ALBERT

Description: 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.

Description: This paper presents a quantitative comparison of the four most commonly used receptor models, namely Absolute Principal Component Scores (APCS), Pragmatic Mass Closure (PMC), Chemical Mass Balance (CMB), and Positive Matrix Factorization (PMF). The models were used to predict the contributions of a wide variety of sources to PM2.5 mass in Halifax, Nova Scotia during the Quantifying the impact of BOReal forest fires on Tropospheric oxidants over the Atlantic using Aircraft and Satellites (BORTAS) experiment. However, particular emphasis was placed on the capacity of the models to predict the boreal wild fire smoke contributions during the BORTAS experiment. Using PMF, a new woodsmoke enrichment factor of 52 was estimated for use in the PMC receptor model. The results indicate that the APCS and PMC receptor models were not able to accurately resolve total PM2.5 mass concentrations below 2.0 μg m−3. CMB was better able to resolve these low PM2.5 concentrations, but it could not be run on 9 of the 45 days of PM2.5 samples. PMF was found to be the most robust of the four models since it was able to resolve PM2.5 mass below 2.0 μg m−3, predict PM2.5 mass on all 45 days, and utilized an unambiguous woodsmoke chemical marker. The median woodsmoke relative contribution to PM2.5 estimated using PMC, APCS, CMB and PMF were found to be 0.08, 0.09, 3.59 and 0.14 μg m−3, respectively. The contribution predicted by the CMB model seems to be clearly too high based on other observations. The use of levoglucosan as a tracer for woodsmoke was found to be vital for identifying this source.

Description: 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.

Description: The source attribution of observed variability of total PM2.5 concentrations over Halifax, Nova Scotia was investigated between 11 July–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 wild fire 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: 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 during the BORTAS-B mission.

Description: During the MILAGRO campaign centered in the Mexico City area, Pacific Northwest National Laboratory (PNNL) and Argonne National Laboratory (ANL) operated atmospheric profiling systems at Veracruz and at two locations on the Central Mexican Plateau in the region around Mexico City. These systems included radiosondes, wind profilers, a sodar, and an aerosol backscatter lidar. An additional wind profiler was operated by the University of Alabama in Huntsville (UAH) at the Mexican Petroleum Institue (IMP) near the center of Mexico City. Because of the opportunity afforded by collocation of profilers, radiosondes, and a lidar, and because of the importance of boundary layer depth for aerosol properties, we have carried out a comparison of mixing layer depth as determined independently from these three types of measurement systems during the campaign. We have then used results of this comparison and additional measurements to develop a detailed description of the daily structure and evolution of the boundary layer on the Central Mexican Plateau during MILAGRO. Our analysis indicates that the profilers were more consistently successful in establishing the mixing layer depth during the daytime. The boundary layer growth was similar at the three locations, although the mixing layer tended to be slightly deeper in the afternoon in central Mexico City. The sodar showed that convection began about an hour after sunrise. Maximum daily mixing layer depths always reached 2000 m a.g.l. and frequently extended to 4000 m. The rate and variability of mixing layer growth was essentially the same as that observed during the IMADA-AVER campaign in the same season in 1997. This growth did not seem to be related to whether deep convection was reported on a given day. Wind speeds within the boundary layer exhibited a daily low-altitude maximum in the late afternoon with lighter winds aloft, consistent with previous reports of diurnal regional circulations. Norte events, which produced high winds at Veracruz, did not appreciably modulate the winds on the plateau. Finally, despite the typically dry conditions at the surface, radiosonde profiles showed that relative humidity often exceeded 50% in the early morning and in the upper part of the boundary layer. This suggests that aerosol particles would have experienced hygroscopic growth within the boundary layer on many days.

Description: The main purpose of the NASA Goddard Space Flight Center TROPospheric OZone DIfferential Absorption Lidar (GSFC TROPOZ DIAL) is to measure the vertical distribution of tropospheric ozone for science investigations. Because of the important health and climate impacts of tropospheric ozone, it is imperative to quantify background photochemical ozone concentrations and ozone layers aloft, especially during air quality episodes. For these reasons, this paper addresses the necessary procedures to validate the TROPOZ retrieval algorithm and confirm that it is properly representing ozone concentrations. This paper is focused on ensuring the TROPOZ algorithm is properly quantifying ozone concentrations, and a following paper will focus on a systematic uncertainty analysis. This methodology begins by simulating synthetic lidar returns from actual TROPOZ lidar return signals in combination with a known ozone profile. From these synthetic signals, it is possible to explicitly determine retrieval algorithm biases from the known profile. This was then systematically performed to identify any areas that need refinement for a new operational version of the TROPOZ retrieval algorithm. One immediate outcome of this exercise was that a bin registration error in the correction for detector saturation within the original retrieval was discovered and was subsequently corrected for. Another noticeable outcome was that the vertical smoothing in the retrieval algorithm was upgraded from a constant vertical resolution to a variable vertical resolution to yield a statistical uncertainty of

Description: The MILAGRO field campaign was a multi-agency international collaborative project to evaluate the regional impacts of the Mexico City air pollution plume as a means of understanding urban impacts on the global climate. Mexico City lies on an elevated plateau with mountains on three sides and has complex mountain and surface-driven wind flows. This paper asks what the wind transport was in the basin during the field campaign and how representative it was of the climatology. Surface meteorology and air quality data, radiosoundings and radar wind profiler data were collected at sites in the basin and its vicinity. Cluster analysis is used to identify the dominant wind patterns both during the campaign and within the past 10 years of operational data from the warm dry season. Our analysis shows that March 2006 was representative of typical flow patterns experienced in the basin. Six episode types were identified for the basin scale circulation providing a way of interpreting atmospheric chemistry and particulate data collected during the campaign. Decoupling between surface winds and those aloft had a strong influence in leading to convection and poor air quality episodes. Hourly characterisation of wind circulation during the MILAGRO, MCMA-2003 and IMADA field campaigns will enable the comparisons of similar air pollution episodes and the evaluation of the impact of wind transport on measurements of the atmospheric chemistry taking place in the basin.

Description: Tropospheric ozone profiles have been retrieved from the new ground-based National Aeronautics and Space Administration (NASA) Goddard Space Flight Center TROPospheric OZone DIfferential Absorption Lidar (GSFC TROPOZ DIAL) in Greenbelt, MD (38.99° N, 76.84° W, 57 m a.s.l.), from 400 m to 12 km a.g.l. Current atmospheric satellite instruments cannot peer through the optically thick stratospheric ozone layer to remotely sense boundary layer tropospheric ozone. In order to monitor this lower ozone more effectively, the Tropospheric Ozone Lidar Network (TOLNet) has been developed, which currently consists of five stations across the US. The GSFC TROPOZ DIAL is based on the DIAL technique, which currently detects two wavelengths, 289 and 299 nm, with multiple receivers. The transmitted wavelengths are generated by focusing the output of a quadrupled Nd:YAG laser beam (266 nm) into a pair of Raman cells, filled with high-pressure hydrogen and deuterium, using helium as buffer gas. With the knowledge of the ozone absorption coefficient at these two wavelengths, the range-resolved number density can be derived. An interesting atmospheric case study involving the stratospheric–tropospheric exchange (STE) of ozone is shown, to emphasize the regional importance of this instrument as well as to assess the validation and calibration of data. There was a low amount of aerosol aloft, and an iterative aerosol correction has been performed on the retrieved data, which resulted in less than a 3 ppb correction to the final ozone concentration. The retrieval yields an uncertainty of 16–19% from 0 to 1.5 km, 10–18% from 1.5 to 3 km, and 11–25% from 3 to 12 km according to the relevant aerosol concentration aloft. There are currently surface ozone measurements hourly and ozonesonde launches occasionally, but this system will be the first to make routine tropospheric ozone profile measurements in the Baltimore–Washington, D.C. area.

Description: Tropospheric ozone profiles have been retrieved from the new ground based National Aeronautics and Space Administration (NASA) Goddard Space Flight Center TROPospheric OZone DIfferential Absorption Lidar (GSFC TROPOZ DIAL) in Greenbelt, MD (38.99° N, 76.84° W, 57 m a.s.l.) from 400 m to 12 km a.g.l. Current atmospheric satellite instruments cannot peer through the optically thick stratospheric ozone layer to remotely sense boundary layer tropospheric ozone. In order to monitor this lower ozone more effectively, the Tropospheric Ozone Lidar Network (TOLNet) has been developed, which currently consists of five stations across the US. The GSFC TROPOZ DIAL is based on the Differential Absorption Lidar (DIAL) technique, which currently detects two wavelengths, 289 and 299 nm. Ozone is absorbed more strongly at 289 nm than at 299 nm. The DIAL technique exploits this difference between the returned backscatter signals to obtain the ozone number density as a function of altitude. The transmitted wavelengths are generated by focusing the output of a quadrupled Nd:YAG laser beam (266 nm) into a pair of Raman cells, filled with high pressure hydrogen and deuterium. Stimulated Raman Scattering (SRS) within the focus generates a significant fraction of the pump energy at the first Stokes shift. With the knowledge of the ozone absorption coefficient at these two wavelengths, the range resolved number density can be derived. An interesting atmospheric case study involving the Stratospheric–Tropospheric Exchange (STE) of ozone is shown to emphasize the regional importance of this instrument as well as assessing the validation and calibration of data. The retrieval yields an uncertainty of 16–19% from 0–1.5 km, 10–18% from 1.5–3 km, and 11–25% from 3 km to 12 km. There are currently surface ozone measurements hourly and ozonesonde launches occasionally, but this system will be the first to make routine tropospheric ozone profile measurements in the Baltimore–Washington DC area.

Description: The Super Dual Auroral Radar Network (SuperDARN) network of HF coherent backscatter radars form a unique global diagnostic of large-scale ionospheric and magnetospheric dynamics in the Northern and Southern Hemispheres. Currently the ground projections of the HF radar returns are routinely determined by a simple rangefinding algorithm, which takes no account of the prevailing, or indeed the average, HF propagation conditions. This is in spite of the fact that both direct E- and F-region backscatter and 1½-hop E- and F-region backscatter are commonly used in geophysical interpretation of the data. In a companion paper, Chisham et al. (2008) have suggested a new virtual height model for SuperDARN, based on average measured propagation paths. Over shorter propagation paths the existing rangefinding algorithm is adequate, but mapping errors become significant for longer paths where the roundness of the Earth becomes important, and a correct assumption of virtual height becomes more difficult. The SuperDARN radar at Hankasalmi has a propagation path to high power HF ionospheric modification facilities at both Tromsø on a ½-hop path and SPEAR on a 1½-hop path. The SuperDARN radar at Þykkvibǽr has propagation paths to both facilities over 1½-hop paths. These paths provide an opportunity to quantitatively test the available SuperDARN virtual height models. It is also possible to use HF radar backscatter which has been artificially induced by the ionospheric heaters as an accurate calibration point for the Hankasalmi elevation angle of arrival data, providing a range correction algorithm for the SuperDARN radars which directly uses elevation angle. These developments enable the accurate mappings of the SuperDARN electric field measurements which are required for the growing number of multi-instrument studies of the Earth's ionosphere and magnetosphere.