ALBERT

Description: Wildfires raged throughout western Russia and parts of Eastern Europe during a persistent heat wave in the summer of 2010. Anomalously high surface temperatures (35–41 °C) and low relative humidity (9–25 %) from mid-June to mid-August 2010 shown by analysis of radiosonde data from multiple sites in western Russia were ideal conditions for the wildfires to thrive. Measurements of outgoing longwave radiation (OLR) from the Atmospheric Infrared Sounder (AIRS) over western Russian indicate persistent subsidence during the heat wave. Daily three-day back-trajectories initiated over Moscow reveal a persistent anti-cyclonic circulation for 18 days in August, coincident with the most intense period of fire activity observed by Moderate Resolution Imaging Spectroradiometer (MODIS). This unfortunate meteorological coincidence allowed transport of polluted air from the region of intense fires to Moscow and the surrounding area. We demonstrate that the 2010 Russian wildfires are unique in the record of observations obtained by remote-sensing instruments on-board NASA satellites: Aura and Aqua (part of the A-Train Constellation) and Terra. Analysis of the distribution of MODIS fire products and aerosol optical thickness (AOT), UV aerosol index (AI) and single-scattering albedo (SSA) from Aura's Ozone Monitoring Instrument (OMI), and total column carbon monoxide (CO) from Aqua's Atmospheric Infrared Sounder (AIRS) show that the region in the center of western Russia surrounding Moscow (52°–58° N, 33°–43° E) is most severely impacted by wildfire emissions. Over this area, AIRS CO, OMI AI, and MODIS AOT are significantly enhanced relative to the historical satellite record during the first 18 days in August when the anti-cyclonic circulation persisted. By mid-August, the anti-cyclonic circulation was replaced with westerly transport over Moscow and vicinity. The heat wave ended as anomalies of surface temperature and relative humidity, and OLR disappeared. After 18 August the fire activity greatly diminished over western Russia and levels of the satellite smoke tracers returned to values typical of previous years.

Description: Saharan dust was observed over the Caribbean basin during the summer 2007 NASA Tropical Composition, Cloud, and Climate Coupling (TC4) field experiment. Airborne Cloud Physics Lidar (CPL) and satellite observations from MODIS suggest a barrier to dust transport across Central America into the eastern Pacific. We use the NASA GEOS-5 atmospheric transport model with online aerosol tracers to perform simulations of the TC4 time period in order to understand the nature of this barrier. Our simulations are driven by the Modern Era Retrospective-Analysis for Research and Applications (MERRA) meteorological analyses. Compared to observations from MODIS and CALIOP, GEOS-5 reproduces the observed location and magnitude of observed dust events, but our baseline simulation does not develop as strong a barrier to dust transport across Central America as observations suggest. Analysis of the dust transport dynamics and loss processes suggest that while both mechanisms play a role in defining the dust transport barrier, loss processes by wet removal of dust are about twice as important as transport. Sensitivity analyses with our model showed that the dust barrier would not exist without convective scavenging over the Caribbean. The best agreement between our model and the observations was obtained when dust wet removal was parameterized to be more aggressive, treating the dust as we do hydrophilic aerosols.

Description: We use aircraft observations obtained during the Arctic Research of the Composition of the Troposphere from Aircraft and Satellites (ARCTAS) mission to examine the distributions and source attributions of O3 and NOy in the Arctic and sub-Arctic region. Using a number of marker tracers, we distinguish various air masses from the background troposphere and examine their contributions to NOx, O3, and O3 production in the Arctic troposphere. The background Arctic troposphere has a mean O3 of ~60 ppbv and NOx of ~25 pptv throughout spring and summer with CO decreasing from ~145 ppbv in spring to ~100 ppbv in summer. These observed mixing ratios are not notably different from the values measured during the 1988 ABLE-3A and the 2002 TOPSE field campaigns despite the significant changes in emissions and stratospheric ozone layer in the past two decades that influence Arctic tropospheric composition. Air masses associated with stratosphere-troposphere exchange are present throughout the mid and upper troposphere during spring and summer. These air masses, with mean O3 concentrations of 140–160 ppbv, are significant direct sources of O3 in the Arctic troposphere. In addition, air of stratospheric origin displays net O3 formation in the Arctic due to its sustainable, high NOx (75 pptv in spring and 110 pptv in summer) and NOy (~800 pptv in spring and ~1100 pptv in summer). The air masses influenced by the stratosphere sampled during ARCTAS-B also show conversion of HNO3 to PAN. This active production of PAN is the result of increased degradation of ethane in the stratosphere-troposphere mixed air mass to form CH3CHO, followed by subsequent formation of PAN under high NOx conditions. These findings imply that an adequate representation of stratospheric NOy input, in addition to stratospheric O3 influx, is essential to accurately simulate tropospheric Arctic O3, NOx and PAN in chemistry transport models. Plumes influenced by recent anthropogenic and biomass burning emissions observed during ARCTAS show highly elevated levels of hydrocarbons and NOy (mostly in the form of NOx and PAN), but do not contain O3 higher than that in the Arctic tropospheric background except some aged biomass burning plumes sampled during spring. Convection and/or lightning influences are negligible sources of O3 in the Arctic troposphere but can have significant impacts in the upper troposphere in the continental sub-Arctic during summer.

Description: We derive tropospheric column BrO during the ARCTAS and ARCPAC field campaigns in spring 2008 using retrievals of total column BrO from the satellite UV nadir sensors OMI and GOME-2 using a radiative transfer model and stratospheric column BrO from a photochemical simulation. We conduct a comprehensive comparison of satellite-derived tropospheric BrO column to aircraft in-situ observations of BrO and related species. The aircraft profiles reveal that tropospheric BrO, when present during April 2008, was distributed over a broad range of altitudes rather than being confined to the planetary boundary layer (PBL). Perturbations to the total column resulting from tropospheric BrO are the same magnitude as perturbations due to longitudinal variations in the stratospheric component, so proper accounting of the stratospheric signal is essential for accurate determination of satellite-derived tropospheric BrO. We find reasonably good agreement between satellite-derived tropospheric BrO and columns found using aircraft in-situ BrO profiles, particularly when satellite radiances were obtained over bright surfaces (albedo 〉0.7), for solar zenith angle

Description: Global aerosol distributions provided by the NASA Modern Era Retrospective Analysis for Research and Applications aerosol reanalysis (MERRAero) are evaluated using the aerosol types identified by the CALIOP vertical feature mask (VFM) algorithm, focusing especially on Saharan dust distributions during July 2009. MERRAero is comprised of an aerosol simulation produced in the Goddard Earth Observing System version 5 (GEOS-5) Earth system model and incorporates assimilation of MODIS-derived aerosol optical thickness to constrain column aerosol loadings. For comparison to the CALIOP VFM we construct two synthetic VFMs using the MERRAero aerosol distributions: a Level 2 VFM in which simulated MERRAero total attenuated backscatter and estimated particulate depolarization ratios are input directly to the CALIOP VFM typing algorithm, and a Level 3 VFM in which we map the aerosol species in MERRAero to the CALIOP VFM types. By comparing the simulated MERRAero-Level 2 VFM to CALIOP VFM we can diagnose the aerosol transport and speciation in MERRAero. By comparing the MERRAero-Level 2 and MERRAero-Level 3 simulated VFMs we perform a simple Observing System Simulation Experiment (OSSE), which is useful for identifying shortcomings in the CALIOP VFM algorithm itself. We find that despite having our column AOT constrained by MODIS, comparison to the CALIOP VFM reveals a greater occurrence of dusty aerosol layers in our MERRAero-Level 2 VFM, due to errors in MERRAero aerosol speciation. Additionally, we find that the CALIOP VFM algorithm classification for desert dust and polluted dust should be reconsidered for aerosol features that contain dust mixtures in low aerosol loadings, as our application of the CALIOP VFM to MERRAero distributions flagged a greater presence of dusty vs. marine aerosols when our two MERRAero VFMs were compared.

Description: An aerosol optical depth (AOD) three-dimensional variational data assimilation technique is developed for the Gridpoint Statistical Interpolation (GSI) system for which WRF-Chem forecasts are performed with a detailed sectional model, the Model for Simulating Aerosol Interactions and Chemistry (MOSAIC). Within GSI, forward AOD and adjoint sensitivities are performed using Mie computations from the WRF-Chem optical properties module, providing consistency with the forecast. GSI tools such as recursive filters and weak constraints are used to provide correlation within aerosol size bins and upper and lower bounds for the optimization. The system is used to perform assimilation experiments with fine vertical structure and no data thinning or re-gridding on a 12 km horizontal grid over the region of California, USA, where improvements on analyses and forecasts is demonstrated. A first set of simulations was performed, comparing the assimilation impacts of using the operational MODIS (Moderate Resolution Imaging Spectroradiometer) dark target retrievals to those using observationally constrained ones, i.e., calibrated with AERONET (Aerosol RObotic NETwork) data. It was found that using the observationally constrained retrievals produced the best results when evaluated against ground based monitors, with the error in PM2.5 predictions reduced at over 90% of the stations and AOD errors reduced at 100% of the monitors, along with larger overall error reductions when grouping all sites. A second set of experiments reveals that the use of fine mode fraction AOD and ocean multi-wavelength retrievals can improve the representation of the aerosol size distribution, while assimilating only 550 nm AOD retrievals produces no or at times degraded impact. While assimilation of multi-wavelength AOD shows positive impacts on all analyses performed, future work is needed to generate observationally constrained multi-wavelength retrievals, which when assimilated will generate size distributions more consistent with AERONET data and will provide better aerosol estimates.

Description: 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 ~

Description: We use the NASA GEOS-5 transport model with tagged tracers to investigate the contributions of different regional sources of CO and black carbon (BC) to their concentrations in the Western Arctic (i.e., 50–90° N and 190–320° E) in spring and summer 2008. The model is evaluated by comparing the results with airborne measurements of CO and BC from the NASA Arctic Research of the Composition of the Troposphere from Aircraft and Satellites (ARCTAS) field campaigns to demonstrate the strengths and limitations of our simulations. We also examine the reliability of tagged CO tracers in characterizing air mass origins using the measured fossil fuel tracer of dichloromethane and the biomass burning tracer of acetonitrile. Our tagged CO simulations suggest that most of the enhanced CO concentrations (above background level from CH4 production) observed during April originate from Asian anthropogenic emissions. Boreal biomass burning emissions and Asian anthropogenic emissions are of similar importance in July domain wise, although the biomass burning CO fraction is much larger in the area of the ARCTAS field experiments. The fraction of CO from Asian anthropogenic emissions is larger in spring than in summer. European sources make up no more than 10% of CO levels in the campaign domain during either period. Comparisons of CO concentrations along the flight tracks with regional averages from GEOS-5 show that the along-track measurements are representative of the concentrations within the large domain of the Western Arctic in April but not in July.

Description: We derive estimates of tropospheric BrO column amounts during two Arctic field campaigns in 2008 using information from the satellite UV nadir sensors Ozone Monitoring Instrument (OMI) and the second Global Ozone Monitoring Experiment (GOME-2) as well as estimates of stratospheric BrO columns from a model simulation. The sensitivity of the satellite-derived tropospheric BrO columns to various parameters is investigated using a radiative transfer model. We conduct a comprehensive analysis of satellite-derived tropospheric BrO columns including a detailed comparison with aircraft in-situ observations of BrO and related species obtained during the field campaigns. In contrast to prior expectation, tropospheric BrO, when present, existed over a broad range of altitudes. Our results show reasonable agreement between tropospheric BrO columns derived from the satellite observations and columns found using aircraft in-situ BrO. After accounting for the stratospheric contribution to total BrO column, several events of rapid BrO activation due to surface processes in the Arctic are apparent in both the OMI and GOME-2 based tropospheric columns. The wide orbital swath of OMI allows examination of the evolution of tropospheric BrO on about hourly time intervals near the pole. Low pressure systems, strong surface winds, and high planetary boundary layer heights are associated with the observed tropospheric BrO activation events.

Description: We analyze the aircraft observations obtained during the Arctic Research of the Composition of the Troposphere from Aircraft and Satellite (ARCTAS) mission together with the GEOS-5 CO simulation to examine O3 and NOy in the Arctic and sub-Arctic region and their source attribution. Using a number of marker tracers and their probability density distributions, we distinguish various air masses from the background troposphere and examine their contribution to NOx, O3, and O3 production in the Arctic troposphere. The background Arctic troposphere has mean O3 of ~60 ppbv and NOx of ~25 pptv throughout spring and summer with CO decreases from ~145 ppbv in spring to ~100 ppbv in summer. These observed CO, NOx and O3 mixing ratios are not notably different from the values measured during the 1988 ABLE-3A and the 2002 TOPSE field campaigns despite the significant changes in the past two decades in processes that could have changed the Arctic tropospheric composition. Air masses associated with stratosphere-troposphere exchange are present throughout the mid and upper troposphere during spring and summer. These air masses with mean O3 concentration of 140–160 ppbv are the most important direct sources of O3 in the Arctic troposphere. In addition, air of stratospheric origin is the only notable driver of net O3 formation in the Arctic due to its sustainable high NOx (75 pptv in spring and 110 pptv in summer) and NOy (~800 pptv in spring and ~1100 pptv in summer) levels. The ARCTAS measurements present observational evidence suggesting significant conversion of nitrogen from HNO3 to NOx and then to PAN (a net formation of ~120 pptv PAN) in summer when air of stratospheric origin is mixed with tropospheric background during stratosphere-to-troposphere transport. These findings imply that an adequate representation of stratospheric O3 and NOy input are essential in accurately simulating O3 and NOx photochemistry as well as the atmospheric budget of PAN in tropospheric chemistry transport models of the Arctic. Anthropogenic and biomass burning pollution plumes observed during ARCTAS show highly elevated hydrocarbons and NOy (mostly in the form of NOx and PAN), but do not contribute significantly to O3 in the Arctic troposphere except in some of the aged biomass burning plumes sampled during spring. Convection and/or lightning influences are negligible sources of O3 in the Arctic troposphere but can have significant impacts in the upper troposphere in the continental sub-Arctic during summer.