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PACE Technical Report Series, Volume 7: Ocean Color Instrument (OCI) Concept Design Studies

Extending OCI hyperspectral radiance measurements in the ultraviolet to 320 nm on the blue spectrograph enables quantitation of atmospheric total column ozone (O3) for use in ocean color atmospheric correction algorithms. The strong absorption by atmospheric ozone below 340 nm enables the quantification of total column ozone. Other applications are possible but were not investigated due to their exploratory nature and lower priority.The first step in the atmospheric correction processing, which converts top-of-the-atmosphere radiances to water-leaving radiances, is removal of the absorbance by atmospheric trace gases such as water vapor, oxygen, ozone and nitrogen dioxide. Details of the atmospheric correction process currently used by the Ocean Biology Processing Group (OBPG) and will be employed for PACE with appropriate modifications, are described by Mobley et al. [2016]. Atmospheric ozone absorbs within the visible to near-infrared spectrum between ~450 nm and 800nm and most appreciably between 530 nm and 650 nm, a spectral region critical for maintaining NASA's chlorophyll-a climate data record and for PACE algorithms planned to characterize phytoplankton community composition and other ocean color products.While satellite-based observations will likely be available during PACE's mission lifetime, the difference in acquisition time with PACE, the coarseness in their spatial resolution, and differences in viewing geometries will introduce significant levels of uncertainties in PACE ocean color data products.

Cetinic, Ivona↗

Attribution of Chemistry-Climate Model Initiative (CCMI) Ozone Radiative Flux Bias from Satellites

The top-of-atmosphere (TOA) outgoing longwave flux over the 9.6-μm ozone band is a fundamental quantity for understanding chemistry-climate coupling. However, observed TOA fluxes are hard to estimate as they exhibit considerable variability in space and time that depend on the distributions of clouds, ozone (O3), water vapor (H2O), air temperature (Ta), and surface temperature (Ts). Benchmarking present day fluxes and quantifying the relative influence of their drivers is the first step for estimating climate feedbacks from ozone radiative forcing and predicting radiative forcing evolution. To that end, we constructed observational instantaneous radiative kernels (IRKs) under clear-sky conditions, representing the sensitivities of the TOA flux in the 9.6-μm ozone band to the vertical distribution of geophysical variables, including O3, H2O, Ta, and Ts based upon the Aura Tropospheric Emission Spectrometer (TES) measurements. Applying these kernels to present-day simulations from the Chemistry-Climate Model Initiative (CCMI) project as compared to a 2006 reanalysis assimilating satellite observations, we show that the models have large differences in TOA flux, attributable to different geophysical variables. In particular, model simulations continue to diverge from observations in the tropics, as reported in previous studies of the Atmospheric Chemistry Climate Model Inter-comparison Project (ACCMIP) simulations. The principal culprits are tropical mid and upper tropospheric ozone followed by tropical lower tropospheric H2O. Five models out of the eight studied here have TOA flux biases exceeding 100 mWm-2 attributable to tropospheric ozone bias. Another set of five models have flux biases over 50 mWm-2 due to H2O. On the other hand, Ta radiative bias is negligible in all models (no more than 30 mWm-2). We found that AM3 and CMAM have the lowest TOA flux biases globally but are a result of cancellation of opposite biases due to difference processes. Overall, the multi-model ensemble mean bias is –133±98 mWm-2, indicating that they are too atmospherically opaque due to trapping too much radiation in the atmosphere by overestimated tropical tropospheric O3 and H2O. Having too much O3 and H2O in the troposphere would have different impacts on the sensitivity of TOA flux to O3 and these competing effects add more uncertainties on the ozone radiative forcing. We find that the inter-model TOA outgoing longwave radiation (OLR) difference is well anti-correlated with their ozone band flux bias. This suggests that there is significant radiative compensation in the calculation of model outgoing longwave radiation.

Aura Tropospheric Emission Spectrometer (TES) meas↗

Airborne DIAL Ozone and Aerosol Trends Observed at High Latitudes Over North America from February to May 2000

Ozone (O3) and aerosol scattering ratio profiles were obtained from airborne lidar measurements on thirty-eight aircraft flights over seven aircraft deployments covering the latitudes of 40 deg.-85 deg.N between 4 February and 23 May 2000 as part of the TOPSE (Tropospheric Ozone Production about the Spring Equinox) field experiment. The remote and in situ O3 measurements were used together to produce a vertically-continuous O3 profile from near the surface to above the tropopause. Ozone, aerosol, and potential vorticity (PV) distributions were used together to identify the presence of pollution plumes and stratospheric intrusions. The number of observed pollution plumes was found to increase into the spring along with a significant increase in aerosol loading. Ozone was found to increase in the middle free troposphere (4-6 km) at high latitudes (60 deg.-85 deg. N) by an average of 4.3 ppbv/mo from about 55 ppbv in early February to over 72 ppbv in mid-May. The average aerosol scattering ratios in the same region increased at an average rate of 0.37/mo from about 0.35 to over 1.7. Ozone and aerosol scattering were highly correlated over entire field experiment. Based on the above results and the observed aircraft in-situ measurements, it was estimated that stratospherically-derived O3 accounted for less than 20% of the observed increase in mid tropospheric O3 at high latitudes. The primary cause of the observed O3 increase was found to be the photochemical production of O3 in pollution plumes.

Hair, Jonathan W.↗

Analysis of the Latitudinal Variability of Tropospheric Ozone in the Arctic Using the Large Number of Aircraft and Ozonesonde Observations in Early Summer 2008

The goals of the paper are to: (1) present tropospheric ozone (O3) climatologies in summer 2008 based on a large amount of measurements, during the International Polar Year when the Polar Study using Aircraft, Remote Sensing, Surface Measurements, and Models of Climate Chemistry, Aerosols, and Transport (POLARCAT) campaigns were conducted (2) investigate the processes that determine O3 concentrations in two different regions (Canada and Greenland) that were thoroughly studied using measurements from 3 aircraft and 7 ozonesonde stations. This paper provides an integrated analysis of these observations and the discussion of the latitudinal and vertical variability of tropospheric ozone north of 55oN during this period is performed using a regional model (WFR-Chem). Ozone, CO and potential vorticity (PV) distributions are extracted from the simulation at the measurement locations. The model is able to reproduce the O3 latitudinal and vertical variability but a negative O3 bias of 6-15 ppbv is found in the free troposphere over 4 km, especially over Canada. Ozone average concentrations are of the order of 65 ppbv at altitudes above 4 km both over Canada and Greenland, while they are less than 50 ppbv in the lower troposphere. The relative influence of stratosphere-troposphere exchange (STE) and of ozone production related to the local biomass burning (BB) emissions is discussed using differences between average values of O3, CO and PV for Southern and Northern Canada or Greenland and two vertical ranges in the troposphere: 0-4 km and 4-8 km. For Canada, the model CO distribution and the weak correlation ( 30) of O3 and PV suggests that stratosphere-troposphere exchange (STE) is not the major contribution to average tropospheric ozone at latitudes less than 70oN, due to the fact that local biomass burning (BB) emissions were significant during the 2008 summer period. Conversely over Greenland, significant STE is found according to the better O3 versus PV correlation ( 40) and the higher 75th PV percentile. A weak negative latitudinal summer ozone gradient -6 to -8 ppbv is found over Canada in the mid troposphere between 4 and 8 km. This is attributed to an efficient O3 photochemical production due to the BB emissions at latitudes less than 65oN, while STE contribution is more homogeneous in the latitude range 55oN to 70oN. A positive ozone latitudinal gradient of 12 ppbv is observed in the same altitude range over Greenland not because of an increasing latitudinal influence of STE, but because of different long range transport from multiple mid-latitude sources (North America, Europe and even Asia for latitudes higher than 77oN).

climatologies↗

Airborne Measurements of Ozone and Other Trace Gases Captured by the Alpha Jet Atmospheric eXperiment (AJAX) During the 2016 California Baseline Ozone Transport Study (CABOTS)

In October 2015, the Environmental Protection Agency lowered the National Ambient Air Quality Standard for ozone (O3) from 75 ppbv to 70 ppbv. However, meeting the stricter air standards is a challenge for certain areas of California, like the San Joaquin Valley (SJV), where O3 levels are typically high due to topography, meteorology, and local emissions. Another factor potentially contributing to increased surface O3 is the trans-Pacific transport of O3 from Asia. The extent of which O3stems from local emissions or is transported across the Pacific, however, is unclear. The California Ozone Transport Study (CABOTS), a joint effort between the California Air Resource Board, the National Oceanic and Atmospheric Administration, and San Jose State University, was conducted during the spring and summer of 2016 in an attempt to answer this question.Nearly 10 science flights were carried out by the Alpha Jet Atmospheric eXperiment (AJAX) between June and August 2016, based out of the NASA Ames Research Center. A summary of airborne O3, CO2, CH4, H2O, formaldehyde (HCHO), and 3D wind measurements will be presented. AJAX flights connect the fixed-location measurements at Visalia (TOPAZ ozone lidar) and Bodega Bay (ozonesondes), while exploring the spatial heterogeneity of O3 concentrations across California and at various offshore locations. Preliminary analyses of these flights will investigate connections between offshore O3 and Central Valley O3. Vertical profiles, time series, and tracer-tracer correlations will be employed to identify the sources of O3 during these flights.

Iraci, Laura T.↗

The Dynamical Role of the Chesapeake Bay on the Local Ozone Pollution Using Mesoscale Modeling—A Case Study

This study investigated the dynamic influence of the Chesapeake Bay (CB) on local ozone (O3) concentration and distribution using a weather forecasting model. The Weather Research and Forecasting model coupled with Chemistry (WRF–Chem) was employed to simulate O3 production and transportation near the CB. Baseline (water) as well as sensitivity (nowater) model experiments of bay circulation were carried out with and without bay water by changing the water surface from water to land (loam). First, the model performance simulating O3 was evaluated using the baseline experiment results and AirNow surface wind and O3 observations. The results showed that the model overestimates surface O3 by up to 20–30%. Further, the comparisons of the baseline and sensitivity experiments revealed higher O3 mixing ratios, primarily due to the resulting bay breeze circulation. These increases, after considering model overestimation, represent a mean bay dynamics circulation-induced contribution of up to 10% at night and 5% during the day. Furthermore, the boundary layer over northern CB, where it is at its narrowest width, was higher (by 1.2 km on average) during daytime due to higher surface temperatures observed. The boundary layer depth difference between the northern, central, and southern regions of the bay leads to a differential in the role of bay circulation dynamics in the observed O3 increase. The relatively wider swath of water surface over southern CB resulted in a lower boundary layer depth and stronger breeze circulation and this circulation contributed to O3 concentrations. Moreover, since the case selected has a minimal bay breeze circulation, the associated surface ozone enhancements represent what is expected at least at a minimum.

Chesapeak Bay↗

Improved Assessment of Recent Trends in NOx and VOC Emissions and Ozone Production Sensitivity Regimes Using Satellite Data

This presentation highlights results from a NASA Aura Science Team and Atmospheric Composition Modeling and Analysis Program (ACMAP) project which study the capability to observe and model trends in ozone (O3) production regimes using spaceborne sensors. Ultraviolet– visible (UV–Vis) tropospheric column satellite retrievals of formaldehyde (HCHO) (a proxy for volatile organic compound [VOC] reactivity) and nitrogen dioxide (NO2) (a proxy for nitrogen oxides [NOx]) are frequently used to investigate the sensitivity of O3 production to emissions of NOx and VOCs. There are challenges that come from using satellite-derived ratios of HCHO and NO2 (FNR) to study O3 production sensitivity with the largest uncertainties associated with specific spaceborne sensor’s retrieval biases and errors. This study quantifies the differences and improvements in satellite retrievals of O3 production sensitivity regimes using FNRs when moving from legacy polar orbiting satellites such as the Ozone Monitoring Instrument (OMI) onboard NASA’s Aura satellite and Ozone Mapping and Profiler Suite Nadir Mapper (OMPS-NM) onboard the NASA/NOAA Suomi-NPP platform to newer, higher spatiotemporal resolution satellite sensors TROPOspheric Monitoring Instrument (TROPOMI) and eventually the recently launched NASA geostationary sensor Tropospheric Emissions: Monitoring of Pollution (TEMPO). Furthermore, we investigate how using retrievals of NO2 and HCHO from these different satellites to constrain model predictions impacts the ability to accurately simulate O3 chemistry including chemical production regimes. To this end, we have conducted inverse model simulations, using the WRF-CMAQ-DDM data assimilation system at 12 km × 12 km, to constrain emissions of NOx and VOCs over the contiguous United States (CONUS) when assimilating OMI and TROPOMI retrievals of NO2 and HCHO. Two advantages of this are that we a) account for each satellite’s errors/biases in the emission estimation and b) update the prior profile to ensure that only radiance information is used for optimizing the emissions. This presentation will demonstrate: a) the varying accuracy of different satellite retrieved FNRs and ability to capture known sub-annual emission trends (e.g., seasonal, weekend/weekday) and emission anomalies during the COVID-19 lockdown of 2020, b) the differences and improvements in top-down emission estimates of NOx and VOCs when constrained by newer satellite sensors compared to legacy systems, and c) multi-sensor optimized emission estimates of summer-time NOx and VOCs between 2019-2021.

Data↗

Lidar Observations Revealing Transport of O3 in the Presence of a Nocturnal Low-Level Jet: Regional Implications for "Next-Day" Pollution

Remotely sensed profiles of ozone (O3) and wind are presented continuously for the first time during anocturnal low-level jet (NLLJ) event occurring after a severe O3 episode in the Baltimore-Washington D.C.(BW) urban corridor throughout 11-12 June 2015. High-resolution O3 lidar observations indicate a well mixedand polluted daytime O3 reservoir, which decayed into a contaminated nocturnal residual layer(RL) with concentrations between 70 and 100 ppbv near 1 km above the surface. Observations indicatethe onset of the NLLJ was responsible for transporting polluted O3 away from the region, while simultaneouslyaffecting the height and location of the nocturnal residual layer. High-resolution modelinganalyses and next-day (12 June) lidar, surface, and balloon-borne observations indicate the trajectory ofthe NLLJ and polluted residual layer corresponds with ''next-day'' high O3 at sites throughout thesouthern New England region (New York, Connecticut, Massachusetts). The novel O3 lidar observationsare evidence of both nocturnal advection (via high NLLJ wind fields) and entrainment of the pollutedresidual layer in the presence of the ''next-day'' convectively growing boundary layer. In the greatercontext, the novel observational suite described in this work has shown that the chemical budget in areasdownwind of major urban centers can be altered significantly overnight during transport events such asthe NLLJ.

ozone↗

A21I-1875: Leveraging TEMPO Formaldehyde Observations to Assess Surface Air Quality

Surface ozone (O3) pollution is detrimental to human health, crop yields, and ecosystem productivity. Ground-based ozone observations are sparse and surface ozone retrievals from space are challenging. The process of producing ozone from the oxidation of volatile organic compounds (VOCs) in the presence of nitrogen oxides (NOx) results in formaldehyde (HCHO), which can be observed from satellite and by surface-based remote sensing. From limited field campaign observations, column formaldehyde has been shown to exhibit a strong relationship with surface ozone and, therefore, could be an useful proxy for detecting unmonitored regions of elevated ozone pollution. The spatiotemporal characteristics of this relationship are explored using ground-based Pandora spectrometers and airborne remote sensing data with surface ozone monitors across the United States during recent field campaigns over major cities (TRACER-AQ and STAQS). We extend our analysis to take advantage of HCHO column observations from recently launched Tropospheric Emissions: Monitoring of Pollution (TEMPO), a geostationary satellite over North America. TEMPO observations show preliminary promise in mapping regions of elevated surface ozone from space using column HCHO. We demonstrate the use of column HCHO in assessing the strength of the surface monitoring network, and in detecting the extent of regional ozone exceedances.

Prajjwal Rawat↗

How Well Satellite Remote Sensing Can Inform Surface Level Ozone Production Sensitivity to Precursor Trace Gas Emissions?

Surface-level ozone (O3) pollution mitigation strategies rely on a clear understanding of the atmospheric chemical processes involving O3, NOx (nitric oxide (NO) + nitrogen dioxide (NO2)) and volatile organic compounds (VOCs). A robust spatiotemporal classification of O3 photochemical regimes with relative chemical sensitivity of local O3 formation to emission reductions of NOx (NOx-limited regime) versus VOCs (radical-limited regime) is required to design anthropogenic emission reduction policies in order to improve surface air quality. Numerous studies found that the ratio of satellite-retrieved Vertical Column Densities (VCDs) of formaldehyde (HCHO) to NO2 can diagnose O3 production sensitivity. However, uncertainty still remains about the accuracy of such estimates using satellite-based retrievals. This study conducts an investigation to identify how well satellite data can inform surface-level O3 sensitivity by validating satellite-based estimates against aircraft-based retrievals taken during the Long Island Sound Tropospheric Ozone Study (LISTOS-2018) and Ozone Water-Land Environmental Transition Study (OWLETS-2) field campaigns. For this study, we use HCHO and NO2 retrievals from the Ozone Monitoring Instrument (OMI) onboard the Aura satellite, and high spatiotemporal resolution TROPOspheric Monitoring Instrument (TROPOMI) onboard the Sentinel-5 Precursor (S5P) satellite. The Community Multiscale Air Quality (CMAQ) modelling system is used to provide trace gas vertical profiles to recalculate air mass factor for deriving consistent satellite-based VCDs. To demonstrate the ability of satellites to diagnose O3 production regimes, we validate satellite-derived O3 sensitivity regimes, along with the OMI and TROPOMI products applied, using HCHO and NO2 retrievals from the aircraft-based instruments: Geostationary Trace gas and Aerosol Sensor Optimization (GeoTASO) spectrometer and Geostationary Coastal and Air Pollution Events Airborne Simulator (GCAS) instruments deployed during the LISTOS-2018 and OWLETS-2 campaigns. The results of this work will advance our fundamental knowledge of the spatiotemporal evolution of the complex O3-NOx-VOC chemistry, and will advance our understanding about the quality of remote-sensing, suborbital, and satellite data for accurately observing surface-level O3 production sensitivity.

Satellite↗

Tropospheric Ozone Changes, Radiative Forcing and Attribution to Emissions in the Atmospheric Chemistry and Climate Model Intercomparison Project (ACCMIP)

Ozone (O3) from 17 atmospheric chemistry models taking part in the Atmospheric Chemistry and Climate Model Intercomparison Project (ACCMIP) has been used to calculate tropospheric ozone radiative forcings (RFs). All models applied a common set of anthropogenic emissions, which are better constrained for the present-day than the past. Future anthropogenic emissions follow the four Representative Concentration Pathway (RCP) scenarios, which define a relatively narrow range of possible air pollution emissions. We calculate a value for the pre-industrial (1750) to present-day (2010) tropospheric ozone RF of 410 mW m−2. The model range of pre-industrial to present-day changes in O3 produces a spread (+/-1 standard deviation) in RFs of +/-17%. Three different radiation schemes were used - we find differences in RFs between schemes (for the same ozone fields) of +/-10 percent. Applying two different tropopause definitions gives differences in RFs of +/-3 percent. Given additional (unquantified) uncertainties associated with emissions, climate-chemistry interactions and land-use change, we estimate an overall uncertainty of +/-30 percent for the tropospheric ozone RF. Experiments carried out by a subset of six models attribute tropospheric ozone RF to increased emissions of methane (44+/-12 percent), nitrogen oxides (31 +/- 9 percent), carbon monoxide (15 +/- 3 percent) and non-methane volatile organic compounds (9 +/- 2 percent); earlier studies attributed more of the tropospheric ozone RF to methane and less to nitrogen oxides. Normalising RFs to changes in tropospheric column ozone, we find a global mean normalised RF of 42 mW m(−2) DU(−1), a value similar to previous work. Using normalised RFs and future tropospheric column ozone projections we calculate future tropospheric ozone RFs (mW m(−2); relative to 1750) for the four future scenarios (RCP2.6, RCP4.5, RCP6.0 and RCP8.5) of 350, 420, 370 and 460 (in 2030), and 200, 300, 280 and 600 (in 2100). Models show some coherent responses of ozone to climate change: decreases in the tropical lower troposphere, associated with increases in water vapour; and increases in the sub-tropical to mid-latitude upper troposphere, associated with increases in lightning and stratosphere-to-troposphere transport. Climate change has relatively small impacts on global mean tropospheric ozone RF.

climate change↗

Impact of Biomass Burning and Stratospheric Intrusions in the Remote South Pacific Ocean Troposphere

The ozone mixing ratio spatiotemporal variability in the pristine South Pacific Ocean is studied, for the first time, using 21-year-long ozone (O3) records from the entire southern tropical and subtropical Pacific between 1994 and 2014. The analysis considered regional O3 vertical observations from ozonesondes, surface carbon monoxide (CO) observations from flasks, and three-dimensional chemistry-transport model simulations of the global troposphere. Two 21-year-long numerical simulations, with and without biomass burning emissions, were performed to disentangle the importance of biomass burning relative to stratospheric intrusions for ambient ozone levels in the region. Tagged tracers of O3 from the stratosphere and CO from various biomass burning regions have been used to track the impact of these different regions on the southern tropical Pacific O3 and CO levels. Patterns have been analyzed based on atmospheric dynamics variability. Considering the interannual variability in the observations, the model can capture the observed ozone gradients in the troposphere with a positive bias of 7.5 % in the upper troposphere/lower stratosphere (UTLS) as well as near the surface. Remarkably, even the most pristine region of the global ocean is affected by distant biomass burning emissions by convective outflow through the mid and high troposphere and subsequent subsidence over the pristine oceanic region. Therefore, the biomass burning contribution to tropospheric CO levels maximizes in the UTLS. The Southeast Asian open fires have been identified as the major contributing source to CO from biomass burning in the tropical South Pacific, contributing on average for the study period about 8.5 and 13 ppbv of CO at Rapa Nui and Samoa, respectively, at an altitude of around 12 km during the burning season in the spring of the Southern Hemisphere. South America is the second-most important biomass burning source region that influences the study area. Its impact maximizes in the lower troposphere (6.5 ppbv for Rapa Nui and 3.8 ppbv for Samoa). All biomass burning sources contribute about 15–23 ppbv of CO at Rapa Nui and Samoa and account for about 25 % of the total CO in the entire troposphere of the tropical and subtropical South Pacific. This impact is also seen on tropospheric O3, to which biomass burning O3 precursor emissions contribute only a few ppbv during the burning period, while the stratosphere–troposphere exchange is the most important source of O3 for the mid troposphere of the South Pacific Ocean, contributing about 15–20 ppbv in the subtropics.

Tropospheric ozone↗

Balloon-borne measurements of ClO, NO, and O3 in a volcanic cloud: An analysis of heterogeneous chemistry between 20 and 30 km

Balloon profiles of chlorine monoxide (ClO), nitric oxide (NO), and ozone (O3) were measured on March 11, 1992 from 100 to 10 mb over Greenland (67.0 deg N, 50.6 deg W). Measurements from SAGE II indicate that the aerosol surface area in the region was enhanced by sulfur from the eruption of Mt. Pinatubo, reaching 50 times background near 20 km. Concentrations of ClO were enhanced and concentrations of NO were suppressed relative to low aerosol conditions consistent with the effects of hydrolysis of N2O5 on the surface of sulfuric acid aerosols. The data are consistent with a value of 2 x 10(exp -4) for the reaction probability of the heterogeneous hydrolysis of ClONO2, indicating a minor role for this reaction at as temperature of 220 K. At these temperatures, we find no evidence for the catastrophic loss of ozone predicted to occur under conditions of enhanced aerosol surface area.

Dessler, A. E.↗

Balloon-Borne Measurements of CLO, NO and O3 in a Volcanic Cloud: An Analysis of Heterogeneous Chemistry between 20 and 30 KM

Balloon profiles of chlorine monoxide (ClO), nitric oxide (NO), and ozone (O3) were measured on March 11, 1992 from 100 to 10 mb over Greenland (67.0 deg N, 50.6 deg W). Measurements from SAGE II indicate that the aerosol surface area in the region was enhanced by sulfur from the eruption of Mt. Pinatubo, reaching 50 times background near 20 km. Concentrations of ClO were enhanced and concentrations of NO were suppressed relative to low aerosol conditions consistent with the effects of hydrolysis of N2O5 on the surface of sulfuric acid aerosols. The data are consistent with a value of 2 x 10(exp -4) for the reaction probability of the heterogeneous hydrolysis of ClONO2, indicating a minor role for this reaction at a temperature of 220 K. At these temperatures, we find no evidence for the catastrophic loss of ozone predicted to occur under conditions of enhanced aerosol surface area.

Dessler, A. E.↗

Ozone Measurements with the US EPA UV-DIAL: Preliminary Results

A compact airborne down-looking lidar system was developed at the Environmental Protection Agency in Las Vegas. This differential absorption lidar (DIAL) was designed to simultaneously measure range-resolved concentrations of ozone (O3) and sulfur dioxide (SO2) in the lower troposphere, together with an indication of the aerosol distribution. The five laser wavelengths (i.e., lambda(sub 1) = 277 nm, lambda(sub 2) = 292 nm, lambda(sub 3) = 313 nm, lambda(sub4) = 319 nm, lambda(sub 5) = 369 nm) were generated via Raman conversion of a focused KrF excimer laser. The system is currently installed in a truck-based mobile laboratory. For the ground testing, an opening in the truck floor together with a folding mirror under the truck makes a horizontal, or upwardly inclined direction of measurement possible. Initial ground testing has been performed in the vicinity of a Desert Research Institute (DRI) ambient air monitoring site, located at Cottonwood Cove approximately 85 km south east of Las Vegas, Nevada. At this site O3 and SO2 concentrations are continuously monitored with an average accuracy better than +/- 10 percent. A temporary ozone measurement station with identical accuracy was set up at a distance to get a second point of comparison for the range-resolved DIAL measurements.

Moosmueller, H.↗

Design, development, and field testing of Infrared Heterodyne Radiometer (IHR) for remote profiling of tropospheric and stratospheric species

The performance of a dual-channel infrared heterodyne radiometer, designed to remotely monitor the concentration and vertical distribution of selected atmospheric species, is described. Ground based solar viewing measurement using the IHR were performed at selected laser transitions for ammonia (NH3 and ozone O3). Flight tests were conducted aboard the Galileo II, NASA Ames CV-990, on the Latitude Survey Mission. Ozone was the selected atmospheric species for the airborne flight measurements because of the scientific interest in this atmospheric species, the availability of in situ monitors, the coordinated ozone measurements, and the availability of ground truth data. The IHS was operated in the solar viewing mode to determine ozone distributions in the stratosphere and in the nadir viewing mode to determine the ozone distribution in the troposphere. Airborne atmospheric propagation measurements also were carried out at selected CO2 laser transitions.

Lange, R.↗

Arctic Tropospheric Ozone: Assessment of Current Knowledge and Model Performance

As the third most important greenhouse gas (GHG) after carbon dioxide (CO2) and methane (CH4), tropospheric ozone (O3) is also an air pollutant causing damage to human health and ecosystems. This study brings together recent research on observations and modeling of tropospheric O3 in the Arctic, a rapidly warming and sensitive environment. At different locations in the Arctic, the observed surface O3 seasonal cycles are quite different. Coastal Arctic locations, for example, have a minimum in the springtime due to O3 depletion events resulting from surface bromine chemistry. In contrast, other Arctic locations have a maximum in the spring. The 12 state-of-the-art models used in this study lack the surface halogen chemistry needed to simulate coastal Arctic surface O3 depletion in the springtime; however, the multi-model median (MMM) has accurate seasonal cycles at non-coastal Arctic locations. There is a large amount of variability among models, which has been previously reported, and we show that there continues to be no convergence among models or improved accuracy in simulating tropospheric O3 and its precursor species. The MMM underestimates Arctic surface O3 by 5 % to 15 % depending on the location. The vertical distribution of tropospheric O3 is studied from recent ozonesonde measurements and the models. The models are highly variable, simulating free-tropospheric O3 within a range of ±50 % depending on the model and the altitude. The MMM performs best, within ±8 % for most locations and seasons. However, nearly all models overestimate O3 near the tropopause (∼300 hPa or ∼8 km), likely due to ongoing issues with underestimating the altitude of the tropopause and excessive downward transport of stratospheric O3 at high latitudes. For example, the MMM is biased high by about 20 % at Eureka. Observed and simulated O3 precursors (CO, NOx, and reservoir PAN) are evaluated throughout the troposphere. Models underestimate wintertime CO everywhere, likely due to a combination of underestimating CO emissions and possibly overestimating OH. Throughout the vertical profile (compared to aircraft measurements), the MMM underestimates both CO and NOx but overestimates PAN. Perhaps as a result of competing deficiencies, the MMM O3 matches the observed O3 reasonably well. Our findings suggest that despite model updates over the last decade, model results are as highly variable as ever and have not increased in accuracy for representing Arctic tropospheric O3.

Arctic↗

Investigating Sources of Ozone over California Using AJAX Airborne Measurements and Models: Assessing the Contribution from Long Range Transport

High ozone (O3) concentrations at low altitudes (1.5e4 km) were detected from airborne Alpha Jet Atmospheric eXperiment (AJAX) measurements on 30 May 2012 off the coast of California (CA). We investigate the causes of those elevated O3 concentrations using airborne measurements and various models. GEOS-Chem simulation shows that the contribution from local sources is likely small. A back trajectory model was used to determine the air mass origins and how much they contributed to the O3 over CA. Low-level potential vorticity (PV) from Modern Era Retrospective analysis for Research and Applications 2 (MERRA-2) reanalysis data appears to be a result of the diabatic heating and mixing of airs in the lower altitudes, rather than be a result of direct transport from stratospheric intrusion. The Q diagnostic, which is a measure of the mixing of the air masses, indicates that there is sufficient mixing along the trajectory to indicate that O3 from the different origins is mixed and transported to the western U.S.The back-trajectory model simulation demonstrates the air masses of interest came mostly from the mid troposphere (MT, 76), but the contribution of the lower troposphere (LT, 19) is also significant compared to those from the upper troposphere/lower stratosphere (UTLS, 5). Air coming from the LT appears to be mostly originating over Asia. The possible surface impact of the high O3 transported aloft on the surface O3 concentration through vertical and horizontal transport within a few days is substantiated by the influence maps determined from the Weather Research and Forecasting Stochastic Time Inverted Lagrangian Transport (WRF-STILT) model and the observed increases in surface ozone mixing ratios. Contrasting this complex case with a stratospheric-dominant event emphasizes the contribution of each source to the high O3 concentration in the lower altitudes over CA. Integrated analyses using models, reanalysis, and diagnostic tools, allows high ozone values detected by in-situ measurements to be attributed to multiple source processes.

Ryoo, Ju-Mee↗