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At least 91 records · Page 5

Tropical Tropospheric Ozone from SHADOZ (Southern Hemisphere ADditional Ozonesondes) Network: A Project for Satellite Research, Process Studies, Education

The first climatological overview of total, stratospheric and tropospheric ozone in the southern hemisphere tropical and subtropics is based on ozone sounding data from 10 sites comprising the Southern Hemisphere Additional OZonesondes (SHADOZ) network. The period covered is 1998-2000. Observations were made over: Ascension Island; Nairobi, Kenya; Irene, South Africa; Reunion Island; Watukosek, Java; Fiji; Tahiti; American Samoa; San Cristobal, Galapagos; Natal, Brazil. Campaign data were collected on a trans-Atlantic oceanographic cruise and during SAFARI-2000 in Zambia. The ozone data, with simultaneous temperature profiles to approx. 7 hPa and relative humidity to approx. 200 hPa, reside at: . SHADOZ ozone time-series and profiles give a perspective on tropical total, stratospheric and tropospheric ozone. Prominent features are highly variable tropospheric ozone and a zonal wave-one pattern in total (and tropospheric) column ozone. Total, stratospheric and tropospheric column ozone amounts peak between August and November and are lowest between March and May. Tropospheric ozone variability over the Indian and Pacific Ocean displays influences of the Indian Ocean Dipole and convective mixing. Pollution transport from Africa and South America is a seasonal feature. Tropospheric ozone seasonality over the Atlantic Basin shows effects of regional subsidence and recirculation as well as biomass burning. Dynamical and chemical influences appear to be of comparable magnitude though model studies are needed to quantify this.

Thompson, Anne M.↗

Characterization of Transport Errors in Chemical Forecasts from a Global Tropospheric Chemical Transport Model

We propose a new methodology to characterize errors in the representation of transport processes in chemical transport models. We constrain the evaluation of a global three-dimensional chemical transport model (GEOS-CHEM) with an extended dataset of carbon monoxide (CO) concentrations obtained during the Transport and Chemical Evolution over the Pacific (TRACE-P) aircraft campaign. The TRACEP mission took place over the western Pacific, a region frequently impacted by continental outflow associated with different synoptic-scale weather systems (such as cold fronts) and deep convection, and thus provides a valuable dataset. for our analysis. Model simulations using both forecast and assimilated meteorology are examined. Background CO concentrations are computed as a function of latitude and altitude and subsequently subtracted from both the observed and the model datasets to focus on the ability of the model to simulate variability on a synoptic scale. Different sampling strategies (i.e., spatial displacement and smoothing) are applied along the flight tracks to search for systematic model biases. Statistical quantities such as correlation coefficient and centered root-mean-square difference are computed between the simulated and the observed fields and are further inter-compared using Taylor diagrams. We find no systematic bias in the model for the TRACE-P region when we consider the entire dataset (i.e., from the surface to 12 km ). This result indicates that the transport error in our model is globally unbiased, which has important implications for using the model to conduct inverse modeling studies. Using the First-Look assimilated meteorology only provides little improvement of the correlation, in comparison with the forecast meteorology. These general statements can be refined when the entire dataset is divided into different vertical domains, i.e., the lower troposphere (less than 2 km), the middle troposphere (2-6 km), and the upper troposphere (greater than 6 km). The best agreement between the observations and the model is found in the lower and middle troposphere. Downward displacements in the lower troposphere provide a better fit with the observed value, which could indicate a problem in the representation of boundary layer height in the model. Significant improvement is also found for downward and southward displacements in the upper troposphere. There are several potential sources of errors in our simulation of the continental outflow in the upper troposphere which could lead to such biases, including the location and/or the strength of deep convective cells as well as that of wildfires in Southeast Asia.

Bey, I.↗

Reactive Nitrogen Distribution and Partitioning in the North American Troposphere and Lowermost Stratosphere

A comprehensive group of reactive nitrogen species (NO, NO2, HNO3, HO2NO2, PANs, alkyl nitrates, and aerosol-NO3) were measured in the troposphere and lowermost stratosphere over North America and the Atlantic during July/August 2004 (INTEX-A) from the NASA DC-8 platform (0.1-12 km). Less reactive nitrogen species (HCN and CH3CN), that are also unique tracers of biomass combustion, were also measured along with a host of other gaseous (CO, VOC, OVOC, halocarbon) and aerosol tracers. Clean background air as well as air with influences from biogenic emissions, anthropogenic pollution, biomass combustion, and stratosphere was sampled both over continental U. S., Atlantic and Pacific. The North American upper troposphere was found to be greatly influenced by both lightning NO(x) and surface pollution lofted via convection and contained elevated concentrations of PAN, ozone, hydrocarbons, and NO(x). Under polluted conditions PAN was a dominant carrier of reactive nitrogen in the upper troposphere while nitric acid dominated in the lower troposphere. Peroxynitric acid (HO2NO2) was present in sizable concentrations always peaking at around 8 km. Aerosol nitrate appeared to be mostly contained in large soil based particles in the lower troposphere. Plumes from Alaskan fires contained large amounts of PAN and very little enhancement in ozone. Observational data suggest that lightning was a far greater contributor to NO(x) in the upper troposphere than previously believed. NO(x) and NO(y) reservoir appeared to be in steady state only in the middle troposphere where NO(x)/NO(y) was independent of air mass age. A first comparison of observed data with simulations from four 3-D models shows significant differences between observations and models as well as among models. These uncertainties likely propagate themselves in satellites derived NOx data. Observed data are interpreted to suggest that soil sinks of HCN/CH3CN are at best very small. We investigate the partitioning and interplay of the reactive nitrogen species within characteristic air masses and further examine their role in ozone formation.

Singh, H. B.↗

Climate Response to the Increase in Tropospheric Ozone since Preindustrial Times: A Comparison between Ozone and Equivalent CO2 Forcings

We examine the characteristics of the climate response to anthropogenic changes in tropospheric ozone. Using a general circulation model, we have carried out a pair of equilibrium climate simulations with realistic present-day and preindustrial ozone distributions. We find that the instantaneous radiative forcing of 0.49 W m(sup -2) due to the increase in tropospheric ozone since preindustrial times results in an increase in global mean surface temperature of 0.28 C. The increase is nearly 0.4 C in the Northern Hemisphere and about 0.2 C in the Southern Hemisphere. The largest increases (greater than 0.8 C) are downwind of Europe and Asia and over the North American interior in summer. In the lower stratosphere, global mean temperatures decrease by about 0.2 C due to the diminished upward flux of radiation at 9.6 micrometers. The largest stratospheric cooling, up to 1.0 C, occurs over high northern latitudes in winter, with possibly important implications for the formation of polar stratospheric clouds. To identify the characteristics of climate forcing unique to tropospheric ozone, we have conducted two additional climate equilibrium simulations: one in which preindustrial tropospheric ozone concentrations were increased everywhere by 18 ppb, producing the same global radiative forcing as present-day ozone but without the heterogeneity; and one in which CO2 was decreased by 25 ppm relative to present day, with ozone at present-day values, to again produce the same global radiative forcing but with the spectral signature of CO2 rather than ozone. In the first simulation (uniform increase of ozone), the global mean surface temperature increases by 0.25 C, with an interhemispheric difference of only 0.03 C, as compared with nearly 0.2 C for the heterogeneous ozone increase. In the second simulation (equivalent CO2), the global mean surface temperature increases by 0.36 C, 30% higher than the increase from tropospheric ozone. The stronger surface warming from CO2 is in part because CO2 forcing (obscured by water vapor) is shifted relatively poleward where the positive ice-albedo feedback amplifies the climate response and in part because the magnitude of the CO2 forcing in the mid-troposphere is double that of ozone. However, we find that CO2 is far less effective than tropospheric ozone in driving lower stratospheric cooling at high northern latitudes in winter.

Mickley L. J.↗

Software for Generating Troposphere Corrections for InSAR Using GPS and Weather Model Data

Atmospheric errors due to the troposphere are a limiting error source for spaceborne interferometric synthetic aperture radar (InSAR) imaging. This software generates tropospheric delay maps that can be used to correct atmospheric artifacts in InSAR data. The software automatically acquires all needed GPS (Global Positioning System), weather, and Digital Elevation Map data, and generates a tropospheric correction map using a novel algorithm for combining GPS and weather information while accounting for terrain. Existing JPL software was prototypical in nature, required a MATLAB license, required additional steps to acquire and ingest needed GPS and weather data, and did not account for topography in interpolation. Previous software did not achieve a level of automation suitable for integration in a Web portal. This software overcomes these issues. GPS estimates of tropospheric delay are a source of corrections that can be used to form correction maps to be applied to InSAR data, but the spacing of GPS stations is insufficient to remove short-wavelength tropospheric artifacts. This software combines interpolated GPS delay with weather model precipitable water vapor (PWV) and a digital elevation model to account for terrain, increasing the spatial resolution of the tropospheric correction maps and thus removing short wavelength tropospheric artifacts to a greater extent. It will be integrated into a Web portal request system, allowing use in a future L-band SAR Earth radar mission data system. This will be a significant contribution to its technology readiness, building on existing investments in in situ space geodetic networks, and improving timeliness, quality, and science value of the collected data

Moore, Angelyn W.↗

Global Free Tropospheric NO2 Abundances Derived Using a Cloud Slicing Technique Applied to Satellite Observations from the Aura Ozone Monitoring Instrument (OMI)

We derive free-tropospheric NO2 volume mixing ratios (VMRs) and stratospheric column amounts of NO2 by applying a cloud slicing technique to data from the Ozone Monitoring Instrument (OMI) on the Aura satellite. In the cloud-slicing approach, the slope of the above-cloud NO2 column versus the cloud scene pressure is proportional to the NO2 VMR. In this work, we use a sample of nearby OMI pixel data from a single orbit for the linear fit. The OMI data include cloud scene pressures from the rotational-Raman algorithm and above-cloud NO2 vertical column density (VCD) (defined as the NO2 column from the cloud scene pressure to the top-of-the-atmosphere) from a differential optical absorption spectroscopy (DOAS) algorithm. Estimates of stratospheric column NO2 are obtained by extrapolating the linear fits to the tropopause. We compare OMI-derived NO2 VMRs with in situ aircraft profiles measured during the NASA Intercontinental Chemical Transport Experiment Phase B (INTEX-B) campaign in 2006. The agreement is generally within the estimated uncertainties when appropriate data screening is applied. We then derive a global seasonal climatology of free-tropospheric NO2 VMR in cloudy conditions. Enhanced NO2 in the free troposphere commonly appears near polluted urban locations where NO2 produced in the boundary layer may be transported vertically out of the boundary layer and then horizontally away from the source. Signatures of lightning NO2 are also shown throughout low and middle latitude regions in summer months. A profile analysis of our cloud slicing data indicates signatures of uplifted and transported anthropogenic NO2 in the middle troposphere as well as lightning-generated NO2 in the upper troposphere. Comparison of the climatology with simulations from the Global Modeling Initiative (GMI) for cloudy conditions (cloud optical thicknesses > 10) shows similarities in the spatial patterns of continental pollution outflow. However, there are also some differences in the seasonal variation of free-tropospheric NO2 VMRs near highly populated regions and in areas affected by lightning-generated NOx. Stratospheric column NO2 obtained from cloud slicing agrees well with other independently-generated estimates, providing further confidence in the free-tropospheric results.

NO2↗

Global-scale distribution of ozone in the remote troposphere from ATom and HIPPO airborne field missions

Ozone is a key constituent of the troposphere, where it drives photochemical processes, impacts air quality, and acts as a climate forcer. Large-scale in situ observations of ozone commensurate with the grid resolution of current Earth system models are necessary to validate model outputs and satellite retrievals. In this paper, we examine measurements from the Atmospheric Tomography (ATom; four deployments in 2016–2018) and the HIAPER Pole-to-Pole Observations (HIPPO; five deployments in 2009–2011) experiments, two global-scale airborne campaigns covering the Pacific and Atlantic basins. ATom and HIPPO represent the first global-scale, vertically resolved measurements of O3 distributions throughout the troposphere, with HIPPO sampling the atmosphere over the Pacific and ATom sampling both the Pacific and Atlantic. Given the relatively limited temporal resolution of these two campaigns, we first compare ATom and HIPPO ozone data to longer-term observational records to establish the representativeness of our dataset. We show that these two airborne campaigns captured on average 53 %, 54 %, and 38 % of the ozone variability in the marine boundary layer, free troposphere, and upper troposphere–lower stratosphere (UTLS), respectively, at nine well-established ozonesonde sites. Additionally, ATom captured the most frequent ozone concentrations measured by regular commercial aircraft flights in the northern Atlantic UTLS. We then use the repeated vertical profiles from these two campaigns to confirm and extend the existing knowledge of tropospheric ozone spatial and vertical distributions throughout the remote troposphere. We highlight a clear hemispheric gradient, with greater ozone in the Northern Hemisphere, consistent with greater precursor emissions and consistent with previous modeling and satellite studies. We also show that the ozone distribution below 8 km was similar in the extra-tropics of the Atlantic and Pacific basins, likely due to zonal circulation patterns. However, twice as much ozone was found in the tropical Atlantic as in the tropical Pacific, due to well-documented dynamical patterns transporting continental air masses over the Atlantic. Finally, we show that the seasonal variability of tropospheric ozone over the Pacific and the Atlantic basins is driven year-round by transported continental plumes and photochemistry, and the vertical distribution is driven by photochemistry and mixing with stratospheric air. This new dataset provides additional constraints for global climate and chemistry models to improve our understanding of both ozone production and loss processes in remote regions, as well as the influence of anthropogenic emissions on baseline ozone.

ATom, aircraft profiles, Atlantic pollution, ozone↗

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↗

Impact of Surface Emissions to the Zonal Variability of Tropical Tropospheric Ozone and Carbon Monoxide for November 2004

The chemical and dynamical processes governing the zonal variability of tropical tropospheric ozone and carbon monoxide are investigated for November 2004 using satellite observations, in-situ measurements, and chemical transport models in conjunction with inverse-estimated surface emissions. Vertical ozone profile estimates from the Tropospheric Emission Spectrometer (TES) and ozone sonde measurements from the Southern Hemisphere Additional Ozonesondes (SHADOZ) network show the so called zonal 'wave-one' pattern, which is characterized by peak ozone concentrations (70-80 ppb) centered over the Atlantic, as well as elevated concentrations of ozone over Indonesia and Australia (60-70 ppb) in the lower troposphere. Observational evidence from TES CO vertical profiles and Ozone Monitoring Instrument (OMI) NO2 columns point to regional surface emissions as an important contributor to the elevated ozone over Indonesia. This contribution is investigated with the GEOS-Chem chemistry and transport model using surface emission estimates derived from an optimal inverse model, which was constrained by TES and Measurements Of Pollution In The Troposphere (MOPITT) CO profiles (Jones et al., 2007). These a posteriori estimates, which were over a factor of 2 greater than climatological emissions, reduced differences between GEOS-Chem and TES ozone observations by 30-40% and led to changes in GEOS-Chem upper tropospheric ozone of up to 40% over Indonesia. The remaining residual differences can be explained in part by upper tropospheric ozone produced from lightning NOx in the South Atlantic. Furthermore, model simulations from GEOS-Chem indicate that ozone over Indonesian/Australian is more sensitive to changes in surface emissions of NOx than ozone over the tropical Atlantic.

tropical tropospheric ozone↗

Quantifying isentropic stratosphere-troposphere exchange of ozone

There is increased evidence that stratosphere-troposphere exchange (STE) of ozone has a significant impact on tropospheric chemistry and radiation. Traditional diagnostics of STE consider the ozone budget in the lowermost stratosphere (LMS) as a whole. However, this can only render the hemispherically integrated ozone flux and therefore does not distinguish the exchange of ozone into low latitudes from that into high latitudes. The exchange of ozone at different latitudes may have different tropospheric impacts. This present study extends the traditional approach from the entire LMS to individual isentropic layers in the LMS and therefore gives the meridional distribution of STE by the latitudes where each isentropic surface intersects the tropopause. The specified dynamics version of the Whole Atmosphere Community Climate Model is used to estimate the STE ozone flux on each isentropic surface. It is found that net troposphere-to-stratosphere ozone transport occurs in low latitudes along the 350–380 K isentropic surfaces and that net stratosphere-to-troposphere ozone transport takes place in the extratropics along the 280–350 K isentropes. Particularly, the seasonal cycle of extratropical STE ozone flux in the Northern Hemisphere displays a maximum in late spring and early summer, following the seasonal migration of the upper tropospheric jet and associated isentropic mixing. Moreover, differential diabatic heating and isentropic mixing tend to induce STE ozone fluxes in opposite directions, but the net effect results in a spatiotemporal pattern similar to the STE ozone flux associated with isentropic mixing.

54 ENVIRONMENTAL SCIENCES↗

(abstract) Tropospheric Calibration for the Mars Observer Gravity Wave Experiment

In spring 1993, microwave radiometer-based tropospheric calibration was provided for the Mars Observer gravitational wave search. The Doppler shifted X-band radio signals propagating between Earth and the Mars Observer satellite were precisely measured to determine path length variations that might signal passage of gravitational waves. Experimental sensitivity was restricted by competing sources of variability in signal transit time. Principally, fluctuations in the solar wind and ionospheric plasma density combined with fluctions in tropospheric refractivity determined the detection limit. Troposphere-induced path delay fluctions are dominated by refractive changes caused by water vapor inhomogeneities blowing through the signal path. Since passive microwave remote sensing techniques are able to determine atmospheric propagation delays, radiometer-based tropospheric calibration was provided at the Deep Space Network Uranus tracking site (DSS-15). Two microwave water vapor radiometers (WVRs), a microwave temperature profiler (MTP), and a ground based meterological station were deployed to determine line-of-sight vapor content and vertical temperature profile concurrently with Mars Observer tracking measurements. This calibration system provided the capability to correct Mars Observer Doppler data for troposphere-induced path variations. We present preliminary analysis of the Doppler and WVR data sets illustrating the utility of WVRs to calibrate Doppler data. This takes an important step toward realizing the ambitious system required to support future Ka-band Cassini satellite gravity wave tropospheric calibration system.

atmospheric water vapor microwave remote sensing↗

Linkages Between Ozone-depleting Substances, Tropospheric Oxidation and Aerosols

Coupling between the stratosphere and the troposphere allows changes in stratospheric ozone abundances to affect tropospheric chemistry. Large-scale effects from such changes on chemically produced tropospheric aerosols have not been systematically examined in past studies. We use a composition-climate model to investigate potential past and future impacts of changes in stratospheric ozone depleting substances (ODS) on tropospheric oxidants and sulfate aerosols. In most experiments, we find significant responses in tropospheric photolysis and oxidants, with small but significant effects on methane radiative forcing. The response of sulfate aerosols is sizeable when examining the effect of increasing future nitrous oxide (N2O) emissions. We also find that without the regulation of chlorofluorocarbons (CFCs) through the Montreal Protocol, sulfate aerosols could have increased by 2050 by a comparable amount to the decreases predicted due to relatively stringent sulfur emissions controls. The individual historical radiative forcings of CFCs and N2O through their indirect effects on methane (−22.6mW/sq. m for CFCs and −6.7mW/sq. m for N2O) and sulfate aerosols (−3.0mW/sq. m for CFCs and +6.5mW/sq. m for N2O when considering the direct aerosol effect) discussed here are non-negligible when compared to known historical ODS forcing. Our results stress the importance of accounting for stratosphere-troposphere, gas-aerosol and composition-climate interactions when investigating the effects of changing emissions on atmospheric composition and climate.

troposphere↗

A New Differential Absorption Lidar to Measure Sub-Hourly Fluctuation of Tropospheric Ozone Profiles in the Baltimore - Washington D.C. Region

Tropospheric ozone profiles have been retrieved from the new ground based National Aeronautics and Space Administration (NASA) Goddard Space Flight Center TROPospheric OZone DIfferential Absorption Lidar (GSFC TROPOZ DIAL) in Greenbelt, MD (38.99 N, 76.84 W, 57 meters ASL) from 400 m to 12 km AGL. Current atmospheric satellite instruments cannot peer through the optically thick stratospheric ozone layer to remotely sense boundary layer tropospheric ozone. In order to monitor this lower ozone more effectively, the Tropospheric Ozone Lidar Network (TOLNet) has been developed, which currently consists of five stations across the US. The GSFC TROPOZ DIAL is based on the Differential Absorption Lidar (DIAL) technique, which currently detects two wavelengths, 289 and 299 nm. Ozone is absorbed more strongly at 289 nm than at 299 nm. The DIAL technique exploits this difference between the returned backscatter signals to obtain the ozone number density as a function of altitude. The transmitted wavelengths are generated by focusing the output of a quadrupled Nd:YAG laser beam (266 nm) into a pair of Raman cells, filled with high pressure hydrogen and deuterium. Stimulated Raman Scattering (SRS) within the focus generates a significant fraction of the pump energy at the first Stokes shift. With the knowledge of the ozone absorption coefficient at these two wavelengths, the range resolved number density can be derived. An interesting atmospheric case study involving the Stratospheric-Tropospheric Exchange (STE) of ozone is shown to emphasize the regional importance of this instrument as well as assessing the validation and calibration of data. The retrieval yields an uncertainty of 16-19 percent from 0-1.5 km, 10-18 percent from 1.5-3 km, and 11-25 percent from 3 km to 12 km. There are currently surface ozone measurements hourly and ozonesonde launches occasionally, but this system will be the first to make routine tropospheric ozone profile measurements in the Baltimore-Washington DC area.

Stimulated Raman Scattering↗

Pre-industrial to End 21st Century Projections of Tropospheric Ozone from the Atmospheric Chemistry and Climate Model Intercomparison Project (ACCMIP)

Present day tropospheric ozone and its changes between 1850 and 2100 are considered, analysing 15 global models that participated in the Atmospheric Chemistry and Climate Model Intercomparison Project (ACCMIP). The ensemble mean compares well against present day observations. The seasonal cycle correlates well, except for some locations in the tropical upper troposphere. Most (75 %) of the models are encompassed with a range of global mean tropospheric ozone column estimates from satellite data, but there is a suggestion of a high bias in the Northern Hemisphere and a low bias in the Southern Hemisphere, which could indicate deficiencies with the ozone precursor emissions. Compared to the present day ensemble mean tropospheric ozone burden of 337+/-23 Tg, the ensemble mean burden for 1850 time slice is approx. 30% lower. Future changes were modelled using emissions and climate projections from four Representative Concentration Pathways (RCPs). Compared to 2000, the relative changes in the ensemble mean tropospheric ozone burden in 2030 (2100) for the different RCPs are: −4% (−16 %) for RCP2.6, 2% (−7%) for RCP4.5, 1% (−9%) for RCP6.0, and 7% (18 %) for RCP8.5. Model agreement on the magnitude of the change is greatest for larger changes. Reductions in most precursor emissions are common across the RCPs and drive ozone decreases in all but RCP8.5, where doubled methane and a 40-150% greater stratospheric influx (estimated from a subset of models) increase ozone. While models with a high ozone burden for the present day also have high ozone burdens for the other time slices, no model consistently predicts large or small ozone changes; i.e. the magnitudes of the burdens and burden changes do not appear to be related simply, and the models are sensitive to emissions and climate changes in different ways. Spatial patterns of ozone changes are well correlated across most models, but are notably different for models without time evolving stratospheric ozone concentrations. A unified approach to ozone budget specifications and a rigorous investigation of the factors that drive tropospheric ozone is recommended to help future studies attribute ozone changes and inter-model differences more clearly.

Troposphere↗

Northern Winter Climate Change: Assessment of Uncertainty in CMIP5 Projections Related to Stratosphere-Troposphere Coupling

Future changes in the stratospheric circulation could have an important impact on northern winter tropospheric climate change, given that sea level pressure (SLP) responds not only to tropospheric circulation variations but also to vertically coherent variations in troposphere-stratosphere circulation. Here we assess northern winter stratospheric change and its potential to influence surface climate change in the Coupled Model Intercomparison Project-Phase 5 (CMIP5) multimodel ensemble. In the stratosphere at high latitudes, an easterly change in zonally averaged zonal wind is found for the majority of the CMIP5 models, under the Representative Concentration Pathway 8.5 scenario. Comparable results are also found in the 1% CO2 increase per year projections, indicating that the stratospheric easterly change is common feature in future climate projections. This stratospheric wind change, however, shows a significant spread among the models. By using linear regression, we quantify the impact of tropical upper troposphere warming, polar amplification, and the stratospheric wind change on SLP. We find that the intermodel spread in stratospheric wind change contributes substantially to the intermodel spread in Arctic SLP change. The role of the stratosphere in determining part of the spread in SLP change is supported by the fact that the SLP change lags the stratospheric zonally averaged wind change. Taken together, these findings provide further support for the importance of simulating the coupling between the stratosphere and the troposphere, to narrow the uncertainty in the future projection of tropospheric circulation changes.

climate change↗

Highlights from the 11-Year Record of Tropospheric Ozone from OMI/MLS and Continuation of that Long Record Using OMPS Measurements

Since October 2004 the Ozone Monitoring Instrument (OMI) and Microwave Limb Sounder (MLS) onboard the Aura satellite have provided over 11 years of continuous tropospheric ozone measurements. These OMI/MLS measurements have been used in many studies to evaluate dynamical and photochemical effects caused by ENSO, the Madden-Julian Oscillation (MJO) and shorter timescales, as well as long-term trends and the effects of deep convection on tropospheric ozone. Given that the OMI and MLS instruments have now extended well beyond their expected lifetimes, our goal is to continue their long record of tropospheric ozone using recent Ozone Mapping Profiler Suite (OMPS) measurements. The OMPS onboard the Suomi National Polar-orbiting Partnership NPP satellite was launched on October 28, 2011 and is comprised of three instruments: the nadir mapper, the nadir profiler, and the limb profiler. Our study combines total column ozone from the OMPS nadir mapper with stratospheric column ozone from the OMPS limb profiler to measure tropospheric ozone residual. The time period for the OMPS measurements is March 2012 present. For the OMPS limb profiler retrievals, the OMPS v2 algorithm from Goddard is tested against the University of Saskatchewan (USask) Algorithm. The retrieved ozone profiles from each of these algorithms are evaluated with ozone profiles from both ozonesondes and the Aura Microwave Limb Sounder (MLS). Effects on derived OMPS tropospheric ozone caused by the 2015-2016 El Nino event are highlighted. This recent El Nino produced anomalies in tropospheric ozone throughout the tropical Pacific involving increases of approximately 10 DU over Indonesia and decreases approximately 5-10 DU in the eastern Pacific. These changes in ozone due to El Nino were predominantly dynamically-induced, caused by the eastward shift in sea-surface temperature and convection from the western to the eastern Pacific.

MJO↗

Western US Tropospheric Ozone: An Assessment of Vertical and Seasonal Variations over California and Nevada

In the rural western US free-tropospheric O3 has risen in recent years as a result of rising Asian emissions, deep stratospheric intrusions and more frequent wildfires. This increasing O3 trend combined with the high surface elevation of much of the western US, which aids mixing between boundary layer and free-troposphere, pose challenges in attaining the more stringent O3 National Ambient Air Quality Standard (NAAQS) at many western US rural surface sites. As such, the ability to identify various sources and transport mechanisms that contribute towards surface O3 is increasingly important. This paper analyzes vertical profiles of O3 from the Alpha Jet Atmospheric eXperiment (AJAX) over California and Nevada, ozonesondes from Trinidad Head, CA and tropospheric ozone profiles from the differential absorption lidar (DIAL) at the JPL Table Mountain Facility, CA. Surface O3 from the US EPA Clean air Status and Trends Network (CASNET) are used to discuss surface trends. GEOS-Chem determines the trends in regional O3 and assess the contributions of various sources on surface O3. And Realtime Air Quality Modeling System (RAQMS) is used to forecast and interpret free-tropospheric observations. Specifically we will address the following questions: What are the effects of the lowered NAAQS? Do we observe elevated O3 during 2012 at surface sites reported in previous studies? And if so, what are the causes? How variable is free-tropospheric O3 over California and Nevada? How frequently do we observe high O3 lamina in the free troposphere and what are the surface impacts?

tropospheric↗

Impact of Regional Northern Hemisphere Mid-latitude Anthropogenic Sulfur Dioxide Emissions on Local and Remote Tropospheric Oxidants

The unintended consequences of reductions in regional anthropogenic sulfur dioxide (SO2) emissions implemented to protect human health are poorly understood. SO2 decreases began in the 1970s in the US and Europe and are expected to continue into the future, while recent emissions decreases in China are also projected to continue. In addition to the well-documented climate effects (warming) from reducing aerosols, tropospheric oxidation is impacted via aerosol modification of photolysis rates and radical sinks. Impacts on the hydroxyl radical and other trace constituents directly affect climate and air quality metrics such as surface ozone levels. We use the Geophysical Fluid Dynamics Laboratory Atmospheric Model version 3 nudged towards National Centers for Environmental Prediction (NCEP) reanalysis wind velocities to estimate the impact of SO2 emissions from the US, Europe, and China by differencing a control simulation with an otherwise identical simulation in which 2015 anthropogenic SO2 emissions are set to zero over one of the regions. Springtime sulfate aerosol changes occur both locally to the emission region and also throughout the Northern Hemispheric troposphere, including remote oceanic regions and the Arctic. Hydroperoxy (HO2) radicals are directly removed via heterogeneous chemistry on aerosol surfaces, including sulfate, in the model, and we find that sulfate aerosol produced by SO2 emissions from the three individual northern mid-latitude regions strongly reduces both HO2 and hydroxyl (OH) by up to 10 % year-round throughout most of the troposphere north of 30∘ N latitude. Regional SO2 emissions significantly increase nitrogen oxides (NOx) by about 5 %–8 % throughout most of the free troposphere in the Northern Hemisphere by increasing the NOx lifetime as the heterogeneous sink of HO2 on sulfate aerosol declines. Despite the NOx increases, tropospheric ozone decreases at northern mid-latitudes by 1 %–4 % zonally averaged and by up to 5 ppbv in summertime surface air over China, where the decreases in HO2 and OH suppress O3 production. Since 2015 anthropogenic SO2 emissions in China exceed those in the US or Europe, the oxidative response is greatest for the China perturbation simulation. Chemical effects of aerosols on oxidation (reactive uptake) dominate over radiative effects (photolysis rates), the latter of which are only statistically significant locally for the large perturbation over China. We find that the SO2 emissions decrease in China, which has yet to be fully realized, will have the largest impact on oxidants and related species in the Northern Hemisphere free troposphere compared to future decreases in Europe or the US. Our results bolster previous calls for a multipollutant strategy for air pollution mitigation to avoid the unintended consequence of aerosol removal leading to surface ozone increases that offset or mask surface ozone gains achieved by regulation of other pollutants, especially in countries where current usage of high-sulfur emitting fuels may be phased out in the future.

anthropogenic sulfur dioxide emissions↗