Springtime high surface ozone events over the western United States: Quantifying the role of stratospheric intrusions

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

Quantifying TOLNet ozone lidar accuracy during the 2014 DISCOVER-AQ and FRAPPE campaigns

The Tropospheric Ozone Lidar Network (TOLNet) is a unique network of lidar systems that measure high-resolution atmospheric profiles of ozone. The accurate characterization of these lidars is necessary to determine the uniformity of the network calibration. 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 ozone variations from the boundary layer to the top of the troposphere. This study presents the analysis of the intercomparison between the TROPOZ, TOPAZ, and LMOL lidars, along with comparisons between the lidars and other in situ ozone instruments including ozonesondes and a P-3B airborne chemiluminescence sensor. The TOLNet lidars measured vertical ozone structures with an accuracy generally better than ±15 % within the troposphere. Larger differences occur at some individual altitudes in both the near-field and far-field range of the lidar systems, largely as expected. In terms of column average, the TOLNet lidars measured ozone with an accuracy better than ±5 % for both the intercomparison between the lidars and between the lidars and other instruments. These results indicate that these three TOLNet lidars are suitable for use in air quality, satellite validation, and ozone modeling efforts

The California baseline ozone transport study (CABOTS)

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

Quantifying TOLNet Ozone Lidar Accuracy During the 2014 DISCOVER-AQ and FRAPP Campaigns

The Tropospheric Ozone Lidar Network (TOLNet) is a unique network of lidar systems that measure high-resolution atmospheric profiles of ozone. The accurate characterization of these lidars is necessary to determine the uniformity of the network calibration. 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 xperiment (FRAPP) to measure ozone variations from the boundary layer to the top of the troposphere. This study presents the analysis of the intercomparison between the TROPOZ, TOPAZ, and LMOL lidars, along with comparisons between the lidars and other in situ ozone instruments including ozonesondes and a P-3B airborne chemiluminescence sensor. The TOLNet lidars measured vertical ozone structures with an accuracy generally better than 15 % within the troposphere. Larger differences occur at some individual altitudes in both the near-field and far-field range of the lidar systems, largely as expected. In terms of column average, the TOLNet lidars measured ozone with an accuracy better than 5 % for both the intercomparison between the lidars and between the lidars and other instruments. These results indicate that these three TOLNet lidars are suitable for use in air quality, satellite validation, and ozone modeling efforts

TOLNet - A Tropospheric Ozone Lidar Profiling Network for Satellite Continuity and Process Studies

NASA initiated an interagency ozone lidar observation network under the name TOLNet to promote cooperative multiple-station ozone-lidar observations to provide highly time-resolved (few minutes) tropospheric-ozone vertical profiles useful for air-quality studies, model evaluation, and satellite validation

Evaluating A Priori Ozone Profile Information Used in TEMPO Tropospheric Ozone Retrievals

Ozone (O3) is a greenhouse gas and toxic pollutant which plays a major role in air quality. Typically, monitoring of surface air quality and O3 mixing ratios is primarily conducted using in situ measurement networks. This is partially due to high-quality information related to air quality being limited from space-borne platforms due to coarse spatial resolution, limited temporal frequency, and minimal sensitivity to lower tropospheric and surface-level O3. The Tropospheric Emissions: Monitoring of Pollution (TEMPO) satellite is designed to address these limitations of current space-based platforms and to improve our ability to monitor North American air quality. TEMPO will provide hourly data of total column and vertical profiles of O3 with high spatial resolution to be used as a near-real-time air quality product. TEMPO O3 retrievals will apply the Smithsonian Astrophysical Observatory profile algorithm developed based on work from GOME, GOME-2, and OMI. This algorithm uses a priori O3 profile information from a climatological data-base developed from long-term ozone-sonde measurements (tropopause-based (TB) O3 climatology). It has been shown that satellite O3 retrievals are sensitive to a priori O3 profiles and covariance matrices. During this work we investigate the climatological data to be used in TEMPO algorithms (TB O3) and simulated data from the NASA GMAO Goddard Earth Observing System (GEOS-5) Forward Processing (FP) near-real-time (NRT) model products. These two data products will be evaluated with ground-based lidar data from the Tropospheric Ozone Lidar Network (TOLNet) at various locations of the US. This study evaluates the TB climatology, GEOS-5 climatology, and 3-hourly GEOS-5 data compared to lower tropospheric observations to demonstrate the accuracy of a priori information to potentially be used in TEMPO O3 algorithms. Here we present our initial analysis and the theoretical impact on TEMPO retrievals in the lower troposphere

Ozone Lidar Observations for Air Quality Studies

Tropospheric ozone lidars are well suited to measuring the high spatio-temporal variability of this important trace gas. Furthermore, lidar measurements in conjunction with balloon soundings, aircraft, and satellite observations provide substantial information about a variety of atmospheric chemical and physical processes. Examples of processes elucidated by ozone-lidar measurements are presented, and modeling studies using WRF-Chem, RAQMS, and DALES/LES models illustrate our current understanding and shortcomings of these processes

Characterizing sources of high surface ozone events in the southwestern US with intensive field measurements and two global models

The detection and attribution of high background ozone (O3) events in the southwestern US is challenging but relevant to the effective implementation of the lowered National Ambient Air Quality Standard (NAAQS; 70&thinsp;ppbv). Here we leverage intensive field measurements from the Fires, Asian, and Stratospheric Transport&minus;Las Vegas Ozone Study (FAST-LVOS) in May&ndash;June&nbsp;2017, alongside high-resolution simulations with two global models (GFDL-AM4 and GEOS-Chem), to study the sources of O3 during high-O3 events. We show possible stratospheric influence on 4 out of the 10 events with daily maximum 8&thinsp;h average (MDA8) surface O3 above 65&thinsp;ppbv in the greater Las Vegas region. While O3 produced from regional anthropogenic emissions dominates pollution events in the Las Vegas Valley, stratospheric intrusions can mix with regional pollution to push surface O3 above 70&thinsp;ppbv. GFDL-AM4 captures the key characteristics of deep stratospheric intrusions consistent with ozonesondes, lidar profiles, and co-located measurements of O3, CO, and water vapor at Angel Peak, whereas GEOS-Chem has difficulty simulating the observed features and underestimates observed O3 by &sim;20&thinsp;ppbv at the surface. On days when observed MDA8 O3 exceeds 65&thinsp;ppbv and the AM4 stratospheric ozone tracer shows 20&ndash;40&thinsp;ppbv enhancements, GEOS-Chem simulates &sim;15&thinsp;ppbv lower US background O3 than GFDL-AM4. The two models also differ substantially during a wildfire event, with GEOS-Chem estimating &sim;15&thinsp;ppbv greater O3, in better agreement with lidar observations. At the surface, the two models bracket the observed MDA8 O3 values during the wildfire event. Both models capture the large-scale transport of Asian pollution, but neither resolves some fine-scale pollution plumes, as evidenced by aerosol backscatter, aircraft, and satellite measurements. US background O3 estimates from the two models differ by 5&thinsp;ppbv on average (greater in GFDL-AM4) and up to 15&thinsp;ppbv episodically. Uncertainties remain in the quantitative attribution of each event. Nevertheless, our multi-model approach tied closely to observational analysis yields some process insights, suggesting that elevated background O3 may pose challenges to achieving a potentially lower NAAQS level (e.g., 65&thinsp;ppbv) in the southwestern US. </div

TOLNET – A Tropospheric Ozone Lidar Profiling Network for Satellite Continuity and Process Studies

Ozone lidars measure continuous, high-resolution ozone profiles critical for process studies and for satellite validation in the lower troposphere. However, the effectiveness of lidar validation by using single-station data is limited. Recently, NASA initiated an interagency ozone lidar observation network under the name TOLNet to promote cooperative multiple-station ozone-lidar observations to provide highly timeresolved (few minutes) tropospheric-ozone vertical profiles useful for air-quality studies, model evaluation, and satellite validation. This article briefly describes the concept, stations, major specifications of the TOLNet instruments, and data archiving