ALBERT

Description: In the fall of 2017, an airborne field campaign was conducted from the NASA Armstrong Flight Research Center in Palmdale, California, to advance the remote sensing of aerosols and clouds with multi-angle polarimeters (MAP) and lidars. The Aerosol Characterization from Polarimeter and Lidar (ACEPOL) campaign was jointly sponsored by NASA and the Netherlands Institute for Space Research (SRON). Six instruments were deployed on the ER-2 high-altitude aircraft. Four were MAPs: the Airborne Hyper Angular Rainbow Polarimeter (AirHARP), the Airborne Multiangle SpectroPolarimetric Imager (AirMSPI), the Airborne Spectrometer for Planetary EXploration (SPEX airborne), and the Research Scanning Polarimeter (RSP). The remainder were lidars, including the Cloud Physics Lidar (CPL) and the High Spectral Resolution Lidar 2 (HSRL-2). The southern California base of ACEPOL enabled observation of a wide variety of scene types, including urban, desert, forest, coastal ocean, and agricultural areas, with clear, cloudy, polluted, and pristine atmospheric conditions. Flights were performed in coordination with satellite overpasses and ground-based observations, including the Ground-based Multiangle SpectroPolarimetric Imager (GroundMSPI), sun photometers, and a surface reflectance spectrometer. ACEPOL is a resource for remote sensing communities as they prepare for the next generation of spaceborne MAP and lidar missions. Data are appropriate for algorithm development and testing, instrument intercomparison, and investigations of active and passive instrument data fusion. They are freely available to the public. The DOI for the primary database is https://doi.org/10.5067/SUBORBITAL/ACEPOL2017/DATA001 (ACEPOL Science Team, 2017), while for AirMSPI it is https://doi.org/10.5067/AIRCRAFT/AIRMSPI/ACEPOL/RADIANCE/ELLIPSOID_V006 and https://doi.org/10.5067/AIRCRAFT/AIRMSPI/ACEPOL/RADIANCE/TERRAIN_V006 (ACEPOL AirMSPI 75 Science Team, 2017a, b). GroundMSPI data are at https://doi.org/10.5067/GROUND/GROUNDMSPI/ACEPOL/RADIANCE_v009 (GroundMSPI Science Team, 2017). Table 3 lists further details of these archives. This paper describes ACEPOL for potential data users and also provides an outline of requirements for future field missions with similar objectives.

Description: Four summer seasons of nitrogen oxide (NO) concentrations were obtained at the South Pole (SP) during the Sulfur Chemistry in the Antarctic Troposphere (ISCAT) program (1998 and 2000) and the Antarctic Tropospheric Chemistry Investigation (ANTCI) in (2003, 2005, 2006–2007). Together, analyses of the data collected from these studies provide insight into the large- to small-scale meteorology that sets the stage for extremes in NO and the significant variability that occurs day to day, within seasons, and year to year. In addition, these observations reveal the interplay between physical and chemical processes at work in the stable boundary layer of the high Antarctic plateau. We found a systematic evolution of the large-scale wind system over the ice sheet from winter to summer that controls the surface boundary layer and its effect on NO: initially in early spring (Days 280–310) the transport of warm air and clouds over West Antarctica dominates the environment over the SP; in late spring (Days 310–340), the winds at 300 hPa exhibit a bimodal behavior alternating between northwest and southeast quadrants, which is of significance to NO; in early summer (Days 340–375), the flow aloft is dominated by winds from the Weddell Sea; and finally, during late spring, winds aloft from the southeast are strongly associated with clear skies, shallow stable boundary layers, and light surface winds from the east – it is under these conditions that the highest NO occurs. Examination of the winds at 300 hPa from 1961 to 2013 shows that this seasonal pattern has not changed significantly, although the last twenty years have seen an increasing trend in easterly surface winds at the SP. What has also changed is the persistence of the ozone hole, often into early summer. With lower total ozone column density and higher sun elevation, the highest actinic flux responsible for the photolysis of snow nitrate now occurs in late spring under the shallow boundary layer conditions optimum for high accumulation of NO. This may occur via the non-linear HOX–NOx chemistry proposed after the first ISCAT field programs and NOx recycling to the surface where quantum yields may be large under the low-snow-accumulation regime of the Antarctic plateau. During the 2003 field program a sodar made direct measurements of the stable boundary layer depth (BLD), a key factor in explaining the chemistry of the high NO concentrations. Because direct measurements were not available in the other years, we developed an estimator for BLD using direct observations obtained in 2003 and step-wise linear regression with meteorological data from a 22 m tower (that was tested against independent data obtained in 1993). These data were then used with assumptions about the column abundance of NO to estimate surface fluxes of NOx. These results agreed in magnitude with results at Concordia Station and confirmed significant daily, intraseasonal and interannual variability in NO and its flux from the snow surface. Finally, we found that synoptic to mesoscale eddies governed the boundary layer circulation and accumulation pathways for NO at the SP rather than katabatic forcing. It was the small-scale features of the circulation including the transition from cloudy to clear conditions that set the stage for short-term extremes in NO, whereas larger-scale features were associated with more moderate concentrations.

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

Description: We measured levels of ambient volatile organic compounds (VOCs) at seven sites in the Pearl River Delta (PRD) region of China during the Air Quality Monitoring Campaign spanning 4 October to 3 November 2004. Two of the sites, Guangzhou (GZ) and Xinken (XK), were intensive sites at which we collected multiple daily canister samples. The observations reported here provide a look at the VOC distribution, speciation, and photochemical implications in the PRD region. Alkanes constituted the largest percentage (〉40%) in mixing ratios of the quantified VOCs at six sites; the exception was one major industrial site that was dominated by aromatics (about 52%). Highly elevated VOC levels occurred at GZ during two pollution episodes; however, the chemical composition of VOCs did not exhibit noticeable changes during these episodes. We calculated the OH loss rate to estimate the chemical reactivity of all VOCs. Of the anthropogenic VOCs, alkenes played a predominant role in VOC reactivity at GZ, whereas the contributions of reactive aromatics were more important at XK. Our preliminary analysis of the VOC correlations suggests that the ambient VOCs at GZ came directly from local sources (i.e., automobiles); those at XK were influenced by both local emissions and transportation of air mass from upwind areas.

Description: The NASA Studies of Emissions and Atmospheric Composition, Clouds and Climate Coupling by Regional Surveys (SEAC4RS) project included goals related to aerosol particle life cycle in convective regimes. Using the University of Wisconsin High Spectral Resolution Lidar system at Huntsville, Alabama, USA, and the NASA DC-8 research aircraft, we investigate the altitude dependence of aerosol, water vapor and Altocumulus (Ac) properties in the free troposphere from a canonical 12 August 2013 convective storm case as a segue to a presentation of a mission-wide analysis. It stands to reason that any moisture detrainment from convection must have an associated aerosol layer. Modes of covariability between aerosol, water vapor and Ac are examined relative to the boundary layer entrainment zone, 0 ∘C level, and anvil, a region known to contain Ac clouds and a complex aerosol layering structure (Reid et al., 2017). Multiple aerosol layers in regions warmer than 0 ∘C were observed within the planetary boundary layer entrainment zone. At 0 ∘C there is a proclivity for aerosol and water vapor detrainment from storms, in association with melting level Ac shelves. Finally, at temperatures colder than 0 ∘C, weak aerosol layers were identified above Cumulus congestus tops (∼0 and ∼-20 ∘C). Stronger aerosol signals return in association with anvil outflow. In situ data suggest that detraining particles undergo aqueous-phase or heterogeneous chemical or microphysical transformations, while at the same time larger particles are being scavenged at higher altitudes leading to enhanced nucleation. We conclude by discussing hypotheses regarding links to aerosol emissions and potential indirect effects on Ac clouds.

Description: The NASA Studies of Emissions & Atmospheric Composition, Clouds & Climate Coupling by Regional Surveys (SEAC4RS) project included goals related to aerosol particle lifecycle in convective regimes. Using the University of Wisconsin High Spectral Resolution Lidar system at Huntsville, Alabama USA and the NASA DC-8 research aircraft, we investigate the altitude dependence of aerosol, water vapor and Altocumulus (Ac) properties in the free troposphere from a canonical August 12, 2013 convective storm case as a segue to a presentation of a mission wide analysis. It stands to reason that any moisture detrainment from convection must have an associated aerosol layer. Modes of covariability between aerosol, water vapor and Ac are examined relative to the boundary layer entrainment zone, 0 °C level, and anvil, a region known to contain Ac clouds and a complex aerosol layering structure (Reid et al., 2017). Multiple aerosol layers in regions warmer than 0 °C were observed within the PBL entrainment zone. At 0 °C there is a proclivity for aerosol and water vapor detrainment from storms, in association with melting level Ac shelves. Finally, at temperatures colder than 0 °C, weak aerosol layers were identified above Cumulus congestus tops (~0 °C and ~ 20 °C). Stronger aerosol signals return in association with anvil outflow. In situ data suggest that detraining particles undergo aqueous phase or heterogeneous chemical or microphysical transformations, while at the same time larger particles are being scavenged at higher altitudes leading to enhanced nucleation. We conclude by discussing hypotheses regarding links to aerosol emissions and potential indirect effects on Ac clouds.

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

Description: Four summer seasons of nitrogen oxide (NO) concentrations were obtained at the South Pole during the Sulfur Chemistry in the Antarctic Troposphere (ISCAT) program (1998 and 2000) and the Antarctic Tropospheric Chemistry Investigation (ANTCI) in (2003, 2006–7). Together, analyses of their data here provide insight into the large-to-small scale meteorology that sets the stage for high NO and the significant variability that occurs day-to-day, within seasons and year-to-year. In addition, these observations reveal the interplay between physical and chemical processes at work in the stable boundary layer of the high Antarctic plateau. We found a systematic evolution of the large-scale wind system over the ice sheet from winter to summer that controls the surface boundary layer and its effect on NO: Initially in early spring (Days 280–310) the transport of warm air and clouds over West Antarctica dominates the environment over the South Pole; In late spring (Days 310–340), of significance to NO, the winds at 300-hPa exhibit a bimodal behavior alternating between NW and SE; In early summer (Days 340–375), the flow aloft is dominated by winds from the Weddell Sea. During late spring, winds aloft from the SE are strongly associated with clear skies, shallow stable boundary layers, and light surface winds from the east: it is under these conditions that the highest NO occurs. Examination of the winds at 300 hPa from 1961 to 2013 shows that this seasonal pattern has not changed significantly although the last twenty years have seen an increasing trend in easterly surface winds at the South Pole. What has also changed is the persistence of the ozone hole, often into early summer. With lower total ozone column density and higher sun elevation, the highest actinic flux responsible for the photolysis of snow nitrate now occurs in late spring under the shallow boundary layer conditions optimum for high accumulation of NO. This may occur via the non-linear HOX-NOX chemistry proposed after the first ISCAT field programs and NOX recycling to the surface where quantum yields may be large under the low-snow-accumulation regime of the Antarctic plateau. During the 2003 field program a sodar made direct measurements of the stable boundary layer depth (BLD), a key factor in explaining the chemistry of the high NO concentrations. Because direct measurements were not available in the other years, we developed an estimator for BLD using direct observations obtained in 2003 and step-wise linear regression with meteorological data from a 22-m tower (that was tested against independent data obtained in 1993). These data were then used with assumptions about the column abundance of NO to estimate surface fluxes of NOX. These results agreed in magnitude with results at Concordia Station and confirmed significant daily, intraseasonal and interannual variability in NO and its flux from the snow surface. Finally, we found that synoptic to mesoscale eddies governed the boundary layer circulation and accumulation pathways for NO at the South Pole rather than katabatic forcing. It was the small scale features of the circulation including the transition from cloudy to clear conditions that set the stage for short-term extremes in NO whereas larger-scale features were associated with more moderate concentrations.

Description: Radon-222 (222Rn) is a short-lived radioactive gas naturally emitted from land surfaces and has long been used to assess convective transport in atmospheric models. In this study, we simulate 222Rn using the GEOS-Chem chemical transport model to improve our understanding of 222Rn emissions and surface concentration seasonality and characterize convective transport associated with two Goddard Earth Observing System (GEOS) meteorological products, the Modern-Era Retrospective analysis for Research and Applications (MERRA) and GEOS Forward Processing (GEOS-FP). We evaluate four global 222Rn emission scenarios by comparing model results with observations at 51 surface sites. The default emission scenario in GEOS-Chem yields a moderate agreement with surface observations globally (68.9 % of data within a factor of 2) and a large underestimate of winter surface 222Rn concentrations at Northern Hemisphere midlatitudes and high latitudes due to an oversimplified formulation of 222Rn emission fluxes (1 atom cm−2 s−1 over land with a reduction by a factor of 3 under freezing conditions). We compose a new global 222Rn emission scenario based on Zhang et al. (2011) and demonstrate its potential to improve simulated surface 222Rn concentrations and seasonality. The regional components of this scenario include spatially and temporally varying emission fluxes derived from previous measurements of soil radium content and soil exhalation models, which are key factors in determining 222Rn emission flux rates. However, large model underestimates of surface 222Rn concentrations still exist in Asia, suggesting unusually high regional 222Rn emissions. We therefore propose a conservative upscaling factor of 1.2 for 222Rn emission fluxes in China, which was also constrained by observed deposition fluxes of 210Pb (a progeny of 222Rn). With this modification, the model shows better agreement with observations in Europe and North America (〉 80 % of data within a factor of 2) and reasonable agreement in Asia (close to 70 %). Further constraints on 222Rn emissions would require additional concentration and emission flux observations in the central United States, Canada, Africa, and Asia. We also compare and assess convective transport in model simulations driven by MERRA and GEOS-FP using observed 222Rn vertical profiles in northern midlatitude summer and from three short-term airborne campaigns. While simulations with both GEOS products are able to capture the observed vertical gradient of 222Rn concentrations in the lower troposphere (0–4 km), neither correctly represents the level of convective detrainment, resulting in biases in the middle and upper troposphere. Compared with GEOS-FP, MERRA leads to stronger convective transport of 222Rn, which is partially compensated for by its weaker large-scale vertical advection, resulting in similar global vertical distributions of 222Rn concentrations between the two simulations. This has important implications for using chemical transport models to interpret the transport of other trace species when these GEOS products are used as driving meteorology.