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NASA NTRS2001

Photolysis Rate Coefficient Calculations in Support of SOLVE Campaign

The objectives for this SOLVE project were 3-fold. First, we sought to calculate a complete set of photolysis rate coefficients (j-values) for the campaign along the ER-2 and DC-8 flight tracks. En route to this goal, it would be necessary to develop a comprehensive set of input geophysical conditions (e.g., ozone profiles), derived from various climatological, aircraft, and remotely sensed datasets, in order to model the radiative transfer of the atmosphere accurately. These j-values would then need validation by comparison with flux-derived j-value measurements. The second objective was to analyze chemistry along back trajectories using the NASA/Goddard chemistry trajectory model initialized with measurements of trace atmospheric constituents. This modeling effort would provide insight into the completeness of current measurements and the chemistry of Arctic wintertime ozone loss. Finally, we sought to coordinate stellar occultation measurements of ozone (and thus ozone loss) during SOLVE using the MSX/UVISI satellite instrument. Such measurements would determine ozone loss during the Arctic polar night and represent the first significant science application of space-based stellar occultation in the Earth's atmosphere.

Lloyd, Steven A.↗
NASA NTRS2001

Evidence of Stratosphere-to-Troposphere Transport Within a Mesoscale Model and Total Ozone Mapping Spectrometer Total Ozone

We evaluate evidence for stratospheric mass transport into, and mass remaining in, the troposphere during an intense midlatitude cyclone. Mesoscale forecast model analysis fields from the Mesoscale Analysis and Prediction System were matched with total ozone observations from the Total Ozone Measurement Spectrometer. Combined with parcel back trajectory calculations, the analyses imply that two mechanisms contributed to the mass exchange: (1) An area of dynamically induced exchange was observed on the cyclone's southern edge. Parcels originally in the stratosphere crossed the jet core and were diluted through turbulent mixing with tropospheric air; (2) Diabetic effects reduced parcel potential vorticity (PC) for trajectories traversing precipitation regions, creating a 'PV hole' signature in the center of the cyclone. Air with characteristics of ozone and water vapor found in the lower stratosphere remained in the troposphere. The strength of the latter process may be unusual. Combined with other research, these results suggest that precipitation-induced diabetic effects can significantly modify (either decreasing or increasing) parcel potential vorticity, depending on parcel trajectory configuration with respect to maximum heating regions and jet core. The diabetic heating effect on stratosphere-troposphere exchange (STE) is more important to tropopause erosion than to altering parcel trajectories. In addition, these results underline the importance of using not only PC but also chemical constituents for diagnoses of STE.

Olsen, Mark A.↗
NASA NTRS1999

Effects of Aircraft On Aerosol Abundance in the Upper Troposphere

A significant increase in sulfuric acid aerosol concentration was detected above 10 km pressure altitude during a cross-corridor flight out of Shannon on October 23, 1997. The source of this aerosol is ascribed to commercial aircraft operations in flight corridors above 10 km, because (1) a stable atmosphere prevented vertical air mass exchanges and thus eliminated surface sources, (2) air mass back trajectories documented the absence of remote continental sources, and (3) temperature profiler data showed the tropopause at least one kilometers above flight altitude throughout the flight. Particle volatility identified 70% H2SO4, 20% (NH4)2SO4 and 10% nonvolatile aerosol in the proximity of flight corridors, and (10-30)% H2SO4, up to 50% (NH4)2SO4, and (40-60)% nonvolatile aerosols in air that was not affected by aircraft operations below 10 km. Only a very small fraction of the nonvolatile particles (determined with a condensation nucleus counter) could be morphologically identified as soot aerosol (validated by scanning electron microscopy of wire impactor samples). The newly formed H2SO4 particles did not measurably affect surface area and volume of the background aerosol due to their small size, hence did not affect radiative transfer directly.

Ferry, G. V.↗
NASA NTRS2002

Cloud Condensation Nuclei in FIRE III

Yum and Hudson showed that the springtime Arctic aerosol is probably a result of long-range transport at high altitudes. Scavenging of particles by clouds reduces the low level concentrations by a factor of 3. This produces a vertical gradient in particle concentrations when low-level clouds are present. Concentrations are uniform with height when clouds are not present. Low-level CCN (cloud condensation nuclei) spectra are similar to those in other maritime areas as found by previous projects including FIRE 1 and ASTEX, which were also supported on earlier NASA-FIRE grants. Wylie and Hudson carried this work much further by comparing the CCN spectra observed during ACE with back trajectories of air masses and satellite photographs. This showed that cloud scavenging reduces CCN concentrations at all altitudes over the springtime Arctic, with liquid clouds being more efficient scavengers than frozen clouds. The small size of the Arctic Ocean seems to make it more susceptible to continental and thus anthropogenic aerosol influences than any of the other larger oceans.

Hudson, James G.↗
NASA NTRS2002

A Comparison of the Age-Spectra from Data Assimilation Models

We use kinematic and diabatic back trajectory calculations, driven by winds from a general circulation model (GCM) and two different data assimilation systems (DAS), to compute the age spectrum at three latitudes in the lower stratosphere. The age-spectra are compared to chemical transport model (CTM) calculations, and the mean ages from all of these studies are compared to observations. The age spectra computed using the GCM winds show a reasonably well-isolated tropics in good agreement with observations; however, the age spectra determined from the DAS differ from the GCM spectra. For the diabatic trajectory calculations, the age spectrum is too broad as a result of too much exchange between the tropics and mid-latitudes. The age spectrum determined using the kinematic trajectory calculation is less broad and lacks an age offset; both of these features are due to excessive vertical dispersion of parcels. The tropical and mid-latitude mean age difference between the diabatically and kinematically determined age-spectra is about one year, the former being older. The CTM calculation of the age spectrum using the DAS winds shows the same dispersive characteristics of the kinematic trajectory calculation. These results suggest that the current DAS products will not give realistic trace gas distributions for long integrations; they also help explain why the mean ages determined in a number of previous DAS driven CTM's are too young compared with observations. Finally, we note trajectory-generated age spectra show significant age anomalies correlated with the seasonal cycles, and these anomalies can be linked to year-to-year variations in the tropical heating rate. These anomalies are suppressed in the CTM spectra suggesting that the CTM transport is too diffusive.

Schoeberl, Mark R.↗
NASA NTRS2002

Clouds in the Winter Arctic Tropopause Region

Water vapor in the winter arctic tropopause region is important because, after the tropical tropopause region, the winter arctic tropopause has the coldest temperatures in the tropospheric northern hemisphere. This suggests the potential for cloud formation that can remove water vapor from a part of the atmosphere where radiatively active gases (such as water) exert a disproportionate influence on the earth's radiation budget. Previous work by the same authors has shown that this cloud formation extends into the stratosphere, with 20% of the parcels having ozone values of 300-350 ppbv experiencing ice saturation in any given 10 day period period during the late winter. In fact, temperatures are cold enough that 5-10% of the parcels experience saturation even if the water content is below the prevailing stratospheric value of 5 ppmv. This work describes a case study of clouds observed by aircraft near the winter arctic tropopause during the SAGE Ozone Loss and Validation Experiment (SOLVE). This provided a unique opportunity to examine dehydration processes in this region since in situ water, tracer, cloud particle, and meteorological data were all available simultaneously. During this period, temperatures were cold enough at the tropopause to produce saturation mixing ratios of 3-4 ppmv. Thus, clouds were actually observed within the stratosphere. Back trajectories indicate that the air in these clouds came from lower latitudes and altitudes. The study describes the nature of the clouds, the history of the air, and the possible implications for the upper tropospheric water budget.

Pfister, Leonhard↗
NASA NTRS2002

A Comparison of the Lower Stratospheric Age-Spectra Derived from a General Circulation Model and Two Data Assimilation Systems

We use kinematic and diabatic back trajectory calculations, driven by winds from a general circulation model (GCM) and two different data assimilation systems (DAS), to compute the age spectrum at three latitudes in the lower stratosphere. The age-spectra are compared to chemical transport model (CTM) calculations, and the mean ages from all of these studies are compared to observations. The age spectra computed using the GCM winds show a reasonably isolated tropics in good agreement with observations; however, the age spectra determined from the DAS differ from the GCM spectra. For the DAS diabatic trajectory calculations there is too much exchange between the tropics and mid-latitudes. The age spectrum is thus too broad and the tropical mean age is too old as a result of mixing older mid latitude air with tropical air. Likewise the mid latitude mean age is too young due to the in mixing of tropical air. The DAS kinematic trajectory calculations show excessive vertical dispersion of parcels in addition to excessive exchange between the tropics and mid latitudes. Because air is moved rapidly to the troposphere from the vertical dispersion, the age spectrum is shifted toward the young side. The excessive vertical and meridional dispersion compensate in the kinematic case giving a reasonable tropical mean age. The CTM calculation of the age spectrum using the DAS winds shows the same vertical and meridional dispersive characteristics of the kinematic trajectory calculation. These results suggest that the current DAS products will not give realistic trace gas distributions for long integrations; they also help explain why the extra tropical mean ages determined in a number of previous DAS driven CTM s are too young compared with observations. Finally, we note trajectory-generated age spectra . show significant age anomalies correlated with the seasonal cycles. These anomalies can be linked to year-to-year variations in the tropical heating rate. The anomalies are suppressed in the CTM spectra suggesting that the CTM transport scheme is too diffusive.

Schoeberl, Mark R.↗
NASA NTRS2003

Studies of Trace Gas Chemical Cycles Using Inverse Methods and Global Chemical Transport Models

We report progress in the first year, and summarize proposed work for the second year of the three-year dynamical-chemical modeling project devoted to: (a) development, testing, and refining of inverse methods for determining regional and global transient source and sink strengths for long lived gases important in ozone depletion and climate forcing, (b) utilization of inverse methods to determine these source/sink strengths using either MATCH (Model for Atmospheric Transport and Chemistry) which is based on analyzed observed wind fields or back-trajectories computed from these wind fields, (c) determination of global (and perhaps regional) average hydroxyl radical concentrations using inverse methods with multiple titrating gases, and (d) computation of the lifetimes and spatially resolved destruction rates of trace gases using 3D models. Important goals include determination of regional source strengths of methane, nitrous oxide, methyl bromide, and other climatically and chemically important biogenic/anthropogenic trace gases and also of halocarbons restricted by the Montreal protocol and its follow-on agreements and hydrohalocarbons now used as alternatives to the restricted halocarbons.

Prinn, Ronald G.↗
NASA NTRS2003

Large Scale Water Vapor Sources Relative to the October 2000 Piedmont Flood

Very intense mesoscale or synoptic-scale rainfall events can occasionally be observed in the Mediterranean region without any deep cyclone developing over the areas affected by precipitation. In these perplexing cases the synoptic situation can superficially look similar to cases in which very little precipitation occurs. These situations could possibly baffle the operational weather forecasters. In this article, the major precipitation event that affected Piedmont (Italy) between 13 and 16 October 2000 is investigated. This is one of the cases in which no intense cyclone was observed within the Mediterranean region at any time, only a moderate system was present, and yet exceptional rainfall and flooding occurred. The emphasis of this study is on the moisture origin and transport. Moisture and energy balances are computed on different space- and time-scales, revealing that precipitation exceeds evaporation over an area inclusive of Piedmont and the northwestern Mediterranean region, on a time-scale encompassing the event and about two weeks preceding it. This is suggestive of an important moisture contribution originating from outside the region. A synoptic and dynamic analysis is then performed to outline the potential mechanisms that could have contributed to the large-scale moisture transport. The central part of the work uses a quasi-isentropic water-vapor back trajectory technique. The moisture sources obtained by this technique are compared with the results of the balances and with the synoptic situation, to unveil possible dynamic mechanisms and physical processes involved. It is found that moisture sources on a variety of atmospheric scales contribute to this event. First, an important contribution is caused by the extratropical remnants of former tropical storm Leslie. The large-scale environment related to this system allows a significant amount of moisture to be carried towards Europe. This happens on a time- scale of about 5-15 days preceding the Piedmont event. Second, water-vapor intrusions from the African Inter-Tropical Convergence Zone and evaporation from the eastern Atlantic contribute on the 2-5 day time-scale. The large-scale moist dynamics appears therefore to be one important factor enabling a moderate Mediterranean cyclone to produce heavy precipitation. Finally, local evaporation from the Mediterranean, water-vapor recycling, and orographically-induced low-level convergence enhance and concentrate the moisture over the area where heavy precipitation occurs. This happens on a 12-72 hour time-scale.

Turato, Barbara↗
NASA NTRS2003

Chemical and Physical Properties of Bulk Aerosols within Four Sectors Observed during TRACE-P

Chemical and physical aerosol data collected on the DC-8 during TRACE-P were grouped into four sectors based on back trajectories. The four sectors represent long-range transport from the west (WSW), regional circulation over the western Pacific and Southeast Asia (SE Asia), polluted transport from Northern Asia with substantial sea salt at low altitudes (NNW) and a substantial amount of dust (Channel). WSW has generally low mixing ratios at both middle and high altitudes, with the bulk of the aerosol mass due to non-sea-salt water-soluble inorganic species. Low altitude SE Asia also has low mean mixing ratios in general, with the majority of the aerosol mass comprised of non-sea-salts, however, soot is also relatively important m this region. "w had the highest mean sea salt mixing ratios, with the aerosol mass at low altitudes (a km) evenly divided between sea salts, mm-sea-salts, and dust. The highest mean mixing ratios of water-soluble ions and soot were observed at the lowest altitudes (a km) in the Channel sector. The bulk of the aerosol mass exported from Asia emanates h m Channel at both low and midaltitudes, due to the prevalence of dust compared to other sectors. Number densities show enhanced fine particles for Channel and NNW, while their volume distributions are enhanced due to sea salt and dust Low-altitude Channel exhibits the highest condensation nuclei ((34) number densities along with enhanced scattering coefficients, compared to the other sectors. At midaltitudes (2-7 km), low mean CN number densities coupled with a high proportion of nonvolatile particles (265%) observed in polluted sectors (Channel and NNW) are attributed to wet scavenging which removes hygroscopic CN particles. Low single scatter albedo m SE Asia reflects enhanced soot

Jordan, C. E.↗
NASA NTRS2004

Investigation of Polar Stratospheric Cloud Solid Particle Formation Mechanisms Using ILAS and AVHRR Observations in the Arctic

Satellite observations of denitrification and ice clouds in the Arctic lower stratosphere in February 1997 are used with Lagrangian microphysical box model calculations to evaluate nucleation mechanisms of solid polar stratospheric cloud (PSC) particles. The occurrences of ice clouds are not correlated in time and space with the locations of back trajectories of denitrified air masses, indicating that ice particle surfaces are not always a prerequisite for the formation of solid PSCs that lead to denitrification. In contrast, the model calculations incorporating a pseudoheterogeneous freezing process occurring at the vapor-liquid interface can quantitatively explain most of the observed denitrification when the nucleation activation free energy for nitric acid dihydrate formation is raised by only approx.10% relative to the current published values. Once nucleated, the conversion of nitric acid dihydrate to the stable trihydrate phase brings the computed levels of denitrification closer to the measurements. INDEX TERMS: 0305 Atmospheric Composition and Structure: Aerosols and particles (0345, 4801); 0320 Atmospheric Composition and Sb~lctureC: loud physics and chemistry; 0340 Atmospheric Composition and Structure: Middle atmosphere-composition and chemistry

Irie, H.↗
NASA NTRS2007

Characterizing Aerosols over Southeast Asia using the AERONET Data Synergy Tool

Biomass burning, urban pollution and dust aerosols have significant impacts on the radiative forcing of the atmosphere over Asia. In order to better quanti@ these aerosol characteristics, the Aerosol Robotic Network (AERONET) has established over 200 sites worldwide with an emphasis in recent years on the Asian continent - specifically Southeast Asia. A total of approximately 15 AERONET sun photometer instruments have been deployed to China, India, Pakistan, Thailand, and Vietnam. Sun photometer spectral aerosol optical depth measurements as well as microphysical and optical aerosol retrievals over Southeast Asia will be analyzed and discussed with supporting ground-based instrument, satellite, and model data sets, which are freely available via the AERONET Data Synergy tool at the AERONET web site (http://aeronet.gsfc.nasa.gov). This web-based data tool provides access to groundbased (AERONET and MPLNET), satellite (MODIS, SeaWiFS, TOMS, and OMI) and model (GOCART and back trajectory analyses) databases via one web portal. Future development of the AERONET Data Synergy Tool will include the expansion of current data sets as well as the implementation of other Earth Science data sets pertinent to advancing aerosol research.

Giles, David M.↗
NASA NTRS2007

Summer Dust Aerosols Detected from CALIPSO Observations over the Tibetan Plateau

Summertime Tibetan dust aerosol plumes are detected from the Cloud-Aerosol Lidar and Infrared Pathfinder Satellite Observations (CALIPSO) satellite. CALIPSO reveals that dust storms occur 4 times more frequently than previously found from Tibetan surface observations because few surface sites were available over remote northwestern Tibet. The Tibetan dust aerosol is characterized by column-averaged depolarization and color ratios around 21% and 0.83, respectively. The dust layers appear most frequently around 4-7 km above mean sea level. The depolarization ratio for about 90% of the dust particles is less than 10% at low altitudes (3-5 km), while only about 50% of the particles have a greater depolarization ratio at higher altitudes (7-10 km) suggesting a separation of larger irregular particles from smaller, near spherical ones during transport. The 4-day back trajectory analyses show that these plumes probably originate from the nearby Taklimakan desert surface and accumulate over the northern slopes of the Tibetan Plateau. These dust outbreaks can affect the radiation balance of the atmosphere of Tibet because they both absorb and reflect solar radiation.

Huang, Jianping↗
NASA NTRS2008

3D Air Quality and the Clean Air Interstate Rule: Lagrangian Sampling of CMAQ Model Results to Aid Regional Accountability Metrics

The Clean Air Interstate Rule (CAIR) is expected to reduce transport of air pollutants (e.g. fine sulfate particles) in nonattainment areas in the Eastern United States. CAIR highlights the need for an integrated air quality observational and modeling system to understand sulfate as it moves in multiple dimensions, both spatially and temporally. Here, we demonstrate how results from an air quality model can be combined with a 3d monitoring network to provide decision makers with a tool to help quantify the impact of CAIR reductions in SO2 emissions on regional transport contributions to sulfate concentrations at surface monitors in the Baltimore, MD area, and help improve decision making for strategic implementation plans (SIPs). We sample results from the Community Multiscale Air Quality (CMAQ) model using ensemble back trajectories computed with the NASA Langley Research Center trajectory model to provide Lagrangian time series and vertical profile information, that can be compared with NASA satellite (MODIS), EPA surface, and lidar measurements. Results are used to assess the regional transport contribution to surface SO4 measurements in the Baltimore MSA, and to characterize the dominant source regions for low, medium, and high SO4 episodes.

Fairlie, T. D.↗
NASA NTRS2006

Influence of Ohio River Valley Emissions on Fine Particle Sulfate Measured from Aircraft over Large Regions of the Eastern United States and Canada during INTEX-NA

Aircraft measurements of fine inorganic aerosol composition were made with a particle-into-liquid sampler coupled to dual ion chromatographs (PILS-IC) as part of the NASA INTEX-NA study. The sampling campaign, which lasted from 1 July to 14 August 2004, centered over the eastern United States and Canada and showed that sulfate was the dominant inorganic species measured. The highest sulfate concentrations were observed at altitudes below 2 km, and back trajectory analyses showed a distinct difference between air masses that had or had not intercepted the Ohio River valley (ORV) region. Air masses encountered below 2 km with a history over the ORV had sulfate concentrations that were higher by a factor of 3.2 and total sulfur (S) concentrations higher by 2.5. The study's highest sulfate concentrations were found in these air masses. The sulfur of the ORV air masses was also more processed with a mean sulfate to total sulfur molar ratio of 0.5 compared to 0.3 in non-ORV measurements. Results from a second, independent trajectory model agreed well with those from the primary analysis. These ORV-influenced air masses were encountered on multiple days and were widely spread across the eastern United States and western Atlantic region.

Hennigan, Christopher J.↗
NASA NTRS2007

OMI Tropospheric NO2 from Lightning in Observed Convective Events

Lightning is responsible for an estimated 15 percent of total NO emissions, and is one of the most prominent sources in the upper troposphere. In this study, we present evidence of lightning-generated NO2 (LNO2) using data from the Ozone Monitoring Instrument (OMI), which has observed tropospheric NO2 since its launch in 2004. Although LNO2 has been also reported in previous satellite studies from the Global Ozone Monitoring Experiment (GOME) and SCIAMACHY, OMI is better suited for such measurements by virtue of its higher spatial resolution and daily global coverage. We will present data clearly showing the LNO2 signal in the OMI tropospheric NO2 product on two days over and downwind of specific convective systems in the US Midwest. Gridded monthly mean tropospheric NO 2 data are subtracted from the daily gridded data to obtain the presumed LNO2 signal. Observed cloud-to-ground (CG) lightning flashes from the National Lightning Detection Network (NLDN) were counted along middle and upper tropospheric back trajectories that were run from the regions containing the LNO2 signal. A vertically-weighted average number of upwind CG flashes was obtained using a profile of LNO(x) mass obtained from a series of midlatitude cloud-resolved storm chemistry simulations. The number of CG flashes was scaled up to total flashes (intracloud (IC) flashes plus CG) using a climatological IC/CG ratio. The number of moles of LNO(x) in the region considered was estimated by assuming that LNO2 is 30 percent of LNO(x). This value was divided by the number of upwind flashes to obtain an average estimate of the number of moles produced per flash. Results yield values in the range obtained through other estimation techniques (e.g., aircraft measurements, models). We will also present a similar analysis over northern Australia during the SCOUT-O3/ACTIVE field campaigns in November and December 2005, in which we will compare the OMI LNOx signals with aircraft observations from the storm anvils.

Pickering, Kenneth↗
NASA NTRS2008

The Relationship of Loss, Mean Age of Air and the Distribution of CFC's to Stratospheric Circulation and Implications for Atmospheric Lifetimes

Model-derived estimates of the annually integrated destruction and lifetime for various ozone depleting substances (ODSs) depend on the simulated stratospheric transport and mixing in the global model used to produce the estimate. Observations in the middle and high latitude lower stratosphere show that the mean age of an air parcel (i.e., the time since its stratospheric entry) is related to the fractional release for the ODs (i.e., the amount of the ODS that has been destroyed relative to the amount at the time of stratospheric entry). We use back trajectory calculations to produce an age spectrum, and explain the relationship between the mean age and the fractional release by showing that older elements in the age spectrum have experienced higher altitudes and greater ODs destruction than younger elements. In our study, models with faster circulations produce distributions for the age-of-air that are 'young' compared to a distribution derived from observations. These models also fail to reproduce the observed relationship between the mean age of air and the fractional release. Models with slower circulations produce both realistic distributions for mean age and a realistic relationship between mean age and fractional release. These models also produce a CFCl3 lifetime of approximately 56 years, longer than the 45 year lifetime used to project future mixing ratios. We find that the use of flux boundary conditions in assessment models would have several advantages, including consistency between ODS evolution and simulated loss even if the simulated residual circulation changes due to climate change.

Douglas, A. R.↗
NASA NTRS2004

Observational Evidence Against Mountain-Wave Generation of Ice Nuclei as a Prerequisite for the Formation of Three Solid Nitric Acid Polar Stratospheric Clouds Observed in the Arctic in Early December 1999

A number of recently published papers suggest that mountain-wave activity in the stratosphere, producing ice particles when temperatures drop below the ice frost point, may be the primary source of large NAT particles. In this paper we use measurements from the Advanced Very High Resolution Radiometer (AVHRR) instruments on board the National Oceanic and Atmospheric Administration (NOAA) polar-orbiting satellites to map out regions of ice clouds produced by stratospheric mountain-wave activity inside the Arctic vortex. Lidar observations from three DC-8 flights in early December 1999 show the presence of solid nitric acid (Type Ia or NAT) polar stratospheric clouds (PSCs). By using back trajectories and superimposing the position maps on the AVHRR cloud imagery products, we show that these observed NAT clouds could not have originated at locations of high-amplitude mountain-wave activity. We also show that mountain-wave PSC climatology data and Mountain Wave Forecast Model 2.0 (MWFM-2) raw hemispheric ray and grid box averaged hemispheric wave temperature amplitude hindcast data from the same time period are in agreement with the AVHRR data. Our results show that ice cloud formation in mountain waves cannot explain how at least three large scale NAT clouds were formed in the stratosphere in early December 1999.

MOUNTAIN WAVES↗