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NASA NTRS2019

Investigating the Utility of Hyperspectral Sounders in the 9.6 μm Band to Improve Ozone Analyses

Currently, hyperspectral sounder brightness temperatures assimilated in the Goddard Earth Observing System - Atmospheric Data Assimilation System (GEOS-ADAS) are limited to assimilating temperature and moisture. The ozone sensitive 9.6 micron region is sensed by several hyperspectral sounders including AIRS (Atmospheric InfraRed Sounder), IASI (Infrared Atmospheric Sounding Interferometer), and CrIS (Cross-track Infrared Sounder). Direct assimilation of brightness temperatures in the 9.6 micron region have been used previously to improve ozone analyses. This has recently been achieved by ECMWF (European Centre for Medium-Range Weather Forecast) (Dragani and McNally, 2013; Eresmaa et al., 2017), and while every system presents its challenges, it should be possible to take advantage of this spectral region using the GEOS-ADAS. For this study, channels were selected from available operational subsets evaluating information content, and minimizing inter-channel correlation. Additionally, information such as channel selections made by other studies, and vertical sensitivities of ozone and temperature were considered in developing the study. The analyses produced show improvements verified against ozonesondes taken from SHADOZ (Southern Hemisphere Additional Ozonesondes), and WOUDC (World Ozone and Ultraviolet Data Center). The addition of ozone channels does degrade forecast skill in the Tropics, on the border of statistical significance. Overall, the addition of these channels in some form could improve ozone analyses in the GEOS-ADAS.

Karpowicz, Bryan M.↗
NASA NTRS2019

Improvements to Ozone Analyses using Hyperspectral Sounders in the 9.6 μm Band

Previously, hyperspectral sounder brightness temperatures assimilated in the Goddard Earth Observing System Atmospheric Data Assimilation System (GEOS-ADAS) were limited to assimilating temperature and moisture. The ozone sensitive 9.6 m region is sensed by several hyperspectral sounders including AIRS (Atmospheric InfraRed Sounder), IASI (Infrared Atmospheric Sounding Interferometer), and CrIS (Cross-track Infrared Sounder). Direct assimilation of brightness temperatures in the 9.6 m region have been operational at ECMWF for several years (Dragani and McNally, 2013; Eresmaa et al., 2017). With this study, similar improvements using the GEOS-ADAS are presented. Channels were selected from available operational subsets evaluating information content and minimizing inter-channel correlation. Additionally, information such as channel selections made by other studies, and vertical sensitivities of ozone and temperature were considered in developing the study. The analyses produced show improvements verified against ozonesondes taken from SHADOZ (Southern Hemisphere Additional Ozonesondes). It is anticipated that inclusion of these ozone sensitive channels will be used to improve NASA GMAO products in the near future.

GEOS-ADAS↗
NASA NTRS2019

Improvements to Ozone Analyses Using Hyperspectral Sounders in the 9.6 μm Band

Previously, hyperspectral sounder brightness temperatures assimilated in the Goddard Earth Observing System Atmospheric Data Assimilation System (GEOS-ADAS) were limited to assimilating temperature and moisture. The ozone sensitive 9.6 m region is sensed by several hyperspectral sounders including AIRS (Atmospheric InfraRed Sounder), IASI (Infrared Atmospheric Sounding Interferometer), and CrIS (Cross-track Infrared Sounder). Direct assimilation of brightness temperatures in the 9.6 m region have been operational at ECMWF for several years (Dragani and McNally, 2013; Eresmaa et al., 2017). With this study, similar improvements using the GEOS-ADAS are presented. Channels were selected from available operational subsets evaluating information content and minimizing inter-channel correlation. Additionally, information such as channel selections made by other studies, and vertical sensitivities of ozone and temperature were considered in developing the study. The analyses produced show improvements verified against ozonesondes taken from SHADOZ (Southern Hemisphere Additional Ozonesondes), and WOUDC (World Ozone and Ultraviolet Data Center). Inclusion of inter-channel correlation error to the selected ozone channels are expected to improve ozone analyses further along with improve analyses overall. It is anticipated that inclusion of these ozone sensitive channels will be used to improve NASA GMAO products in the near future.

GEOS-ADAS↗
NASA NTRS2019

Improved Ozone Analyses Using Direct Assimilation of 9.6μm Radiances from Hyperspectral Sounders

Previously, hyperspectral sounder brightness temperatures assimilated in the Goddard Earth Observing System Atmospheric Data Assimilation System (GEOS-ADAS) were limited to assimilating temperature and moisture. The ozone sensitive 9.6 m region is sensed by several hyperspectral sounders including AIRS (Atmospheric InfraRed Sounder), IASI (Infrared Atmospheric Sounding Interferometer), and CrIS (Cross-track Infrared Sounder). Direct assimilation of brightness temperatures in the 9.6 m region have been operational at ECMWF for several years (Dragani and McNally, 2013; Eresmaa et al., 2017). With this study, similar improvements using the GEOS-ADAS are presented. Channels were selected from available operational subsets evaluating information content and minimizing inter-channel correlation. Additionally, information such as channel selections made by other studies, and vertical sensitivities of ozone and temperature were considered. The analyses produced show improvements verified against ozonesondes taken from SHADOZ (Southern Hemisphere Additional Ozonesondes), and WOUDC (World Ozone and Ultraviolet Data Center). While care was taken to minimize inter-channel correlation through channel selection, a key feature available in the GEOS-ADAS is the ability to account for correlated error. The importance of inter-channel correlated error is highlighted by performing assimilation experiments with and without inter-channel correlation in the GEOS-ADAS. It is anticipated that inclusion of these ozone sensitive channels will be used to improve NASA GMAO products in the near future.

Karpowicz, Bryan M.↗
NASA NTRS2021

Investigating the Utility of Hyperspectral Sounders in the 9.6 μm Band to Improve Ozone Analyses

Hyperspectral sounder brightness temperatures assimilated in the Global Earth Observing System Atmospheric Data Assimilation System (GEOS-ADAS) were previously limited to assimilating temperature and moisture. The ozone-sensitive 9.6 𝜇 m region is sensed by several hyperspectral sounders including AIRS (Atmospheric InfraRed Sounder), IASI (Infrared Atmospheric Sounding Interferometer), and CrIS (Cross-track Infrared Sounder). Direct assimilation of brightness temperatures in the 9.6 𝜇 m region have been operational at ECMWF for several years. With this study, similar improvements using the GEOS-ADAS are presented. Channels were selected from available operational subsets evaluating information content and minimizing inter-channel correlation. Additionally, information such as channel selections made by other studies, and vertical sensitivities of ozone and temperature were considered. The analyses produced show improvements verified against ozonesondes taken from SHADOZ (Southern Hemisphere Additional Ozonesondes) and WOUDC (World Ozone and Ultraviolet Data Center). This work will be added to the GEOS-ADAS and will provide an improved source of ozone data in NASA Global Modeling and Assimilation Office products.

Ozone↗
NASA NTRSDate not supplied

Regional and Seasonal Trends in Tropical Ozone from SHADOZ Profiles: Reference for Models and Satellite Products

Understanding lowermost stratosphere (LMS) ozone variability is an important topic in the trends and climate assessment communities because of feedbacks among changing temperature, dynamics, water vapor and ozone. LMS evaluations are usually based on satellite observations. Free tropospheric (FT) ozone assessments typically rely on profiles from commercial aircraft. Ozonesonde measurements constitute an independent dataset encompassing both LMS and FT. We used Southern Hemisphere Additional Ozonesondes (SHADOZ) data from 1998-2019 in the GSFC Multiple Linear Regression (MLR) model to analyze monthly mean FT and LMS ozone across five well-distributed tropical sites, three based on combination of nearby individual stations (Figure 1). Our findings: (1) both FT (defined as 5-15 km) and LMS (15-20 km) ozone trends exhibit marked regional and seasonal variability. (2) Stations with the largest FT ozone increases, in the equatorial Americas and western Pacific/east Indian Ocean, show these trends most strongly in February-May when there is convectively-driven wave activity. (3) LMS ozone losses are greatest in the 2nd half of the year (solid lines in Figure 2) when the losses are correlated with an increase in tropopause height (TH) as derived from SHADOZ radiosonde data. ( 4) When the upper FT and LMS are defined by tropopause-relative coordinates, the LMS ozone trend calculated by MLR becomes insignificant, as shown in the dashed lines in Figure 2. Thus, the 20-year decline in tropical LMS ozone reported in recent satellite- and model-based studies does not point to a chemical loss but is rather a signature of a tropopause that has been perturbed by a changing climate. Output based on our regional and monthly averaged FT and LMS ozone trends will be available as a reference for satellite- and model-based analyses.

Free Tropospheric (FT) ozone assessments↗
NASA NTRS2022

Tropospheric Ozone Retrieval By A Combination of TROPOMI/S5P Measurements With BASCOE Assimilated Data

We present a new tropospheric ozone dataset based on TROPOspheric Monitoring Instrument (TROPOMI)/Sentinel-5 Precursor (S5P) total ozone measurements combined with stratospheric ozone data from the Belgian Assimilation System for Chemical ObsErvations (BASCOE) constrained by assimilating ozone observations from the Microwave Limb Sounder (MLS). The BASCOE stratospheric data are interpolated to the S5P observations and subtracted from the TROPOMI total ozone data. The difference is equal to the tropospheric ozone residual column from the surface up to the tropopause. The tropospheric ozone columns are retrieved at the full spatial resolution of the TROPOMI sensor (5.5×3.5 km 2 ) with daily global coverage. Compared to the Ozone Mapping and Profiler Suite Modern-Era Retrospective analysis for Research and Applications 2 (OMPS-MERRA-2) data, a global mean positive bias of 3.3 DU is found for the analysed period April 2018 to June 2020. A small negative bias of about −0.91 DU is observed in the tropics relative to the operational TROPOMI tropical tropospheric data based on the convective cloud differential (CCD) algorithm throughout the same period. The new tropospheric ozone data (S5P-BASCOE) are compared to a set of globally distributed ozonesonde data integrated up to the tropopause level. We found 2254 comparisons with cloud-free TROPOMI observations within 25 km of the stations. In the global mean, S5P-BASCOE deviates by 2.6 DU from the integrated ozonesondes. Depending on the latitude the S5P-BASCOE deviate from the sondes and between −4.8 and 7.9 DU, indicating a good agreement. However, some exceptional larger positive deviations up to 12 DU are found, especially in the northern polar regions (north of 70∘). The monthly mean tropospheric column and time series for selected areas showed the expected spatial and temporal pattern, such as the wave one structure in the tropics or the seasonal cycle, including a summer maximum, in the mid-latitudes.

Satellite Retrieval↗
NASA NTRSDate not supplied

Observation of Pollution Events at Low Altitude During TRACER-AQ – The Advantage of Adaptive Resolution Lidar

The TRACER-AQ campaign happened in August-September 2021 in Houston, Texas. Its objective was to better understand the pollution events in the coastal environment and to evaluate models and satellite observations. As a supporting instrument, NASA’s Langley Mobile Ozone Lidar (LMOL) was installed on the Houston campus, adjacent to University of Houston’s air-quality site, and performed observations of ozone and aerosols. Co-located instrumentation included a Pandora spectrophotometer, in-situ trace-gas measurements, and ozonesonde launches. Thanks to an adaptive resolution retrieval scheme, LMOL was able to detect thin-layer O3 structures at low (~200m) altitude that are not captured by the ozonesondes, and would ordinarily be missed with traditional coarse TOLNet lidar vertical averaging. We show that some of these features are not present in the models and are likely coming from local, industry-generated, emissions.

Guillaume Gronoff↗
NASA NTRS2016

Why Do Models Overestimate Surface Ozone in the Southeast United States?

Ozone pollution in the Southeast US involves complex chemistry driven by emissions of anthropogenic nitrogen oxide radicals (NO(x) triple bond NO + NO2) and biogenic isoprene. Model estimates of surface ozone concentrations tend to be biased high in the region and this is of concern for designing effective emission control strategies to meet air quality standards. We use detailed chemical observations from the SEAC(exp 4)RS aircraft campaign in August and September 2013, interpreted with the GEOS-Chem chemical transport model at 0.25 deg x 0.3125 deg horizontal resolution, to better understand the factors controlling surface ozone in the Southeast US. We find that the National Emission Inventory (NEI) for NO(x) from the US Environmental Protection Agency (EPA) is too high. This finding is based on SEAC(exp 4)RS observations of NO(x) and its oxidation products, surface network observations of nitrate wet deposition fluxes, and OMI satellite observations of tropospheric NO2 columns. Our results indicate that NEI NO(x) emissions from mobile and industrial sources must be reduced by 30-60%, dependent on the assumption of the contribution by soil NO(x) emissions. Upper-tropospheric NO2 from lightning makes a large contribution to satellite observations of tropospheric NO2 that must be accounted for when using these data to estimate surface NO(x) emissions. We find that only half of isoprene oxidation proceeds by the high-NO(x) pathway to produce ozone; this fraction is only moderately sensitive to changes in NO(x) emissions because isoprene and NO(x) emissions are spatially segregated. GEOS-Chem with reduced NO(x) emissions provides an unbiased simulation of ozone observations from the aircraft and reproduces the observed ozone production efficiency in the boundary layer as derived from a regression of ozone and NO(x) oxidation products. However, the model is still biased high by 6 plus or minus 14 ppb relative to observed surface ozone in the Southeast US. Ozonesondes launched during midday hours show a 7 ppb ozone decrease from 1.5 km to the surface that GEOS-Chem does not capture. This bias may reflect a combination of excessive vertical mixing and net ozone production in the model boundary layer.

Oxidation↗
NASA NTRS2019

The Effects of a 1998 Observing System Change on MERRA-2-Based Ozone Profile Simulations

Model simulations of ozone (O3) driven by meteorological reanalyses are useful for filling observational gaps and interpreting observed O3 variability and trends. However, the transport circulation of reanalysis products is impacted by changes to the observing system (the data assimilated into the reanalyses). We examine the impacts of these changes on simulated O3 from two models, Global Modeling Initiative (GMI) Chemistry Transport Model (GMI CTM) and Modern‐Era Retrospective Analysis for Research Applications version 2 (MERRA‐2) GMI Replay (M2 GMI Replay) simulation, using observations from global ozonesondes (>50,000 profiles) and satellites from 1980 to 2016. Both models are constrained by meteorology from the NASA MERRA‐2 reanalysis, and both use versions of NASA's GMI chemical mechanism. We focus on an observing system change affecting simulated O3 after 1998, associated with the assimilation of temperature and humidity data from new microwave profiling satellites. A large post‐1998 O3 increase, mainly confined to 15–20‐km altitude, of ~10 Dobson units (DU) in midlatitudes occurs in the GMI CTM, worsening the bias compared to observations. In contrast, an increase in M2 GMI Replay simulation O3 of ~10 DU is observed only near −60° latitude, reducing the bias compared to observations. The GMI CTM O3 high biases display a Quasi‐Biennial Oscillation (QBO)‐like periodicity that result from excessive transport from the tropical stratosphere to the midlatitude lower stratosphere during the QBO westerly phase. We quantify O3 discontinuities caused by MERRA‐2 observing system changes and demonstrate how the MERRA‐2 Global Modeling Initiative Replay simulation dampens the effects of these changes and QBO‐driven artifacts on simulated lower stratospheric and total O3. We caution against using simulations driven by a reanalysis to derive multidecadal O3 trends, especially prior to 1998.

Replay↗
NASA NTRS2019

Characterizing Spatio-Temporal Ozone Gradients Along Coastal Boundaries: Sondes and Mobile Measurements from OWLETS-2

One of the major difficulties for the modeling and satellite communities is the validation of O3 levels in sharp coastal transition regions within metropolitan areas. Land-water gradients of ozone as well as its precursors can be significant due to differences in emissions, land use, surface deposition, boundary layer height, and mesoscale wind patterns. The Ozone Water-Land Environmental Transition Study (OWLETS-2) was a follow-on field campaign spearheaded by NASA GSFC and LaRC's Tropospheric Ozone Lidar Network (TOLnet) conducted in the summer of 2018 within the Upper Chesapeake region to better characterize spatial and vertical distribution of various pollutants across the coastal boundary. Supporting this campaign, 40 ozonesondes were simultaneously launched directly in the marine environment on Hart Miller Island (HMI) and on two land sites: both the University of Maryland, Baltimore County (UMBC) and Howard University-Beltsville (HUBV). In addition, Personal Ozone Monitors (POMs) - small sensors - were deployed in a variety of environments - car, boat, and drone, to name a few - to quantify ozone across fine spatial and temporal thresholds. The purpose of these measurements is multifaceted: to provide both ozone pollution information to coastal metropolitan communities and validation to satellite, modeling, and forecasting communities, especially in current and future satellite endeavors such as TROPOMI and TEMPO.

coastal pollution↗
NASA NTRS2022

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↗
NASA NTRSDate not supplied

From the Ground Up: Stratospheric Aerosol and Gas Experiment III on the International Space Station (SAGE III/ISS) Comparison of Vertical Profiles with 2022 Student Airborne Research Program (SARP) In Situ Data

The Stratospheric Aerosol and Gas Experiment III (SAGE III) instrument, installed on the International Space Station (ISS) in 2017, has completed over five years of data collection and the accompanying production of science data products. SAGE III/ISS is a solar and lunar occultation instrument that scans the light from the Sun and Moon through the limb of the Earth’s atmosphere to produce vertical profiles of aerosol, ozone, water vapor, and other trace gasses. This year provided the unique opportunity to compare in situ data collected during the NASA Student Airborne Research Program (SARP) summer airborne campaign with data collected by SAGE III/ISS on coincident overpasses.​ ​ SARP, a summer internship program typically for rising undergraduate seniors, provides students with an opportunity to gain hands-on experience making earth system measurements using NASA’s airborne science platforms. The NASA DC-8 flying laboratory collected in-situ measurements of ozone and other trace gasses during the summer 2022 SARP campaign. While the general focus with SARP is on the airborne research component, this year, a suite of 10 ozonesonde launches spatially and temporally co-located with the research flights collected atmospheric state and in-situ ozone measurements from inland southern California. This presentation shows the results of comparing SAGE III/ISS vertical profiles with those of in situ data collected during the summer 2022 SARP campaign.​

In Situ↗
NASA NTRSDate not supplied

Homogenized Ground-Based and Profile Ozone Datasets From the TOAR-II/HEGIFTOM Project: Methods and Station Trends

Within the framework of the second phase of the Tropospheric Ozone Assessment Report (TOAR-II), it was recognized that an essential first step for deriving accurate trends from the ground-based networks that monitor ozone in the free troposphere is putting the measurements on the same basis with respect to absolute references and processing methods. The relevant procedures are referred to as “harmonization” or “homogenization”. The TOAR II working group, “HEGIFTOM” (Harmonization and Evaluation of Ground-based Instruments for Free-Tropospheric Ozone Measurements), has carried out harmonization for five types of network (Figure below) instruments (mid-1990s to 2020): ozonesondes, commercial aircraft IAGOS landing/takeoff profiles, Fourier-Transform Infrared spectrometer (FTIR), tropospheric Lidar, and Brewer/Dobson Umkehr. First, we summarize the homogenization effort for each network that provides new quality-assessed ozone profile or segment (partial column) data sets, including uncertainty estimates and quality flags. Second, with the HEGIFTOM datasets forming the basis for a global assessment of tropospheric ozone column trends, results derived with various trend detection algorithms will be presented. The ultimate goal is evaluation of the consistency of the calculated trends among different techniques at selected stations and/or regions.

ozone↗
DOE OSTI2024

Characterizing Overwater High Ozone Events in the Houston–Galveston–Brazoria Region during the 2021 GO3 and TRACER-AQ Campaigns

Photochemical modeling outputs showing high ozone concentrations over the Gulf of Mexico and Galveston Bay during ozone episodes in the Houston–Galveston–Brazoria (HGB) region have not been previously verified using in situ observations. Such data were collected systematically, for the first time, from July to October 2021 from three boats deployed for the Galveston Offshore Ozone Observations (GO3) and Tracking Aerosol Convection Interactions Experiment—Air Quality (TRACER-AQ) field campaigns. A pontoon boat and a commercial vessel operated in Galveston Bay, while another commercial vessel operated in the Gulf of Mexico offshore of Galveston. All three boats had continuously operating sampling systems that included ozone analyzers and weather stations, and the two boats operating in Galveston Bay had a ceilometer. The sampling systems operated autonomously on the two commercial boats as they traveled their daily routes. Thirty-seven ozonesondes were launched over water on forecast high ozone days in Galveston Bay and the Gulf of Mexico. During the campaigns, multiple periods of ozone exceeding 100 ppbv were observed over water in Galveston Bay and the Gulf of Mexico. These events included previously identified conditions for high ozone events in the HGB region, such as the bay/sea-breeze recirculation and postfrontal environments, as well as a localized coastal high ozone event after the passing of a tropical system (Hurricane Nicholas) that was not well forecast.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2023

Test Flights of NOAA Ozone Photometer for Uncrewed Aerial Systems (UAS)/Balloon-Based Studies (OPUS) during TRACER (Field Campaign Report)

We proposed to integrate and fly the National Oceanic and Atmospheric Administration (NOAA) Ozone Photometer for Uncrewed Aerial Systems (UAS)/Balloon-Based Studies (OPUS) on the U.S. Department of Energy (DOE) Atmospheric Radiation Measurement (ARM) user facility’s tethered balloon system (TBS) during the second phase (August 1-15) of the 2022 Tracking Aerosol Convection Interactions Experiment (TRACER) in southwest Houston, Texas. The two main goals were: 1) Test fly the sensor to discover and address any potential problems such as interface and communication with other instruments, interferences with other instruments and radio, and 2) If OPUS performs well, then inter-compare OPUS with the EN-SCI ozonesondes that will also be flown on the TBS. The collaborating institutions are DOE Sandia National Laboratories TBS team, the University of Houston, and St. Edward's University.

47 OTHER INSTRUMENTATION↗
DOE OSTI2022

Australian wildfire smoke in the stratosphere: the decay phase in 2020/2021 and impact on ozone depletion

Abstract. Record-breaking wildfires raged in southeastern Australia in late December 2019 and early January 2020. Rather strong pyrocumulonimbus (pyroCb) convection developed over the fire areas and lofted enormous amounts of biomass burning smoke into the tropopause region and caused the strongest wildfire-related stratospheric aerosol perturbation ever observed around the globe. We discuss the geometrical, optical, and microphysical properties of the stratospheric smoke layers and the decay of this major stratospheric perturbation. A multiwavelength polarization Raman lidar at Punta Arenas (53.2∘ S, 70.9∘ W), southern Chile, and an elastic backscatter Raman lidar at Río Grande (53.8∘ S, 67.7∘ W) in southern Argentina, were operated to monitor the major record-breaking event until the end of 2021. These lidar measurements can be regarded as representative for mid to high latitudes in the Southern Hemisphere. A unique dynamical feature, an anticyclonic, smoke-filled vortex with 1000 km horizontal width and 5 km vertical extent, which ascended by about 500 m d−1, was observed over the full last week of January 2020. The key results of the long-term study are as follows. The smoke layers extended, on average, from 9 to 24 km in height. The smoke partly ascended to more than 30 km height as a result of self-lofting processes. Clear signs of a smoke impact on the record-breaking ozone hole over Antarctica in September–November 2020 were found. A slow decay of the stratospheric perturbation detected by means of the 532 nm aerosol optical thickness (AOT) yielded an e-folding decay time of 19–20 months. The maximum smoke AOT was around 1.0 over Punta Arenas in January 2020 and thus 2 to 3 orders of magnitude above the stratospheric aerosol background of 0.005. After 2 months with strongly varying smoke conditions, the 532 nm AOT decreased to 0.03-0.06 from March–December 2020 and to 0.015–0.03 throughout 2021. The particle extinction coefficients at 532 nm were in the range of 10–75 Mm−1 in January 2020 and, later on, mostly between 1 and 5 Mm−1. Combined lidar–photometer retrievals revealed typical smoke extinction-to-backscatter ratios of 69 ± 19 sr (at 355 nm), 91 ± 17 sr (at 532 nm), and 120 ± 22 sr (at 1064 nm). An ozone reduction of 20 %–25 % in the 15–22 km height range was observed over Antarctica and New Zealand ozonesonde stations in the smoke-polluted air, with particle surface area concentrations of 1–5 µm2 cm−3.

Ohneiser, Kevin↗
DOE OSTI2023

Arctic tropospheric ozone: assessment of current knowledge and model performance

As the third most important greenhouse gas (GHG) after carbon dioxide (CO 2 ) and methane (CH 4 ), tropospheric ozone (O 3 ) is also an air pollutant causing damage to human health and ecosystems. This study brings together recent research on observations and modeling of tropospheric O 3 in the Arctic, a rapidly warming and sensitive environment. At different locations in the Arctic, the observed surface O 3 seasonal cycles are quite different. Coastal Arctic locations, for example, have a minimum in the springtime due to O 3 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 O 3 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 O 3 and its precursor species. The MMM underestimates Arctic surface O 3 by 5% to 15% depending on the location. The vertical distribution of tropospheric O 3 is studied from recent ozonesonde measurements and the models. The models are highly variable, simulating free-tropospheric O 3 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 O 3 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 O 3 at high latitudes. For example, the MMM is biased high by about 20% at Eureka. Observed and simulated O 3 precursors (CO, NO x , 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 NO x but overestimates PAN. Perhaps as a result of competing deficiencies, the MMM O 3 matches the observed O 3 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 O 3 .

54 ENVIRONMENTAL SCIENCES↗