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Importance of a Priori Vertical Ozone Profiles for TEMPO Air Quality Retrievals

Ozone (O3) is a toxic pollutant which plays a major role in air quality. Typically, monitoring of surface air quality and O3 mixing ratios is conducted using in situ measurement networks. This is partially due to high-quality information related to air quality being limited from space-borne platforms due to coarse spatial resolution, limited temporal frequency, and minimal sensitivity to lower tropospheric and surface-level O3. The Tropospheric Emissions: Monitoring of Pollution (TEMPO) satellite is designed to address the limitations of current space-based platforms and to improve our ability to monitor North American air quality. TEMPO will provide hourly data of total column and vertical profiles of O3 with high spatial resolution to be used as a near-real-time air quality product. TEMPO O3 retrievals will apply the Smithsonian Astrophysical Observatory profile algorithm developed based on work from GOME (Global Ozone Monitoring Experiment), GOME-2, and OMI (Ozone Monitoring Instrument). This algorithm is suggested to use a priori O3 profile information from a climatological data-base developed from long-term ozone-sonde measurements (tropopause-based (TB-Clim) O3 climatology). This study evaluates the TB-Clim dataset and model simulated O3 profiles, which could potentially serve as a priori O3 profile information in TEMPO retrievals, from near-real-time data assimilation model products (NASA GMAO's (Global Modeling and Assimilation Office) operational GEOS-5 (Goddard Earth Observing System, Version 5) FP (Forecast Products) model and reanalysis data from MERRA2 (Modern-Era Retrospective analysis for Research and Applications, Version 2)) and a full chemical transport model (CTM), GEOS-Chem. In this study, vertical profile products are evaluated with surface (0-2 kilometers) and tropospheric (0-10 kilometers) TOLNet (Tropospheric Ozone Lidar Network) observations and the theoretical impact of individual a priori profile sources on the accuracy of TEMPO O3 retrievals in the troposphere and at the surface are presented. Results indicate that while the TB-Clim climatological dataset can replicate seasonally-averaged tropospheric O3 profiles, model-simulated profiles from a full CTM resulted in more accurate tropospheric and surface-level O3 retrievals from TEMPO when compared to hourly and daily-averaged TOLNet observations. Furthermore, it is shown that when large surface O3 mixing ratios are observed, TEMPO retrieval values at the surface are most accurate when applying CTM a priori profile information compared to all other data products.

Priori↗

Interhemispheric differences in polar stratospheric HNO3, H2O, ClO, and O3

Simultaneous global measurements of nitric acid (HNO3), water (H2O), chlorine monoxide (ClO), and ozone (O3) in the stratosphere have been obtained over complete annual cycles in both hemispheres by the Microwave Limb Sounder on the Upper Atmosphere Research Satellite. A sizeable decrease in gas-phase HNO3 was evident in the lower stratospheric vortex over Antarctica by early June 1992, followed by a significant reduction in gas-phase H2O after mid-July. By mid-August, near the time of peak ClO, abundances of gas-phase HNO3 and H2O were extremely low. The concentrations of HNO3 and H2O over Antarctica remained depressed into November, well after temperatures in the lower stratosphere had risen above the evaporation threshold for polar stratospheric clouds, implying that denitrification and dehydration had occurred. No large decreases in either gas-phase HNO3 or H2O were observed in the 1992-1993 Arctic winter vortex. Although ClO was enhanced over the Arctic as it was over the Antarctic, Arctic O3 depletion was substantially smaller than that over Antarctica. A major factor currently limiting the formation of an Arctic ozone 'hole' is the lack of denitrification in the northern polar vortex, but future cooling of the lower stratosphere could lead to more intense denitrification and consequently larger losses of Arctic ozone.

Santee, M. L.↗

Evaluating a Priori Ozone Profile Information Used in TEMPO Tropospheric Ozone Retrievals

Ozone (O3) is a greenhouse gas and toxic pollutant which plays a major role in air quality. Typically, monitoring of surface air quality and O3 mixing ratios is primarily conducted using in situ measurement networks. This is partially due to high-quality information related to air quality being limited from space-borne platforms due to coarse spatial resolution, limited temporal frequency, and minimal sensitivity to lower tropospheric and surface-level O3. The Tropospheric Emissions: Monitoring of Pollution (TEMPO) satellite is designed to address these limitations of current space-based platforms and to improve our ability to monitor North American air quality. TEMPO will provide hourly data of total column and vertical profiles of O3 with high spatial resolution to be used as a near-real-time air quality product.TEMPO O3 retrievals will apply the Smithsonian Astrophysical Observatory profile algorithm developed based on work from GOME, GOME-2, and OMI. This algorithm uses a priori O3 profile information from a climatological data-base developed from long-term ozone-sonde measurements (tropopause-based (TB) O3 climatology). It has been shown that satellite O3 retrievals are sensitive to a priori O3 profiles and covariance matrices. During this work we investigate the climatological data to be used in TEMPO algorithms (TB O3) and simulated data from the NASA GMAO Goddard Earth Observing System (GEOS-5) Forward Processing (FP) near-real-time (NRT) model products. These two data products will be evaluated with ground-based lidar data from the Tropospheric Ozone Lidar Network (TOLNet) at various locations of the US. This study evaluates the TB climatology, GEOS-5 climatology, and 3-hourly GEOS-5 data compared to lower tropospheric observations to demonstrate the accuracy of a priori information to potentially be used in TEMPO O3 algorithms. Here we present our initial analysis and the theoretical impact on TEMPO retrievals in the lower troposphere.

TEMPO↗

Evaluating A Priori Ozone Profile Information Used in TEMPO Tropospheric Ozone Retrievals

Ozone (O3) is a greenhouse gas and toxic pollutant which plays a major role in air quality. Typically, monitoring of surface air quality and O3 mixing ratios is primarily conducted using in situ measurement networks. This is partially due to high-quality information related to air quality being limited from space-borne platforms due to coarse spatial resolution, limited temporal frequency, and minimal sensitivity to lower tropospheric and surface-level O3. The Tropospheric Emissions: Monitoring of Pollution (TEMPO) satellite is designed to address these limitations of current space-based platforms and to improve our ability to monitor North American air quality. TEMPO will provide hourly data of total column and vertical profiles of O3 with high spatial resolution to be used as a near-real-time air quality product. TEMPO O3 retrievals will apply the Smithsonian Astrophysical Observatory profile algorithm developed based on work from GOME, GOME-2, and OMI. This algorithm uses a priori O3 profile information from a climatological data-base developed from long-term ozone-sonde measurements (tropopause-based (TB) O3 climatology). It has been shown that satellite O3 retrievals are sensitive to a priori O3 profiles and covariance matrices. During this work we investigate the climatological data to be used in TEMPO algorithms (TB O3) and simulated data from the NASA GMAO Goddard Earth Observing System (GEOS-5) Forward Processing (FP) near-real-time (NRT) model products. These two data products will be evaluated with ground-based lidar data from the Tropospheric Ozone Lidar Network (TOLNet) at various locations of the US. This study evaluates the TB climatology, GEOS-5 climatology, and 3-hourly GEOS-5 data compared to lower tropospheric observations to demonstrate the accuracy of a priori information to potentially be used in TEMPO O3 algorithms. Here we present our initial analysis and the theoretical impact on TEMPO retrievals in the lower troposphere.

ozone↗

Global Multi-Year O3-CO Correlation Patterns from Models and TES Satellite Observations

The correlation between measured tropospheric ozone (O3) and carbon monoxide (CO) has been used extensively in tropospheric chemistry studies to explore the photochemical characteristics of different regions and to evaluate the ability of models to capture these characteristics. Here, we present the first study that uses multi-year, global, vertically resolved, simultaneous and collocated O3 and CO satellite (Tropospheric Emission Spectrometer) measurements, to determine this correlation in the middle/lower free troposphere for two different seasons, and to evaluate two chemistry-climate models. We find results that are fairly robust across different years, altitudes and timescales considered, which indicates that the correlation maps presented here could be used in future model evaluations. The highest positive correlations (around 0.8) are found in the northern Pacific during summer, which is a common feature in the observations and the G-PUCCINI model. We make quantitative comparisons between the models using a single-figure metric (C), which we define as the correlation coefficient between the modeled and the observed O3-CO correlations for different regions of the globe. On a global scale, the G-PUCCINI model shows a good performance in the summer (C =0.71) and a satisfactory performance in the winter (C = 0.52). It captures midlatitude features very well, especially in the summer, whereas the performance in regions like South America or Central Africa is weaker. The UKCA model (C = 0.46/0.15 for July-August/December-January on a global scale) performs better in certain regions, such as the tropics in winter, and it captures some of the broad characteristics of summer extratropical correlations, but it systematically underestimates the O3-CO correlations over much of the globe. It is noteworthy that the correlations look very different in the two models, even though the ozone distributions are similar. This demonstrates that this technique provides a powerful global constraint for understanding modeled tropospheric chemical processes. We investigated the sources of the correlations by performing a series of sensitivity experiments. In these, the sign of the correlation is, in most cases, insensitive to removing different individual emissions, but its magnitude changes downwind of emission regions when applying such perturbations. Interestingly, we find that the O3-CO correlation does not solely reflect the strength of O3 photochemical production, as often assumed by earlier studies, but is more complicated and may reflect a mixture of different processes such as transport.

Voulgarakis, A.↗

Active and Widespread Halogen Chemistry in the Tropical and Subtropical Free Troposphere

Halogens in the troposphere are increasingly recognized as playing an important role for atmospheric chemistry, and possibly climate. Bromine and iodine react catalytically to destroy ozone (O3), oxidize mercury, and modify oxidative capacity that is relevant for the lifetime of greenhouse gases. Most of the tropospheric O3 and methane (CH4) loss occurs at tropical latitudes. Here we report simultaneous measurements of vertical profiles of bromine oxide (BrO) and iodine oxide (IO) in the tropical and subtropical free troposphere (10degN to 40degS), and show that these halogens are responsible for 34% of the column-integrated loss of tropospheric O3. The observed BrO concentrations increase strongly with altitude (approx.3.4 pptv at 13.5 km), and are 2-4 times higher than predicted in the tropical free troposphere. BrO resembles model predictions more closely in stratospheric air. The largest model low bias is observed in the lower tropical transition layer (TTL) over the tropical eastern Pacific Ocean, and may reflect a missing inorganic bromine source supplying an additional 2.5-6.4 pptv total inorganic bromine (Bry), or model overestimated Bry wet scavenging. Our results highlight the importance of heterogeneous chemistry on ice clouds, and imply an additional Bry source from the debromination of sea salt residue in the lower TTL. The observed levels of bromine oxidize mercury up to 3.5 times faster than models predict, possibly increasing mercury deposition to the ocean. The halogen-catalyzed loss of tropospheric O3 needs to be considered when estimating past and future ozone radiative effects.

Wang, Siyuan↗

Evaluation of NASA's High-Resolution Global Composition Simulations: Understanding a Pollution Event in the Chesapeake Bay During the Summer 2017 OWLETS Campaign

Recirculation of pollutants due to a bay breeze effect is a key meteorological mechanism impacting air quality near urban coastal areas, but regional and global chemical transport models have historically struggled to capture this phenomenon. We present a case study of a high ozone (O3) episode observed over the Chesapeake Bay during the NASA Ozone Water-Land Environmental Transition Study (OWLETS) in summer 2017. OWLETS included a complementary suite of ground-based and airborne observations, with which we characterize the meteorological and chemical context of this event and develop a framework to evaluate model performance. Two publicly-available NASA global high-resolution coupled chemistry-meteorology models (CCMMs) are investigated: GEOS-CF and MERRA2-GMI. The GEOS-CF R squared value for comparisons between the NASA Sherpa C-23 aircraft measurements to the GEOS-CF resulted in good agreement (R squared: 0.67) on July 19th and fair agreement (R squared: 0.55) for July 20th. Compared to surface observations, we find the GEOS-CF product with a 25 x 25 km squared grid box, at an hourly (R squared: 0.62 to 0.87) and 15-minute (R squared: 0.64 to 0.87) interval for six regional sites outperforms the hourly nominally 50 x 50 km squared gridded MERRA2-GMI (R squared: 0.53 to 0.76) for four of the six sites, suggesting it is better capable of simulating complex chemical and meteorological features associated with ozone transport within the Chesapeake Bay airshed. When the GEOS-CF product was compared to the TOLNet LiDAR observations at both NASA Langley Research Center (LaRC) and the Chesapeake Bay Bridge Tunnel (CBBT), the median differences at LaRC were -6 to 8% and at CBBT were ± 7% between 400 to 2000 m ASL. This indicates that, for this case study, the GEOS-CF is able to simulate surface level ozone diurnal cycles and vertical ozone profiles at small scales between the surface level and 2000 m ASL. Evaluating global chemical model simulations at sub-regional scales will help air quality scientists understand the complex processes occurring at small spatial and temporal scales within complex surface terrain changes, simulating nighttime chemistry and deposition, and the potential to use global chemical transport simulations in support of regional and sub-regional field campaigns.

NASA Ozone Water-Land Environmental Transition Stu↗

Response of the rat erythrocyte to ozone exposure

Sprague-Dawley rats were exposed to high (6-8 ppm) and moderate (1.5 ppm) amounts of ozone (O3) for various time periods. Response of the rat erythrocyte to ozone was monitored with red blood cell potassium (rubidium) influx studies, with storage stress combined with ultrastructural studies and with levels of erythrocyte glutathione peroxidase and superoxide dismutase. Erythrocytes of rats exposed to O3 showed no significant changes either in their potassium influx or in their glutathione peroxidase and superoxide dismutase activities compared to controls. Erythrocyte differential counts on O3-exposed animals showed significant changes initially as well as following storage stress compared to controls. Rats exposed to 8 ppm O3 for 4 h showed a marked increase in echinocytes. These consistent transformations from discocytes to echinocytes following O3 exposure suggest latent erythrocyte damage has occurred.

Larkin, E. C.↗

Airborne lidar observations in the wintertime Arctic stratosphere - Ozone

Large-scale distributions of ozone (O3) were measured with an airborne lidar system as part of the 1989 Airborne Arctic Stratospheric Expedition. Measurements of O3 distributions were obtained between January 6 and February 15, 1989, on 15 long-range flights into the polar vortex from the Solar Air Station, Norway. The observed O3 distribution was found to clearly indicate the edge of the polar vortex and to be an effective tracer of dynamical processes in the lower stratosphere. On the last two flights of the expedition, large regions with reduced O3 levels were observed by the lidar inside the polar vortex. Ozone had decreased by as much as 17 percent in the center of these areas, and using the in situ measurements made on the ER-2 aircraft, it was concluded that this decline was due to chemical O3 destruction.

Browell, E. V.↗

PyroCbs from Australia Fires and its Impact Using Satellite Observations from CrIS and TROPOMI and Reanalysis Data

Pyrocumulonimbus (pyroCb) clouds are thunder clouds created by intense heat from the Earth’s surface. They are formed similarly to cumulonimbus clouds, but the intense heat that results in the vigorous updraft comes from fire, either large wildfires or volcanic eruptions. Australia’s unprecedented fire disasters at the end of 2019 to early 2020 emitted huge amounts of carbon monoxide (CO) and fire aerosol particles to the atmosphere, particularly during the pyroCb outbreak that occurred in southeast Australia between 29 December 2019 and 4 January 2020. It was estimated that at least 18 pyroCbs were generated during this episode, and some of them injected ice, smoke, and biomass burning gases above the local tropopause. An unprecedented abundance of H2O and CO in the stratosphere, and the displacement of background ozone (O3) and N2O from rapid ascent of air from the troposphere and lower stratosphere were found from satellite observations. Some other studies also found that the fire emissions and their long-range transport resulted in stratospheric aerosol, temperature, and O3 anomalies after the 2020 Australian bushfires and altered the Antarctic ozone and vortex, posing great impact to local air quality and climate change. Further study on the atmospheric thermodynamic status of atmosphere associated with these pyroCbs, and the change of the cloud properties and trace gases during this unprecedented Australia fires will be made using a new single Field of View (SFOV) Sounder Atmospheric Products (SiFSAP). SiFSAP was developed by NASA using the Cross-track Infrared Sounder (CrIS) and Advanced Technology Microwave Sounder (ATMS) onboard SNPP and JPSS-1, and will soon be available to the public at NASA DAAC. Since this product has a spatial resolution of 15 km at nadir, which is better than most global weather and climate models and other current operational sounding products, a process-oriented analysis of the dynamic transport of CO and fire plumes during this unprecedented fire disasters will be made in this study. Based on a Principal Component Radiative Transfer Model (PCRTM) and an optimized estimation retrieval algorithm, a simultaneously retrieval is made using the whole spectral information measured by CrIS, and the derived SiFSAP include temperature, water vapor, trace gases (such as O3, CO2, CO, CH4 and N2O), cloud properties and surface properties. Use of ATMS together with CrIS allows SiFSAP to get accurate retrieval products under thick pyroCb conditions, and an algorithm to detect pyroCb based on the hyperspectral infrared sounder spectrum from CrIS will be developed and verified. In addition to SiFSAP sounding products, other products like CO, O3, NO2 from TROPOMI, O3 from OMPS will be used for retrospective analysis. The wind fields from the NASA’s Modern-Era Retrospective Analysis for Research and Applications Version-2 (MERRA-2) and ERA5 will be used to characterize the transport, and the SiFSAP temperature and water vapor profiles within and around pyroCbs will be compared with MERRA-2 and ERA5 products.

Xiaozhen (Shawn) Xiong↗

Observation of Stratospheric Intrusions and Ozone Transport using CrIS SiFSAP Products

The Single Field of View (SFOV) ozone (O3) profiles derived from the Cross-track Infrared Sounder (CrIS) onboard Suomi National Polar-Orbiting Partnership (SNPP), with a high horizontal resolution of approximately 14 km at nadir and good sensitivity to O3 in the upper troposphere and lower stratosphere (UTLS), provide a prominent opportunity to examine stratosphere to troposphere (STT) transport. A process-oriented analysis was performed to examine the fine-scale features of a stratospheric intrusion (SI) event on June 11-13, 2017 in the southwestern US using the CrIS SFOV products together with wind and potential velocity (PV) from models. It was found that the location and strength of O3 enhancement correlate well with the PV contours, and the intrusion depth can be characterized using the vertical cross-sections of O3 and relative humidity (RH). In addition, the capability to use total column ozone (TCO) to identify SI events was confirmed through analysis of TCO from CrIS SFOV and other satellite and reanalysis products. The ozone/PV ratio was derived using SFOV O3 and model PV, and the values, ranging from 23.2 to 35.8 ppbv PVU-1 (1 PV unit (PVU) = 10-6 km2 kg-1 s-1), are in the lower end of previous estimations. These results demonstrate the advantages of the SFOV products in monitoring the fine-scale ozone transport and thermodynamic structure of SI events, as well as their potential value for weather and climate study.

Xiaozhen Xiong↗

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

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

Laminates↗

Hemispheric Differences in the Annual Cycle of Tropical Lower Stratosphere Transport and Tracers

Transport in the tropical lower stratosphere plays a major role in determining the composition of the entire stratosphere. Previous studies that quantified the relative role of transport processes have generally assumed well-mixed tropics and focused on tropical-wide average characteristics. However, it has recently been shown that there is a hemispheric difference in the annual cycle of tropical lower stratosphere ozone and other tracers, with a larger amplitude in the northern tropics (NT) than in the southern tropics (ST). In this study, we examined the ability of chemistry climate models (CCMs) to reproduce the hemispheric differences in ozone (O3) and other tracers (i.e., hydrochloric acid, or HCl and nitrous oxide, or N2O), and then use the CCMs to examine the cause of these differences. Examination of CCM simulations from the CCMVal-2 project shows that the majority of the CCMs produce the observed feature of a larger annual cycle in the NT than ST O3 and other tracers. However, only around a third of the models produce an ozone annual cycle similar to that observed. Transformed Eulerian Mean analysis of two of the CCMs shows that seasonality in vertical advection drives the seasonality in ST O3 and N2O while seasonality of horizontal mixing drives the seasonality in NT O3 and N2O, with a large increase in horizontal mixing during northern summer (associated with the Asian monsoon). Thus, latitudinal and longitudinal variations within the tropics have to be considered to fully understand the balance between transport processes in tropical lower stratosphere.

transport↗

Formation and Destruction of Ozone in Ices Relevant to Planetary and Satellite Surfaces

Ozone, O3, has been observed on the surfaces of Ganymede and the Saturnian satellites Dione and Rhea. It is generally accepted that in each case the O3 is formed by the magnetospheric irradiation of oxygen, O2, within water-rich icy surfaces. Carbon dioxide ice, which has been detected on a number of planetary-satellite surfaces, is another possible source of O3 after irradiation. Laboratory work to date has focused on O3 formation from irradiated O2 at 10 K using < 1O eV and 5 keV electrons and 100 keV protons. The temperature-dependent formation of O3 in solid O2 from 11 to 30 K using 5 keV electrons also has been examined. The objectives of the present laboratory study are (1) to compare O3 formation in O2 and CO2 ices using MeV proton and 10 keV electron bombardment at different temperatures, and (2) to examine ozone's thermal stability in different icy matrices (O2, CO2, H2O) during warming. Our results will aid in the understanding of these possible abiotic ozone sources, which is necessary when assessing O3 as a potential biomarker.

Moore, Marla H.↗

The evolution of ozone observed by UARS MLS in the 1992 late winter southern polar vortex

The evolution of ozone (O3) observed by the Microwave Limb Sounder on board the Upper Atmosphere Research Satellite is described for 14 Aug through 20 Sep 1992, in relation to the polar vortex. The development of an ozone hole is observed in column O3, and a corresponding decrease is seen in O3 mixing ratio in the polar lower stratosphere, consistent with chemical destruction. The observations also suggest that poleward transport associated with episodes of strong planetary wave activity is important in increasing O3 in the mid-stratosphere.

Manney, G. L.↗

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.↗