Tropospheric Ozone Lidar Network Research Articles

Evaluation of WRF-Chem air quality forecasts during the AEROMMA and STAQS 2023 field campaigns

ABSTRACT A real-time air quality forecasting system was developed using the Weather Research and Forecasting model coupled with Chemistry (WRF-Chem) to provide support for flight planning activities during the NOAA Atmospheric Emissions and Reactions Observed from Megacities to Marine Areas (AEROMMA) and NASA Synergistic TEMPO Air Quality Science (STAQS) 2023 field campaigns. The forecasting system operated on two separate domains centered on Chicago, IL, and New York City, NY, and provided 72-hour predictions of atmospheric composition, aerosols, and clouds. This study evaluates the Chicago-centered forecasting system’s 1-, 2-, and 3-day ozone (O3) forecast skill for Chiwaukee Prairie, WI, a rural area downwind of Chicago that often experiences high levels of O3 pollution. Comparisons to vertical O3 profiles collected by a Tropospheric Ozone Lidar Network (TOLNet) instrument revealed that forecast skill decreases as forecast lead time increases. When compared to surface measurements, the forecasting system tended to underestimate O3 concentrations on high O3 days and overestimate on low O3 days at Chiwaukee Prairie regardless of forecast lead time. Using July 25, 2023, as a case study, analyses show that the forecasts underestimated peak O3 levels at Chiwaukee Prairie during this regionwide bad air quality day. Wind speed and direction data indicates that this underestimation can partially be attributed to lake breeze simulation errors. Surface fine particulate matter (PM2.5) measurements, Geostationary Operational Environmental Satellite-16 (GOES-16) aerosol optical depth (AOD) data, and back trajectories from the NOAA Hybrid Single-Particle Lagrangian Integrated Trajectory (HYSPLIT) model show that transported Canadian wildfire smoke impacted the Lake Michigan region on this day. Errors in the forecasted chemical composition and transport of the smoke plumes also contributed to underpredictions of O3 levels at Chiwaukee Prairie on July 25, 2023. The results of this work help identify improvements that can be made for future iterations of the WRF-Chem forecasting system. Implications: Air quality forecasting is an important tool that can be used to inform the public about upcoming high pollution days so that individuals may plan accordingly to limit their exposure to health-damaging air pollutants. Forecasting also helps scientists make decisions about where to make observations during air quality field campaigns. A variety of observational datasets were used to evaluate the accuracy of an air quality forecasting system that was developed for NOAA and NASA field campaigns that occurred in the summer of 2023. These evaluations inform areas of improvement for future development of this air quality forecasting system.

TOLNet validation of satellite ozone profiles in the troposphere: impact of retrieval wavelengths

Abstract. The Tropospheric Ozone Lidar Network (TOLNet) was used to validate retrievals of ozone (O3) profiles in the troposphere from the TROPOspheric Monitoring Instrument (TROPOMI) ultraviolet (UV), Cross-track Infrared Sounder (CrIS) infrared (IR), and a combined UV + IR wavelength retrieval from TROPOMI/CrIS. Observations from six separate ground-based lidar systems and various locations of ozonesondes distributed throughout North America and in the Netherlands were used to quantify systematic bias and random errors for each satellite retrieval. Furthermore, TOLNet data were used to intercompare idealized UV, IR, and UV + IR convolved lidar profiles of O3 in the troposphere during case studies representative of high-O3 events. This study shows that the improved sensitivity and vertical resolution in UV + IR retrievals in the middle- and upper-troposphere resulted in tropospheric degree of freedom (DOF) values ∼ 33 % higher compared to UV- and IR-only retrievals. The increased DOFs in the UV + IR retrievals allowed for improved reproduction of mid- and upper-tropospheric O3 enhancements and, to a lesser degree, near-surface pollution enhancements compared to single-wavelength satellite products. The validation of O3 profiles in the troposphere retrieved with the UV-only, IR-only, and UV + IR Tikhonov regularised Ozone Profile retrievAl with SCIATRAN (TOPAS) algorithm developed at the Institute for Environmental Physics, University of Bremen, demonstrated the utility of using TOLNet as a satellite evaluation data set. TOPAS UV-only, IR-only, and UV + IR wavelength retrievals had systematic biases, quantified with normalized mean bias, throughout the troposphere of 11.2 ppb (22.1 %), −1.7 ppb (−0.3 %), and 3.5 ppb (7.8 %), respectively, which meet the tropospheric systematic bias requirements defined by the science teams for the TROPOMI and CrIS sensors. The primary drivers of systematic bias were determined to be solar zenith angle, surface albedo, and cloud fraction. Random errors, representative of uncertainty in the retrievals and quantified by root mean squared errors (RMSEs), were large for all three retrievals, with UV-only, IR-only, and UV + IR wavelength retrievals having RMSEs throughout the troposphere of 17.4 ppb (19.8 % of mean tropospheric column values), 10.5 ppb (12.6 % of mean tropospheric column values), and 14.0 ppb (14.6 % of mean tropospheric column values), respectively. TOPAS UV-only profiles did not meet the uncertainty requirements defined for TROPOMI for the troposphere; however, CrIS IR-only retrievals did meet the uncertainty requirements defined by this mission. The larger random errors reflect the challenge of retrieving daily O3 profiles due to the limited sensitivity and vertical resolution of these retrievals in the troposphere. Tropospheric systematic biases and random error were lower in IR-only and combined UV + IR retrievals compared to UV-only products due to the increased sensitivity in the troposphere allowing the retrievals to deviate further from the a priori profiles. Observations from TOLNet demonstrated that the performance of the three satellite products varied by season and altitude in the troposphere. TOLNet was shown to result in similar validation statistics compared to ozonesonde data, which are a commonly used satellite evaluation data source, demonstrating that TOLNet is a sufficient source of satellite O3 profile validation data in the troposphere, which is critical as this data source is the primary product identified for the tropospheric O3 validation of the recently launched Tropospheric Emissions: Monitoring of Pollution (TEMPO) mission.

Retrieval of UVB aerosol extinction profiles from the ground-based Langley Mobile Ozone Lidar (LMOL) system

Abstract. Aerosols emitted from wildfires are becoming one of the main sources of poor air quality on the US mainland. Their extinction in UVB (the wavelength range from 280 to 315 nm) is difficult to retrieve using simple lidar techniques because of the impact of ozone (O3) absorption and the lack of information about the lidar ratios at those wavelengths. Improving the characterization of lidar ratios at the abovementioned wavelengths will enable aerosol monitoring with different instruments and will also permit the correction of the aerosol impact on O3 lidar data. The 2018 Long Island Sound Tropospheric Ozone Study (LISTOS) campaign in the New York City region utilized a comprehensive set of instruments that enabled the characterization of the lidar ratio for UVB aerosol retrieval. The NASA Langley High Altitude Lidar Observatory (HALO) produced the 532 nm aerosol extinction product along with the lidar ratio for this wavelength using a high-spectral-resolution technique. The Langley Mobile Ozone Lidar (LMOL) is able to compute the extinction provided that it has the lidar ratio at 292 nm. The lidar ratio at 292 nm and the Ångström exponent (AE) between 292 and 532 nm for the aerosols were retrieved by comparing the two observations using an optimization technique. We evaluate the aerosol extinction error due to the selection of these parameters, usually done empirically for 292 nm lasers. This is the first known 292 nm aerosol product intercomparison between HALO and Tropospheric Ozone Lidar Network (TOLNet) O3 lidar. It also provides the characterization of the UVB optical properties of aerosols in the lower troposphere affected by transported wildfire emissions.

A Case Study of Ozone Diurnal Variation in the Convective Boundary Layer in the Southeastern United States Using Multiple Observations and Large-Eddy Simulation

We investigated the diurnal ozone variation on 6 September 2013 in a midsize urban environment using multiple in situ and remote-sensing measurements along with the Dutch atmospheric large-eddy simulation (DALES) model coupled with a chemical module and a dry deposition module that we added for this study. Our study area was Huntsville, Alabama, USA, a typical midsize city in the Southeastern United States. The ozone variation in the convective boundary layer (CBL) resulted mainly from local emissions and photochemical production stemming from weather conditions controlled by an anticyclonic system on that day. Local chemical production contributes approximately two thirds of the ozone enhancement in the CBL and, in this case, dynamical processes including ozone transport from the free troposphere (FT) to the CBL through the entrainment processes contributed the remainder. The numerical experiments performed by the large-eddy simulation (LES) model showed acceptable agreement with the TOLNet (The tropospheric ozone lidar network)/RO3QET (Rocket-city ozone quality evaluation in the troposphere) ozone DIAL (differential absorption lidar) observations. This study indicated the need for fine-scale, three-dimensional ozone observations with high temporal and spatial resolution for air quality studies at the urban scale and smaller.

Validation of the TOLNet lidars: the Southern California Ozone Observation Project (SCOOP)

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

Evaluation of potential sources of a priori ozone profiles for TEMPO tropospheric ozone retrievals

Abstract. Potential sources of a priori ozone (O3) profiles for use in Tropospheric Emissions: Monitoring of Pollution (TEMPO) satellite tropospheric O3 retrievals are evaluated with observations from multiple Tropospheric Ozone Lidar Network (TOLNet) systems in North America. An O3 profile climatology (tropopause-based O3 climatology (TB-Clim), currently proposed for use in the TEMPO O3 retrieval algorithm) derived from ozonesonde observations and O3 profiles from three separate models (operational Goddard Earth Observing System (GEOS-5) Forward Processing (FP) product, reanalysis product from Modern-era Retrospective Analysis for Research and Applications version 2 (MERRA2), and the GEOS-Chem chemical transport model (CTM)) were: (1) evaluated with TOLNet measurements on various temporal scales (seasonally, daily, and hourly) and (2) implemented as a priori information in theoretical TEMPO tropospheric O3 retrievals in order to determine how each a priori impacts the accuracy of retrieved tropospheric (0–10 km) and lowermost tropospheric (LMT, 0–2 km) O3 columns. We found that all sources of a priori O3 profiles evaluated in this study generally reproduced the vertical structure of summer-averaged observations. However, larger differences between the a priori profiles and lidar observations were calculated when evaluating inter-daily and diurnal variability of tropospheric O3. The TB-Clim O3 profile climatology was unable to replicate observed inter-daily and diurnal variability of O3 while model products, in particular GEOS-Chem simulations, displayed more skill in reproducing these features. Due to the ability of models, primarily the CTM used in this study, on average to capture the inter-daily and diurnal variability of tropospheric and LMT O3 columns, using a priori profiles from CTM simulations resulted in TEMPO retrievals with the best statistical comparison with lidar observations. Furthermore, important from an air quality perspective, when high LMT O3 values were observed, using CTM a priori profiles resulted in TEMPO LMT O3 retrievals with the least bias. The application of near-real-time (non-climatological) hourly and daily model predictions as the a priori profile in TEMPO O3 retrievals will be best suited when applying this data to study air quality or event-based processes as the standard retrieval algorithm will still need to use a climatology product. Follow-on studies to this work are currently being conducted to investigate the application of different CTM-predicted O3 climatology products in the standard TEMPO retrieval algorithm. Finally, similar methods to those used in this study can be easily applied by TEMPO data users to recalculate tropospheric O3 profiles provided from the standard retrieval using a different source of a priori.

TOLNet ozone lidar intercomparison during the discover-aq and frappé campaigns

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.

Coordinated profiling of stratospheric intrusions and transported pollution by the Tropospheric Ozone Lidar Network (TOLNet) and NASA Alpha Jet experiment (AJAX): Observations and comparison to HYSPLIT, RAQMS, and FLEXPART

Ground-based lidars and ozonesondes belonging to the NASA-supported Tropospheric Ozone Lidar Network (TOLNet) are used in conjunction with the NASA Alpha Jet Atmospheric eXperiment (AJAX) to investigate the transport of stratospheric ozone and entrained pollution into the lower troposphere above the United States on May 24–25, 2013. TOLNet and AJAX measurements made in California, Nevada, and Alabama are compared to tropospheric ozone retrievals from the Atmospheric Infrared Sounder (AIRS), to back trajectories from the NOAA Air Resources Laboratory (ARL) Hybrid Single Particle Lagrangian Integrated Trajectory (HYSPLIT) model, and to analyses from the NOAA/NESDIS Real-time Air Quality Modeling System (RAQMS) and FLEXPART particle dispersion model. The measurements and model analyses show much deeper descent of ozone-rich upper tropospheric/lower stratospheric air above the Desert Southwest than above the Southeast, and comparisons to surface measurements from regulatory monitors reporting to the U.S. EPA Air Quality System (AQS) suggest that there was a much greater surface impact in the Southwest including exceedances of the 2008 National Ambient Air Quality Standard (NAAQS) of 0.075 ppm in both Southern California and Nevada. Our analysis demonstrates the potential benefits to be gained by supplementing the existing surface ozone network with coordinated upper air observations by TOLNet.

Quantifying TOLNet Ozone Lidar Accuracy during the 2014 DISCOVER-AQ and FRAPPÉ 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 cross-instrument 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. In terms of the range-resolving capability, 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 very good measurement accuracy for these three TOLNet lidars, making them suitable for use in air quality, satellite validation, and ozone modeling efforts.

Evaluating Summer-Time Ozone Enhancement Events in the Southeast United States

This study evaluates source attribution of ozone (O3) in the southeast United States (US) within O3 lamina observed by the University of Alabama in Huntsville (UAH) Tropospheric Ozone Lidar Network (TOLNet) system during June 2013. This research applies surface-level and airborne in situ data and chemical transport model simulations (GEOS-Chem) in order to quantify the impact of North American anthropogenic emissions, wildfires, lightning NOx, and long-range/stratospheric transport on the observed O3 lamina. During the summer of 2013, two anomalous O3 layers were observed: (1) a nocturnal near-surface enhancement and (2) a late evening elevated (3–6 km above ground level) O3 lamina. A “brute force” zeroing method was applied to quantify the impact of individual emission sources and transport pathways on the vertical distribution of O3 during the two observed lamina. Results show that the nocturnal O3 enhancement on 12 June 2013 below 3 km was primarily due to wildfire emissions and the fact that daily maximum anthropogenic emission contributions occurred during these night-time hours. During the second case study it was predicted that above average contributions from long-range/stratospheric transport was largely contributing to the O3 lamina observed between 3 and 6 km on 29 June 2013. Other models, remote-sensing observations, and ground-based/airborne in situ data agree with the source attribution predicted by GEOS-Chem simulations. Overall, this study demonstrates the dynamic atmospheric chemistry occurring in the southeast US and displays the various emission sources and transport processes impacting O3 enhancements at different vertical levels of the troposphere.

Characterizing the Vertical Processes of Ozone in Colorado’s Front Range Using the GSFC Ozone DIAL

Although characterizing the interactions of ozone throughout the entire troposphere are important for health and climate processes, there is a lack of routine measurements of vertical profiles within the United States. In order to monitor this lower ozone more effectively, the National Aeronautics and Space Administration (NASA) Goddard Space Flight Center TROPospheric OZone DIfferential Absorption Lidar (GSFC TROPOZ DIAL) has been developed and validated within the Tropospheric Ozone Lidar Network (TOLNet). Two scientifically interesting ozone episodes are presented that were observed during the 2014 Deriving Information on Surface Conditions from Column and Vertically Resolved Observations Relevant to Air Quality (DISCOVER AQ) campaign at Ft. Collins, Colorado.The first case study, occurring between 22-23 July 2014, indicates enhanced concentrations of ozone at Ft. Collins during nighttime hours, which was due to the complex recirculation of ozone within the foothills of the Rocky Mountain region. Although quantifying the ozone increase aloft during recirculation episodes has been historically difficult, results indicate that an increase of 20 - 30 ppbv of ozone at the Ft. Collins site has been attributed to this recirculation. The second case, occurring between Aug 4-8th 2014, characterizes a dynamical exchange of ozone between the stratosphere and the troposphere. This case, along with seasonal model parameters from previous years, is used to estimate the stratospheric contribution to the Rocky Mountain region. Results suggest that a large amount of stratospheric air is residing in the troposphere in the summertime near Ft. Collins, CO. The results also indicate that warmer tropopauses are correlated with an increase in stratospheric air below the tropopause in the Rocky Mountain Region.

A mobile differential absorption lidar to measure sub-hourly fluctuation of tropospheric ozone profiles in the Baltimore–Washington, D.C. region

Abstract. Tropospheric ozone profiles have been retrieved from the new ground-based National Aeronautics and Space Administration (NASA) Goddard Space Flight Center TROPospheric OZone DIfferential Absorption Lidar (GSFC TROPOZ DIAL) in Greenbelt, MD (38.99° N, 76.84° W, 57 m a.s.l.), from 400 m to 12 km a.g.l. Current atmospheric satellite instruments cannot peer through the optically thick stratospheric ozone layer to remotely sense boundary layer tropospheric ozone. In order to monitor this lower ozone more effectively, the Tropospheric Ozone Lidar Network (TOLNet) has been developed, which currently consists of five stations across the US. The GSFC TROPOZ DIAL is based on the DIAL technique, which currently detects two wavelengths, 289 and 299 nm, with multiple receivers. The transmitted wavelengths are generated by focusing the output of a quadrupled Nd:YAG laser beam (266 nm) into a pair of Raman cells, filled with high-pressure hydrogen and deuterium, using helium as buffer gas. With the knowledge of the ozone absorption coefficient at these two wavelengths, the range-resolved number density can be derived. An interesting atmospheric case study involving the stratospheric–tropospheric exchange (STE) of ozone is shown, to emphasize the regional importance of this instrument as well as to assess the validation and calibration of data. There was a low amount of aerosol aloft, and an iterative aerosol correction has been performed on the retrieved data, which resulted in less than a 3 ppb correction to the final ozone concentration. The retrieval yields an uncertainty of 16–19% from 0 to 1.5 km, 10–18% from 1.5 to 3 km, and 11–25% from 3 to 12 km according to the relevant aerosol concentration aloft. There are currently surface ozone measurements hourly and ozonesonde launches occasionally, but this system will be the first to make routine tropospheric ozone profile measurements in the Baltimore–Washington, D.C. area.