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At least 73 records · Page 4

Ozone measurements from a global network of surface sites

From a network of surface ozone monitoring sites distributed primarily over the Atlantic and Pacific Oceans, the seasonal, day-to-day, and diurnal patterns are delineated. At most of the NH (Northern Hemisphere) sites there is a spring maximum and late summer or autumn minimum. At Barrow, AK (70 deg N) and Barbados (14 deg N), however, there is a winter maximum, but the mechanisms producing the maximum are quite different. All the sites in the SH (Southern Hemisphere) show winter maxima and summer minima. At the subtropical and tropical sites, there are large day-to-day variations that reflect the changes in flow patterns. Air of tropical origin has much lower ozone concentrations than air from higher latitudes. At the two tropical sites (Barbados and Samoa), there is a marked diurnal ozone variation with highest amounts in the early morning and lowest values in the afternoon. At four of the locations (Barrow, AK; Mauna Loa, HI; American Samoa; and South Pole), there are 15- through 20-year records which allow us to look at longer term changes. At Barrow there has been a large summer increase over the 20 years of measurements. At South Pole, on the other hand, summer decreases have led to an overall decline in surface ozone amounts.

Oltmans, Samuel J.↗

An analysis of the impacts of global climate and emissions changes on regional tropospheric ozone

Many of the synergistic impacts resulting from future changes in emissions as well as changes in ambient temperature, moisture, and UV flux have not been quantified. A three-dimensional regional-scale photo-chemical model (STEM-2) is used in this study to evaluate these perturbations to trace gas cycles over the eastern half of the United States of America. The model was successfully used to simulate a regional-scale ozone episode (base case - June 1984) and four perturbations scenarios - viz., perturbed emissions, temperature, water vapor column, and incoming UV flux cases, and a future scenario (for the year 2034). The impact of these perturbation scenarios on the distribution of ozone and other major pollutants such as SO2 and sulfates were analyzed in detail. The spatial distribution and the concentration of ozone at the surface increased by about 5-15 percent for most cases except for the perturbed water vapor case. The regional scale surface ozone concentration distribution for the year 2034 (future scenario) showed an increase of non-attainment areas. The rural areas of Pennsylvania, West Virginia, and Georgia showed the largest change in the surface ozone field for the futuristic scenario when compared to the base case.

John, Kuruvilla↗

The impact of Los Angeles Basin pollution and stratospheric intrusions on the surrounding San Gabriel Mountains as seen by surface measurements, lidar, and numerical models

In this work, the impact of Los Angeles Basin pollution transport and stratospheric intrusions on the surface ozone levels observed in the San Gabriel Mountains is investigated based on a combination of surface and lidar measurements as well as WRF-Chem (Weather Research and Forecasting with Chemistry) and WACCM (Whole Atmosphere Community Climate Model) runs. The number of days with observed surface ozone levels exceeding the National Ambient Air Quality Standards exhibit a clear seasonal pattern, with a maximum during summer, when models suggest a minimum influence of stratospheric intrusions and the largest impact from Los Angeles Basin pollution transport. Additionally, measured and modeled surface ozone and PM10 were analyzed as a function of season, time of the day, and wind direction. Measurements and models are in good qualitative agreement, with maximum surface ozone observed for southwest and west winds. For the prevailing summer wind direction, slightly south of the ozone maximum and corresponding to south-southwest winds, lower ozone levels were observed. Back trajectories suggest that this is associated with transport from the central Los Angeles Basin, where titration limits the amount of surface ozone. A quantitative comparison of the lidar profiles with WRF-Chem and WACCM models revealed good agreement near the surface, with models showing an increasing positive bias as function of altitude, reaching 75 % at 15 km above sea level. Finally, three selected case studies covering the different mechanisms affecting the near-surface ozone concentration over the San Gabriel Mountains, namely stratospheric intrusions and pollution transport, are analyzed based on surface and ozone lidar measurements, as well as co-located ceilometer measurements and models.

Impact↗

How Well Satellite Remote Sensing Can Inform Surface Level Ozone Production Sensitivity to Precursor Trace Gas Emissions?

Surface-level ozone (O3) pollution mitigation strategies rely on a clear understanding of the atmospheric chemical processes involving O3, NOx (nitric oxide (NO) + nitrogen dioxide (NO2)) and volatile organic compounds (VOCs). A robust spatiotemporal classification of O3 photochemical regimes with relative chemical sensitivity of local O3 formation to emission reductions of NOx (NOx-limited regime) versus VOCs (radical-limited regime) is required to design anthropogenic emission reduction policies in order to improve surface air quality. Numerous studies found that the ratio of satellite-retrieved Vertical Column Densities (VCDs) of formaldehyde (HCHO) to NO2 can diagnose O3 production sensitivity. However, uncertainty still remains about the accuracy of such estimates using satellite-based retrievals. This study conducts an investigation to identify how well satellite data can inform surface-level O3 sensitivity by validating satellite-based estimates against aircraft-based retrievals taken during the Long Island Sound Tropospheric Ozone Study (LISTOS-2018) and Ozone Water-Land Environmental Transition Study (OWLETS-2) field campaigns. For this study, we use HCHO and NO2 retrievals from the Ozone Monitoring Instrument (OMI) onboard the Aura satellite, and high spatiotemporal resolution TROPOspheric Monitoring Instrument (TROPOMI) onboard the Sentinel-5 Precursor (S5P) satellite. The Community Multiscale Air Quality (CMAQ) modelling system is used to provide trace gas vertical profiles to recalculate air mass factor for deriving consistent satellite-based VCDs. To demonstrate the ability of satellites to diagnose O3 production regimes, we validate satellite-derived O3 sensitivity regimes, along with the OMI and TROPOMI products applied, using HCHO and NO2 retrievals from the aircraft-based instruments: Geostationary Trace gas and Aerosol Sensor Optimization (GeoTASO) spectrometer and Geostationary Coastal and Air Pollution Events Airborne Simulator (GCAS) instruments deployed during the LISTOS-2018 and OWLETS-2 campaigns. The results of this work will advance our fundamental knowledge of the spatiotemporal evolution of the complex O3-NOx-VOC chemistry, and will advance our understanding about the quality of remote-sensing, suborbital, and satellite data for accurately observing surface-level O3 production sensitivity.

Satellite↗

Evaluation of the production and the destruction of ozone in the lower atmosphere

Observed surface ozone mixing ratio X(sub ob) is partitioned into two parts; X(sub tr), transported from the free troposphere and X(sub ch), chemically produced or destructed in the boundary layer. X(sub tr) is estimated from the ozone concentration in the free troposphere and the wind speed. The ozone in the free troposphere estimated from surface ozone observations is consistent with that of ozonesonde data. X(sub ch) is obtained from the difference between X(sub ob) and X(sub tr). X(sub tr) increases with wind speed, while X(sub ch) shows maximum at hourly wind speed of 1-2 m/s in the daytime. Contribution of X(sub tr) to X(sub ob) is larger than X(sub ch) except for a short period in summer. X(sub ch) is positive for April-October, but X(sub ch) can be negative in winter, showing the net chemical destruction in the boundary layer. X(sub ch) increases linearly with solar radiation, and is negative for daily global solar radiation below 8 MJ/sq m, which is about equal to the monthly mean in winter.

Muramatsu, H.↗

Total ozone and surface temperature correlations during 1972 - 1981

Ten years of Dobson spectrophotometer total ozone measurements and surface temperature observations were used to construct monthly mean values of the two parameters. The variability of both parameters is greatest in the months of January and February. Indeed, in January there is an apparent correlation between high total ozone values and abnormally low surface temperatures. However, the correlation does not hold in February. By reviewing the history of stratospheric warmings during this period, it is argued that the ozone and surface temperature correlation is influenced by the advection or lack of advection of ozone rich arctic air resulting from sudden stratospheric warmings.

Parsons, C. L.↗

Analysis of Atmospheric Conditions Responsible for an Ozone Exceedance Event in Southeast Virginia on June 15, 2022

On June 15, 2022, the Virginia Department of Environmental Quality monitoring site at Suffolk/Holland, a rural site in southeast Virginia, recorded its first ozone exceedance since 2016. An ozone exceedance day occurs when the daily maximum 8-hour average surface ozone concentration is greater than 70 ppb. On this day, it was 75 ppb. This event is also noteworthy due to the rapid increase in surface ozone between 6 am and 9 am EDT as well as the hourly maximum ozone concentration of 82 ppb that was measured at 1 pm EDT. In this analysis, we utilize various observational and model data to determine the atmospheric conditions responsible for this ozone exceedance event. The analysis is conducted in two parts: (1) an evaluation of the accuracy of the GEOS-CF and WRF-Chem model forecasts and (2) an investigation of the mechanisms responsible for the high surface ozone at the Virginia DEQ Suffolk/Holland monitoring site. Comparisons of model forecasted ozone time-height cross sections with measured ozone by lidars from the Tropospheric Ozone Lidar Network (TOLNet) at NASA Langley and NASA Goddard reveal that both models forecasted ozone reasonably well near the surface. Model and observational data reveal that an upper-level ridge was present over much of the eastern United States, with a broad anticyclonic circulation near the surface, resulting in north-northeasterly flow over southeast Virginia. Back trajectory calculations using the Hybrid Single-Particle Lagrangian Integrated Trajectory model (HYSPLIT) and model data suggest that a low-level plume rich in ozone and precursor species originating from the New York City and New Jersey region was transported along the east coast between June 14 and June 15, arriving in southeast Virginia around 6 am EDT on June 15. In the early morning hours, this plume mixed down to the surface, elevating the background ozone mixing ratio as well as the mixing ratios of several precursor species. Other potential contributions are also explored and discussed. Lastly, the authors note that this work represents the analysis of the authors and not the Virginia Department of Environmental Quality.

Daniel B Phoenix↗

Stratospheric Instrusion Catalog: A 10-Year Compilation of Events Identified by using TRACK with NASA's MERRA-2 Reanalysis

Stratospheric intrusions "the introduction of ozone-rich stratospheric air into the troposphere" have been linked with surface ozone air quality exceedances, especially at the high elevations in the western USA in springtime. However, the impact of stratospheric intrusions in the remaining seasons and over the rest of the USA is less clear. A new approach to the study of stratospheric intrusions uses NASA's Goddard Earth Observing System Model (GEOS) model and assimilation products with an objective feature tracking algorithm to investigate the atmospheric dynamics that generate stratospheric intrusions and the different mechanisms through which stratospheric intrusions may influence tropospheric chemistry and surface air quality seasonally over both the western and the eastern USA. A catalog of stratospheric intrusions identified in the MERRA-2 reanalysis was produced for the period 2004-2015 and validated against surface ozone observations (focusing on those which exceed the national air quality standard) and a recent data set of stratospheric intrusion-influenced air quality exceedance flags from the US Environmental Protection Agency (EPA). Considering not all ozone exceedances have been flagged by the EPA, a collection of stratospheric intrusions can support air quality agencies for more rapid identification of the impact of stratospheric air on surface ozone and demonstrates that future operational analyses may aid in forecasting such events. An analysis of the spatiotemporal variability of stratospheric intrusions over the continental US was performed, and while the spring over the western USA does exhibit the largest number of stratospheric intrusions affecting the lower troposphere, the number of intrusions in the remaining seasons and over the eastern USA is sizable. By focusing on the major modes of variability that influence weather in the USA, such as the Pacific North American (PNA) teleconnection index, predicative meteorological patterns associated with stratospheric intrusions and their regional effects on tropospheric ozone were identified. Improved understanding of the connections between large-scale climate variability and local-scale dynamically-driven air quality events may support improved seasonal prediction of such events.

PN↗

The effect of paleoatmospheric ozone on surface temperature

Photochemical and radiative-convective calculations are performed to evaluate the influence of ozone in determining the surface temperature of the paleoatmosphere prior to the buildup of molecular oxygen to its present atmospheric level. Possible effects of atmospheric dynamics on the photochemistry and thermal structure of the paleoatmosphere are neglected, and the present atmospheric values are assumed for the tropospheric water-vapor relative-humidity distribution and lapse rate as well as for the fractional cloud amount and cloud reflectivity. It is found that the radiative effects (at IR and solar wavelengths) of ozone for a molecular oxygen level of one-tenth the present atmospheric level resulted in a globally averaged surface-temperature increase of about 4.5 K for the present solar constant. Implications of the results for paleoclimate are briefly considered.

Levine, J. S.↗

Mid-21st Century Ozone Air Quality and Health Burden in China Under Emissions Scenarios and Climate Change

Despite modest emissions reductions of air pollutants in recent years, China still suffers from poor air quality, and the outlook for future air quality in China is uncertain. We explore the impact of two disparate 2050 emissions scenarios relative to 2015 in the context of a changing climate with the Geophysical Fluid Dynamics Laboratory Atmospheric Model version 3 (GFDL-AM3) chemistry-climate model. We impose the same near-term climate change for both emission scenarios by setting global sea surface temperature (SST) and sea ice cover (SIC) to the average over 2010–2019 and 2046–2055, respectively, from a three-member ensemble of GFDL coupled climate model simulations under the RCP8.5 (Representative Concentration Pathway) scenario. By the 2050s, annual mean surface ozone increases throughout China by up to 8 ppbv from climate change alone (estimated by holding air pollutants at 2015 levels while setting SIC and SST to 2050 conditions in the model) and by 8–12 ppbv in a scenario in which emissions of ozone precursors nitrogen oxides (NO (sub x) ) and anthropogenic volatile organic compounds (VOCs) increase by ~10%. In a scenario in which NO (sub x) and anthropogenic VOC emissions decline by 60%, annual mean surface ozone over China decreases by 16–20 ppbv in the 2050s relative to the 2010s. The ozone increase from climate change alone results in an additional 62 000 premature deaths in China as compared to 330 000 fewer premature deaths by the 2050s under a strong emissions mitigation scenario. In springtime over Southwestern China in the 2050s, the model projects 9–12 ppbv enhancements to surface ozone from the stratosphere (diagnosed with a model tracer) and from international anthropogenic emissions (diagnosed by differencing AM3 simulations with the same emissions within China but higher versus lower emissions in the rest of the world). Our findings highlight the effectiveness of emissions controls in reducing the health burden in China due to air pollution, and also the potential for climate change and rising global emissions to offset, at least partially, some of the ozone decreases attained with regional emission reductions in China.

Westervelt, D. M.↗

Bromoalkane production by Antarctic ice algae

Ice microalgae, collected from the underside of annual sea ice in McMurdo Sound, Antarctica, were found to contain and release to seawater a number of brominated hydrocarbons. These included bromoform, dibromomethane, mixed bromochloromethanes, and methyl bromide. Atmospheric measurements in the McMurdo Sound vicinity revealed the presence of bromoform and methyl bromide in the lower atmosphere, with lowest concentrations inland, further indicating that biogenic activity in the Sound is a source of organic bromine gases to the Antarctic atmosphere. This may have important implications for boundary layer chemistry in Antarctica. In the Arctic, the presence of bromoform has been linked to loss of surface ozone in the spring. We report here preliminary evidence for similar surface ozone loss at McMurdo Station.

Sturges, W. T.↗

A three-dimensional dynamical-chemical model of atmospheric ozone

A three-year integration of a global three-dimensional model including dynamics and simple photochemistry is used to predict ozone. Good agreement with observation is obtained for stratospheric motion patterns, meridional circulations, ozone density as a function of height and latitude, eddy transports of ozone, surface destruction of ozone, and correlations of ozone with other variables. The annual cycle of columnar ozone in high latitudes is present, but at a smaller amplitude than observed. Vertical transport of ozone downward from the main generation level at 30 km is accomplished primarily by small-scale eddy diffusion between 20 and 30 km and again near the ground; large-scale vertical transport dominates in between. The model predicts a secondary maximum in ozone mixing ratio at 45 km somewhat equatorward of the winter polar-night zone. This feature, recently observed from satellite measurements, is thought to be caused by the temperature dependence of reaction rates in the Chapman scheme. The principal deficiency of the model is an underprediction of the spring ozone concentration in high latitudes in the lower stratosphere.

Cunnold, D.↗

Sensitivity of Tropospheric Ozone Over the Southeast USA to Dry Deposition

Dry deposition (DD) is a major loss process for tropospheric ozone and some reactive nitrogen and carbon precursors. We investigate the response of summertime ozone and its production chemistry over the Southeast United States (USA) to variability in this sink. Turning off DD of oxidized nitrogen, ozone, or all species over the United States in the Geophysical Fluid Dynamics Laboratory AM3 model increases regional mean surface ozone by 5, 18, or 25 ppb, respectively. Additional sensitivity simulations demonstrate that, assuming linearity, surface ozone has a similar sensitivity to ozone DD as to NOx emissions. Trends in ozone production efficiency derived from observed relationships between ozone and precursor oxidation products may not solely reflect precursor emission changes if ozone DD varies (e.g., with meteorology). We conclude that DD variability merits consideration when interpreting observed ozone trends. Quantifying the impact of changes in sinks versus sources will require long‐term DD measurements across the region of interest.

dry deposition↗

NASA's High-Resolution GEOS Forecasting and Reanalysis Products: Support for TOLNet

Stratospheric intrusions (SIs) the introduction of ozone-rich stratospheric air into the troposphere – have been the interest of decades of research for their link with surface ozone air quality exceedances, especially at the high elevations in the western USA in springtime; however, the impact of SIs in the remaining seasons and over the rest of the USA is less clear. We can expect MERRA-2 to realistically represent both atmospheric dynamics and composition. The operational GEOS weather forecasting system, GEOS-FP, has a similar ozone observing system to MERRA-2, while NASA's new global high-resolution air quality forecast system, GEOS-CF, combines the operational GEOS weather forecasting model with the state-of-the-science GEOS-Chem chemistry module (version 12), simulating a wide range of additional air pollutants and tracers which strengthens this detailed analysis of the intrusions and the sources for the high ozone concentrations. Using a multitude of observational datasets, including lidar, air craft, ozonesondes and air quality monitoring surface sites, in combination with the GEOS forecast and reanalysis products, we aim to provide the public with tools which are available in near-real time to enhance their capability to identify the impact of stratospheric air on surface ozone concentrations separate from anthropogenic sources. In particular, improved understanding of the connections between large-scale climate variability and local-scale dynamically-driven air quality events may support improved seasonal prediction of SI events.

Knowland, K. Emma↗

Ensemble Statistical Post-Processing of the National Air Quality Forecast Capability: Enhancing Ozone Forecasts in Baltimore, Maryland

An ensemble statistical post-processor (ESP) is developed for the National Air Quality Forecast Capability (NAQFC) to address the unique challenges of forecasting surface ozone in Baltimore, MD. Air quality and meteorological data were collected from the eight monitors that constitute the Baltimore forecast region. These data were used to build the ESP using a moving-block bootstrap, regression tree models, and extreme-value theory. The ESP was evaluated using a 10-fold cross-validation to avoid evaluation with the same data used in the development process. Results indicate that the ESP is conditionally biased, likely due to slight overfitting while training the regression tree models. When viewed from the perspective of a decision-maker, the ESP provides a wealth of additional information previously not available through the NAQFC alone. The user is provided the freedom to tailor the forecast to the decision at hand by using decision-specific probability thresholds that define a forecast for an ozone exceedance. Taking advantage of the ESP, the user not only receives an increase in value over the NAQFC, but also receives value for An ensemble statistical post-processor (ESP) is developed for the National Air Quality Forecast Capability (NAQFC) to address the unique challenges of forecasting surface ozone in Baltimore, MD. Air quality and meteorological data were collected from the eight monitors that constitute the Baltimore forecast region. These data were used to build the ESP using a moving-block bootstrap, regression tree models, and extreme-value theory. The ESP was evaluated using a 10-fold cross-validation to avoid evaluation with the same data used in the development process. Results indicate that the ESP is conditionally biased, likely due to slight overfitting while training the regression tree models. When viewed from the perspective of a decision-maker, the ESP provides a wealth of additional information previously not available through the NAQFC alone. The user is provided the freedom to tailor the forecast to the decision at hand by using decision-specific probability thresholds that define a forecast for an ozone exceedance. Taking advantage of the ESP, the user not only receives an increase in value over the NAQFC, but also receives value for

ozone↗

Air Quality Science and Regulatory Efforts Require Geostationary Satellite Measurements

Air quality scientists and regulatory agencies would benefit from the high spatial and temporal resolution trace gas and aerosol data that could be provided by instruments on a geostationary platform. More detailed time-resolved data from a geostationary platform could be used in tracking regional transport and in evaluating mesoscale air quality model performance in terms of photochemical evolution throughout the day. The diurnal cycle of photochemical pollutants is currently missing from the data provided by the current generation of atmospheric chemistry satellites which provide only one measurement per day. Often peak surface ozone mixing ratios are reached much earlier in the day during major regional pollution episodes than during local episodes due to downward mixing of ozone that had been transported above the boundary layer overnight. The regional air quality models often do not simulate this downward mixing well enough and underestimate surface ozone in regional episodes. Having high time-resolution geostationary data will make it possible to determine the magnitude of this lower-and mid-tropospheric transport that contributes to peak eight-hour average ozone and 24-hour average PM2.5 concentrations. We will show ozone and PM(sub 2.5) episodes from the CMAQ model and suggest ways in which geostationary satellite data would improve air quality forecasting. Current regulatory modeling is typically being performed at 12 km horizontal resolution. State and regional air quality regulators in regions with complex topography and/or land-sea breezes are anxious to move to 4-km or finer resolution simulations. Geostationary data at these or finer resolutions will be useful in evaluating such models.

Pickering, Kenneth E.↗

An Intercomparative Study of the Effects of Aircraft Emissions on Surface Air Quality

This study intercompares, among five global models, the potential impacts of all commercial aircraft emissions worldwide on surface ozone and particulate matter (PM (sub 2.5)). The models include climate-response models (CRMs) with interactive meteorology, chemical-transport models (CTMs) with prescribed meteorology, and models that integrate aspects of both. Model inputs are harmonized in an effort to achieve a consensus about the state of understanding of impacts of 2006 commercial aviation emissions. Models find that aircraft increase near-surface ozone (0.3 to 1.9 percent globally), with qualitatively similar spatial distributions, highest in the Northern Hemisphere. Annual changes in surface-level PM (sub 2.5) in the CTMs (0.14 to 0.4 percent) and CRMs (-1.9 to 1.2 percent) depend on differences in nonaircraft baseline aerosol fields among models and the inclusion of feedbacks between aircraft emissions and changes in meteorology. The CTMs tend to result in an increase in surface PM (sub 2.5) primarily over high-traffic regions in the North American midlatitudes. The CRMs, on the other hand, demonstrate the effects of aviation emissions on changing meteorological fields that result in large perturbations over regions where natural emissions (e.g., soil dust and sea spray) occur. The changes in ozone and PM (sub 2.5) found here may be used to contextualize previous estimates of impacts of aircraft emissions on human health.

Air quality↗

The Equilibrium Response of Climate and Composition to Lightning

Climate change can affect atmospheric composition through perturbation of natural processes, leading to complex feedbacks. The primary atmospheric oxidants OH and ozone are very sensitive to emissions of nitrogen oxides (NO x ) from lightning, and therefore so are the subsequent chemical perturbations to long-lived greenhouse gases (e.g., methane) and aerosol chemistry and physics. Meanwhile, cloud electrification responds to both meteorology and composition (aerosol particles). Key to understanding the ultimate impact of lightning on air quality and climate is the long-term methane feedback. Here, we present simulations from the GISS ModelE2.1 chemistry-climate model in which we isolate the response of Earth’s radiative budget and composition to lightning NO x in the present day and at the end of this century by allowing the model to re-equilibrate following removal of the source. Whereas lightning initially contributes to surface ozone enhancements, longer-term responses amplified by the methane lifetime feedback reduce surface ozone on multi-decadal time scales in the northern midlatitudes. Lightning consequently contributes a strong negative radiative effect in the present day (-0.5 W m -2 ), stronger than that estimated for the anthropogenic NOx source. In addition to influencing tropospheric composition, we find significant changes in stratospheric dynamics and composition. We test the sensitivity of our results to multiple parameterizations for global lightning activity.

Lightning↗