air within the surface boundary layer, up to heights of 1 to 1.6 km above ground. The ozone mixing ratio measured in the polluted boundary layer air directly above the oil sands industry was equal to or less than the background ozone mixing ratio. On one of the flights, the lidar measurements detected a layer of forest fire smoke above the surface boundary layer in which the ozone mixing ratio was substantially greater than the background. Measurements of the linear depolarization ratio in the aerosol backscatter were obtained with a ground-based lidar and this aided in the discrimination between the separate emission sources from industry and forest fires. The retrieval of ozone abundance from the lidar measurements required the development of a method to account for the interference from the substantial aerosol content within the polluted boundary layer.

Biomass burning from wildfires is a significant global source of aerosol and trace gases which impact air quality, tropospheric and stratospheric composition, and climate. During the summer of 2019, wildfire activity in central and eastern Siberia occurred during the Fire Influence on Regional to Global Environments and Air Quality (FIREX-AQ) campaign conducted in the United States between July 24 and September 6, 2019. Ground-based lidar observations from the Autonomous Mobile Ozone Lidar for Tropospheric Experiments (AMOLITE) system in Alberta, Canada retrieved frequent ozone (O3) and aerosol lamina in the free troposphere during the campaign. Simulated data from NASA's GEOS Composition Forecast (GEOS-CF) coupled chemistry meteorology model, TROPOspheric Monitoring Instrument (TROPOMI), and ground-based in situ measurements were applied to define the trans-Pacific and trans-Arctic transport pathways of Siberian biomass burning emissions resulting in the enhanced O3 and aerosol lamina observed by AMOLITE in western Canada. Siberian wildfires had some influence on North American air quality resulting in enhancements of surface carbon monoxide (CO) and fine particulate matter (PM2.5) concentrations in western Canada; however, minimal increases in surface-level O3 were measured as well as modeled by GEOS-CF. The impact in western Canada was larger in the free troposphere, demonstrated by GEOS-CF modeled and AMOLITE observed O3 lamina >20 ppb above background values and coincident model-predicted PM2.5 lamina >30 μg m−3. This study demonstrated that the Siberian biomass burning emissions in the summer of 2019 impacted tropospheric composition in western Canada, and potentially could have influenced areas in the vicinity of FIREX-AQ airborne and ground-based measurements in the United States, and should be considered in future studies.

Results of a recently developed water vapor Raman lidar instrument at Environment Canada's Center for Atmospheric Research Experiments (CARE) are shown for selected days of summer and winter seasons. The basic components of the Raman water vapor lidar consist of a 30 Hz, Q-switched Nd:YAG high-powered laser utilizing the third harmonic (355 nm), beam steering optics, a 0.76 m Cassegrain telescope and three detection channels to simultaneously observe the vertical profiles of aerosols, water vapor, and nitrogen from near ground up to 9.5 km. By manipulating the inelastic backscattering lidar signals from the Raman nitrogen channel (386.7 nm) and Raman water vapor channel (407.5 nm), vertical profiles of water vapor mixing ratio (WVMR) are deduced, calibrated, and compared against WVMR profiles obtained from coincident and collocated radiosonde profiles. The average standard deviation, in the water vapor mixing ratio, is estimated to be less than 10% between the sonde and lidar measurements. In addition, comparisons between simultaneous WVMR profiles and aerosol profiles obtained from a simple aerosol backscatter lidar, also located at the CARE facility, provide insight into the complex dynamic mixing of the lower atmosphere and their subsequent impact on climate and air quality.

In July and August 2012, a combination of dry weather and record-breaking temperatures led to an unusually intense wildfire season in Boreal Asia. Based on model results and satellite observations it is thought that a portion of the smoke output from these fires was carried across the Pacific to North America in quantities sufficient to adversely affect air quality in southwestern British Columbia. CORALNet lidar observations taken in Vancouver during these months revealed aerosol layers in the free troposphere followed by relative increases in backscatter ratio within the boundary layer peaking on July 7–10 and again on August 9–15. Depolarization ratios in the boundary layer and for layers in the free troposphere during this period were consistent with high concentrations of smoke. Throughout July and August, Total Suspended Particulate (TSP) monitors throughout the lower Fraser Valley of British Columbia revealed several days with a significant increase in PM2.5 concentrations and nine of the twenty highest daily average PM2.5 concentrations of 2012 coincide with increases in backscatter in the lidar observations indicating that these events were accompanied by a substantial increase in particulate concentrations near the surface.

We describe the design and execution of the BORTAS (Quantifying the impact of BOReal forest fires on Tropospheric oxidants using Aircraft and Satellites) experiment, which has the overarching objective of understanding the chemical aging of airmasses that contain the emission products from seasonal boreal wildfires and how these airmasses 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. The planned July 2010 deployment of the ARA was postponed by 12 months because of activities related to the dispersal of material emitted by the Eyjafjallajökull volcano. However, most other planned model and measurement activities, including ground-based measurements at the Dalhousie University Ground Station (DGS), enhanced ozonesonde launches, and measurements at the Pico Atmospheric Observatory in the Azores, went ahead and constituted phase A of the experiment. Phase B of BORTAS in July 2011 included the same measurements, but included the ARA, special satellite observations and a more comprehensive measurement suite at the DGS. The high-frequency aircraft data provided a comprehensive snapshot of the pyrogenic plumes from wildfires. 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. We coordinated aircraft vertical profiles and overpasses of the NASA Tropospheric Emission Spectrometer and the Canadian Atmospheric Chemistry Experiment. These space-borne data, while less precise than other data, helped to relate the two-week measurement campaign to larger geographical and longer temporal scales. We interpret these data using a range of chemistry models: from a near-explicit gas-phase chemical mechanism, which tests out understanding of the underlying chemical mechanism, to regional and global 3-D models of atmospheric transport and lumped chemistry, which helps to assess the performance of the simplified chemical mechanism and effectively act as intermediaries between different measurement types. We also present an overview of some of the new science that has originated from this project from the mission planning and execution to the analysis of the ground-based, aircraft, and space-borne data.

Among the many well-documented cases of springtime trans-Pacific transport of crustal dust from Asia to North America (significant events include those of 1998, 2001, and 2005), the events of March and April 2010 were extraordinary both in the extent of the dust distribution and in the unique meteorological conditions that caused the dust layers in the free troposphere to linger and be detectable across Canada and the northern United States for over a month. This study focuses on extending previous research by combining data from CORALNet (Canadian Operational Research Aerosol Lidar Network) lidars in Vancouver, BC, and Egbert, ON, with AERONET (AErosol RObotic NETwork) sunphotometer retrievals and model results from HYSPLIT (HYbrid Single-Particle Lagrangian Integrated Trajectory) and NAAPS (Navy Aerosol Analysis and Prediction System) to monitor the arrival and distribution of dust layers across North America. This is the first documented instance of lidar detection of Asian dust from the Egbert CORALNet installation, where layers identified as dust using depolarization ratios corresponded with retrievals of coarse-mode optical depth at the co-located AEROCAN/AERONET site. In Vancouver dust layer depolarization ratios varied from 0.27 for dust above 6 km to less than 0.10 for the first 1.5–2 km above the surface. Similar layers of elevated dust exhibited much lower volume depolarization ratios for all altitudes in Egbert, ON, where maximum depolarization ratios stayed below 0.15 for all layers from 2–8 km with no clear variation with altitude, or over time. The relative lack of variation is an indication that as the layers of dust were transported across North America the rates of change in their optical properties slowed. HYSPLIT back trajectories performed throughout the free troposphere above these sites showed a majority of air parcels originating from central Asia on the days in question. Using these techniques, it was shown that elevated layers of aerosol reaching the west coast of North America as early as 17 March also included dust from the same central Asian sources, extending the known duration of the 2010 event by almost a full month.

The Canadian Network for the Detection of Atmospheric Change and Environment Canada DIAL lidar located at the Polar Environment Atmospheric Research Laboratory (PEARL) in Eureka, Nunavut, has been upgraded to measure water vapour mixing ratio profiles. The lidar is capable of measuring water vapour in the dry Arctic atmosphere up to the tropopause region. Measurements were obtained in the February to March polar sunrise during 2007, 2008 and 2009 as part of the Canadian Arctic ACE (Atmospheric Chemistry Experiment) Validation Campaign. Before such measurements can be used to address important questions in understanding dynamics and chemistry, the lidar measurements must be calibrated against an independent determination of water vapour. Here, radiosonde measurements of relative humidity have been used to empirically calibrate the lidar measurements. It was found that the calibration varied significantly between each year's campaign. However, the calibration of the lidar during an individual polar sunrise campaign agrees on average with the local radiosonde measurements to better than 12%. To independently validate the calibration of the lidar derived from the radiosondes, comparisons are made between the calibrated lidar measurements and water vapour measurements from the ACE satellite-borne Fourier Transform Spectrometer (ACE-FTS). The comparisons between the lidar and satellite-borne spectrometer for both a campaign average and single overpasses show favourable agreement between the two instruments and help validate the lidar's calibration. The 39 nights of high-Arctic water vapour measurements obtained offer the most detailed high spatial-temporal resolution measurement set available for understanding this time of transition from the long polar night to polar day.

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.

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.

A ground-based lidar system that has been deployed in Whistler, British Columbia, Canada, since the spring of 2010 provides a means of evaluating vertical aerosol structure in a mountainous environment. This information is used to help to determine when an air chemistry observatory atop Whistler Mountain (2182 m MSL) is within the free troposphere or is influenced by the valley-based planetary boundary layer (PBL). Three case studies are presented in which 1-day time series images of backscatter data from the lidar are analyzed along with concurrent meteorological and air-chemistry datasets from the mountaintop site. The cases were selected to illustrate different scenarios of diurnal PBL evolution that are expected to be common during their respective seasons. The lidar images corroborate assumptions about PBL influence as derived from analysis of diurnal trends in water vapor, condensation nuclei, and ozone. Use of all of these datasets together bolsters efforts to determine which atmospheric layer the site best represents, which is important when evaluating the provenance of air samples.

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.

Forest fires in Northern California and Oregon were responsible for two significant regional scale aerosol transport events observed in southern British Columbia during summer 2008. A combination of ground based (CORALNet) and satellite (CALIPSO) lidar, sunphotometry and high altitude chemistry observations permitted unprecedented characterization of forest fire plume height and mixing as well as description of optical properties and physicochemistry of the aerosol. In southwestern BC, lidar observations show the smoke to be mixed through a layer extending to 5–6 km a.g.l. where the aerosol was confined by an elevated inversion in both cases. Depolarization ratios for a trans-Pacific dust event (providing a basis for comparison) and the two smoke events were consistent with observations of dust and smoke events elsewhere and permit discrimination of aerosol events in the region. Based on sunphotometry, the Aerosol Optical Thicknesses (AOT) reached maxima of ~0.7 and ~0.4 for the two events respectively. Dubovik-retrieval values of reff, f during both the June/July and August events varied between about 0.13 and 0.15 μm and confirm the dominance of accumulation mode size particles in the forest fire plumes. Both Whistler Peak and Mount Bachelor Observatory data show that smoke events are accompanied by elevated CO and O3 concentrations as well as elevated K+/SO4 ratios. In addition to documenting the meteorology and physic-chemical characteristics of two regional scale biomass burning plumes, this study demonstrates the positive analytical synergies arising from the suite of measurements now in place in the Pacific Northwest, and complemented by satellite borne instruments.

On 30 August 2009, intense forest fires in interior British Columbia (BC) coupled with winds from the east and northeast resulted in transport of a broad forest fire plume across southwestern BC. The physico-chemical and optical characteristics of the plume as observed from Saturna Island (AERONET), CORALNet-UBC and the Whistler Mountain air chemistry facility were consistent with forest fire plumes that have been observed elsewhere in continental North America. However, the importance of three-dimensional transport in relation to the interpretation of mountaintop chemistry observations is highlighted on the basis of deployment of both a CL31 ceilometer and a single particle mass spectrometer (SPMS) in a mountainous setting. The SPMS is used to identify the biomass plume based on levoglucosan and potassium markers. Data from the SPMS are also used to show that the biomass plume was correlated with nitrate, but not correlated with sulphate or sodium. This study not only provides baseline measurements of biomass burning plume physico-chemical characteristics in western Canada, but also highlights the importance of lidar remote sensing methods in the interpretation of mountaintop chemistry measurements.

Aerosol backscatter measurements from a Vaisala CL31 ceilometer are compared directly with a co-located 532/1064 nm lidar in order to validate the CL31 for remote sensing of vertical aerosol structure. The cases examined include a significant aerosol event (biomass burning), which by virtue of its vertical extent, provides a robust measure of the vertical range of the ceilometer for aerosol applications. A second case is presented when the instruments were separated in order to illustrate the utility of a network of such instruments for elucidating spatial patterns in aerosol distribution and the advection of elevated pollutant layers. When co-located, the instruments show remarkable agreement and indicate that the CL31 can detect aerosol layers up to 3000 m AGL in ideal conditions (at night and with high aerosol concentrations as found in biomass burning or dust plumes). When separated, multiple instruments provide an opportunity to examine advection of pollutant layers as well as their evolution. This suggests that installation of a ceilometer network would provide a cost-effective means of examining three-dimensional aspects of regional air quality as well as distinguishing between regional and local sources of pollution

This paper presents extensive validation 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. The ACE satellite instruments operate in the mid-infrared and ultraviolet-visible-near-infrared spectral regions using the solar occultation technique. In order to continue the long-standing record of solar occultation measurements from space, a detailed quality assessment is required to evaluate the ACE data and validate their use for scientific purposes. Here we compare the latest ozone data products from ACE-FTS and ACE-MAESTRO with coincident observations from 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 mean differences range generally between 0 and +10% with a slight but systematic positive bias (typically +5%). At higher altitudes (45-60 km), the ACE-FTS ozone amounts are significantly larger than those of the comparison instruments by up to ~40% (typically +20%). For the ACE-MAESTRO version 1.2 ozone data product, agreement within ±10% (generally better than ±5%) is found between 18 and 40 km for the sunrise and sunset measurements. At higher altitudes (45-55 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 (by as much as -10%), the sunset occultation profiles for ACE-MAESTRO show results that are qualitatively similar to ACE-FTS and indicate a large positive bias (+10 to +30%) in this altitude range. In contrast, there is no significant difference in bias found for the ACE-FTS sunrise and sunset measurements. These systematic effects in the ozone profiles retrieved from the measurements of ACE-FTS and ACE-MAESTRO are being investigated. This work shows that the ACE instruments provide reliable, high quality measurements from the tropopause to the upper stratosphere and can be used with confidence in this vertical domain

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.

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 operate 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.

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 ≈ 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.

[1] Reflectivities recorded by the W-band Cloud Profiling Radar (CPR) aboard NASA's CloudSat satellite and some of CloudSat's retrieval products are compared to Ka-band radar reflectivities and in situ cloud properties gathered by instrumentation on the NRC's Convair-580 aircraft. On 20 February 2007, the Convair flew several transects along a 60 nautical mile stretch of CloudSat's afternoon ground track over southern Quebec. On one of the transects it was well within CloudSat's radar's footprint while in situ sampling a mixed phase boundary layer cloud. A cirrus cloud was also sampled before and after overpass. Air temperature and humidity profiles from ECMWF reanalyses, as employed in CloudSat's retrieval stream, agree very well with those measured by the Convair. The boundary layer cloud was clearly visible, to the eye and lidar, and dominated the region's solar radiation budget. It was, however, often below or near the Ka-band's distance-dependent minimum detectable signal. In situ samples at overpass revealed it to be composed primarily of small, supercooled droplets at the south end and increasingly intermixed with ice northward. Convair and CloudSat CPR reflectivities for the low cloud agree well, but while CloudSat properly ascribed it as overcast, mixed phase, and mostly liquid near the south end, its estimates of liquid water content LWC (and visible extinction coefficient κ) and droplet effective radii are too small and large, respectively. The cirrus consisted largely of irregular crystals with typical effective radii ∼150 μm. While both CPR reflectivities agree nicely, CloudSat's estimates of crystal number concentrations are too large by a factor of 5. Nevertheless, distributions of ice water content and κ deduced from in situ data agree quite well with values retrieved from CloudSat algorithms.

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.

The first documented case of long range transport of Saharan dust over a pathway spanning Asia and the Pacific to Western North America is described. Crustal material generated by North African dust storms during the period 28 February - 3 March 2005 reached western Canada on 13-14 March 2005 and was observed by lidar and sunphotometer in the Vancouver region and by high altitude aerosol instrumentation at Whistler Peak. Global chemical models (GEOS-CHEM and NRL NAAPS) confirm the transport pathway and suggest source attribution was simplified in this case by the distinct, and somewhat unusual, lack of dust activity over Eurasia (Gobi and Takla Makan deserts) at this time. Over western North America, the dust layer, although subsiding close to the boundary layer, did not appear to contribute to boundary layer particulate matter concentrations. Furthermore, sunphotometer observations (and associated inversion products) suggest that the dust layer had only subtle optical impact (Aerosol Optical Thickness (Tau(sub a500)) and Angstrom exponent (Alpha(sub 440-870) were 0.1 and 1.2 respectively) and was dominated by fine particulate matter (modes in aerodynamic diameter at 0.3 and 2.5microns). High Altitude observations at Whistler BC, confirm the crustal origin of the layer (rich in Ca(++) ions) and the bi-modal size distribution. Although a weak event compared to the Asian Trans-Pacific dust events of 1998 and 2001, this novel case highlights the possibility that Saharan sources may contribute episodically to the aerosol burden in western North America.