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Ozone is one of the six “criteria” pollutants identified by the U.S. Clean Air Act Amendment of 1970 as particularly harmful to human health. Concentrations have decreased markedly across the United States over the past 50 years in response to regulatory efforts, but continuing research on its deleterious effects have spurred further reductions in the legal threshold. The South Coast and San Joaquin Valley Air Basins of California remain the only two “extreme” ozone nonattainment areas in the United States. Further reductions of ozone in the West are complicated by significant background concentrations whose relative importance increases as domestic anthropogenic contributions decline and the national standards continue to be lowered. These background concentrations derive largely from uncontrollable sources including stratospheric intrusions, wildfires, and intercontinental transport. Taken together the exogenous sources complicate regulatory strategies and necessitate a much more precise understanding of the timing and magnitude of their contributions to regional air pollution. The California Baseline Ozone Transport Study was a field campaign coordinated across Northern and Central California during spring and summer 2016 aimed at observing daily variations in the ozone columns crossing the North American coastline, as well as the modification of the ozone layering downwind across the mountainous topography of California to better understand the impacts of background ozone on surface air quality in complex terrain.

The Fires, Asian, and Stratospheric Transport-Las Vegas Ozone Study (FAST-LVOS) was conducted in May and June of 2017 to study the transport of ozone (O3) to Clark County, Nevada, a marginal non-attainment area in the Southwestern U.S. (SWUS). This 6-week (20 May–30 June 2017) field campaign used lidar, ozonesonde, aircraft, and in-situ measurements in conjunction with a variety of models to characterize the distribution of O3 and related species above southern Nevada and neighbouring California, and to probe the influence of stratospheric intrusions, wildfires, and local, regional, and Asian pollution on surface O3 concentrations in Las Vegas and the surrounding area. In this paper, we describe the FAST-LVOS campaign and present case studies illustrating the influence of different transport processes on background O3 and air quality attainment in the SWUS. The measurements found elevated O3 layers above Las Vegas on more than 75 % (35 of 45) of the sample days, and show that entrainment of these layers contributed to mean 8-h average background O3 concentrations of 50–55 parts-per-billion by volume (ppbv) across southern Nevada. These background concentrations constitute 70–80 % of the current U.S. National Ambient Air Quality Standard (NAAQS) of 70 ppbv, and illustrate some of the challenges facing air quality managers tasked with O3 attainment in the SWUS during late spring and early summer. The companion paper by Zhang et al. (2020) describes the use of the AM4 and GEOS-Chem global models to estimate the impacts of transported O3 on surface air quality in the Southwestern U.S. and Intermountain West during the FAST-LVOS campaign.

Transport of pollution into pristine wilderness areas is of concern for both federal and state agencies. Assessing such transport in complex terrain is a challenge when relying solely on data from standard federal or state air quality monitoring networks because of the sparsity of network monitors beyond urban areas. During the Front Range air quality study, conducted in the summer of 2008 in the vicinity of Denver, CO, research-grade surface air quality data, vertical wind profiles and mixing heights obtained by radar wind profilers, and ozone profile data obtained by an airborne ozone differential absorption lidar augmented the local regulatory monitoring networks. Measurements from this study were taken on 2 successive days at the end of July 2008. On the first day, the prevailing winds were downslope westerly, advecting pollution to the east of the Front Range metropolitan areas. On this day, chemistry measurements at the mountain and foothills surface stations showed seasonal background ozone levels of approximately 55–68 ppbv (nmol mol–1 by volume). The next day, upslope winds prevailed, advecting pollution from the Plains into the Rocky Mountains and across the Continental Divide. Mountain stations measured ozone values greater than 90 ppbv, comparable to, or greater than, nearby urban measurements. The measurements show the progression of the ozone-enriched air into the mountains and tie the westward intrusion into high-elevation mountain sites to the growth of the afternoon boundary layer. Thus, under deep upslope flow conditions, ozone-enriched air can be advected into wilderness areas of the Rocky Mountains. Our findings highlight a process that is likely to be an important ozone transport mechanism in mountainous terrain adjacent to ozone source areas when the right circumstances come together, namely a deep layer of light winds toward a mountain barrier coincident with a deep regional boundary layer.

International audience; The Soberanes Fire burned 53,470 ha (132,127 acres) along the central California coast between 22 July and 12 October 2016, generating dense smoke and a variety of gaseous compounds that drifted eastward into the San Joaquin Valley Air Basin (SJVAB), an “extreme” nonattainment area for ozone (O3). These gases included nitrogen oxides (NOx) and volatile organic compounds, the photochemical precursors of O3. The fire started during the California Baseline Ozone Transport Study, a field campaign that brought aircraft, surface, and remote sensing measurements of O3 and related species to central California. In this paper, we use the California Baseline Ozone Transport Study measurements to assess the impact of the Soberanes Fire on ozone and particulate air quality in the SJVAB. We focus our analysis on 27 July to 2 August when the smoke haze was heaviest and the highest O3 concentrations in the SJVAB during 2016 were recorded. Our analyses suggest that while 40 to 60 ppbv of fire‐generated O3 was transported to the eastern SJVAB in the 1‐ to 3‐km‐altitude range, relatively little smoke or fire‐generated O3 reached the surface in the Visalia area.

Tropospheric O3 has been decreasing across much of the eastern U.S. but has remained steady or even increased in some western regions. Recent increases in VOC and NOx emissions associated with the production of oil and natural gas (O&NG) may contribute to this trend in some areas. The Northern Front Range of Colorado has regularly exceeded O3 air quality standards during summertime in recent years. This region has VOC emissions from a rapidly developing O&NG basin and low concentrations of biogenic VOC in close proximity to urban-Denver NOx emissions. Here VOC OH reactivity (OHR), O3 production efficiency (OPE), and an observationally constrained box model are used to quantify the influence of O&NG emissions on regional summertime O3 production. Analyses are based on measurements acquired over two summers at a central location within the Northern Front Range that lies between major regional O&NG and urban emission sectors. Observational analyses suggest that mixing obscures any OPE differences in air primarily influenced by O&NG or urban emission sector. The box model confirms relatively modest OPE differences that are within the uncertainties of the field observations. Box model results also indicate that maximum O3 at the measurement location is sensitive to changes in NOx mixing ratio but also responsive to O&NG VOC reductions. Combined, these analyses show that O&NG alkanes contribute over 80% to the observed carbon mixing ratio, roughly 50% to the regional VOC OHR, and approximately 20% to regional photochemical O3 production.

We have observed lower nitrogen dioxide (NO2) and ozone (O3) during a hot weekend (summer 2010) from aircraft over the entire South Coast Air Basin (SoCAB). Surface concentrations of NO2, O3, and temperature from 1996 to 2014 corroborate that this lower O3 on weekends is increasingly likely in recent years. While higher surface O3 on the weekends (weekend ozone effect, WO3E) remains widespread, the spatial extent and the trend in the probability of WO3E occurrences (PWO3E) have decreased significantly compared to a decade ago. This decrease is mostly the result of lower O3 on hot weekends in recent years. PWO3E is lowest in the eastern SoCAB. The major decrease happened during the 2008 economic recession, after which PWO3E has stabilized at a 15–25% lower level throughout most of the basin. Future NOx reductions are likely to be increasingly effective at reducing O3 pollution initially under hot conditions in the coming decade.

The Tropospheric Ozone Lidar Network (TOLNet) is a unique network of lidar systems that measure atmospheric profiles of ozone and aerosols, to contribute to air-quality studies, atmospheric modeling, and satellite validation efforts. The accurate characterization of these lidars is of critical interest, and is necessary to determine cross-instrument calibration uniformity. From July to August 2014, three lidars, the TROPospheric OZone (TROPOZ) lidar, the Tunable Optical Profiler for Aerosol and oZone (TOPAZ) lidar, and the Langley Mobile Ozone Lidar (LMOL), of TOLNet participated in the “Deriving Information on Surface conditions from Column and Vertically Resolved Observations Relevant to Air Quality” (DISCOVER-AQ) mission and the “Front Range Air Pollution and Photochemistry Éxperiment” (FRAPPÉ) to measure sub-hourly ozone variations from near the surface to the top of the troposphere. Although large differences occur at few individual altitudes in the near field and far field range, the TOLNet lidars agree with each other within ±4%. These results indicate excellent measurement accuracy for the TOLNet lidars that is suitable for use in air-quality and ozone modeling efforts.

Recently, two air quality campaigns were conducted in the southwestern United States to study the impact of transported ozone, stratospheric intrusions, and fire emissions on ground-level ozone concentrations. The California Baseline Ozone Transport Study (CABOTS) took place in May – August 2016 covering the central California coast and San Joaquin Valley, and the Fires, Asian, and Stratospheric Transport Las Vegas Ozone Study (FAST-LVOS) was conducted in the greater Las Vegas, Nevada area in May – June 2017. During these studies, nearly 1000 hours of ozone and aerosol profile data were collected with the NOAA TOPAZ lidar. A Doppler wind lidar and a radar wind profiler provided continuous observations of atmospheric turbulence, horizontal winds, and mixed layer height. These measurements allowed us to directly observe the degree to which ozone transport layers aloft were entrained into the boundary layer and to quantify the resulting impact on surface ozone levels. Mixed layer heights in the San Joaquin Valley during CABOTS were generally below 1 km above ground level (AGL), while boundary layer heights in Las Vegas during FAST-LVOS routinely exceeded 3 km AGL and occasionally reached up to 4.5 km AGL. Consequently, boundary layer entrainment was more often observed during FAST-LVOS, while most elevated ozone layers passed untapped over the San Joaquin Valley during CABOTS.

International audience; A series of deep stratospheric intrusions in late May 2013 increased the daily maximum 8 h surface ozone (O 3) concentrations to more than 70 parts per billion by volume (ppbv) at rural and urban surface monitors in California and Nevada. This influx of ozone-rich lower stratospheric air and entrained Asian pollution persisted for more than 5 days and contributed to exceedances of the 2008 8 h national ambient air quality standard of 75 ppbv on 21 and 25 May in Clark County, NV. Exceedances would also have occurred on 22 and 23 May had the new standard of 70 ppbv been in effect. In this paper, we examine this episode using lidar measurements from a high-elevation site on Angel Peak, NV, and surface measurements from NOAA, the Clark County, Nevada Department of Air Quality, the Environmental Protection Agency Air Quality System, and the Nevada Rural Ozone Initiative. These measurements, together with analyses from the National Centers for Environmental Prediction/North American Regional Reanalysis

The NOAA airborne ozone lidar system [Tunable Optical Profiler for Aerosol and Ozone (TOPAZ)] is compared with the fast-response chemiluminescence sensor flown aboard the NOAA WP-3D during the 2006 Texas Air Quality Study (TexAQS). TOPAZ measurements made from the NOAA Twin Otter, flying at an altitude of ~3300 m MSL in the Houston, Texas, area on 31 August, and the Dallas, Texas, area on 13 September, show that the overall uncertainty in the 10-s (~600-m horizontal resolution) TOPAZ profiles is dominated by statistical uncertainties (1σ) of ~8 ppbv (6%–10%) at ranges of ~2300 m from the aircraft (~1000 m MSL), and ~11–27 ppbv (12%–30%) at ranges of ~2800 m (~500 m MSL). These uncertainties are substantially reduced by spatial averaging, and the averages of 11 profiles (of 110 s or 6.6-km horizontal resolution) at ~1000 m MSL are in excellent agreement (±2%) with the in situ measurements at ~500 m MSL. The TOPAZ measurements at lower altitudes on 31 August exhibit a negative bias of up to ~15%, however, when the lidar signals were strongly attenuated by very high ozone levels in the plume from the Houston Ship Channel. This bias appears to result from nonlinear behavior in the TOPAZ signal amplifiers, which is described in the companion paper by Alvarez et al. An empirical correction is presented.

A case study from the Texas Air Quality Study 2000 field campaign illustrates the complex interaction of meteorological and chemical processes that produced a high-pollution event in the Houston area on 30 August 2000. High 1-h ozone concentrations of nearly 200 ppb were measured near the surface, and vertical profile data from an airborne differential-absorption lidar (DIAL) system showed that these high-ozone concentrations penetrated to heights approaching 2 km into the atmospheric boundary layer. This deep layer of pollution was transported over the surrounding countryside at night, where it then mixed out the next day to become part of the rural background levels. These background levels thus increased during the course of the multiday pollution episode. The case study illustrates many processes that numerical forecast models must faithfully represent to produce accurate quantitative predictions of peak pollutant concentrations in coastal locations such as Houston. Such accurate predictions ...

A high-ozone (O3) pollution episode was observed on 22 July 2014 during the concurrent “Deriving Information on Surface Conditions from Column and Vertically Resolved Observations Relevant to Air Quality” (DISCOVER-AQ) and “Front Range Air Pollution and Photochemistry Experiment” (FRAPPE) campaigns in northern Colorado. Surface O3 monitors at three regulatory sites exceeded the Environmental Protection Agency (EPA) 2008 National Ambient Air Quality Standard (NAAQS) daily maximum 8-hr average (MDA8) of 75 ppbv. To further characterize the polluted air mass and assess transport throughout the event, measurements are presented from O3 and wind profilers, O3-sondes, aircraft, and surface monitoring sites. Observations indicate thermally-driven upslope flow was established throughout the Colorado Front Range during the pollution episode. As the thermally-driven flow persisted throughout the day, O3 concentrations increased and affected high-elevation Rocky Mountain sites. These observations, coupled with modeling analyses, demonstrate a westerly return flow of polluted air aloft, indicating the mountain-plains solenoid circulation was established and impacted surface conditions within the Front Range.

Data from the oil- and gas-producing basin of northeastern Utah and a box model are used to assess the photochemical reactions of nitrogen oxides and volatile organic compounds that lead to excessive atmospheric ozone pollution in winter. The US experience with air quality degradation from shale gas extraction presents a measurement and modelling framework relevant to similar developments in other regions projected for the near future. High ozone mixing ratios have been observed in oil and gas producing basins in the United States during winter, but the underlying chemistry involved is not fully understood. This study presents a quantitative assessment of the underlying chemistry responsible for the winter ozone pollution events based on data from an oil and gas basin in Utah and a chemical 'box model' simulation. The results show that very high volatile organic carbon concentrations optimize the ozone production efficiency of nitrogen oxides with carbonyl photolysis as a dominant oxidant source. The United States is now experiencing the most rapid expansion in oil and gas production in four decades, owing in large part to implementation of new extraction technologies such as horizontal drilling combined with hydraulic fracturing. The environmental impacts of this development, from its effect on water quality1 to the influence of increased methane leakage on climate2, have been a matter of intense debate. Air quality impacts are associated with emissions of nitrogen oxides3,4 (NOx = NO + NO2) and volatile organic compounds5,6,7 (VOCs), whose photochemistry leads to production of ozone, a secondary pollutant with negative health effects8. Recent observations in oil- and gas-producing basins in the western United States have identified ozone mixing ratios well in excess of present air quality standards, but only during winter9,10,11,12,13. Understanding winter ozone production in these regions is scientifically challenging. It occurs during cold periods of snow cover when meteorological inversions concentrate air pollutants from oil and gas activities, but when solar irradiance and absolute humidity, which are both required to initiate conventional photochemistry essential for ozone production, are at a minimum. Here, using data from a remote location in the oil and gas basin of northeastern Utah and a box model, we provide a quantitative assessment of the photochemistry that leads to these extreme winter ozone pollution events, and identify key factors that control ozone production in this unique environment. We find that ozone production occurs at lower NOx and much larger VOC concentrations than does its summertime urban counterpart, leading to carbonyl (oxygenated VOCs with a C = O moiety) photolysis as a dominant oxidant source. Extreme VOC concentrations optimize the ozone production efficiency of NOx. There is considerable potential for global growth in oil and gas extraction from shale. This analysis could help inform strategies to monitor and mitigate air quality impacts and provide broader insight into the response of winter ozone to primary pollutants.

One of the objectives of the 1995 Southern Oxidants Study was to assess the extent to which fossil fuel power plants contribute to high ozone episodes that often occur in the Nashville area during summer. Among other instruments, the National Oceanic and Atmospheric Administration airborne ozone and aerosol lidar was used to investigate power plant plumes in the vicinity of Nashville, Tennessee. Owing to its ability to characterize the two-dimensional structure of ozone and aerosols below the aircraft, the airborne lidar is well suited to document the evolution of the size and shape of a power plant plume as well as its impact on ozone concentration levels as the plume is advected downwind. We report on two case studies of the Cumberland power plant plume that were conducted on July 7 and 19, 1995. The meteorological conditions on these 2 days were distinctly different and had a significant impact on the plume characteristics. On July 7, the Cumberland plume was shaped symmetrically and confined to the boundary layer, while on July 19 the plume had an irregular shape and showed two cores, one above and the other within the boundary layer. Close to the Cumberland power plant, we found that ozone in the plume was destroyed at a rate of 5 to 8 ppbv h -1 due to titration at high NO levels. Farther downwind, where plume NOx reacts with ozone precursor gases to form ozone, we measured plume-averaged ozone production rates of 1.5 to 4 ppbv h -1. The results of these two case studies are compared to aircraft in situ measurements of the same power plant plume.

As part of the 1995 Southern Oxidants Study (SOS), the National Oceanic and Atmospheric Administration airborne ozone lidar was deployed during June and July to provide detailed three-dimensional lower tropospheric ozone distribution information in the Nashville, Tennessee, area. The airborne portion of the study included six aircraft instrumented with an assortment of in situ and remote sensors. Results of comparisons between the ozone values obtained using the lidar and the values obtained using in situ instrumentation aboard other aircraft are presented. High resolution (90 m vertical and 520 m horizontal corresponding to 8 s at a flight speed of 65 m/s) was maintained during the analysis of the lidar data which caused statistical variations in the calculated ozone concentrations from 3 ppbv (5% for typical ozone concentrations encountered during the study) at a range of 1500 m from the lidar to 11 ppbv (17%) at a range of 2500 m from the lidar. However, the lidar ozone concentration measurements compare favorably with the in situ values, with the average offset less than 10 ppbv (16%) for each flight, and the average magnitude of the offsets over all the flights at 4.3 ppbv (7%).

This paper reports results from the Southern Oxidants Study field campaign designed to characterize the formation and distribution of ozone and related species in the Nashville urban region. Data from several airborne platforms as well as surface observations on July 3 and 18 are examined to gain insight into the factors that control O{sub 3} formation rates and concentrations in the regional plumes. On both days, well-defined urban and power plant plumes were sampled. Utilizing both aircraft and surface data, a detailed kinetic analysis of the chemical evolution of the urban plume is performed to derive NO{sub x} lifetime, ozone production efficiency, OH concentration, HNO{sub 3} dry deposition rate, and the relative importance of natural and anthropogenic hydrocarbons to O{sub 3} production. Analysis of the urban plume data revealed a very active photochemical system (average [OH]{approximately}1.2{times}10{sup 7}hmoleculeshcm{sup {minus}3}) which consumed 50{percent} of the NO{sub x} within approximately 2 hours, at an ozone production efficiency of 2.5 to 4 molecules for each molecule of NO{sub x}. Anthropogenic hydrocarbons provided approximately 44{percent} of the fuel for ozone production by the urban plume. The dry deposition rate for HNO{sub 3} in the urban plume was estimated to be of the order of 5more » to 7 cmhs{sup {minus}1}. {copyright} 1998 American Geophysical Union« less

A 3-day period of strong, synoptic-scale stagnation, in which daytime boundary-layer winds were light and variable over the region, occurred in mid July of the 1995 Southern Oxidants Study centered on Nashville, Tennessee. Profiler winds showed light and variable flow throughout the mixed layer during the daytime, but at night in the layer between 100 and 2000 m AGL (which had been occupied by the daytime mixed layer) the winds accelerated to 5-10 m s-1 as a result of nocturnal decoupling from surface friction, which producect inertial oscillations. In the present study, we investigate the effects of these wind changes on the buildup and transport of ozone (03). The primary measurement system used in this study was an airborne differential absorption lidar (DIAL) system that profiled 03 in the boundary layer as the airplane flew along. Vertical cross sections showed that 03 concentrations exceeding 120 ppb extended up to nearly 2 km AGL, but that the 03 hardly moved at all horizontally, instead forming a dome of pollution over or near the city. The analysis concentrates on four meteorological processes that determine the 3-D spatial distribution of 03 and the interaction between urban and rural pollution: (1) daytime buildup of 03 over the urban area, (2) the extent of the drift of pollution cloud during the day as it formed, which controls peak 03 concentrations, (3) nighttime transport by the accelerated winds above the surface, and (4) vertical mixing of pollution layers the next day. Other consequences of very light-wind conditions were intra-regional differences in daytime mixed-layer depth over distances of 50 km or less, and indications of an urban heat-island circulation.

[1] The published literature debates the extent to which naturally occurring stratospheric ozone intrusions reach the surface and contribute to exceedances of the U.S. National Ambient Air Quality Standard (NAAQS) for ground-level ozone (75 ppbv implemented in 2008). Analysis of ozonesondes, lidar, and surface measurements over the western U.S. from April to June 2010 show that a global high-resolution (∼50 × 50 km2) chemistry-climate model (GFDL AM3) captures the observed layered features and sharp ozone gradients of deep stratospheric intrusions, representing a major improvement over previous chemical transport models. Thirteen intrusions enhanced total daily maximum 8-h average (MDA8) ozone to ∼70–86 ppbv at surface sites. With a stratospheric ozone tracer defined relative to a dynamically varying tropopause, we find that stratospheric intrusions can episodically increase surface MDA8 ozone by 20–40 ppbv (all model estimates are bias corrected), including on days when observed ozone exceeds the NAAQS threshold. These stratospheric intrusions elevated background ozone concentrations (estimated by turning off North American anthropogenic emissions in the model) to MDA8 values of 60–75 ppbv. At high-elevation western U.S. sites, the 25th–75th percentile of the stratospheric contribution is 15–25 ppbv when observed MDA8 ozone is 60–70 ppbv, and increases to ∼17–40 ppbv for the 70–85 ppbv range. These estimates, up to 2–3 times greater than previously reported, indicate a major role for stratospheric intrusions in contributing to springtime high-O3events over the high-altitude western U.S., posing a challenge for staying below the ozone NAAQS threshold, particularly if a value in the 60–70 ppbv range were to be adopted.

[1] The influence of stratosphere-to-troposphere transport (STT) on surface ozone (O3) concentrations in the greater Los Angeles area during the CalNex and IONS-2010 measurement campaigns has been investigated. Principal component analysis (PCA) of surface O3measurements from 41 sampling stations indicates that ∼13% of the variance in the maximum daily 8-h average (MDA8) O3between May 10 and June 19, 2010 was associated with changes of 2–3 day duration linked to the passage of upper-level troughs. Ozonesondes launched from Joshua Tree National Park and airborne lidar measurements show that these changes coincided with the appearance of stratospheric intrusions in the lower troposphere above southern California. The Lagrangian particle dispersion model FLEXPART reproduces most of these intrusions, and supports the conclusion from the PCA that significant transport of stratospheric air to the surface occurred on May 28–30. This intrusion led to a peak 1-h O3 concentration of 88 ppbv at Joshua Tree National Monument near the ozonesonde launch site on May 28, and widespread entrainment of stratospheric air into the boundary layer increased the local background O3 over the entire area to ∼55 ppbv on May 29–30. This background was 10–15 ppbv higher than the baseline O3 in air transported ashore from the Pacific Ocean, and when combined with locally produced O3 led to several exceedances of the current National Ambient Air Quality Standard (NAAQS) on the following day.

[1] We use airborne lidar measurements of ozone collected during the Texas Air Quality Study (TexAQS) 2000 and TexAQS 2006 field campaigns to compute the horizontal flux of ozone downwind of the Houston and Dallas/Fort Worth metropolitan areas. Fluxes are computed for each aircraft transect by integrating excess ozone (plume ozone minus background ozone) in the urban plumes and multiplying the result by the horizontal wind speed provided by radar wind profilers. In addition, we use the lidar data to estimate ozone production rates and ozone enhancements in the Houston and Dallas/Fort Worth plumes. We found that the average horizontal flux of ozone emanating from the Houston area based on data from six research flights was 3.2 · 1026 molecules per second. This was significantly higher than the flux measured downwind of Dallas/Fort Worth during a single flight. The Houston fluxes exhibited a strong dependence on wind direction. Under southerly or northerly flow, ozone fluxes were about twice as large as under westerly or easterly flow conditions. We estimate that a day's worth of export of ozone from the Houston area could raise regional background ozone by about 10 ppbv over a 40,000 km2 area. This has important ramifications for air quality in communities downwind of Houston as it could raise background ozone levels enough that regions with little or no local pollution sources of their own may violate the federally mandated ozone standard.

[1] The influence of convective mixing on surface ozone in Houston during TexAQS 2006 is examined. We use airborne lidar measurements of ozone and ship-based Doppler lidar measurements of winds, together with ship- and ground-based measurements of surface ozone to characterize horizontal and vertical mixing of ozone plumes from the Houston Ship Channel on two high-ozone days. We show that a stable capping layer trapped the plume in the boundary layer on 31 August, while shallow convection associated with active fair weather cumulus clouds mixed the plume with free tropospheric air on 17 August. Deep convection associated with an isolated air mass thunderstorm further decreased surface ozone near Galveston Bay in the late afternoon. High ozone thus affected a smaller area for a shorter period on 17 August, despite similar background concentrations and local production. We generalize these findings by comparing Houston ozone concentrations to National Weather Service (Lake Charles, LA) radiosondes. We show that for 1 June to 15 September 2006, stable conditions with high background ozone occurred 18% of the days leading to mean daily 8 h concentrations of 73 ± 11 ppbv. Shallow and deep convection associated with moderate to strongly unstable conditions lowered the mean ozone to 50 ± 11 ppbv (∼29% of days), while weaker convection associated with marginally unstable conditions reduced the mean concentrations to 63 ± 13 ppbv (∼11%). We use these observations to derive simple relationships between surface ozone and convective indicators that may prove useful for parameterization of convective venting in air quality models.

[1] Measurements made with a ship-based Doppler wind lidar during the summertime 2006 Texas Air Quality Study are used to study the relationship between lower-tropospheric vertical structure and winds and ozone (O3) concentrations in Houston, Texas, under two different flow regimes. We observed that strong southerly flow regimes, dominated by the subtropical anticyclone (Bermuda high) off the Atlantic coast of the United States, resulted in strong (i.e., high wind speed) onshore nocturnal low-level jets (LLJ) and low O3 and oxidant Ox (where Ox = O3 + NO2) concentrations at night and the following afternoon. In contrast, periods dominated by northerly or easterly flow resulted in relatively weak (low wind speed), but still onshore, nocturnal LLJs associated with higher concurrent and next-day concentrations of O3 and Ox. We present lidar data from 24 h example periods for each of these conditions and demonstrate how each type of flow regime is related to in situ ship-based ozone measurements. We expanded the study to include all days during the study when the ship was near Houston, to demonstrate how the strength of the meridional winds aloft show a better relationship to concurrent ship-measured Ox concentrations than the winds near the surface do. We found a strong relationship between a parameterization of the observed nocturnal jets, which reflect the synoptic conditions, to peak hourly O3 measured the next day at the ship and averaged throughout the Houston/Galveston/Brazoria continuous ambient monitoring stations monitoring network, indicating potential applications for planning air quality.

[1] Airborne lidar measurements of ozone above the Los Angeles Basin on 17 July 2009 show orographic lifting of ozone from the surface to the free troposphere by the San Gabriel Mountains. Mixing ratios in excess of 100 parts-per-billion-by-volume (ppbv) were measured ∼4 km above mean sea level (ASL). These observations are in excellent agreement with published model studies, confirming that topographic venting by the so called “mountain chimney effect” is a potentially important pathway for removal of pollutants from the Los Angeles Basin. The lofting of ozone and other pollutants into the free troposphere also greatly increases the potential for long-range transport from the Basin, and trajectory calculations suggest that some of this ozone may have been transported ∼1000 km to eastern Utah and western Colorado.

[1] Principal Component Analysis (PCA) is used to isolate the common modes of behavior in the daily maximum 8-h average ozone mixing ratios measured at 30 Continuous Ambient Monitoring Stations in the Houston-Galveston-Brazoria area during the Second Texas Air Quality Study field intensive (1 August to 15 October 2006). Three principal components suffice to explain 93% of the total variance. Nearly 84% is explained by the first component, which is attributed to changes in the “regional background” determined primarily by the large-scale winds. The second component (6%) is attributed to changes in the “local background,” that is, ozone photochemically produced in the Houston area and spatially and temporally averaged by local circulations. Finally, the third component (3.5%) is attributed to short-lived plumes containing high ozone originating from industrial areas along Galveston Bay and the Houston Ship Channel. Regional background ozone concentrations derived using the first component compare well with mean ozone concentrations measured above the Gulf of Mexico by the tunable profiler for aerosols and ozone lidar aboard the NOAA Twin Otter. The PCA regional background values also agree well with background values derived using the lowest daily 8-h maximum method of Nielsen-Gammon et al. (2005), provided the Galveston Airport data (C34) are omitted from that analysis. The differences found when Galveston is included are caused by the sea breeze, which depresses ozone at Galveston relative to sites further inland. PCA removes the effects of this and other local circulations to obtain a regional background value representative of the greater Houston area.

The Ozone Profiling Atmospheric Lidar is a scanning four-wavelength ultraviolet differential absorption lidar that measures tropospheric ozone and aerosols. Derived profiles from the lidar data include ozone concentration, aerosol extinction, and calibrated aerosol backscatter. Aerosol calibrations assume a clear air region aloft. Other products include cloud base heights, aerosol layer heights, and scans of particulate plumes from aircraft. The aerosol data range from 280 m to 12 km with 5 m range resolution, while the ozone data ranges from 280 m to about 1.2 km with 100 m resolution. In horizontally homogeneous atmospheres, data from multiple-elevation angles is combined to reduce the minimum altitude of the aerosol and ozone profiles to about 20 m. The lidar design, the characterization of the photomultiplier tubes, ozone and aerosol analysis techniques, and sample data are described. Also discussed is a double-gating technique to shorten the gated turn-on time of the photomultiplier tubes, and thereby reduce the detection of background light and the outgoing laser pulse.

We have used NOAA’s Tunable Optical Profiler for Aerosol and oZone (TOPAZ) ozone lidar to investigate the sources of high surface ozone concentrations in two different regions of the western United States (US): the Uintah Basin in northeast Utah and Clark County in southern Nevada, which includes the city of Las Vegas. The Uintah Basin is a booming oil and gas producing region that often suffers from very high wintertime ozone concentrations. Clark County experiences violations of the US ozone standard primarily in spring and early summer despite a lack of any major local pollution sources. TOPAZ lidar observations, in conjunction with surface in situ measurements and model results, provided strong evidence that the high wintertime ozone concentrations in the Uintah Basin are primarily driven by local emissions associated with oil and gas exploration, whereas the Clark County ozone exceedances are often caused by ozone-rich air that is transported from the lower stratosphere all the way down to the earth’s surface.

[1] Time series from two ozone monitoring stations are evaluated, one on an island several km off the New England coast, the other several km inland in New Hampshire. In the summer of 2002, during the New England Air Quality Study 2002 (NEAQS-2002), ozone measurements at the island station, Appledore Island (ADI), were consistently higher than at the inland station, Thompson Farm (TF). We hypothesized that the differences in ozone concentrations were due to transport differences driven by mesoscale meteorology, since neither site was in a source region. We found that the Appalachian Trough, coastal cold fronts and coastal stationary fronts at times caused TF to have westerly component flow while ADI had southerly component flow. In these situations, the southwesterly flow along the New England coast brought ozone and precursors to ADI from metropolitan areas to the southwest (e.g., Boston). Conversely, the air transported to TF from the west was contaminated by fewer upstream sources, and therefore the ozone was lower at TF. The sea breeze was also a factor, which tended to have the contrasting effect of nearly equalizing the ozone concentrations at the two sites by transporting ozone-rich air already impacting ADI inland to TF. Enhanced measurements from the NEAQS-2002 study were used in the analysis, including radar wind profilers, Doppler and ozone profiling lidars, and radiosondes launched from a ship. We also assessed model performance for two models, WRF/Chem and MM5/Chem, for four key days.

[1] This paper investigates linkages between weather, climate, and air quality that contributed to the large difference in the number of ozone exceedances encountered in the northeastern United States (U.S.) during 2002 and 2004. Major air quality research field campaigns were conducted in the northeast during July and August of each year. Both the 2002 New England Air Quality Study (NEAQS-02) and the International Consortium for Atmospheric Research on Transport and Transformation 2004 field study (ICARTT-04) had research components focused on regional air quality. The primary environmental difference between the two field campaigns was the underlying climatic conditions. The July–August period in 2002 was much sunnier, warmer, and drier than normal. In contrast, the July–August period in 2004 was cloudier, cooler, and much wetter than normal. We conclude that these extreme climatic conditions were the underlying cause for the significant difference in the number of ozone exceedances that occurred during NEAQS-02 and ICARTT-04. We rule out the impact of other meteorological processes as the primary cause of this difference. We gauge horizontal transport using surface and upper air wind observations collected on Appledore Island (ADI), off the coast of New Hampshire and Maine, along with back trajectories based solely on wind observations collected by profiler networks deployed for each study. The wind conditions that favor pollutant transport to the northeast were more prevalent in 2004 than in 2002, yet the number of ozone exceedances in 2004 was more than a factor of three less than in 2002. Neither was daytime boundary layer mixing the cause for this discrepancy. Unlike other parts of the U.S. where poor air quality is generally associated with shallow boundary layers, in New England the boundary layers were deeper on high-ozone days than on clean days because the same sunny, warm, and dry conditions that favor boundary layer ozone production also produce deeper boundary layers. Both field campaigns were synoptically active. Lulls in synoptic activity explained most of the high-ozone events observed in 2002, whereas even an extended lull in synoptic activity during the summer of 2004 did not produce a single high-ozone day.

[1] Petrochemical industrial facilities can emit large amounts of highly reactive hydrocarbons and NOx to the atmosphere; in the summertime, such colocated emissions are shown to consistently result in rapid and efficient ozone (O3) formation downwind. Airborne measurements show initial hydrocarbon reactivity in petrochemical source plumes in the Houston, TX, metropolitan area is primarily due to routine emissions of the alkenes propene and ethene. Reported emissions of these highly reactive compounds are substantially lower than emissions inferred from measurements in the plumes from these sources. Net O3 formation rates and yields per NOx molecule oxidized in these petrochemical industrial source plumes are substantially higher than rates and yields observed in urban or rural power plant plumes. These observations suggest that reductions in reactive alkene emissions from petrochemical industrial sources are required to effectively address the most extreme O3 exceedences in the Houston metropolitan area.

[1] Two consecutive increases in surface ozone, occurring after the cessation of photochemical ozone production, are investigated. A unique suite of instruments, including an ozone profiling lidar, a Doppler lidar, surface chemistry sensors, surface meteorological sensors, and a radar wind profiler, was deployed during the Southern Oxidants Study of 1999 in Nashville, Tennesee. Time series of ozone at 10, 405, and 1035 m above ground level (AGL) on 22 June 1999 showed variations in the vertical gradient of ozone over the course of the afternoon and evening. Analysis of time series of vertical velocity at 8 m AGL and its standard deviation, the variance in Doppler lidar calculated horizontal wind speed from near the surface to 500 m AGL, wind profiles, and meteorological surface station data, revealed mechanisms responsible for these changes in ozone. An early evening rise in surface ozone occurred with the passage of a thunderstorm gust front. Analysis showed that downward mixing of ozone-rich air from a residual layer (RL) of ozone above 400 m caused a sharp rise in ozone at the surface and a decrease of ozone in the RL. Doppler lidar measurements showed details of the postgust front wind flow, such as the depth of the air mass behind the front, the turbulent wake region, and inferred vertical velocities throughout a layer several hundred meters deep. The second rise in surface ozone was caused by turbulent mixing due to elevated directional wind shear, which mixed ozone-rich air down to the surface.

First measurements of ozone vertical fluxes with a ground-based ozone DIAL/Doppler lidar combination are presented. The vertically pointing ozone DIAL and Doppler lidar yield highly resolved measurements of ozone density and vertical wind speed from which ozone fluxes are retrieved directly using the eddy correlation technique. The time resolution of the ozone density and vertical wind speed measurements is 30 s and the vertical resolution is 120 m. With the current setup ozone flux profiles can be retrieved between 800 and 1500 m above ground level.

The NOAA Environmental Technology Laboratory (ETL) and the NCAR Atmospheric Technology Division (ATD) participated in the 1995 Southern Oxidants Study (SOS) Nashville summer intensive campaign. The airborne UV-DIAL ozone lidar operated jointly by these laboratories was deployed as part of the large suite of instruments used in this study.