Observing Lower-tropospheric Ozone Spatiotemporal Variability with Airborne Lidar and Surface Monitors in Houston, Texas
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Mary Angelique G Demetillo↗
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Observing Lower-Tropospheric Ozone Spatiotemporal Variability with Airborne Lidar and Surface Monitors in Houston, Texas
Explore the source record for details and available documents.
Mary Angelique G Demetillo↗
Low ozone dry deposition rates to sea ice during the MOSAiC field campaign: Implications for the Arctic boundary layer ozone budget
Dry deposition to the surface is one of the main removal pathways of tropospheric ozone (O 3 ). We quantified for the first time the impact of O 3 deposition to the Arctic sea ice on the planetary boundary layer (PBL) O 3 concentration and budget using year-round flux and concentration observations from the Multidisciplinary drifting Observatory for the Study of Arctic Climate (MOSAiC) campaign and simulations with a single-column atmospheric chemistry and meteorological model (SCM). Based on eddy-covariance O 3 surface flux observations, we find a median surface resistance on the order of 20,000 s m –1 , resulting in a dry deposition velocity of approximately 0.005 cm s –1 . This surface resistance is up to an order of magnitude larger than traditionally used values in many atmospheric chemistry and transport models. The SCM is able to accurately represent the yearly cycle, with maxima above 40 ppb in the winter and minima around 15 ppb at the end of summer. However, the observed springtime ozone depletion events are not captured by the SCM. In winter, the modelled PBL O 3 budget is governed by dry deposition at the surface mostly compensated by downward turbulent transport of O 3 towards the surface. Advection, which is accounted for implicitly by nudging to reanalysis data, poses a substantial, mostly negative, contribution to the simulated PBL O 3 budget in summer. During episodes with low wind speed (<5 m s –1 ) and shallow PBL (<50 m), the 7-day mean dry deposition removal rate can reach up to 1.0 ppb h –1 . Our study highlights the importance of an accurate description of dry deposition to Arctic sea ice in models to quantify the current and future O 3 sink in the Arctic, impacting the tropospheric O 3 budget, which has been modified in the last century largely due to anthropogenic activities.
54 ENVIRONMENTAL SCIENCES↗
Analysis of Ozone in Cloudy Versus Clear Sky Conditions
Convection impacts ozone concentrations by transporting ozone vertically and by lofting ozone precursors from the surface, while the clouds and lighting associated with convection affect ozone chemistry. Observations of the above-cloud ozone column (Ziemke et al., 2009) derived from the OMI instrument show geographic variability, and comparison of the above-cloud ozone with all-sky tropospheric ozone columns from OMI indicates important regional differences. We use two global models of atmospheric chemistry, the GMI chemical transport model (CTM) and the GEOS-5 chemistry climate model, to diagnose the contributions of transport and chemistry to observed differences in ozone between areas with and without deep convection, as well as differences in clean versus polluted convective regions. We also investigate how the above-cloud tropospheric ozone from OMI can provide constraints on the relationship between ozone and convection in a free-running climate simulation as well as a CTM.
Cloud↗
The Central Role of Air Quality Observations in NASA's GEOS Composition Forecasting Model
The NASA GEOS composition forecast model (GEOS-CF) provides global, high-resolution (25 km) air quality forecasts in near-real time. This system combines the operational GEOS-5 weather forecasting model with the state-of-the-science GEOS-Chem chemistry module to provide detailed chemical analysis of a wide range of air pollutants such as ozone, carbon monoxide, nitrogen oxides, and fine particulate matter (PM2.5). The resolution of the forecasts is the highest compared to current, publicly-available global composition forecasts.Air quality observations are an indispensable tool to evaluate the model's ability to capture the strong temporal and spatial gradients of air pollutants across the globe. We show how comparisons against near-real time observations available through OpenAQ (www.openaq.org) demonstrate the model's overall success in reproducing surface concentrations of ozone, nitrogen dioxide, and PM2.5. This analysis also helps identifying current limitations of the model, for example over South America. The model-observation mismatches are most likely caused by uncertainties in the emissions data. Using the example of Rio de Janeiro, we show how the model skill can be improved by using local, high-resolution emission inventories in combination with air quality data.
Keller, Christoph A.↗
Stratospheric Ozone Response in Experiments G3 and G4 of the Geoengineering Model Intercomparison Project (GeoMIP)
Geoengineering with stratospheric sulfate aerosols has been proposed as a means of temporarily cooling the planet, alleviating some of the side effects of anthropogenic CO2 emissions. However, one of the known side effects of stratospheric injections of sulfate aerosols is a decrease in stratospheric ozone. Here we show results from two general circulation models and two coupled chemistry climate models that have simulated stratospheric sulfate aerosol geoengineering as part of the Geoengineering Model Intercomparison Project (GeoMIP). Changes in photolysis rates and upwelling of ozone-poor air in the tropics reduce stratospheric ozone, suppression of the NOx cycle increases stratospheric ozone, and an increase in available surfaces for heterogeneous chemistry modulates reductions in ozone. On average, the models show a factor 20-40 increase of the sulfate aerosol surface area density (SAD) at 50 hPa in the tropics with respect to unperturbed background conditions and a factor 3-10 increase at mid-high latitudes. The net effect for a tropical injection rate of 5 Tg SO2 per year is a decrease in globally averaged ozone by 1.1-2.1 DU in the years 2040-2050 for three models which include heterogeneous chemistry on the sulfate aerosol surfaces. GISS-E2-R, a fully coupled general circulation model, performed simulations with no heterogeneous chemistry and a smaller aerosol size; it showed a decrease in ozone by 9.7 DU. After the year 2050, suppression of the NOx cycle becomes more important than destruction of ozone by ClOx, causing an increase in total stratospheric ozone. Contribution of ozone changes in this experiment to radiative forcing is 0.23 W m-2 in GISS-E2-R and less than 0.1 W m-2 in the other three models. Polar ozone depletion, due to enhanced formation of both sulfate aerosol SAD and polar stratospheric clouds, results in an average 5 percent increase in calculated surface UV-B.
aerosol↗
Lusaka, Zambia during SAFARI-2000: A Collection Point for Ozone Pollution
In August and September, throughout south central Africa, seasonal clearing of dry vegetation and other fire-related activities lead to intense smoke haze and ozone formation. The first ozone soundings in the heart of the southern African burning region were taken at Lusaka, Zambia (155 deg S, 28 deg E) in early September 2000. Over 90 ppbv ozone was recorded at the surface (1.3 km elevation) and column tropospheric ozone was greater than 50 DU during a stagnant period. These values are much higher than concurrent measurements over Nairobi (1 deg S, 38 deg E) and Irene (25 deg S, 28 deg E, near Pretoria). The heaviest ozone pollution layer (800-500 hPa) over Lusaka is due to recirculated trans-boundary ozone. Starting out over Zambia, Angola, and Namibia, ozone heads east to the Indian Ocean, before turning back over Mozambique and Zimbabwe, heading toward Lusaka. Thus, Lusaka is a collection point for pollution, consistent with a picture of absolutely stable layers recirculating in a gyre over southern Africa.
Thompson, Anne M.↗
TPSAS-NF1676L-19256-DND
The NASA/GEWEX (Global Energy and Water Exchanges project) Surface Radiation Budget (SRB) project produces longwave and shortwave radiative fluxes for the surface and top-of-atmosphere (TOA) (see, Stackhouse et al., 2011, GEWEX News). The primary inputs of cloud and meteorology data have been undergoing improvements in quality and spatial and temporal resolution. In anticipation of the release of these data, the SRB longwave flux algorithm has been updated both to accommodate these data and to improve the algorithm used in deriving radiative fluxes. Changes in the inputs and algorithm are as follows: - Synchronized algorithm with version used by NASA CERES (Rose et al. 2006). - Atmospheric aerosols were added. - Beta version of ISCCP H cloud properties used. - Beta version of ISCCP nnHIRS temperature and humidity used. - Option of using a newly derived beta Princeton land surface temperature and diurnal Seaflux sea surface temperature as surface skin temperature added - Updated ozone profile with GISS ozone and MEaSUREs GOZCARDS. - Updated maps of surface topography, vegetation type, and snow/ice by ISCCP. The beta GLW v4 IP has enhanced the output fluxes by adding pristine-sky (no clouds or aerosols) fluxes. The new version also computes fluxes at selected atmospheric levels (including the tropopause) rather than just at the surface and TOA. The purpose of this study is to explore the effect of the above changes on the surface and top-of-atmosphere fluxes. These fluxes are compared to the previous version (release 3.1). We show preliminary results for the mid-seasonal months of 2007.
J Colleen Mikovitz↗
Tropospheric Ozone Retrieval By A Combination of TROPOMI/S5P Measurements With BASCOE Assimilated Data
We present a new tropospheric ozone dataset based on TROPOspheric Monitoring Instrument (TROPOMI)/Sentinel-5 Precursor (S5P) total ozone measurements combined with stratospheric ozone data from the Belgian Assimilation System for Chemical ObsErvations (BASCOE) constrained by assimilating ozone observations from the Microwave Limb Sounder (MLS). The BASCOE stratospheric data are interpolated to the S5P observations and subtracted from the TROPOMI total ozone data. The difference is equal to the tropospheric ozone residual column from the surface up to the tropopause. The tropospheric ozone columns are retrieved at the full spatial resolution of the TROPOMI sensor (5.5×3.5 km 2 ) with daily global coverage. Compared to the Ozone Mapping and Profiler Suite Modern-Era Retrospective analysis for Research and Applications 2 (OMPS-MERRA-2) data, a global mean positive bias of 3.3 DU is found for the analysed period April 2018 to June 2020. A small negative bias of about −0.91 DU is observed in the tropics relative to the operational TROPOMI tropical tropospheric data based on the convective cloud differential (CCD) algorithm throughout the same period. The new tropospheric ozone data (S5P-BASCOE) are compared to a set of globally distributed ozonesonde data integrated up to the tropopause level. We found 2254 comparisons with cloud-free TROPOMI observations within 25 km of the stations. In the global mean, S5P-BASCOE deviates by 2.6 DU from the integrated ozonesondes. Depending on the latitude the S5P-BASCOE deviate from the sondes and between −4.8 and 7.9 DU, indicating a good agreement. However, some exceptional larger positive deviations up to 12 DU are found, especially in the northern polar regions (north of 70∘). The monthly mean tropospheric column and time series for selected areas showed the expected spatial and temporal pattern, such as the wave one structure in the tropics or the seasonal cycle, including a summer maximum, in the mid-latitudes.
Satellite Retrieval↗
Evaluating the Impact of Chemical Complexity and Horizontal Resolution on Tropospheric Ozone Over the Conterminous US With a Global Variable Resolution Chemistry Model
A new configuration of the Community Earth System Model (CESM)/Community Atmosphere Model with full chemistry (CAM-chem) supporting the capability of horizontal mesh refinement through the use of the spectral element (SE) dynamical core is developed and called CESM/CAM-chem-SE. Horizontal mesh refinement in CESM/CAM-chem-SE is unique and novel in that pollutants such as ozone are accurately represented at human exposure relevant scales while also directly including global feedbacks. CESM/CAM-chem-SE with mesh refinement down to ∼14 km over the conterminous US (CONUS) is the beginning of the Multi-Scale Infrastructure for Chemistry and Aerosols (MUSICAv0). Here MUSICAv0 is evaluated and used to better understand how horizontal resolution and chemical complexity impact ozone and ozone precursors over CONUS as compared to measurements from five aircraft campaigns, which occurred in 2013. This field campaign analysis demonstrates the importance of using finer horizontal resolution to accurately simulate ozone precursors such as nitrogen oxides and carbon monoxide. In general, the impact of using more complex chemistry on ozone and other oxidation products is more pronounced when using finer horizontal resolution where a larger number of chemical regimes are resolved. Large model biases for ozone near the surface remain in the Southeast US as compared to the aircraft observations even with updated chemistry and finer horizontal resolution. This suggests a need for adding the capability of replacing sections of global emission inventories with regional inventories, increasing the vertical resolution in the planetary boundary layer, and reducing model biases in meteorological variables such as temperature and clouds.
MUSICA↗
The Influence of Ozone: Superstoichiometric Oxygen in Atomic Layer Deposition of Fe 2 O 3 Using tert -Butylferrocene and O 3
Understanding the chemical mechanisms at play in atomic layer deposition (ALD) is critical for effective process development and expansion of ALD into more complex classes of materials. In this work, a mechanistic study of iron oxide deposited by ALD using tert-butylferrocene and ozone as reactants is performed. Iron oxide ALD using ozone is a useful model system for mechanistic studies due to the prevalence of ozone-based ALD processes and the uses of iron oxide in ternary and quaternary metal oxides. Results show that saturation conditions require significantly greater exposures of both reactants than is typically reported in the literature, and growths per cycle of greater than one monolayer of Fe 2 O 3 per cycle are observed and explained. A growth mechanism is proposed whereby increased ozone exposure results in uptake of superstoichiometric oxygen into the film. X-ray characterizations reveal the presence of excess oxygen stored near the surface of films deposited with larger ozone exposures and show that increased ozone exposures cause crystalline domain rearrangement and conversion of the film from the γ-maghemite phase to the α-hematite phase. The mechanism described here has implications for the wider class of ozone-based ALD processes, and potential applications of this growth phenomenon are discussed.
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
Photochemistry of tropospheric ozone
A photochemical equilibrium model of minor constituent chemistry in the troposphere was constructed to investigate the photochemistry of tropospheric ozone. We find that photochemical production must be supplemented by additional sources to account for observed ozone levels in clean air, while photochemical loss is more important than surface destruction as an ozone loss mechanism. Photochemically produced ozone is sensitive to the NO(x) background in the model, exhibiting a maximum of about 0.5 ppb of NO(x).
Stewart, R. W.↗
Initial assessment of the stratospheric and climatic impact of the 1991 Mount Pinatubo eruption - Prologue
An overview is given of the techniques employed to evaluate the early effects of the volcanic eruption on the stratosphere and climate, and data are given on the initial eruption yield. Global satellite measurements were taken by TOMS, SAGE II, AVHRR, and other devices, and the initial results indicate an eruption yield of 20 megatons of SO2 and 20-30 megatons of H2SO4/H2O aerosol mass. The predicted effects of the eruption - accelerated global ozone depletion and surface cooling - can be compared to meteorological data to test the validity of present climate models based on these data.
Mccormick, M. P.↗
Diagnostic studies of the HxOy-NxOy-O3 photochemical system using data from NASA GTE field expeditions
The research effort supported in part by the subject grant focused on three related topics. Our major effort was concentrated on the analysis of data gathered during GTE field expeditions. Ancillary efforts were directed at: the development and application of a Global Chemical Transport Model for the study of the atmospheric reactive nitrogen budget; the development and application of a one-dimensional, time dependent cloud model for the study of the impact of in-cloud aqueous phase chemistry on the atmospheric sulfur budget; and mechanistic studies of the chemical processes involved in dry deposition of ozone to vegetative surfaces. In the sections below, we briefly summarize the central conclusions of each of these efforts. These discussions are followed by a listing of the papers completed during the granting period and the graduate students supported by funds from the grant. Reprints and preprints of all papers completed with support from the grant are attached as appendices.
Chameides, W. L.↗
In situ measurements of ClO at mid-latitudes: Is there an effect from Mt. Pinatubo?
Observations of ClO from 20 to 60 deg N made before and after the eruption of Mt. Pinatubo are compared for changes which may result from increased sulfate aerosol surface area. Using ozone as a vertical coordinate and examining data at similar latitudes and seasons, elevated abundances of ClO are found at low latitudes (20 to 30 deg N), an effect which decreases with increasing latitude. For the flights compared, there appear to be no differences, within the uncertainty of the measurements, at latitudes poleward of 40 deg N. These results are consistent with the idea that the hydrolysis of N2O5 on sulfate aerosols becomes saturated at moderate aerosol loadings.
Avallone, L. M.↗
In Situ Measurements of CLO at Mid-Latitudes: Is there an Effect from Mt. Pinatubo?
Observations of ClO from 20 to 60 deg N made before and after the eruption of Mt. Pinatubo are compared for changes which may result from increased sulfate aerosol surface area. Using ozone as a vertical coordinate and examining data at similar latitudes and seasons, elevated abundances of ClO are found at low latitudes (20 to 30 deg N), an effect which decreases with increasing latitude. For the flights compared, there appear to be no differences, within the uncertainty of the measurements, at latitudes poleward of 40 deg N. These results are consistent with the idea that the hydrolysis of N2O5 on sulfate aerosols becomes saturated at moderate aerosol loadings.
Avallone, L. M.↗
TOMS UV Algorithm: Problems and Enhancements
Satellite instruments provide global maps of surface ultraviolet (UV) irradiance by combining backscattered radiance measurements with radiative transfer models. The models are limited by uncertainties in input parameters of the atmosphere and the surface. We evaluate the effects of possible enhancements of the current Total Ozone Mapping Spectrometer (TOMS) surface UV irradiance algorithm focusing on effects of diurnal variation of cloudiness and improved treatment of snow/ice. The emphasis is on comparison between the results of the current (version 1) TOMS UV algorithm and each of the changes proposed. We evaluate different approaches for improved treatment of pixel average cloud attenuation, with and without snow/ice on the ground. In addition to treating clouds based only on the measurements at the local time of the TOMS observations, the results from other satellites and weather assimilation models can be used to estimate attenuation of the incident UV irradiance throughout the day. A new method is proposed to obtain a more realistic treatment of snow covered terrain. The method is based on a statistical relation between UV reflectivity and snow depth. The new method reduced the bias between the TOMS UV estimations and ground-based UV measurements for snow periods. The improved (version 2) algorithm will be applied to re-process the existing TOMS UV data record (since 1978) and to the future satellite sensors (e.g., Quik/TOMS, GOME, OMI on EOS/Aura and Triana/EPIC).
Krotkov, Nickolay↗
Early Results from AIRS/AMSU/HSB
AIRS was launched on EOS Aqua on May 5, 2002, together with AMSU A and HSB, to form a next generation polar orbiting infiared and microwave atmospheric sounding system. The primary products of AIRS/AMSU/HSB are twice daily global fields of atmospheric temperature-humidity profiles, ozone profiles, sea/land surface skin temperature, and cloud related parameters including OLR. The sounding goals of AIRS are to produce 1 km tropospheric layer mean temperatures with an rms error of lK, and layer precipitable water with an rms error of 20%, in cases with up to 80% effective cloud cover. Pre-launch simulation studies indicated that these results should be achievable. Minor modifications have been made to the pre-launch retrieval algorithm as described in this paper. Sample fields of parameters retrieved from AIRS/AMSU/HSB data are presented and validated as a function of retrieved fractional cloud cover. As in simulation, the degradation of retrieval accuracy with increasing cloud cover is small. Select fields are also compared to those contained in the ECMWF analysis, done without the benefit of AIRS data, to demonstrate information that AIRS can add to that already contained in the ECMWF analysis.
Susskind, Joel↗