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Linear depolarization measurement capabilities were added to the CANDAC Rayleigh–Mie–Raman lidar (CRL) at Eureka, Nunavut, in the Canadian High Arctic in 2010. This upgrade enables measurements of the phases (liquid versus ice) of cold and mixed-phase clouds throughout the year, including during polar night. Depolarization measurements were calibrated according to existing methods using parallel- and perpendicular-polarized profiles as discussed in ). We present a new technique that uses the polarization-independent Rayleigh elastic channel in combination with one of the new polarization-dependent channels, and we show that for a lidar with low signal in one of the polarization-dependent channels this method is superior to the traditional method. The optimal procedure for CRL is to determine the depolarization parameter using the traditional method at low resolution (from parallel and perpendicular signals) and then to use this value to calibrate the high-resolution new measurements (from parallel and polarization-independent Rayleigh elastic signals). Due to its use of two high-signal-rate channels, the new method has lower statistical uncertainty and thus gives depolarization parameter values at higher spatial–temporal resolution by up to a factor of 20 for CRL. This method is easily adaptable to other lidar systems which are considering adding depolarization capability to existing hardware.

The Canadian Network for the Detection of Atmospheric Change (CANDAC) Rayleigh–Mie–Raman lidar (CRL) at Eureka, Nunavut, has measured tropospheric clouds, aerosols, and water vapour since 2007. In remote and meteorologically significant locations, such as the Canadian High Arctic, the ability to add new measurement capability to an existing well-tested facility is extremely valuable. In 2010, linear depolarization 532 nm measurement hardware was installed in the lidar's receiver. To minimize disruption in the existing lidar channels and to preserve their existing characterization so far as is possible, the depolarization hardware was placed near the end of the receiver cascade. The upstream optics already in place were not optimized for preserving the polarization of received light. Calibrations and Mueller matrix calculations are used to determine and mitigate the contribution of these upstream optics on the depolarization measurements. The results show that with appropriate calibration, indications of cloud particle phase (ice vs. water) through the use of the depolarization parameter are now possible to a precision of ±0.05 absolute uncertainty ( ≤ 10 % relative uncertainty) within clouds at time and altitude resolutions of 5 min and 37.5 m respectively, with higher precision and higher resolution possible in select cases. The uncertainty is somewhat larger outside of clouds at the same altitude, typically with absolute uncertainty ≤ 0.1. Monitoring changes in Arctic cloud composition, including particle phase, is essential for an improved understanding of the changing climate locally and globally.

We compared star-photometry-derived, polar winter aerosol optical depths (AODs), acquired at Eureka, Nunavut, Canada, and Ny-Ålesund, Svalbard, with GEOS-Chem (GC) simulations as well as ground-based lidar and CALIOP (Cloud-Aerosol Lidar with Orthogonal Polarization) retrievals over a sampling period of two polar winters. The results indicate significant cloud and/or low-altitude ice crystal (LIC) contamination which is only partially corrected using temporal cloud screening. Spatially homogeneous clouds and LICs that remain after temporal cloud screening represent an inevitable systematic error in the estimation of AOD: this error was estimated to vary from 78 to 210 % at Eureka and from 2 to 157 % at Ny-Ålesund. Lidar analysis indicated that LICs appeared to have a disproportionately large influence on the homogeneous coarse-mode optical depths that escape temporal cloud screening. In principle, spectral cloud screening (to yield fine-mode or submicron AODs) reduces pre-cloud-screened AODs to the aerosol contribution if one assumes that coarse-mode (super-micron) aerosols are a minor part of the AOD. Large, low-frequency differences between these retrieved values and their GC analogue appeared to be often linked to strong, spatially extensive planetary boundary layer events whose presence at either site was inferred from CALIOP profiles. These events were either not captured or significantly underestimated by the GC simulations. High-frequency AOD variations of GC fine-mode aerosols at Ny-Ålesund were attributed to sea salt, while low-frequency GC variations at Eureka and Ny-Ålesund were attributable to sulfates. CALIOP profiles and AODs were invaluable as spatial and temporal redundancy support (or, alternatively, as insightful points of contention) for star photometry retrievals and GC estimates of AOD.

A new microwave satellite water vapour retrieval for the polar winter atmosphere is presented. The retrieval builds on the work of Miao et al. (2001) and Melsheimer and Heygster (2008), employing auxiliary information for atmospheric conditions and numerical optimization. It was tested using simulated and actual measurements from the Microwave Humidity Sounder (MHS) satellite instruments. Ground truth was provided by the G-band vapour radiometer (GVR) at Barrow, Alaska. For water vapour columns less than 6 kg m−2, comparisons between the retrieval and GVR result in a root mean square (RMS) deviation of 0.39 kg m−2 and a systematic bias of 0.08 kg m−2. These results are compared with RMS deviations and biases at Barrow for the retrieval of Melsheimer and Heygster (2008), the AIRS and MIRS satellite data products, and the ERA-Interim, NCEP, JRA-55, and ASR reanalyses. When applied to MHS measurements, the new retrieval produces a smaller RMS deviation and bias than for the earlier retrieval and satellite data products. The RMS deviations for the new retrieval were comparable to those for the ERA-Interim, JRA-55, and ASR reanalyses; however, the MHS retrievals have much finer horizontal resolution (15 km at nadir) and reveal more structure. The new retrieval can be used to obtain pan-Arctic maps of water vapour columns of unprecedented quality. It may also be applied to measurements from the Special Sensor Microwave/Temperature 2 (SSM/T2), Advanced Microwave Sounding Unit B (AMSU-B), Special Sensor Microwave Imager/Sounder (SSMIS), Advanced Technology Microwave Sounder (ATMS), and Chinese MicroWave Humidity Sounder (MWHS) instruments.

We present recent progress on nighttime retrievals of aerosol and cloud optical properties over the PEARL (Polar Environmental Atmospheric Research Laboratory) station at Eureka (Nunavut, Canada) in the High Arctic (80° N, 86° W). In the spring of 2011 and 2012, a star photometer was employed to acquire aerosol optical depth (AOD) data, while vertical aerosol and cloud backscatter profiles were measured using the CANDAC Raman Lidar (CRL). We used a simple backscatter coefficient threshold (βthr) to distinguish aerosols from clouds and, assuming that aerosols were largely fine mode (FM)/sub-micron, to distinguish FM aerosols from coarse mode (CM)/super-micron cloud or crystal particles. Using prescribed lidar ratios, we computed FM and CM AODs that were compared with analogous AODs estimated from spectral star photometry. We found (βthr dependent) coherences between the lidar and star photometer for both FM events and CM cloud and crystal events with averaged, FM absolute differences being R2 values were between 0.2 and 0.8. A βthr sensitivity study demonstrated that zero crossing absolute differences and R2 peaks were in comparable regions of the βthr range (or physical reasons were given for their disparity). The utility of spectral vs. temporal cloud screening of star photometer AODs was also illustrated. In general our results are critical to building confidence in the physical fidelity of derived, weak amplitude, star photometry AODs and, in turn, towards the development of AOD climatologies and validation databases for polar winter models and satellite sensors.

Biomass-burning aerosols contribute to aerosol radiative forcing on the climate system. The magnitude of this effect is partially determined by aerosol size distributions, which are functions of source fire characteristics (e.g. fuel type, MCE) and in-plume microphysical processing. The uncertainties in biomass-burning emission number–size distributions in climate model inventories lead to uncertainties in the CCN (cloud condensation nuclei) concentrations and forcing estimates derived from these models. The BORTAS-B (Quantifying the impact of BOReal forest fires on Tropospheric oxidants over the Atlantic using Aircraft and Satellite) measurement campaign was designed to sample boreal biomass-burning outflow over eastern Canada in the summer of 2011. Using these BORTAS-B data, we implement plume criteria to isolate the characteristic size distribution of aged biomass-burning emissions (aged ~ 1–2 days) from boreal wildfires in northwestern Ontario. The composite median size distribution yields a single dominant accumulation mode with Dpm = 230 nm (number-median diameter) and σ = 1.5, which are comparable to literature values of other aged plumes of a similar type. The organic aerosol enhancement ratios (ΔOA / ΔCO) along the path of Flight b622 show values of 0.09–0.17 μg m−3 ppbv−1 (parts per billion by volume) with no significant trend with distance from the source. This lack of enhancement ratio increase/decrease with distance suggests no detectable net OA (organic aerosol) production/evaporation within the aged plume over the sampling period (plume age: 1–2 days), though it does not preclude OA production/loss at earlier stages. A Lagrangian microphysical model was used to determine an estimate of the freshly emitted size distribution corresponding to the BORTAS-B aged size distributions. The model was restricted to coagulation and dilution processes based on the insignificant net OA production/evaporation derived from the ΔOA / ΔCO enhancement ratios. We estimate that the young-plume median diameter was in the range of 59–94 nm with modal widths in the range of 1.7–2.8 (the ranges are due to uncertainty in the entrainment rate). Thus, the size of the freshly emitted particles is relatively unconstrained due to the uncertainties in the plume dilution rates.

We present measurements of a long-range smoke transport event recorded on 20–21 July 2011 over Halifax, Nova Scotia, Canada, during the Quantifying the impact of BOReal forest fires on Tropospheric oxidants over the Atlantic using Aircraft and Satellites (BORTAS-B) campaign. Ground-based Fourier transform spectrometers and photometers detected air masses associated with large wildland fires burning in eastern Manitoba and western Ontario. We investigate a plume with high trace gas amounts but low amounts of particles that preceded and overlapped at the Halifax site with a second plume with high trace gas loadings and significant amounts of particulate material. We show that the first plume experienced a meteorological scavenging event, but the second plume had not been similarly scavenged. This points to the necessity to account carefully for the plume history when considering long-range transport since simultaneous or near-simultaneous times of arrival are not necessarily indicative of either similar trajectories or meteorological history. We investigate the origin of the scavenged plume, and the possibility of an aerosol wet deposition event occurring in the plume ~ 24 h prior to the measurements over Halifax. The region of lofting and scavenging is only monitored on an intermittent basis by the present observing network, and thus we must consider many different pieces of evidence in an effort to understand the early dynamics of the plume. Through this discussion we also demonstrate the value of having many simultaneous remote-sensing measurements in order to understand the physical and chemical behaviour of biomass burning plumes.

We present the results of total column measurements of CO, C2H6 and fine-mode aerosol optical depth (AOD) during the "Quantifying the impact of BOReal forest fires on Tropospheric oxidants over the Atlantic using Aircraft and Satellites" (BORTAS-B) campaign over eastern Canada. Ground-based observations, using Fourier transform spectrometers (FTSs) and sun photometers, were carried out in July and August 2011. These measurements were taken in Halifax, Nova Scotia, which is an ideal location to monitor the outflow of boreal fires from North America, and also in Toronto, Ontario. Measurements of fine-mode AOD enhancements were highly correlated with enhancements in coincident trace gas (CO and C2H6) observations between 19 and 21 July 2011, which is typical for a smoke plume event. In this paper, we focus on the identification of the origin and the transport of this smoke plume. We use back trajectories calculated by the Canadian Meteorological Centre as well as FLEXPART forward trajectories to demonstrate that the enhanced CO, C2H6 and fine-mode AOD seen near Halifax and Toronto originated from forest fires in northwestern Ontario that occurred between 17 and 19 July 2011. In addition, total column measurements of CO from the satellite-borne Infrared Atmospheric Sounding Interferometer (IASI) have been used to trace the smoke plume and to confirm the origin of the CO enhancement. Furthermore, the enhancement ratio – that is, in this case equivalent to the emission ratio (ERC2H6/CO) – was estimated from these ground-based observations. These C2H6 emission results from boreal fires in northwestern Ontario agree well with C2H6 emission measurements from other boreal regions, and are relatively high compared to fires from other geographical regions. The ground-based CO and C2H6 observations were compared with outputs from the 3-D global chemical transport model GEOS-Chem, using the Fire Locating And Modeling of Burning Emissions (FLAMBE) inventory. Agreement within the stated measurement uncertainty (~3% for CO and ~8% for C2H6) was found for the magnitude of the enhancement of the CO and C2H6 total columns between the measured and modelled results. However, there is a small shift in time (of approximately 6 h) of arrival of the plume over Halifax between the results.

The source attribution of observed variability of total PM2.5 concentrations over Halifax, Nova Scotia, was investigated between 11 July and 26 August 2011 using measurements of PM2.5 mass and PM2.5 chemical composition (black carbon, organic matter, anions, cations and 33 elements). This was part of the BORTAS-B (quantifying the impact of BOReal forest fires on Tropospheric oxidants using Aircraft and Satellites) experiment, which investigated the atmospheric chemistry and transport of seasonal boreal wildfire emissions over eastern Canada in 2011. The US EPA Positive Matrix Factorization (PMF) receptor model was used to determine the average mass (percentage) source contribution over the 45 days, which was estimated to be as follows: long-range transport (LRT) pollution: 1.75 μg m−3 (47%); LRT pollution marine mixture: 1.0 μg m−3 (27.9%); vehicles: 0.49 μg m−3 (13.2%); fugitive dust: 0.23 μg m−3 (6.3%); ship emissions: 0.13 μg m−3 (3.4%); and refinery: 0.081 μg m−3 (2.2%). The PMF model describes 87% of the observed variability in total PM2.5 mass (bias = 0.17 and RSME = 1.5 μg m−3). The factor identifications are based on chemical markers, and they are supported by air mass back trajectory analysis and local wind direction. Biomass burning plumes, found by other surface and aircraft measurements, were not significant enough to be identified in this analysis. This paper presents the results of the PMF receptor modelling, providing valuable insight into the local and upwind sources impacting surface PM2.5 in Halifax and a vital comparative data set for the other collocated ground-based observations of atmospheric composition made during BORTAS-B.

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.

As a consequence of dynamically variable meteorological conditions, springtime Arctic ozone levels exhibit significant interannual variability in the lower stratosphere. In winter 2011, the polar vortex was strong and cold for an unusually long time. Our research site, located at Eureka, Nunavut, Canada (80.05° N, 86.42° W), was mostly inside the vortex from October 2010 until late March 2011. The Bruker 125HR Fourier transform infrared spectrometer installed at the Polar Environment Atmospheric Research Laboratory at Eureka acquired measurements from 23 February to 6 April during the 2011 Canadian Arctic Atmospheric Chemistry Experiment Validation Campaign. These measurements showed unusually low ozone, HCl, and HNO3 total columns compared to the previous 14 yr. To remove dynamical effects, we normalized these total columns by the HF total column. The normalized values of the ozone, HCl, and HNO3 total columns were smaller than those from previous years, and confirmed the occurrence of chlorine activation and chemical ozone depletion. To quantify the chemical ozone loss, a three-dimensional chemical transport model, SLIMCAT, and the passive subtraction method were used. The chemical ozone depletion was calculated as the mean percentage difference between the measured ozone and the SLIMCAT passive ozone, and was found to be 35%.

A climatology of particle scattering properties in the wintertime High Arctic troposphere, including vertical distributions and effective radii, is presented. The measurements were obtained using a lidar and cloud radar located at Eureka, Nunavut Territory (80° N, 86° W). Four different particle groupings are considered: boundary-layer ice crystals, ice clouds, mixed-phase clouds, and aerosols. Two-dimensional histograms of occurrence probabilities against depolarization, radar/lidar colour ratio and height are given. Colour ratios are related to particle minimum dimensions (i.e., widths rather than lengths) using a Mie scattering model. Ice cloud crystals have effective radii spanning 25–220 µm, with larger particles observed at lower altitudes. Topographic blowing snow residuals in the boundary layer have the smallest crystals at 15–70 µm. Mixed-phase clouds have water droplets and ice crystal precipitation in the 5–40 µm and 40–220 µm ranges, respectively. Ice cloud crystals have depolarization decreasing with height. The depolarization trend is associated with the large ice crystal sub-population. Small crystals depolarize more than large ones in ice clouds at a given altitude, and show constant modal depolarization with height. Ice clouds in the mid-troposphere are sometimes observed to precipitate to the ground. Water clouds are constrained to the lower troposphere (0.5–3.5 km altitude). Aerosols are most abundant near the ground and are frequently mixed with the other particle types. The data are used to construct a classification chart for particle scattering in wintertime Arctic conditions.

Ice crystals, also known as diamond dust, are suspended in the boundary layer air under clear sky conditions during most of the Arctic winter in Northern Canada. Occasionally ice crystal events can produce significantly thick layers with optical depths in excess of 2.0 even in the absence of liquid water clouds. Four case studies of high optical depth ice crystal events at Eureka in the Nunavut Territory of Canada during the winter of 2006/07 are presented. They show that the measured ice crystal surface infrared downward radiative forcing ranged from 8 to 36 W m−2 in the wavelength band from 5.6 to 20 μm for 532 nm optical depths ranging from 0.2 to 1.7. MODIS infrared and visible images and the operational radiosonde wind profile were used to show that these high optical depth events were caused by surface snow being blown off 600 to 800 m high mountain ridges about 20 to 30 km North-West of Eureka and advected by the winds towards Eureka as they settled towards the ground within the highly stable boundary layer. This work presents the first study that demonstrates the important role that surrounding topography plays in determining the occurrence of high optical depth ice crystal events from residual blowing snow that becomes a source of boundary layer ice crystals distinct from the classical diamond dust phenomenon.