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Intercomparison of SCIAMACHY and OMI Tropospheric NO2 Columns: Observing the Diurnal Evolution of Chemistry and Emissions from Space

Concurrent (August 2006) measurements of tropospheric NO2 columns from OMI aboard Aura (1330 local overpass time) and SCIAMACHY aboard Envisat (1000 local overpass time) offer an opportunity to examine the consistency between the two instruments under tropospheric background conditions and the effect of different observing times. For scenes with tropospheric NO 2 columns <5.0 x 10(exp 15) molecules cm 2, SCIAMACHY and OMI agree within 1.0-2.0 x 10(exp 15) molecules cm 2, consistent with the detection limits of both instruments. We find evidence for a low bias of 0.2 x 10(exp 15) molecules cm 2 in OMI observations over remote oceans. Over the fossil fuel source regions at northern midlatitudes, we find that SCIAMACHY observes up to 40% higher NO2 at 1000 local time (LT) than OMI at 1330 LT. Over biomass burning regions in the tropics, SCIAMACHY observes up to 40% lower NO 2 columns than OMI. These differences are present in the spectral fitting of the data (slant column) and are augmented in the fossil fuel regions and dampened in the tropical biomass burning regions by the expected increase in air mass factor as the mixing depth rises from 1000 to 1330 LT. Using a global 3-D chemical transport model (GEOS-Chem), we show that the 1000-1330 LT decrease in tropospheric NO2 column over fossil fuel source regions can be explained by photochemical loss, dampened by the diurnal cycle of anthropogenic emissions that has a broad daytime maximum. The observed 1000-1330 LT NO2 column increase over tropical biomass burning regions points to a sharp midday peak in emissions and is consistent with a diurnal cycle of emissions derived from geostationary satellite fire counts.

Boersma, K. Folkert↗

Evaluation of GOME Satellite Measurements of Tropospheric NO2 and HCHO using Regional Data from Aircraft Campaigns in the Southeastern United States

We compare tropospheric measurements of nitrogen dioxide (NO2) and formaldehyde (HCHO) from the Global Ozone Monitoring Experiment (GOME) satellite instrument with in situ measurements over eastern Texas and the southeast United States. On aveiage, the GOME and in situ measurements of tropospheric NO2 and HCHO columns are consistent despite pronounced sampling differences. The geometric mean in situ to GOME ratios over the campaign are 1.08 for NO2 and 0.84 for HCHO, with corresponding geometric standard deviations of 1.27 and 1.38. The correlation of the observed column spatial variability between the two NO2 measurement sets is encouraging before (r2 = 0.54, n = 18) and after (r2 = 0.67, n = 18) correcting for a sampling bias. Mean relative vertical profiles of HCHO and NO2 calculated with a global three-dimensional model (GEOS-CHEM) and used in the GOME retrieval are highly consistent with in situ measurements; differences would affect the retrieved NO2 and HCHO columns by a few percent. GOME HCHO columns over eastern Texas include contributions from anthropogenic volatile organic compound (VOC) emissions but are dominated by biogenic VOC emissions at the regional scale in August-September when HCHO columns are within 20% of those over the southeastern United States. In situ measurements show that during summer the lowest 1500 m (the lower mixed layer) contains 75% of the tropospheric NO2 column over Houston and Nashville, and 60% of the HCHO column over Houston. Future validation of space-based measurements of tropospheric NO2 and HCHO columns over polluted regions should include coincident in situ measurements that span the entire satellite footprint, especially in the heterogeneous mixed layer.

Martin, R. V.↗

A New Technique for Retrieval of Tropospheric and Stratospheric Ozone Profiles using Sky Radiance Measurements at Multiple View Angles: Application to a Brewer Spectrometer

This paper describes and applies a new technique for retrieving diurnal variability in tropospheric ozone vertical distribution using ground-based measurements of ultraviolet sky radiances. The measured radiances are obtained by a polarization-insensitive modified Brewer double spectrometer located at Goddard Space Flight Center, in Greenbelt, Maryland, USA. Results demonstrate that the Brewer angular (0-72deg viewing zenith angle) and spectral (303-320 nm) measurements of sky radiance in the solar principal plane provide sufficient information to derive tropospheric ozone diurnal variability. In addition, the Brewer measurements provide stratospheric ozone vertical distributions at least twice per day near sunrise and sunset. Frequent measurements of total column ozone amounts from direct-sun observations are used as constraints in the retrieval. The vertical ozone profile resolution is shown in terms of averaging kernels to yield at least four points in the troposphere-low stratosphere, including good information in Umkehr layer 0 (0-5 km). The focus of this paper is on the derivation of stratospheric and tropospheric ozone profiles using both simulated and measured radiances. We briefly discuss the necessary modifications of the Brewer spectrometer that were used to eliminate instrumental polarization sensitivity so that accurate sky radiances can be obtained in the presence of strong Rayleigh scattering and aerosols. The results demonstrate that including a site-specific and time-dependent aerosol correction, based on Brewer direct-sun observations of aerosol optical thickness, is critical to minimize the sky radiance residuals as a function of observing angle in the optimal estimation inversion algorithm and improve the accuracy of the retrieved ozone profile.

Tzortziou, Maria↗

Evaluation of Satellite-Based Upper Troposphere Cloud Top Height Retrievals in Multilayer Cloud Conditions During TC4

Upper troposphere cloud top heights (CTHs), restricted to cloud top pressures (CTPs) less than 500 hPa, inferred using four satellite retrieval methods applied to Twelfth Geostationary Operational Environmental Satellite (GOES-12) data are evaluated using measurements during the July August 2007 Tropical Composition, Cloud and Climate Coupling Experiment (TC4). The four methods are the single-layer CO2-absorption technique (SCO2AT), a modified CO2-absorption technique (MCO2AT) developed for improving both single-layered and multilayered cloud retrievals, a standard version of the Visible Infrared Solar-infrared Split-window Technique (old VISST), and a new version of VISST (new VISST) recently developed to improve cloud property retrievals. They are evaluated by comparing with ER-2 aircraft-based Cloud Physics Lidar (CPL) data taken during 9 days having extensive upper troposphere cirrus, anvil, and convective clouds. Compared to the 89% coverage by upper tropospheric clouds detected by the CPL, the SCO2AT, MCO2AT, old VISST, and new VISST retrieved CTPs less than 500 hPa in 76, 76, 69, and 74% of the matched pixels, respectively. Most of the differences are due to subvisible and optically thin cirrus clouds occurring near the tropopause that were detected only by the CPL. The mean upper tropospheric CTHs for the 9 days are 14.2 (+/- 2.1) km from the CPL and 10.7 (+/- 2.1), 12.1 (+/- 1.6), 9.7 (+/- 2.9), and 11.4 (+/- 2.8) km from the SCO2AT, MCO2AT, old VISST, and new VISST, respectively. Compared to the CPL, the MCO2AT CTHs had the smallest mean biases for semitransparent high clouds in both single-layered and multilayered situations whereas the new VISST CTHs had the smallest mean biases when upper clouds were opaque and optically thick. The biases for all techniques increased with increasing numbers of cloud layers. The transparency of the upper layer clouds tends to increase with the numbers of cloud layers.

Chang, Fu-Lung↗

Thermal Structure of Titan's Troposphere and Middle Atmosphere

The thermal structure of Titan's atmosphere is reviewed, with particular emphasis on recent Cassini-Huygens results. Titan's has a similar troposphere-stratosphere-mesosphere pattern like Earth, but with a much more extended atmosphere, because of the weaker gravity, and also much lower temperatures, because of its greater distance from the sun. Titan's atmosphere exhibits an unusually large range in radiative relaxation times. In the troposphere, these are long compared to seasonal time scales, but in the stratosphere they are much shorter than a season. An exception is near the winter pole, where the stratospheric relaxation times at 100-170 km become comparable to the seasonal time scale; at the warm stratopause, they are comparable to a Titan day. Hence, seasonal behavior in the troposphere should be muted, but significant in the stratosphere. This is reflected in the small meridional contrast observed in temperatures in the troposphere and the large stratospheric contrasts noted above. A surprising feature of the vertical profiles of temperature is the abrupt transition between these regimes in at high northern latitudes in winter, where the temperatures in the lower stratosphere exhibit a sudden drop with increasing altitude. This could be a radiative effect, not associated with spatial variations in gaseous opacity, but rather from an optically thick condensate at thermal-infrared wavelengths. A curious aspect of Titan's middle atmosphere is that the axis of symmetry of the temperature field is tilted by several degrees relative to the rotational axis of the moon itself. Whether this is driven by solar heating or gravitational perturbations is not known. Titan's surface exhibits weak contrasts in temperature, approximately 3 K in the winter hemisphere. At low latitudes, there is evidence of a weak nocturnal boundary layer on the morning terminator, which is not radiatively controlled, but can be explained in terms of vertical mixing with a small eddy viscosity.

Flasar, F. M.↗

A Global Climatology of Tropospheric and Stratospheric Ozone Derived from Aura OMI and MLS Measurements

A global climatology of tropospheric and stratospheric column ozone is derived by combining six years of Aura Ozone Monitoring Instrument (OMI) and Microwave Limb Sounder (MLS) ozone measurements for the period October 2004 through December 2010. The OMI/MLS tropospheric ozone climatology exhibits large temporal and spatial variability which includes ozone accumulation zones in the tropical south Atlantic year-round and in the subtropical Mediterranean! Asia region in summer months. High levels of tropospheric ozone in the northern hemisphere also persist in mid-latitudes over the eastern North American and Asian continents extending eastward over the Pacific Ocean. For stratospheric ozone climatology from MLS, largest ozone abundance lies in the northern hemisphere in the latitude range 70degN-80degN in February-April and in the southern hemisphere around 40degS-50degS during months August-October. The largest stratospheric ozone abundances in the northern hemisphere lie over North America and eastern Asia extending eastward across the Pacific Ocean and in the southern hemisphere south of Australia extending eastward across the dateline. With the advent of many newly developing 3D chemistry and transport models it is advantageous to have such a dataset for evaluating the performance of the models in relation to dynamical and photochemical processes controlling the ozone distributions in the troposphere and stratosphere.

Ziemke, J.R.↗

A Review of Low Frequency Electromagnetic Wave Phenomena Related to Tropospheric-Ionospheric Coupling Mechanisms

Investigation of coupling mechanisms between the troposphere and the ionosphere requires a multidisciplinary approach involving several branches of atmospheric sciences, from meteorology, atmospheric chemistry, and fulminology to aeronomy, plasma physics, and space weather. In this work, we review low frequency electromagnetic wave propagation in the Earth-ionosphere cavity from a troposphere-ionosphere coupling perspective. We discuss electromagnetic wave generation, propagation, and resonance phenomena, considering atmospheric, ionospheric and magnetospheric sources, from lightning and transient luminous events at low altitude to Alfven waves and particle precipitation related to solar and magnetospheric processes. We review in situ ionospheric processes as well as surface and space weather phenomena that drive troposphere-ionosphere dynamics. Effects of aerosols, water vapor distribution, thermodynamic parameters, and cloud charge separation and electrification processes on atmospheric electricity and electromagnetic waves are reviewed. We also briefly revisit ionospheric irregularities such as spread-F and explosive spread-F, sporadic-E, traveling ionospheric disturbances, Trimpi effect, and hiss and plasma turbulence. Regarding the role of the lower boundary of the cavity, we review transient surface phenomena, including seismic activity, earthquakes, volcanic processes and dust electrification. The role of surface and atmospheric gravity waves in ionospheric dynamics is also briefly addressed. We summarize analytical and numerical tools and techniques to model low frequency electromagnetic wave propagation and solving inverse problems and summarize in a final section a few challenging subjects that are important for a better understanding of tropospheric-ionospheric coupling mechanisms.

Simoes, Fernando↗

Methane from the Tropospheric Emission Spectrometer (TES)

TES V5 CH4 captures latitudinal gradients, regional variability and interannual variation in the free troposphere. V5 joint retrievals offer improved sensitivity to lower troposphere. Time series extends from 2004 to present. V5 reprocessing in progress. Upper tropospheric bias. Mitigated by N2O correction. Appears largely spatially uniform, so can be corrected. How to relate free-tropospheric values to surface emissions.

methane gas (CH4)↗

Correction Technique for Raman Water Vapor Lidar Signal-Dependent Bias and Suitability for Water Wapor Trend Monitoring in the Upper Troposphere

The MOHAVE-2009 campaign brought together diverse instrumentation for measuring atmospheric water vapor. We report on the participation of the ALVICE (Atmospheric Laboratory for Validation, Interagency Collaboration and Education) mobile laboratory in the MOHAVE-2009 campaign. In appendices we also report on the performance of the corrected Vaisala RS92 radiosonde measurements during the campaign, on a new radiosonde based calibration algorithm that reduces the influence of atmospheric variability on the derived calibration constant, and on other results of the ALVICE deployment. The MOHAVE-2009 campaign permitted the Raman lidar systems participating to discover and address measurement biases in the upper troposphere and lower stratosphere. The ALVICE lidar system was found to possess a wet bias which was attributed to fluorescence of insect material that was deposited on the telescope early in the mission. Other sources of wet biases are discussed and data from other Raman lidar systems are investigated, revealing that wet biases in upper tropospheric (UT) and lower stratospheric (LS) water vapor measurements appear to be quite common in Raman lidar systems. Lower stratospheric climatology of water vapor is investigated both as a means to check for the existence of these wet biases in Raman lidar data and as a source of correction for the bias. A correction technique is derived and applied to the ALVICE lidar water vapor profiles. Good agreement is found between corrected ALVICE lidar measurments and those of RS92, frost point hygrometer and total column water. The correction is offered as a general method to both quality control Raman water vapor lidar data and to correct those data that have signal-dependent bias. The influence of the correction is shown to be small at regions in the upper troposphere where recent work indicates detection of trends in atmospheric water vapor may be most robust. The correction shown here holds promise for permitting useful upper tropospheric water vapor profiles to be consistently measured by Raman lidar within NDACC (Network for the Detection of Atmospheric Composition Change) and elsewhere, despite the prevalence of instrumental and atmospheric effects that can contaminate the very low signal to noise measurements in the UT.

MOHAVE-2009↗

Overview of Global/Regional Models Used to Evaluate Tropospheric Ozone in North America

Ozone (O3) is an important greenhouse gas, toxic pollutant, and plays a major role in atmospheric chemistry. Tropospheric O3 which resides in the planetary boundary layer (PBL) is highly reactive and has a lifetime on the order of days, however, O3 in the free troposphere and stratosphere has a lifetime on the order of weeks or months. Modeling O3 mixing ratios at and above the surface is difficult due to the multiple formation/destruction processes and transport pathways that cause large spatio-temporal variability in O3 mixing ratios. This talk will summarize in detail the global/regional models that are commonly used to simulate/predict O3 mixing ratios in the United States. The major models which will be focused on are the: 1) Community Multi-scale Air Quality Model (CMAQ), 2) Comprehensive Air Quality Model with Extensions (CAMx), 3) Goddard Earth Observing System with Chemistry (GEOS-Chem), 4) Real Time Air Quality Modeling System (RAQMS), 5) Weather Research and Forecasting/Chemistry (WRF-Chem) model, National Center for Atmospheric Research (NCAR)'s Model for OZone And Related chemical Tracers (MOZART), and 7) Geophysical Fluid Dynamics Laboratory (GFDL) AM3 model. I will discuss the major modeling components which impact O3 mixing ratio calculations in each model and the similarities/differences between these models. This presentation is vital to the 2nd Annual Tropospheric Ozone Lidar Network (TOLNet) Conference as it will provide an overview of tools, which can be used in conjunction with TOLNet data, to evaluate the complex chemistry and transport pathways controlling tropospheric O3 mixing ratios.

Mixing Ratios↗

Tropospheric Emissions: Monitoring of Pollution Overview

TEMPO is now well into its implementation phase, having passed both its Key Decision Point C and the Critical Design Review (CDR) for the instrument. The CDR for the ground systems will occur in March 2016 and the CDR for the Mission component at a later date, after the host spacecraft has been selected. TEMPO is on schedule to measure atmospheric pollution for greater North America from space using ultraviolet and visible spectroscopy. TEMPO measures from Mexico City to the Canadian oil sands, and from the Atlantic to the Pacific, hourly and at high spatial resolution. TEMPO provides a tropospheric measurement suite that includes the key elements of tropospheric air pollution chemistry. Measurements are from geostationary (GEO) orbit, to capture the inherent high variability in the diurnal cycle of emissions and chemistry. The small product spatial footprint resolves pollution sources at sub-urban scale. Together, this temporal and spatial resolution improves emission inventories, monitors population exposure, and enables effective emission-control strategies. TEMPO takes advantage of a GEO host spacecraft to provide a modest cost mission that measures the spectra required to retrieve O3, NO2, SO2, H2CO, C2H2O2, H2O, aerosols, cloud parameters, and UVB radiation. TEMPO thus measures the major elements, directly or by proxy, in the tropospheric O3 chemistry cycle. Multi-spectral observations provide sensitivity to O3 in the lowermost troposphere, substantially reducing uncertainty in air quality predictions by 50 percent. TEMPO quantifies and tracks the evolution of aerosol loading. It provides near-real-time air quality products that will be made widely, publicly available. TEMPO provides much of the atmospheric measurement capability recommended for GEO-CAPE in the 2007 National Research Council Decadal Survey, Earth Science and Applications from Space: National Imperatives for the Next Decade and Beyond. Instruments from Europe (Sentinel 4) and Asia (GEMS) will form parts of a global GEO constellation for pollution monitoring later this decade, with a major focus on intercontinental pollution transport. TEMPO will launch at a prime time to be a component of this constellation.

Chance, Kelly↗

Tropospheric Ozone Change from 1980 to 2010 Dominated by Equatorward Redistribution of Emissions

Ozone is an important air pollutant at the surface, and the third most important anthropogenic greenhouse gas in the troposphere. Since 1980, anthropogenic emissions of ozone precursors methane, non-methane volatile organic compounds, carbon monoxide and nitrogen oxides (NOx) have shifted from developed to developing regions. Emissions have thereby been redistributed equatorwards, where they are expected to have a stronger effect on the tropospheric ozone burden due to greater convection, reaction rates and NOx sensitivity. Here we use a global chemical transport model to simulate changes in tropospheric ozone concentrations from 1980 to 2010, and to separate the influences of changes in the spatial distribution of global anthropogenic emissions of short-lived pollutants, the magnitude of these emissions, and the global atmospheric methane concentration. We estimate that the increase in ozone burden due to the spatial distribution change slightly exceeds the combined influences of the increased emission magnitude and global methane. Emission increases in Southeast, East and South Asia may be most important for the ozone change, supported by an analysis of statistically significant increases in observed ozone above these regions. The spatial distribution of emissions dominates global tropospheric ozone, suggesting that the future ozone burden will be determined mainly by emissions from low latitudes.

Zhang, Yuqiang↗

Causes of Interannual Variability over the Southern Hemispheric Tropospheric Ozone Maximum

We examine the relative contribution of processes controlling the interannual variability (IAV) of tropospheric ozone over four sub-regions of the southern hemispheric tropospheric ozone maximum (SHTOM) over a 20-year period. Our study is based on hindcast simulations from the National Aeronautics and Space Administration Global Modeling Initiative chemistry transport model (NASA GMI-CTM) of tropospheric and stratospheric chemistry, driven by assimilated Modern Era Retrospective Analysis for Research and Applications (MERRA) meteorological fields. Our analysis shows that over SHTOM region, the IAV of the stratospheric contribution is the most important factor driving the IAV of upper tropospheric ozone (270 hectopascals), where ozone has a strong radiative effect. Over the South Atlantic region, the contribution from surface emissions to the IAV of ozone exceeds that from stratospheric input at and below 430 hectopascals. Over the South Indian Ocean, the IAV of stratospheric ozone makes the largest contribution to the IAV of ozone with little or no influence from surface emissions at 270 and 430 hectopascals in austral winter. Over the tropical South Atlantic region, the contribution from IAV of stratospheric input dominates in austral winter at 270 hectopascals and drops to less than half but is still significant at 430 hectopascals. Emission contributions are not significant at these two levels. The IAV of lightning over this region also contributes to the IAV of ozone in September and December. Over the tropical southeastern Pacific, the contribution of the IAV of stratospheric input is significant at 270 and 430 hectopascals in austral winter, and emissions have little influence.

Global Modeling Initiative chemistry transport mod↗

Impacts of aerosol size-dependent below-cloud scavenging on tropospheric aerosol in the NASA GEOS model

Wet deposition is the major sink for a suite of tropospheric aerosols, and thus largely affects the global distribution and lifetime of aerosols as well as the formation of clouds in the atmosphere. In this study, we implement the aerosol size-dependent below-cloud scavenging (BCS; washout) parameterization of Croft et al. (Atmos. Chem. Phys., 2009; hereafter referred to as C09) in the GOCART bulk aerosol scheme coupled with the NASA Goddard Earth Observing System (GEOS) model, and evaluate the simulated tropospheric aerosols against surface, airborne, and satellite observations. The current below-cloud scavenging in GOCART employs a first-order removal function with a constant scavenging coefficient that is independent of aerosol sizes and precipitation fluxes. The C09 BCS parameterization instead calculates aerosol below-cloud scavenging coefficients based on a size-dependent collision efficiency between aerosol particles and raindrops (or snow crystals). A look-up table of compiled collision efficiencies provides scavenging coefficients for sixty aerosol sizes and nine rain flux rates. We determine instantaneous coefficients according to the C09 BCS look-up table, precipitation fluxes, and a log-normal size distribution of aerosols. The implemented BCS parameterization tends to result in a large diversity of scavenging coefficient values with higher magnitudes, leading to more efficient scavenging. The model-simulated global mean tropospheric Pb-210 aerosol lifetime decreases from 7.4 days to 5.8 days. The separate consideration of rain and snow conditions in the scavenging coefficient lookup table leads to a bi-mode distribution of scavenging coefficients. These changes also cause increased mass fractions of smaller aerosols compared to the current simulation. We examine the impacts of the C09 BCS parameterization on the simulated aerosol vertical profiles, tropospheric lifetimes, and deposition fluxes through comparisons with NASA aircraft measurements (ATom), surface observations of aerosol concentrations (IMPROVE) and wet deposition fluxes (NADP and APQMP), and MODIS aerosol optical depth (AOD) retrievals.

Aerosols↗

Strong Sensitivity of the Isotopic Composition of Methane to the Plausible Range of Tropospheric Chlorine

The C-13 isotopic ratio of methane, δC-13 of CH4, provides additional constraints on the CH4 budget to complement the constraints from CH4 observations. The interpretation of δC-13 observations is complicated, however, by uncertainties in the methane sink. The reaction of CH4 with Cl is highly fractionating, increasing the relative abundance of 13CH4, but there is currently no consensus on the strength of the tropospheric Cl sink. Global model simulations of halogen chemistry differ strongly from one another in terms of both the magnitude of tropospheric Cl and its geographic distribution. This study explores the impact of the inter-model diversity in Cl fields on the simulated δC-13 of CH4. We use a set of GEOS global model simulations with different predicted Cl fields to test the sensitivity of the δC-13 of CH4 to the diversity of Cl output from chemical transport models. We find that δC-13 is highly sensitive to both the amount and geographic distribution of Cl. Simulations with Cl providing 0.28% or 0.66% of the total CH4 loss bracket the δC-13 observations for a fixed set of emissions. Thus, even when Cl provides only a small fraction of the total CH4 loss and has a small impact on total CH4, it provides a strong lever on δC-13. Consequently, it is possible to achieve a good representation of total CH4 using widely different Cl concentrations, but the partitioning of CH4 loss between the OH and Cl reactions leads to strong differences in isotopic composition depending on which model’s Cl field is used. Comparing multiple simulations, we find that altering the tropospheric Cl field leads to approximately a 0.5‰ increase in δ(13)CH4for each percent increase in how much CH4 is oxidized by Cl. The geographic distribution and seasonal cycle of Cl also impacts the hemispheric gradient and seasonal cycle of δC-13. The large effect of Cl on δC-13 compared to total CH4 broadens the range of CH4 source mixtures that can be reconciled with δC-13 observations. Stronger constraints on tropospheric Cl are necessary to improve estimates of CH4 sources from δC-13 observations.

Global model simulations of halogen chemistry↗

Connections Between Upper Tropospheric and Lower Stratospheric Circulation Responses to Increased Co 2

There are a myriad of ways atmospheric circulation responds to increased CO 2 . In the troposphere, the region of the tropical upwelling narrows, the Hadley Cells expand, and the upper level subtropical zonal winds that comprise the subtropical jet strengthen. In the stratosphere, the tropical upwelling narrows and strengthens, enhancing the Brewer-Dobson Circulation. Despite the robustness of these projections, dynamical coupling between the features remains unclear. In this study, we analyze output from the NASA Goddard Institute for Space Studies (GISS) ModelE coupled climate model to examine any connection between the upper tropospheric and lower stratospheric circulation by considering the features’ seasonality, hemispheric asymmetry, scaling, and transient response to a broad range of CO 2 forcings. We find that a narrowing and strengthening of upper tropospheric upwelling occurs with a strengthening of the subtropical jet. There is also a narrowing and strengthening of lower stratospheric upwelling that is related to an equatorward shift in critical latitude for wave breaking and the associated strengthening of the subtropical lower stratosphere’s zonal winds. However, the stratospheric responses display different seasonal, hemispheric, and transient patterns than those in the troposphere, indicating independent circulation changes between the two domains.

Molly E. Menzel↗

An Observation-Based, Reduced-Form Model for Oxidation in the Remote Marine Troposphere

The hydroxyl radical (OH) fuels atmospheric chemical cycling as the main sink for methane and a driver of the formation and loss of many air pollutants, but direct OH observations are sparse. We develop and evaluate an observation-based proxy for short term, spatial variations in OH (Proxy OH ) in the remote marine troposphere using unprecedented and comprehensive measurements from the NASA Atmospheric Tomography (ATom) airborne campaign. Proxy OH is a reduced form of the OH steady-state equation representing the dominant OH production and loss pathways in the remote marine troposphere, according to box model simulations of OH constrained with ATom observations. Proxy OH comprises only eight variables that are generally observed by routine ground- or satellite-based instruments. ProxyOH scales linearly with in situ [OH] spatial variations along the ATom flight tracks (median r 2 = 0.90, interquartile range = 0.80 – 0.94 across 2 km altitude by 20° latitudinal regions). We deconstruct spatial variations in Proxy OH as a first-order approximation of the sensitivity of OH variations to individual terms. Two terms modulate within-region Proxy OH variations—water vapor (H 2 O) and, to a lesser extent, nitric oxide (NO). This implies that a limited set of observations could offer a novel avenue for observation-based mapping of OH spatial variations over much of the remote marine troposphere. Both H 2 O and NO are expected to change with climate, while NO also varies strongly with human activities. We also illustrate the utility of Proxy OH as a process-based approach for evaluating inter-model differences in remote marine tropospheric OH.

Colleen B. Baublitz↗

Evidence of Seasonally Dependent Stratosphere-Troposphere Exchange and Purging of Lower Stratospheric Aeroso from a Multi-Year Lidar Dataset

Tropospheric and lower stratospheric aerosol backscatter data obtained from a calibrated backscatter lidar at Pasadena, California (34 deg N latitude)over the 1984-1993 period clearly indicate tightly coupled aerosol optical properties in the upper troposphere and lower stratosphere in the winter and early spring, due to the active mid-latitude stratospheric-tropospheric (ST) exchange processes occurring at this time of year.

upper tropospheric aerosols↗