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Global tropospheric ozone investigations

Ozone (O3) is one of the most important trace gases in the troposphere, and it is responsible for influencing many critical chemical and radiative processes. Ozone contributes to the formation of the hydroxyl radical (OH), which is central to most chemical reactions in the lower atmosphere, and it absorbs UV, visible, and infrared radiation which affects the energy budget and atmospheric temperatures. In addition, O3 can be used as a tracer of atmospheric pollution and stratosphere troposphere exchange. At elevated concentrations, O3 can also produce detrimental biological and human health effects. The US National Research Council (NRC) Board on Sustainable Development reviewed the US Global Change Research Program (USGCRP) [NRC, 1995], and it identified tropospheric chemistry as one of the high priority areas for the USGCRP in the next decade. The NRC identified the following specific challenges in tropospheric chemistry. Although we understand the reason for the high levels of 03 over several regions of the world, we need to better establish the distribution of O3 in the troposphere in order to document and understand the changes in the abundance of global tropospheric O3. This information is needed to quantify the contribution of O3 to the Earth' s radiative balance and to understand potential impacts on the health of the biosphere. Having recognized the importance of particles in the chemistry of the stratosphere, we must determine how aerosols and clouds affect the chemical processes in the troposphere. This understanding is essential to predict the chemical composition of the atmosphere and to assess the resulting forcing effects in the climate system. We must determine if the self-cleansing chemistry of the atmosphere is changing as a result of human activities. This information is required to predict the rate at which pollutants are removed from the atmosphere. Over nearly two decades, airborne Differential Absorption Lidar (DIAL) systems have been used in over fifteen major field experiments conducted all over the world to address important atmospheric processes affecting the amount and distribution of 03 and aerosols across the troposphere. This paper discusses some of these wide-ranging field experiments and their results and presents a direction for future global studies of O3 and aerosols from space.

Browell, Edward V.↗

Submillimeter and millimeter observations of solar system objects

Microwave spectroscopy of solar system objects was supported. It necessarily involves millimeter and submillimeter wavelengths where rotational transitions reside. The existing national facilities are at OVRO, the 12-meter at Kitt Peak, UC array at Hat Creek, the Caltech CSO on Mauna Kea, and the 14-meter at the Univ. of Massachusetts, near Amherst. The group used all of these instruments in the last year except the Univ. of Massachusetts 14-meter. This wavelength range (0.3 to 3 mm) is about to enjoy an explosion of interest as submillimeter receivers become better and easier to use. This region of the spectrum is rich in transitions of molecules that exist in the planetary atmospheres which can be studied for temperature-pressure profiles, wind tracers, and atmospheric chemistry. The list of solar system objects that have been recently addressed with these techniques include: (1) Venus: CO studies of T-P profiles, winds, and photochemistry; SO2 detections; Continuum mapping remains to be done at 1 mm; (2) Earth H2O, CO, NO, NO2, O(18)O, etc. as a test bed for other atmospheres; (3) Mars: H2O, CO, O(18)O studies of T-P profiles, winds (fall of 1990), and photochemistry; (4) Saturn: Same as Jupiter plus submillimeter and millimeter mapping of the ring system; (5) Uranus and Neptune: Continuum thermal mapping; and (6) Titan: CO, HCN, and HC3NT-P information and photochemistry. Recent results are given.

Muhleman, Duane O.↗

Development and Validation of Water Vapor Tracers as Diagnostics for the Atmospheric Hydrologic Cycle

Understanding of the local and remote sources of water vapor can be a valuable diagnostic in understanding the regional atmospheric hydrologic cycle. In the present study, we have implemented passive tracers as prognostic variables to follow water vapor evaporated in predetermined regions until the water tracer precipitates. The formulation of the sources and sinks of tracer water is generally proportional to the prognostic water vapor variable. Because all water has been accounted for in tracers, the water vapor variable provides the validation of the tracer water and the formulation of the sources and sinks. The tracers have been implemented in a GEOS General Circulation Model (GCM) simulation consisting of several summer periods to determine the source regions of precipitation for the United States and India. The recycling of water and interannual variability of the sources of water will be examined. Potential uses in GCM sensitivity studies, predictability studies and data assimilation will be discussed.

Bosilovich, Michael G.↗

Microwave Investigation of the Mars Atmosphere and Surface

The Microwave Investigation of the Mars Atmosphere and Surface Experiment (MIMAS) is designed to address two major scientific goals: 1) To understand the three dimensional general circulation of the Martian atmosphere, and 2) To understand the hydrologic cycle of water on Mars, including the time-variable sources, sinks, and atmospheric transport of water vapor. The proposed instrument is a submillimeter wave, heterodyne receiver, with both continuum and very high spectral resolution capability. A small reflector antenna will be used to feed the receiver. Instrument heritage comes from the MIRO receiver, currently under design for the ESA Rosetta Mission, and from SWAS, a NASA astrophysics mission. The instrument will be able to measure atmospheric spectral lines from both water and carbon monoxide and use these lines as tracers of atmospheric winds. Measurement objectives of MIMAS are to measure surface temperature, atmospheric temperature from the surface up to an altitude of 60 km or more, the distribution of CO and H2O in the atmosphere, and certain wind fields (zonal and meridional). The global distribution of CO, as well as temperature distributions, will be used as input data for GCMs (general circulation models). Water vapor profiles will be used to understand the sources and sinks of water on Mars and to understand how it is transported globally by the general circulation. Zonal and meridional wind fields will provide further tests of the GCMs. An important aspect of this experiment is that the temperature and humidity measurements are insensitive to dust and ice condensates thereby making the measurement capability independent of the presence of dust clouds and ice particles. Temperature measurements derived from the data can be used in conjunction with infrared measurements to determine dust profiles.

Gulkis, S.↗

FNAS/LDEF Radiation Data Analysis

The radioactive isotope Be-7 was discovered on the forward-facing side of the LDEF satellite in amounts far exceeding that expected from direct cosmic ray activation of the spacecraft material. This prompted an examination of the production of cosmogenic isotopes in the atmosphere and of the processes by which they may be transported to orbital altitudes and absorbed by a spacecraft. Be-7 is only one of several atmospheric cosmogenic isotopes which might be detectable at orbital altitudes and which might prove to be as useful as tracers of atmospheric circulation processes in the mesosphere and thermosphere, as they have been in the lower layers of the atmosphere.

Gregory, John↗

Simulations of 7 Be and 10 Be with the GEOS-Chem global model v14.0.2 using state-of-the-art production rates

The cosmogenic radionuclides 7 Be and 10 Be are useful aerosol tracers for atmospheric transport studies. Combining 7 Be and 10 Be measurements with an atmospheric transport model can not only improve our understanding of the radionuclide transport and deposition processes but also provide an evaluation of the transport process in the model. To simulate these aerosol tracers, it is critical to evaluate the influence of radionuclides production uncertainties on simulations. Here we use the GEOS-Chem chemical transport model driven by the MERRA-2 reanalysis to simulate 7 Be and 10 Be with different production scenarios: the default production rate in GEOS-Chem based on an empirical approach (Lal and Peters, 1967; denoted as LP67), and two production rates from the CRAC:Be (Cosmic Ray Atmospheric Cascade: Beryllium; Poluianov et al., 2016) model considering only geomagnetic cut-off rigidities for a geocentric axial dipole (denoted as P16) or realistic spatial geomagnetic cut-off rigidity variations due to non-dipole moments of the geomagnetic field (denoted as P16spa). The model results are comprehensively evaluated with a large number of measurements including surface air concentrations and deposition fluxes. The model with the P16spa production can reproduce the absolute values and temporal variability of 7 Be and 10 Be surface concentrations and deposition fluxes on annual and sub-annual scales, as well as the vertical profiles of air concentrations. Simulations with the LP67 production tend to overestimate the absolute values of 7 Be and 10 Be concentrations. The P16 simulations suggest less than 10% differences compared to P16spa but tend to produce a significant positive bias (>20%) in the 7 Be deposition fluxes over East Asia. We find that the deposition fluxes are more sensitive to the production in the troposphere and downward transport from the stratosphere. Independent of the production models, surface air concentrations and deposition fluxes from all simulations show similar seasonal variations, suggesting a dominant meteorological influence. The model can also simulate reasonably the stratosphere-troposphere exchange process of 7 Be and 10 Be by producing stratospheric contribution and 10 Be/ 7 Be ratio values that agree with measurements. Finally, we illustrate the importance of including the time-varying solar modulation in the production calculation, which can significantly improve the agreement between model results and measurements, especially at mid- and high- latitudes. Reduced uncertainties in the production rates, as demonstrated in this study, improve the utility of 7 Be and 10 Be as aerosol tracers for evaluating and testing transport and scavenging processes in global models.

Minjie Zheng↗

Evolution of the martian atmosphere

Carbon dioxide, nitrogen, and the nonradiogenic and radiogenic noble gases are tracked from primordial inventories to their present states in a revised model of atmospheric evolution on Mars. Elemental and isotopic abundances evolve by hydrodynamic escape, impact erosion, outgassing, sputtering, photochemical escape of nitrogen, and carbonate formation and recycling. Atmospheric history is divided into early and late evolutionary periods, the first characterized by high CO2 pressures and a possible greenhouse and the second by a low pressure cap-regolith buffered system initiated by polar CO2 condensation approximately 3.7 Gyr ago. During early evolution the Xe isotopes are fractionated to their present composition by hydraulic escape, and CO2 pressure and isotopic history are dictated by the interplay of losses to erosion, sputtering, and carbonate precipitation, additions by outgassing and carbonate recycling, and perhaps also by feedback stabilization under greenhouse conditions. Atmospheric collapse near 3.7 Gyr leads to abrupt increases in the mixing ratios of preexisting Ar, Ne, and N2 at the exobase and their rapid removal by sputtering. Current abundances and isotopic compositions of these light species are therefore entirely determined by the action of sputtering and photochemical escape on gases supplied by outgassing during the late evolutionary epoch. The present atmospheric Kr inventory also derives almost completely from solar-like Kr degassed during this period. Consequently, among current observables, only the Xe isotopes and delta(C-13) survive as isotopic tracers of atmospheric history prior to its transition to low pressure.

Pepin, Robert O.↗

Theoretical and lidar studies of the density response of the mesospheric sodium layer to gravity wave perturbations

The density response of atmospheric layers to gravity waves is developed in two forms, an exact solution and a perturbation series solution. The degree of nonlinearity in the layer density response is described by the series solution whereas the exact solution gives insight into the nature of the responses. Density perturbation in an atmospheric layer are shown to be substantially greater than the atmospheric density perturbation associated with the propagation of a gravity wave. Because of the density gradients present in atmospheric layers, interesting effects were observed such as a phase reversal in the linear layer response which occurs near the layer peak. Once the layer response is understood, the sodium layer can be used as a tracer of atmospheric wave motions. A two dimensional digital signal processing technique was developed. Both spatial and temporal filtering are utilized to enhance the resolution by decreasing shot noise by more han 10 dB. Many of the features associated with a layer density response to gravity waves were observed in high resolution density profiles of the mesospheric sodium layer. These include nonlinearities as well as the phase reversal in the linear layer response.

Shelton, J. D.↗

Thermodynamics of selected trace elements in the Jovian atmosphere

The thermochemistry of several hundred compounds of twelve selected trace elements (Ge, Se, Ga, As, Te, Pb, Sn, Cd, Sb, Tl, In, and Bi) has been investigated for solar composition material along a Jupiter adiabat. The results indicate that AsF3, InBr, TlI, and SbS, in addition to CO, PH3, GeH4, AsH3, H2Se, HCl, HF, and H3BO3 proposed by Barshay and Lewis (1978), may be potential chemical tracers of atmospheric dynamics. The reported observation of GeH4 is interpreted on the basis of new calculations as implying rapid vertical transport from levels where the temperature is greater than or equal to 800 K. Upper limits are also set on the abundances of many gaseous compounds of the elements investigated.

Fegley, B., Jr.↗

Jupiter's atmospheric composition from the Cassini thermal infrared spectroscopy experiment

The Composite Infrared Spectrometer observed Jupiter in the thermal infrared during the swing-by of the Cassini spacecraft. Results include the detection of two new stratospheric species, the methyl radical and diacetylene, gaseous species present in the north and south auroral infrared hot spots; determination of the variations with latitude of acetylene and ethane, the latter a tracer of atmospheric motion; observations of unexpected spatial distributions of carbon dioxide and hydrogen cyanide, both considered to be products of comet Shoemaker-Levy 9 impacts; characterization of the morphology of the auroral infrared hot spot acetylene emission; and a new evaluation of the energetics of the northern auroral infrared hot spot.

Hydrocarbons↗

Tropospheric- Stratospheric Measurement Studies Summary

The two high altitude aircraft, ER-2 NASA #706 and 709 and the DC-8 NASA #717 are in active use in several programs of upper atmospheric research to study polar ozone changes, stratospheric-tropospheric exchange processes and atmospheric effects of aviation aircraft. The ER-2 has participated in seven major missions which mainly concentrated on vortex dynamics and the large losses of Ozone in the Polar regions (Ozone hole) observed in the spring. One mission verified the complex dynamical chemical and physical processes that occur during sunrise and sunset. Stratospheric Tracers of Atmospheric Transport (STRAT) obtained background measurements using the full ER-2 suite of instruments. Photochemistry of Ozone Loss in the Arctic Region in Summer (POLARIS) in 1997 assisted in understanding the mid-latitude and Arctic Ozone losses during the Northern Summer. The DC-8 with the Meteorological Measurement System (MMS) has participated in the Subsonic Aircraft: Cloud and Contrail Effects Special Study (SUCCESS), in 1996 and the Subsonic assessment Ozone and Nitrogen oxide experiment (SONEX) in 1997 missions. The MMS with its sophisticated software accurately measures ground speed and attitude, in-situ static and dynamic pressure total temperature, which are used to calculate the three dimensional wind fields, static pressure, temperature and turbulence values to meteorological accuracy. The meteorological data is not only of interest for its own sake in atmospheric dynamical processes such as mountain waves and flux measurements; but is also required by other ER-2 experiments that simultaneously measure water vapor, O3, aerosols, NO, HCl, CH4, N2O, ClO, BrO, CO2, NOy, HOx and temperature gradients. MMS products are extensively used to assist in the interpretation of their results in understanding the importance of convective effects relative to in-situ chemical changes, as may be noted by examining the list of references attached. The MMS consists of three subsystems: (a) aircraft instrumentation, inertial navigation system (INS), static and dynamic pressure taps, (b) additional dedicated instrumentation measuring angle of attack, yaw, total temperature, and a GPS which on the DC-8 measures position, velocity and attitude (c) an on board data, storage and computing acquisition system. This instrumentation and the associated software requires both an on-going laboratory ground calibration procedure for the total air temperature, static and total pressure inputs, verification of the INS dynamic response and also extensive air measurements and intercomparisons which ultimately verify and calibrate the complete system and its software. More than the usual accuracy is required because of the near cancellation occurring in the difference between the ground speed and true airspeed vectors used to give the wind vector. In the past year we have redesigned, recalibrated and used the MMS system on the NASA DC-8 that was previously used in the SUCCESS mission for the SONEX mission. Two papers were co-authored based on SUCCESS flights. Several reports and handouts were written for SONEX. Calibrations of the DC-8 pressure transducer temperature measuring thermistors was completed and an extensive analysis spanning several years of data files of the DC-8 Rosemount pressure transducer calibrations was done.

Browen, Stuart W.↗

VALENTInE: A Concept for a New Frontiers Class Long Duration In-Situ Balloon Mission to Venus

Venus and Earth are similar in bulk composition, size, density, and approximate distance from the Sun, yet Venus’s modern-day climate and surface geology is distinctly different [1]. Previous missions to Venus revealed unusual volcanic features, possible continental crust, widespread volcanic plains, a weak magnetic field [2], and insights into the Venusian atmosphere [3,4]. Unfortunately, data from these missions were limited in spatial and temporal resolution and global extent. A future mission to Venus is critical to address fundamental questions surrounding the chemical composition and dynamics of the Venusian atmosphere [5], its geologic history [6,7], its internal structure [8,9], and its habitability throughout time [10,11]. We present the Venus Air and Land Expedition: a Novel Trailblazer for In situ Exploration (VALENTInE) mission to meet this need. VALENTInE is a variable altitude balloon that will passively float in Venus’s atmosphere between 45 and 55 km altitude. VALENTInE will acquire atmospheric data at varying latitudes and longitudes in addition to mapping the surface geomorphology and mineralogy across multiple terrains. Mission Objectives: The VALENTInE mission concept is driven by four main science objectives: 1. Determine whether the driving force of the superrotation of Venus’s atmosphere is caused by horizontal or vertical momentum transport. 2. Determine whether the atmospheric composition and noble gas inventory of the Venusian atmosphere is a product of outgassing from the initial protoplanetary source or if there are significant contributions from exogenic sources. 3. Determine whether the tesserae regions (particularly Aphrodite Terra) are felsic and relatively older than surrounding regions. 4. Determine if there is any evidence of a recent dynamo preserved in the rock record of Venus. Mission Overview: A balloon architecture provides a robust system that can survive long-term in the Venusian environment while taking accurate measurements of the lower cloud deck and surface. Two prior balloon missions to Venus, VEGA 1 and VEGA 2 in 1984, have demonstrated the potential for such planetary exploration; however, these missions were short-lived (46 hr), with limited range (54 km). Our spacecraft concept consists of a battery powered balloon with a gondola and flyby carrier stage (Fig. 1). Our novel design allows for at least 15 days of atmospheric exploration, including multiple ascents and descents in the Venus atmosphere. VALENTInE is baselined to launch in 2032, cruise on solar power for 128 days, enter, descend, and inflate (EDI) into Venus’s atmosphere above Aphrodite Terra, and float in Venus’s atmosphere for a total nominal mission duration of 15 days. The balloon, able to control its altitude by changing its buoyancy, will make one full circumnavigation every 4–8 days and move poleward ~1 o latitude per day; it will be passively directed by the horizontal air currents on Venus. The balloon can only be controlled in the z direction, and the expected latitude range is ±10° from EDI. The balloon itself will be a tracer for atmospheric structures such as zonal winds [5, 12]. During the 15-day operational period, there will be five dips to 45 km for a compositional study of the lower atmosphere and geological and magnetic mapping of the surface. Dips are used to take images and measurements closer to the surface and to obtain in situ vertical atmospheric profiles between 45 and 55 km. Instruments: The VALENTInE instrument payload will allow for extensive study of the geology, atmosphere, and interior of Venus. The instrument suite consists of six instruments. The mission profile for each instrument is shown in Fig. 2. Lower Atmosphere Meteorology Analyzer (LAMA) is an atmospheric structure instrument consisting of a thermometer, barometer, and accelerometer to continuously measure temperature and pressure as a function of altitude, longitude, and latitude. TracE and Noble Gas Investigator (TENGI) is aneutral mass spectrometer used to sample the dense atmosphere. TENGI will operate continuously at 45 km and 55 km and will measure D/H ratios, as well as Ne, Ar, and O isotopic ratios. Kilometer Scale Spectral Imager (KSSI) is amultispectral imager (850-1150 nm) used to resolve surface features on the order of km. Near InfraRed Multispectral Photometer (NIRMP) is an Infrared (IR) photometer used to image the surface through the clouds to characterize mineral assemblages at five different areas of the surface. NIRMP will be operated during dwell. ELevation REConnaissance (ELREC) is a light detection and ranging (LIDAR) instrument used for measuring topography at five different areas of the surface. The ELREC data will be combined with those of NIRMP to determine mineral assemblages and how they correlate to topography. Magnetic Exploration and Interior Detective (MEID) is a magnetometer used to detect any near-surface magnetic anomalies. The magnetometer will continuously operate at all altitudes. Mission Design: The spacecraft’s propulsion system will have a wet mass of 930 kg and will be launched on an Atlas V rocket. The spacecraft will jettison the payload upon arrival in Venus’s atmosphere before decelerating to orbital velocity. Figure 2. Notional power-dip profile while the balloon is on the dayside. Risks and Challenges: Raising and lowering the spacecraft to dip beneath the haze layer require a large amount of energy. This issue was partly compensated by limiting the number of dips over the 15 day prime mission. Power needs for pumping helium are reduced by slowing the descent speed, which consequently increases spatial resolution of in situ measurements between 45 and 55 km. The main limitation for the duration of the mission is the need to carry 15 days’ worth of batteries. The bus experiences external Venusian temperatures ranging from ~27°C at 55 km altitude to ~110°C at 45 km altitude. These high atmospheric temperatures require thermal protection for the bus (instruments, electronics, and flight systems) during its descent, dwell at 45 km, and ascent. The bus is maintained at a mechanically safe temperature range of -10°C to 50°C using white external paint, multi-layer insulation (MLI), mechanical/thermal isolation (e.g. Ti, composites), and ~57 kg of Phase Change Materials (PCM). Images and spectra taken below the haze dominate the available data transmission regardless of the time spent at 45 km. Therefore, less time at the lower altitude mainly reduces the coverage of in situ measurements there. Further, we assumed an unrealistically low-density material for the helium storage tanks on the gondola. However, this issue is partially resolved if we were to jettison 75% of the spent helium storage tanks. After the entry process, the balloon volume remains mostly inflated and storage tanks are required only for reducing balloon volume in dipping to 45 km. This mission was planned against an expected New Frontiers 5 (NF5) cost cap of $1B, as the NF5 call had not yet been released. The mission we describe fits within the predicted cost cap if the flyby carrier stage, responsible for powering the spacecraft during cruise and for relaying in situ measurements back to Earth, can be contributed by another space agency. Acknowledgments: We thank the JPL Planetary Science Summer School, especially A. Nash, J. Scully, K. Mitchell, L. Lowes, and J. Armijo, and our mentors from JPL Team X. Thank you to our review panel for their insightful review. References: [1] Kane, S. et al. (2019) JGR:Ps, 124 , 2015–2028. [2] Phillips, J. L., & Russell, C. T. (1987). JGR: Space Physics , 92 (A3), 2253-2263. [3] Nakamura, M. et al. (2018) Earth Planets Space, 70 (1), 144. [4] Svedhem, H. et al. (2009) JGR:P 114 (E5). [5] Limaye et al. (2009) Decadal Survey White Paper . [6] Ivanov, M. and Head, J. (2011) PSS, 59 (13) , 1559-1600. [7] Smrekar, S. et al. (2018) Space Sci Rev, 214 (5), 88. [8] O’Rourke, J. et al. (2018) EPSL, 502 , 46-56. [9] O’Rourke J. et al. (2019) GRL , (46), 5768–5777 [10] Way, M. et al. (2016) GRL, 43 (16), 8376-8383. [11] Way, M. et al. (2020) JGR:P, 125 (5), e2019JE006276. [12] Preston, R. A. et al. (1986) Science, 231 (4744), 1414-1416.

Mission Concept↗

Transport characteristics in the middle atmosphere and two-dimensional modeling

Transport mechanisms of tracers in the atmosphere are briefly discussed from a viewpoint of Lagrangian motions of air parcels. The tracers are retained by air parcels themselves. In this regard, both momentum and energy are quite different from chemical tracers. The present problem is what interpretation is best for understanding transport mechanisms of tracers. A method is reviewed and proposed, although conceptually. The numerical model used was a whole hemispheric global climate model. Annual- and zonal-mean diabatic forcing was assumed to drive the general circulation. Time integrations were carried out for about 100 days. The model quasi-equilibrium states were analyzed.

Kida, H.↗

Investigating Sources of Variability and Error in Simulations of Carbon Dioxide in an Urban Region

Greenhouse gas (GHG) emissions estimation methods that use atmospheric trace gas observations, including inverse modeling techniques, perform better when carbon dioxide (CO2) fluxes are more accurately transported and dispersed in the atmosphere by a numerical model. In urban areas, transport and dispersion is particularly difficult to simulate using current mesoscale meteorological models due, in part, to added complexity from surface heterogeneity and fine spatial/temporal scales. It is generally assumed that the errors in GHG estimation methods in urban areas are dominated by errors in transport and dispersion. Other significant errors include, but are not limited to, those from assumed emissions magnitude and spatial distribution. To assess the predictability of simulated trace gas mole fractions in urban observing systems using a numerical weather prediction model, we employ an Eulerian model that combines traditional meteorological variables with multiple passive tracers of atmospheric CO2 from anthropogenic inventories and a biospheric model. The predictability of the Eulerian model is assessed by comparing simulated atmospheric CO2 mole fractions to observations from four in situ tower sites (three urban and one rural) in the Washington DC/Baltimore, MD area for February 2016. Four different gridded fossil fuel emissions inventories along with a biospheric flux model are used to create an ensemble of simulated atmospheric CO2 observations within the model. These ensembles help to evaluate whether the modeled observations are impacted more by the underlying emissions or transport. The spread of modeled observations using the four emission fields indicates the model's ability to distinguish between the different inventories under various meteorological conditions. Overall, the Eulerian model performs well; simulated and observed average CO2 mole fractions agree within 1% when averaged at the three urban sites across the month. However, there can be differences greater than 10% at any given hour, which are attributed to complex meteorological conditions rather than differences in the inventories themselves. On average, the mean absolute error of the simulated compared to actual observations is generally twice as large as the standard deviation of the modeled mole fractions across the four emission inventories. This result supports the assumption, in urban domains, that the predicted mole fraction error relative to observations is dominated by errors in model meteorology rather than errors in the underlying fluxes in winter months. As such, minimizing errors associated with atmospheric transport and dispersion may help improve the performance of GHG estimation models more so than improving flux priors in the winter months. We also find that the errors associated with atmospheric transport in urban domains are not restricted to certain times of day. This suggests that atmospheric inversions should use CO2 observations that have been filtered using meteorological observations rather than assuming that meteorological modeling is most accurate at certain times of day (such as using only mid-afternoon observations).

CO2↗

Properties of the stratospheric aerosol layer studied with a one-dimensional computer model

Aerosol particle effects are often neglected in theoretical studies of stratospheric phenomena. In reality, the particulate matter normally found above the tropopause may influence the terrestrial radiation balance, catalyze heterogeneous chemical interactions, and serve as a tracer of atmospheric motions. The paper proposes a one-dimensional model of the stratospheric aerosol layer, and it is used to compare aerosol theory with observational data. The model considers gaseous sulfur photochemistry and the physical aerosol processes of nucleation, coagulation, sedimentation, and diffusion. Calculations of the effects on the aerosol layer of stratospheric injections of aluminum oxide particles by Space Shuttle engines and of sulfur dioxide molecules by volcanic activity are performed. The relation between measured aerosol variability and changes in stratospheric air temperatures and vertical transport rates are discussed.

Turco, R. P.↗

Daytime lidar measurements of tidal winds in the mesospheric sodium layer at Urbana, Illinois

For more than 15 years lidar systems have been used to study the chemistry and dynamics of the mesospheric sodium layer. Because the layer is an excellent tracer of atmospheric wave motions, sodium lidar has proven to be particularly useful for studying the influence of gravity waves and tides on mesospheric dynamics. These waves, which originate in the troposphere and stratosphere, propagate through the mesosphere and dissipate their energy near the mesopause making important contributions to the momentum and turbulence budget in this region of the atmosphere. Recently, the sodium lidar was modified for daytime operation so that wave phenomena and chemical effects could be monitored throughout the complete diurnal cycle. The results of continuous 24 hour lidar observations of the sodium layer structure are presented alond with measurement of the semidiurnal tidal winds.

Kwon, K. H.↗

Global average concentration and trend for hydroxyl radicals deduced from ALE/GAGE trichloroethane (methyl chloroform) data for 1978-1990

An optimal estimation inversion scheme is utilized with atmospheric data and emission estimates to determined the globally averaged CH3CCl3 tropospheric lifetime and OH concentration. The data are taken from atmospheric measurements from surface stations of 1,1,1-trichloroethane and show an annual increase of 4.4 +/- 0.2 percent. Industrial emission estimates and a small oceanic loss rate are included, and the OH concentration for the same period (1978-1990) are incorporated at 1.0 +/- 0.8 percent/yr. The positive OH trend is consistent with theories regarding OH and ozone trends with respect to land use and global warming. Attention is given to the effects of the ENSO on the CH3CCl3 data and the assumption of continuing current industrial anthropogenic emissions. A novel tropical atmospheric tracer-transport mechanism is noted with respect to the CH3CCl3 data.

Prinn, R.↗

Regarding tracer transport in Mars' winter atmosphere in the presence of nearly stationary, forced planetary waves

Large-scale transport of volatiles and condensates on Mars, as well as atmospheric dust, is ultimately driven by the planet's global-scale atmospheric circulation. This circulation arises in part from the so-called mean meridional (Hadley) circulation that is associated with rising/poleward motion in low latitudes and sinking/equatorward motion in middle and high latitudes. Intimately connected to the mean circulation is an eddy-driven component due to large-scale wave activity in the planet's atmosphere. During winter this wave activity arises both from traveling weather systems (i.e., barotropic and baroclinic disturbances) and from 'forced' disturbances (e.g., the thermal tides and surface-forced planetary waves). Possible contributions to the effective (net) transport circulation from forced planetary waves are investigated.

Hollingsworth, Jeffrey L.↗