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The TRacking Aerosol Convection ExpeRiment – Air Quality (TRACER-AQ) campaign probed Houston air quality with a comprehensive suite of ground-based and airborne remote sensing measurements during the intensive operating period in September 2021. Two post-frontal high-ozone episodes (6–11 and 23–26 September) were recorded during the aforementioned period. In this study, we evaluated the simulation of the planetary boundary layer (PBL) height and the vertical ozone profile by a high-resolution (1.33 km) 3-D photochemical model, the Weather Research and Forecasting (WRF)-driven GEOS-Chem (WRF-GC). We evaluated the PBL heights with a ceilometer at the coastal site La Porte and the airborne High Spectral Resolution Lidar 2 (HSRL-2) flying over urban Houston and adjacent waters. Compared with the ceilometer at La Porte, the model captures the diurnal variations in the PBL heights with a very strong temporal correlation (R>0.7) and ±20 % biases. Compared with the airborne HSRL-2, the model exhibits a moderate to strong spatial correlation (R=0.26–0.68), with ±20 % biases during the noon and afternoon hours during ozone episodes. For land–water differences in PBL heights, the water has shallower PBL heights compared to land. The model predicts larger land–water differences than the observations because the model consistently underestimates the PBL heights over land compared to water. We evaluated vertical ozone distributions by comparing the model against vertical measurements from the TROPospheric OZone lidar (TROPOZ), the HSRL-2, and ozonesondes, as well as surface measurements at La Porte from a model 49i ozone analyzer and one Continuous Ambient Monitoring Station (CAMS). The model underestimates free-tropospheric ozone (2–3 km aloft) by 9 %–22 % but overestimates near-ground ozone ( m aloft) by 6 %-39 % during the two ozone episodes. Boundary layer ozone (0.5–1 km aloft) is underestimated by 1 %–11 % during 8–11 September but overestimated by 0 %–7 % during 23–26 September. Based on these evaluations, we identified two model limitations, namely the single-layer PBL representation and the free-tropospheric ozone underestimation. These limitations have implications for the predictivity of ozone's vertical mixing and distribution in other models.

Coastal regions are susceptible to multiple complex dynamic and chemical mechanisms and emission sources that lead to frequently observed large tropospheric ozone variations. These large ozone variations occur on a mesoscale and have proven to be arduous to simulate using chemical transport models (CTMs). We present a clustering analysis of multi-dimensional measurements from ozone lidar in conjunction with both an offline GEOS-Chem chemical-transport model (CTM) simulation and the online GEOS-Chem simulation GEOS-CF, to investigate the vertical and temporal variability of coastal ozone during three recent air quality campaigns: 2017 Ozone Water-Land Environmental Transition Study (OWLETS)-1, 2018 OWLETS-2, and 2018 Long Island Sound Tropospheric Ozone Study (LISTOS). We developed and tested a clustering method that resulted in five ozone profile curtain clusters. The established five clusters all varied significantly in ozone magnitude vertically and temporally, which allowed us to characterize the coastal ozone behavior. The lidar clusters provided a simplified way to evaluate the two CTMs for their performance of diverse coastal ozone cases. An overall evaluation of the models reveals good agreement (R≈0.70) in the low-level altitude range (0 to 2000 m), with a low and unsystematic bias for GEOS-Chem and a high systemic positive bias for GEOS-CF. The mid-level (2000–4000 m) performances show a high systematic negative bias for GEOS-Chem and an overall low unsystematic bias for GEOS-CF and a generally weak agreement to the lidar observations (R=0.12 and 0.22, respectively). Evaluating cluster-by-cluster model performance reveals additional model insight that is overlooked in the overall model performance. Utilizing the full vertical and diurnal ozone distribution information specific to lidar measurements, this work provides new insights on model proficiency in complex coastal regions.

A TROPOspheric Monitoring Instrument (TROPOMI) validation campaign was held in the Netherlands based at the CESAR (Cabauw Experimental Site for Atmospheric Research) observatory during September 2019. The TROpomi vaLIdation eXperiment (TROLIX-19) consisted of active and passive remote sensing platforms in conjunction with several balloon-borne and surface chemical (e.g., ozone and nitrogen dioxide) measurements. The goal of this joint NASA-KNMI geophysical validation campaign was to make intensive observations in the TROPOMI domain in order to be able to establish the quality of the L2 satellite data products under realistic conditions, such as non-idealized conditions with varying cloud cover and a range of atmospheric conditions at a rural site. The research presented here focuses on using ozone lidars from NASA's Goddard Space Flight Center to better evaluate the characterization of ozone throughout TROLIX-19. Results of comparisons to the lidar systems with balloon, space-borne and ground-based passive measurements are shown. In addition, results are compared to a global coupled chemistry meteorology model to illustrate the vertical variability and columnar amounts of both tropospheric and stratospheric ozone during the campaign period.

The conventional two-wavelength differential absorption lidar (DIAL) has measured air pollutants such as nitrogen dioxide (NO2). However, high concentrations of aerosol within the planetary boundary layer (PBL) can cause significant retrieval errors using only a two-wavelength DIAL technique to measure NO2. We proposed a new technique to obtain more accurate measurements of NO2 using a three-wavelength DIAL technique based on an optical parametric oscillator (OPO) laser. This study derives the three-wavelength DIAL retrieval equations necessary to retrieve vertical profiles of NO2 in the troposphere. Additionally, two rules to obtain the optimum choice of the three wavelengths applied in the retrieval are designed to help increase the differences in the NO2 absorption cross-sections and reduce aerosol interference. NO2 retrieval relative uncertainties caused by aerosol extinction, molecular extinction, absorption of gases other than the gas of interest and backscattering are calculated using two-wavelength DIAL (438 and 439.5 nm) and three-wavelength DIAL (438, 439.5 and 441 nm) techniques. The retrieval uncertainties in aerosol extinction using the three-wavelength DIAL technique are reduced to less than 2 % of those when using the two-wavelength DIAL technique. Moreover, the retrieval uncertainty analysis indicates that the three-wavelength DIAL technique can reduce more fluctuation caused by aerosol backscattering than the two-wavelength DIAL technique. This study presents NO2 concentration profiles which were obtained using the HU (Hampton University) three-wavelength OPO DIAL. As a first step to assess the accuracy of the HU lidar NO2 profiles, we compared the NO2 profiles to simulated data from the Weather Research and Forecasting Chemistry (WRF-Chem) model. This comparison suggests that the NO2 profiles retrieved with the three-wavelength DIAL technique have similar vertical structure and magnitudes typically within ±0.1 ppb compared to modeled profiles.

A newly upgraded German Weather Service (DWD) ozone and temperature lidar (HOH) located at the Hohenpeißenberg Meteorological Observatory (47.8∘ N, 11.0∘ E) has been evaluated through comparison with the travelling standard lidar operated by NASA's Goddard Space Flight Center (NASA GSFC Stratospheric Ozone (STROZ) lidar), satellite overpasses from the Microwave Limb Sounder (MLS), the Sounding of the Atmosphere using Broadband Emission Radiometry (SABER), the Ozone Mapping and Profiler Suite (OMPS), meteorological radiosondes launched from Munich (65 km northeast), and locally launched ozonesondes. The “blind” evaluation was conducted under the framework of the Network for the Detection of Atmospheric Composition Change (NDACC) using 10 clear nights of measurements in 2018 and 2019. The campaign, referred to as the Hohenpeißenberg Ozone Profiling Study (HOPS), was conducted within the larger context of NDACC validation activities for European lidar stations. There was good agreement between all ozone lidar measurements in the range of 15 to 41 km with relative differences between co-located ozone profiles of less than ±10 %. Differences in the measured ozone number densities between the lidars and the locally launched ozone sondes were also generally less than 5 % below 30 km. The satellite ozone profiles demonstrated some differences with respect to the ground-based lidars which are due to sampling differences and geophysical variation. Both the original and new DWD lidars continue to meet the NDACC standard for lidar ozone profiles by exceeding 3 % accuracy between 16.5 and 43 km. Temperature differences for all instruments were less than ±5 K below 60 km, with larger differences present in the lidar–satellite comparisons above this region. Temperature differences between the DWD lidars met the NDACC accuracy requirements of ±1 K between 17 and 78 km. A unique cross-comparison between the HOPS campaign and a similar, recent campaign at Observatoire de Haute-Provence (Lidar Validation NDACC Experiment; LAVANDE) allowed for an investigation into potential biases in the NASA-STROZ reference lidar. The reference lidar may slightly underestimate ozone number densities above 43 km with respect to the French and German NDACC lidars. Below 20 km, the reference lidar temperatures profiles are 5 to 10 K cooler than the temperatures which are reported by the other instruments.

We report OH reactivity observations by a chemical ionization mass spectrometer–comparative reactivity method (CIMS-CRM) instrument in a suburban forest of the Seoul metropolitan area (SMA) during the Korea–United States Air Quality Study (KORUS-AQ 2016) from mid-May to mid-June of 2016. A comprehensive observational suite was deployed to quantify reactive trace gases inside of the forest canopy including a high-resolution proton transfer reaction time-of-flight mass spectrometer (PTR-ToF-MS). An average OH reactivity of 30.7±5.1 s−1 was observed, while the OH reactivity calculated from CO, NO+NO2 (NOx), ozone (O3), sulfur dioxide (SO2), and 14 volatile organic compounds (VOCs) was 11.8±1.0 s−1. An analysis of 346 peaks from the PTR-ToF-MS accounted for an additional 6.0±2.2 s−1 of the total measured OH reactivity, leaving 42.0 % missing OH reactivity. A series of analyses indicate that the missing OH reactivity most likely comes from VOC oxidation products of both biogenic and anthropogenic origin.

Aerosol retrieval using ozone lidars in the ultraviolet spectral region is challenging but necessary for correcting aerosol interference in ozone retrieval and for studying the ozone–aerosol correlations. This study describes the aerosol retrieval algorithm for a tropospheric ozone lidar, quantifies the retrieval error budget, and intercompares the aerosol retrieval products at 299 nm with those at 532 nm from a high spectral resolution lidar (HSRL) and with those at 340 nm from an AErosol RObotic NETwork radiometer. After the cloud-contaminated data are filtered out, the aerosol backscatter or extinction coefficients at 30 m and 10 min resolutions retrieved by the ozone lidar are highly correlated with the HSRL products, with a coefficient of 0.95 suggesting that the ozone lidar can reliably measure aerosol structures with high spatiotemporal resolution when the signal-to-noise ratio is sufficient. The actual uncertainties of the aerosol retrieval from the ozone lidar generally agree with our theoretical analysis. The backscatter color ratio (backscatter-related exponent of wavelength dependence) linking the coincident data measured by the two instruments at 299 and 532 nm is 1.34±0.11, while the Ångström (extinction-related) exponent is 1.49±0.16 for a mixture of urban and fire smoke aerosols within the troposphere above Huntsville, AL, USA.

A two-part intercomparison campaign was conducted at Observatoire de Haute-Provence (OHP) for the validation of lidar ozone and temperature profiles using the mobile NASA Stratospheric Ozone Lidar (NASA STROZ), satellite overpasses from the Microwave Limb Sounder (MLS), the Sounding of the Atmosphere using Broadband Emission Radiometry (SABER), meteorological radiosondes launched from Nîmes, and locally launched ozonesondes. All the data were submitted and compared “blind”, before the group could see results from the other instruments. There was good agreement between all ozone measurements between 20 and 40 km, with differences of generally less than 5 % throughout this region. Below 20 km, SABER and MLS measured significantly more ozone than the lidars or ozonesondes. Temperatures for all lidars were in good agreement between 30 and 60 km, with differences on the order of ±1 to 3 K. Below 30 km, the OHP lidar operating at 532 nm has a significant cool bias due to contamination by aerosols. Systematic, altitude-varying bias up to ±5 K compared to the lidars was found for MLS at many altitudes. SABER temperature profiles are generally closer to the lidar profiles, with up 3 K negative bias near 50 km. Total uncertainty estimates for ozone and temperature appear to be realistic for nearly all systems. However, it does seem that the very low estimated uncertainties of lidars between 30 and 50 km, between 0.1 and 1 K, are not achieved during Lidar Validation Network for the Detection of Atmospheric Composition Change (NDACC) Experiment (LAVANDE). These estimates might have to be increased to 1 to 2 K.

Nitryl chloride (ClNO2) is a radical reservoir species that releases chlorine radicals upon photolysis. An integrated analysis of the impact of ClNO2 on regional photochemistry in the Seoul metropolitan area (SMA) during the Korea–United States Air Quality Study (KORUS-AQ) 2016 field campaign is presented. Comprehensive multiplatform observations were conducted aboard the NASA DC-8 and at two ground sites (Olympic Park, OP; Taehwa Research Forest, TRF), representing an urbanized area and a forested suburban region, respectively. Positive correlations between daytime Cl2 and ClNO2 were observed at both sites, the slope of which was dependent on O3 levels. The possible mechanisms are explored through box model simulations constrained with observations. The overall diurnal variations in ClNO2 at both sites appeared similar but the nighttime variations were systematically different. For about half of the observation days at the OP site the level of ClNO2 increased at sunset but rapidly decreased at around midnight. On the other hand, high levels were observed throughout the night at the TRF site. Significant levels of ClNO2 were observed at both sites for 4–5 h after sunrise. Airborne observations, box model calculations, and back-trajectory analysis consistently show that these high levels of ClNO2 in the morning are likely from vertical or horizontal transport of air masses from the west. Box model results show that chlorine-radical-initiated chemistry can impact the regional photochemistry by elevating net chemical production rates of ozone by ∼25 % in the morning.

During the May–June 2016 International Cooperative Air Quality Field Study in Korea (KORUS-AQ), light synoptic meteorological forcing facilitated Seoul metropolitan pollution outflow to reach the remote Taehwa Research Forest (TRF) site and cause regulatory exceedances of ozone on 24 days. Two of these severe pollution events are thoroughly examined. The first, occurring on 17 May 2016, tracks transboundary pollution transport exiting eastern China and the Yellow Sea, traversing the Seoul Metropolitan Area (SMA), and then reaching TRF in the afternoon hours with severely polluted conditions. This case study indicates that although outflow from China and the Yellow Sea were elevated with respect to chemically unperturbed conditions, the regulatory exceedance at TRF was directly linked in time, space, and altitude to urban Seoul emissions. The second case studied, which occurred on 9 June 2016, reveals that increased levels of biogenic emissions, in combination with amplified urban emissions, were associated with severe levels of pollution and a regulatory exceedance at TRF. In summary, domestic emissions may be causing more pollution than by transboundary pathways, which have been historically believed to be the major source of air pollution in South Korea. The case studies are assessed with multiple aircraft, model (photochemical and meteorological) simulations, in situ chemical sampling, and extensive ground-based profiling at TRF. These observations clearly identify TRF and the surrounding rural communities as receptor sites for severe pollution events associated with Seoul outflow, which will result in long-term negative effects to both human health and agriculture in the affected areas.

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.

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.

Data from ground-based ozone (O3) vertical profiling platforms operated during the FRAPPE/DISCOVER-AQ campaigns in summer 2014 were used to characterize key processes responsible for establishing O3 profile development in the boundary layer in the Northern Colorado Front Range. Morning mixing from the upper boundary layer and lower free troposphere into the lower boundary layer was the key process establishing the mid-morning boundary layer O3 mixing ratio. Photochemical O3 production throughout the boundary layer builds on the mid-morning profile. From late morning to mid-afternoon the continuing O3 increase was nearly uniform through the depth of the profile measured by the tethersonde (~400 m). Ozonesondes flown on a near daily schedule over a four week period with multiple profiles on a number of days captured the full 1500 to 2000 m vertical extent of O3 enhancements in the mixed boundary layer confirming O3 production throughout the entire boundary layer. Continuous O3 measurements from the Boulder Atmospheric Observatory (BAO) tall tower at 6 m and 300 m showed hourly O3 at the 6 m level ≥75 ppb on 15% of the days. The diurnal variation on these days followed a pattern similar to that seen in the tethersonde profiles. The association of high O3 days at the BAO tower with transport from sectors with intense oil and natural gas production toward the northeast suggests emissions from this industry were an important source of O3 precursors and are crucial in producing peak O3 events in the NCFR. Higher elevation locations to the west of the NCFR plains regularly experience higher O3 values than those in the lower elevation NCFR locations. Exposure of populations in these areas is not captured by the current regulatory network, and likely underestimated in population O3 exposure assessments.

The main purpose of the NASA Goddard Space Flight Center TROPospheric OZone DIfferential Absorption Lidar (GSFC TROPOZ DIAL) is to measure the vertical distribution of tropospheric ozone for science investigations. Because of the important health and climate impacts of tropospheric ozone, it is imperative to quantify background photochemical ozone concentrations and ozone layers aloft, especially during air quality episodes. For these reasons, this paper addresses the necessary procedures to validate the TROPOZ retrieval algorithm and confirm that it is properly representing ozone concentrations. This paper is focused on ensuring the TROPOZ algorithm is properly quantifying ozone concentrations, and a following paper will focus on a systematic uncertainty analysis. This methodology begins by simulating synthetic lidar returns from actual TROPOZ lidar return signals in combination with a known ozone profile. From these synthetic signals, it is possible to explicitly determine retrieval algorithm biases from the known profile. This was then systematically performed to identify any areas that need refinement for a new operational version of the TROPOZ retrieval algorithm. One immediate outcome of this exercise was that a bin registration error in the correction for detector saturation within the original retrieval was discovered and was subsequently corrected for. Another noticeable outcome was that the vertical smoothing in the retrieval algorithm was upgraded from a constant vertical resolution to a variable vertical resolution to yield a statistical uncertainty of opt) has been effective in retrieving nearly 200 m lower to the surface. Also, as compared to the previous version of the retrieval, the TROPOZopt had an overall mean improvement of 3.5 %, and large improvements (upwards of 10–15 % as compared to the previous algorithm) were apparent between 4.5 and 9 km. Finally, to ensure the TROPOZopt retrieval algorithm is robust enough to handle actual lidar return signals, a comparison is shown between four nearby ozonesonde measurements. The ozonesondes are mostly within the TROPOZopt retrieval uncertainty bars, which implies that this exercise was quite successful.

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.