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

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.

Ground-based lidar for atmospheric boundary layer ozone measurements.

Ground-based lidars are suitable for long-term ozone monitoring as a complement to satellite and ozonesonde measurements. However, current ground-based lidars are unable to consistently measure ozone below 500 m above ground level (AGL) due to both engineering issues and high retrieval sensitivity to various measurement errors. In this paper, we present our instrument design, retrieval techniques, and preliminary results that focus on the high-temporal profiling of ozone within the atmospheric boundary layer (ABL) achieved by the addition of an inexpensive and compact mini-receiver to the previous system. For the first time, to the best of our knowledge, the lowest, consistently achievable observation height has been extended down to 125 m AGL for a ground-based ozone lidar system. Both the analysis and preliminary measurements demonstrate that this lidar measures ozone with a precision generally better than ±10% at a temporal resolution of 10 min and a vertical resolution from 150 m at the bottom of the ABL to 550 m at the top. A measurement example from summertime shows that inhomogeneous ozone aloft was affected by both surface emissions and the evolution of ABL structures.

Ozone Variability and Anomalies Observed during SENEX and SEAC4RS Campaigns in 2013.

Tropospheric ozone variability occurs because of multiple forcing factors including surface emission of ozone precursors, stratosphere-to-troposphere transport (STT), and meteorological conditions. Analyses of ozonesonde observations made in Huntsville, AL, during the peak ozone season (May to September) in 2013 indicate that ozone in the planetary boundary layer was significantly lower than the climatological average, especially in July and August when the Southeastern United States (SEUS) experienced unusually cool and wet weather. Because of a large influence of the lower stratosphere, however, upper-tropospheric ozone was mostly higher than climatology, especially from May to July. Tropospheric ozone anomalies were strongly anti-correlated (or correlated) with water vapor (or temperature) anomalies with a correlation coefficient mostly about 0.6 throughout the entire troposphere. The regression slopes between ozone and temperature anomalies for surface up to mid-troposphere are within 3.0-4.1 ppbv·K-1. The occurrence rates of tropospheric ozone laminae due to STT are ≥50% in May and June and about 30% in July, August and September suggesting that the stratospheric influence on free-tropospheric ozone could be significant during early summer. These STT laminae have a mean maximum ozone enhancement over the climatology of 52±33% (35±24 ppbv) with a mean minimum relative humidity of 2.3±1.7%.

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.

Fourier transform infrared spectroscopy of size-segregated aerosol deposits on foil substrates.

A method based on Fourier transform infrared (FTIR) double-pass transmittance spectroscopy was developed for determining functional group loading in size-segregated ambient aerosol deposits. The impactor employed for sample collection utilized rotating stages, which produced uniform particulate matter (PM) deposits on standard Al foil substrates. Each sample was analyzed without extraction using an FTIR spectrometer equipped with a reflectometer accessory. The use of the reflectometer obviated the need for infrared window materials as substrates. (NH(4))(2)SO(4) aerosol generated under laboratory conditions were used to calibrate deposit mass to the band strength of the relatively isolated nu(4) bending mode of SO(2-)(4) centered near 620 cm(-1). Atmospheric PM was sampled during the summer of 2004 in Huntsville, Ala. Sulfate concentrations determined in this initial study correlated well with measurements made by collocated EPA air samplers.

Tropospheric ozone profiles from a ground-based ultraviolet spectrometer: a new retrieval method.

We present, to the best of our knowledge, a new method to retrieve tropospheric ozone (O3) profiles from ground-based ultraviolet spectroscopic measurements. This method utilizes radiance spectra in the Huggins bands (i.e., 300-340 nm) measured at three off-axis angles (e.g., 45 degrees, 75 degrees, and 85 degrees) normalized to direct-Sun irradiances or zenith-sky radiances with the total column O3 derived from direct-Sun or zenith-sky measurements as a constraint. The vertical resolution of the retrieved O3 values ranges from approximately 3 km near the surface to approximately 12 km at 20 km altitude. This method can be used to measure diurnal variation of tropospheric O3 profiles and is complementary to the Umkehr method that mainly measures ozone profiles in the stratosphere.

Mapping tropospheric ozone profiles from an airborne ultraviolet-visible spectrometer.

We present a novel technique for retrieving ozone (O3) profiles and especially tropospheric O3 from airborne UV/visible spectrometer measurements. This technique utilizes radiance spectra from one down-looking and two up-looking (85 degrees and 75 degrees) directions, taking advantage of the O3 absorption structure in the Huggins (300-340-nm) and Chappuis (530-650-nm) bands. This technique is especially sensitive to tropospheric O3 below and < or =8 km above the aircraft with a vertical resolution of 2-6 km and is sensitive to lower and middle stratospheric O3 with a vertical resolution of 8-15 km. It can measure tropospheric O3 at spatial resolutions of 2 km x 2 km or higher and is therefore well suited for regional air-quality studies and validation of satellite measurements.

Optimal eigenanalysis for the treatment of aerosols in the retrieval of atmospheric composition from transmission measurements.

The separation of the individual contributions of aerosol and gases to the total attenuation of radiation through the atmosphere has been the subject of much scientific investigation since remote sensing experiments first began. We describe a new scheme to account for the spectral variation of the aerosol extinction in the inversion of transmission data from occultation measurements. Because the spectral variation of the aerosol extinction is generally unknown,the inversion problem is underdetermined and cannot be solved without a reduction in the number of unknowns in the set of equations used to describe the attenuation at each wavelength. This reduction can be accomplished by a variety of methods, including use of a priori information, the parameterization of the aerosol spectral attenuation, and the specification of the form of the aerosol size distribution. We have developed and implemented a parameterization scheme based on existing empirical and modeled information about the microphysical properties of aerosols. This scheme employs the eigenvectors from an extensive set of simulations to parameterize the aerosol extinction coefficient for incorporation into the inversion algorithm. We examine the accuracy of our method using data sets containing over 24,000 extinction spectra and compare it with that of another scheme that is currently implemented in the Polar Ozone and Aerosol Measurement (POAM) satellite experiment. In simulations using 80 wavelengths in the UV-visible-near-IR spectral range of the Stratospheric Aerosol and Gas Experiment III (SAGE) instrument, we show that, for our optimal parameterization, errors below 1% are observed in 80% of cases, whereas only approximately 20% of all cases are as accurate as this in a quadratic parameterization employing the logarithm of the wavelength.

Atmospheric Trace Molecule Spectroscopy (ATMOS) Experiment Version 3 data retrievals.

Version 3 of the Atmospheric Trace Molecule Spectroscopy (ATMOS) experiment data set for some 30 trace and minor gas profiles is available. From the IR solar-absorption spectra measured during four Space Shuttle missions (in 1985, 1992, 1993, and 1994), profiles from more than 350 occultations were retrieved from the upper troposphere to the lower mesosphere. Previous results were unreliable for tropospheric retrievals, but with a new global-fitting algorithm profiles are reliably returned down to altitudes as low as 6.5 km (clouds permitting) and include notably improved retrievals of H2O, CO, and other species. Results for stratospheric water are more consistent across the ATMOS spectral filters and do not indicate a net consumption of H2 in the upper stratosphere. A new sulfuric-acid aerosol product is described. An overview of ATMOS Version 3 processing is presented with a discussion of estimated uncertainties. Differences between these Version 3 and previously reported Version 2 ATMOS results are discussed. Retrievals are available at http://atmos.jpl.nasa.gov/atmos.