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Hipskind, R. Stephen

Publications and source records attributed to Hipskind, R. Stephen.

At least 19 records

Vertical Mass, Momentum, Moisture, and Heat Fluxes in Hurricanes above 10 km during CAMEX-3 and CAMEX-4

The third and fourth NASA Convection and Moisture Experiments (CAMEX-3 and CAMEX-4) during the Atlantic hurricane seasons of 1998 and 2001, respectively, have yielded comprehensive multi-aircraft datasets using, both remote and in-situ instrumentation. Among these are high-frequency in-situ measurements of vertical wind, horizontal wind, temperature, and water vapor, made from NASA's DC-8 aircraft in the upper portions of the hurricane (typically above 10 km). Wind and temperature measurements were made at 20 hz by the NASA/Ames Meteorological Measurement System, while water vapor was measured at 1 hz by the NASA/JPL Laser Hygrometer. Fluxes of heat, momentum, and moisture at these levels are important, since modeling studies have shown that ice processes, which are dominant at temperatures below -40C (where the DC-8 flies) are important for hurricane intensification. Also, there are indications from satellite studies that latent heat release at DC-8 levels is significant, perhaps a third of those in the mid-troposphere. Preliminary results show that typical updrafts in the eyewall region are comparable to or higher than previous observations of tropical convection, with several instances of updraft magnitudes of 15 meters per second (the maximum observed was 21 meters per second). They also show significant supersaturations (10-20% or more) in the updrafts, which would enhance the latent heat release at the upper levels of the hurricane. This paper will examine the magnitude and distribution of small and mesoscale vertical fluxes of mass, momentum, moisture, and heat. The goal is to examine the role of these fluxes in the overall budgets of the respective quantities in the upper portions of the hurricane.

Pfister, Leonhard

In-Situ Measurements of HCN and CH3CN In the Pacific Troposphere: Sources, Sinks, and Comparisons with Satellite Observations

A new capillary gas chromatographic method using a Reduction Gas Detector was developed to measure HCN and CH3CN in the remote troposphere. This instrumental configuration was deployed for the very first time in the Trace-P field mission performed during the spring of 2001. The NASA DC-8 aircraft afforded an opportunity to measure HCN and CH3CN in polluted and pristine environments over the Pacific to a maximum altitude of 12 km. These are some of the first in situ measurements of the distribution of HCN and CH3CN over the Pacific. Large background concentrations of both nitriles were found to be present and significant variability was observed. The abundance of HCN and CH3CN was strongly impacted by outflow of pollution from Asia. In general there appeared to be a direct but nonlinear relationship between the mixing ratios of HCN and CH3CN. The vertical structure of these chemicals shows direct evidence of the presence of a significant oceanic sink. These observations will be compared with the column content HCN data from satellites and other available measurements. A large body of data have been collected and are being analyzed, both statistically and with the help of models, to better understand the sources and sinks of these nitriles. These results will be presented.

Singh, Hanwant B.

Overview of ACE-Asia Spring 2001 Investigations On Aerosol-Radiation Interactions

ACE-Asia's extensive measurements from land, ocean, air and space quantified aerosol-radiation interactions. Results from each platform type, plus satellite-suborbital combinations, include: 1. Time series of multiwavelength aerosol optical depth (ADD), Angstrom exponent (alpha), single-scattering albedo (SSA), and size distribution from AERONET radiometry at 13 stations. In China and Korea AOD and alpha were strongly anticorrelated (reflecting transient dust events); dust volume-size modes peaked near 8 microns diameter; and SSA(dust) greater than SSA(pollution). 2. Calculations and measurements of photosynthetically active radiation and aerosols in China yield 24-h average downward surface radiative forcing per AOD(500 nm) of -27 W/sq m (400-700 nm). 3. The Hawaii-Japan cruise sampled a gradient with AOD(500 nm) extremes of 0.1 and 1.1. Shipboard measurements showed that adding dust to pollution increased SSA(550 nm, 55% RH), typically from -0.91 to approx. 0.97. Downwelling 8-12 micron radiances showed aerosol effects, especially in the major April dust event, with longwave forcing estimated at -5 to 15 W/sq m. 4. Extinction profiles from airborne sunphotometry and total-direct-diffuse radiometry show wavelength dependence often varying strongly with height, reflecting layering of dust-dominated over pollution-dominated aerosols. Comparing sunphotometric extinction profiles to those from in situ measurements (number and composition vs size, or scattering and absorption) shows layer heights agree, but extinction sometimes differs. 5. Airborne solar spectral flux radiometry yields absorption spectra for layers. Combining with AOD spectra yields best-fit aerosol single scattering albedo spectra. 6. Visible, NIR and total solar fluxes combined with AOD give radiative forcing efficiencies at surface and aloft.

Russell, P. B.

Measurements of Oxygenated Organic Chemicals In the Pacific Troposphere During TRACE-P: Higher Aldehydes (less than C(sub 1)), Their Sources, and Potential Role In Atmospheric Oxidation

Airborne measurements of a large number of oxygenated organics were carried out in the Pacific troposphere (to 12 km) in the Spring of 2001 (Feb. 24-April 10). Specifically these measurements included acetaldehyde, propanaldehyde, acetone, methylethyl ketone, methanol, ethanol, PAM and organic nitrates. Independent measurements of formaldehyde, peroxides, and tracers were also available. Highly polluted as well as pristine air masses were sampled. Oxygenated organics were abundant in the clean In troposphere and were greatly enhanced in the outflow regions from Asia. Extremely high concentrations of aldehydes could be measured in the troposphere. It is not possible to explain the large abundances of aldehydes in the background troposphere without invoking significant oceanic sources. A strong correlation between the observed mixing ratios of formaldehyde and acetaldehyde is present. We infer that higher aldehydes (such as acetaldehyde and propanaldehyde) may provide a large source of formaldehyde and sequester Cox throughout the troposphere. The atmospheric behavior of acetone, methylethyl ketone, and methanol is generally indicative of their common terrestrial sources with a Image contribution from biomass/biofuel burning. A vast body of data has been collected and it is being analyzed both statistically and with the help of models to better understand the role that oxygenated organics play in the atmosphere and to unravel their sources and sinks. These results will be presented.

Singh, Hanwant B.

Coordinated Airborne, Spaceborne, and Ground-Based Measurements of Massive, Thick Aerosol Layers During the Dry Season in Southern Africa

During the dry-season airborne campaign of the Southern African Regional Science Initiative (SAFARI 2000), unique coordinated observations were made of massive, thick aerosol layers. These layers were often dominated by aerosols from biomass burning. We report on airborne Sunphotometer measurements of aerosol optical depth (lambda=354-1558 nm), columnar water vapor, and vertical profiles of aerosol extinction and water vapor density that were obtained aboard the University of Washington's Convair-580 research aircraft. We compare these with ground-based AERONET Sun/sky radiometer results, with ground based lidar data MPL-Net), and with measurements from a downward-pointing lidar aboard the high-flying NASA ER-2 aircraft. Finally, we show comparisons between aerosol optical depths from the Sunphotometer and those retrieved over land and over water using four spaceborne sensors (TOMS (Total Ozone Mapping Spectrometer), MODIS (Moderate Resolution Imaging Spectrometer), MISR (Multiangle Imaging Spectroradiometer) and ATSR-2 (Along Track Scanning Radiometer)).

Schmid, B.

Rationalizing Burned Carbon with Carbon Monoxide Exported from South America

We present several estimates cross-checking the fluxes of carbon to the atmosphere from burning, comparing models that are based on simple land-surface parameterizations and atmospheric transport dynamics. Both estimates made by NASA Ames and USP modeling techniques are quite high compared to some detailed satellite/land-use studies of emissions. The flux of carbon liberated to the atmosphere via biomass burning is important for several reasons. This flux is a fundamental statistic for the parameterization of the large-scale flux of gases controlling the reactive greenhouse gases methane and ozone. Similarly, it is central to the estimation of the translocation of nitrogen and pyrodenitrification in the tropics. Thirdly, CO2 emitted from rainforest clearing contributes directly to carbon lost from the rainforest system as it contributes to greenhouse gas forcing. While CO2 from pasturage, agriculture, etc, is considered to be reabsorbed seasonally, and so "off budget" for the carbon cycle, it must also be accounted. CO2 anomalies related to daily weather and interannual climatic variation are strong enough to perturb our scientific perception of long-term carbon storage trends. We compare fluxes deduced from land-use statistics (originally, W.M. Hao) and from satellite hot pixels (A. Setzer) with atmospheric fluxes determined by the mesoscale/continental scale models RAMS and MM5, and point to some new work with highly resolved global models (the NASA Data Assimilation Office's GEOS4). Our simulations are tied to events, so that measured tracers like CO tie the models directly to the burning and meteorology of a specific period. We point out a particular sensitivity in estimates based on CO, and indicate how analysis of CO2 along with other biomass-burning tracers may lead to an improved multi-species estimator of carbon burned.

Chatfield, R.

Airborne Sunphotometer Measurements of Aerosol Optical Depth and Water Vapor in ACE-Asia and Their Comparisons to Correlative Measurements

In the Spring 2001 phase of the Asian Pacific Regional Aerosol Characterization Experiment (ACE-Asia), the 6-channel NASA Ames Airborne Tracking Sunphotometer (AATS-6) operated on 15 of the 19 research flights of the NCAR C-130, while its 14-channel counterpart (AATS-14) flew successfully on all 19 research flights of the CIRPAS Twin Otter. ACE-Asia studied aerosol outflow from the Asian continent to the Pacific basin. It was designed to integrate suborbital and satellite measurements and models to reduce the uncertainty in calculations of the climate forcing due to aerosols. AATS-6 and AATS-14 measured solar beam transmission at six and 14 wavelengths (380-1021 and 354-1558 nm, respectively), yielding aerosol optical depth (AOD) spectra and columnar water vapor (CWV). Vertical differentiation in profiles yielded aerosol extinction spectra and water vapor concentration. In this paper, we plan to present examples of the following, preliminary findings that are based in part on our airborne sunphotometer measurements: (1) The wavelength dependence of sunphotometer-derived AOD and extinction indicates that supermicron dust was often a major component of the aerosol, frequently extending to high altitudes. The percentage of full-column AOD (525 nm) that Jay above 3 km was typically 34+/-13%. In contrast, the analogous percentage of columnar water vapor was only 10+/-4%; (2) Initial comparison studies between AOD data obtained by AATS-6 and AATS-14 during coordinated low-level flight legs show agreement well within the instruments' error bars; (3) Aerosol extinction has been derived from airborne in situ measurements of scattering (nephelometers) and absorption (particle soot/ absorption photometer, PSAP) or calculated from particle size distribution measurements (mobility analyzers and aerodynamic particle sizers). Comparison with corresponding extinction values derived from the Ames airborne sunphotometer measurements shows good agreement for the vertical distribution of aerosol layers. However, the level of agreement in absolute magnitude of the derived aerosol extinction/optical depth varied among the aerosol layers sampled; (4) Initial comparisons of sunphotometer and satellite-derived AOD using SeaWiFS, MISR and AVHRR show promising results. We also plan to include comparisons with MODIS and TOMS: (5) Initial comparisons of sunphotometer-derived AOD and aerosol extinction profiles with lidars in Tokyo and on a ship show reasonable agreement.

Schmid, B.

Airborne Sunphotometer Measurements of Aerosol Optical Depth and Columnar Water Vapor During the Puerto Rico Dust Experiment, and Comparison with Land, Aircraft, and Satellite Measurements

Analyses of aerosol optical depth (AOD) and columnar water vapor (CWV) measurements obtained with the six-channel NASA Ames Airborne Tracking Sunphotometer (AATS-6) mounted on a twin-engine aircraft during the summer 2000 Puerto Rico Dust Experiment are presented. In general, aerosol extinction values calculated from AATS-6 AOD measurements acquired during aircraft profiles up to 5 km ASL reproduce the vertical structure measured by coincident aircraft in-situ measurements of total aerosol number and surface area concentration. Calculations show that the spectral dependence of AOD was small (mean Angstrom wavelength exponents of approximately 0.20) within three atmospheric layers defined as the total column beneath the top of each aircraft profile, the region beneath the trade wind inversion, and the region within the Saharan Air Layer (SAL) above the trade inversion. This spectral behavior is consistent with attenuation of incoming solar radiation by large dust particles or by dust plus sea salt. Values of CWV calculated from profile measurements by AATS-6 at 941.9 nm and from aircraft in-situ measurements by a chilled mirror dewpoint hygrometer agree to within approximately 4% (0.13 g/sq cm). AATS-6 AOD values measured on the ground at Roosevelt Roads Naval Air Station and during low altitude aircraft runs over the adjacent Cabras Island aerosol/radiation ground site agree to within 0.004 to 0.030 with coincident data obtained with an AERONET Sun/sky Cimel radiometer located at Cabras Island. For the same observation times, AERONET retrievals of CWV exceed AATS-6 values by a mean of 0.74 g/sq cm (approximately 21 %) for the 2.9-3.9 g/sq cm measured by AATS-6. Comparison of AATS-6 aerosol extinction values obtained during four aircraft ascents over Cabras Island with corresponding values calculated from coincident aerosol backscatter measurements by a ground-based micro-pulse lidar (MPL-Net) located at Cabras yields a similar vertical structure above the trade inversion. Finally, AATS-6 AOD values measured during low altitude aircraft traverses over the ocean are compared with corresponding AOD values retrieved over water from upwelling radiance measurements by the MODIS, TOMS, and GOES-8 Imager satellite sensors, with mixed results. These exercises highlight the need for continued satellite sensor comparison/validation studies to improve satellite AOD retrieval algorithms, and the usefulness of airborne sunphotometer measurements in the validation process.

Livingston, John M.

In-Situ Measurements of HCN and CH3CN in the Pacific Troposphere: Sources, Sinks, and Comparisons with Spectroscopic Observations

We report the first in-situ measurements of hydrogen cyanide (HCN) and acetonitrile (CH3CN) from the Pacific troposphere (0-12 km) obtained during the NASA/Trace-P mission (Feb.-April, 2001). Mean HCN and CH3CN mixing ratios of 243 (+/-118) ppt and 149 (+/-56) ppt respectively, were measured. The in-situ observations correspond to a total HCN column of 4.4-4.9 x 10(exp 15) molec. cm(exp -2) and a CH3CN column of 2.8-3.0 x 10(exp 15) molec. cm(exp -2). This HCN column is in good agreement with available spectroscopic observations. The atmospheric concentrations of HCN and CH3CN were greatly influenced by outflow of pollution from Asia. There is a linear relationship between the mixing ratios of HCN and CH3CN, and in turn these are well correlated with tracers of biomass combustion (e.g. CH3Cl, CO). Relative enhancements with respect to known tracers of biomass combustion within selected plumes in the free troposphere, and pollution episodes in the boundary layer allow an estimation of a global biomass burning source of 0.8+/-0.4 Tg (N)/y for HCN and 0.4+/-0.1 Tg (N)/y for CH3CN. In comparison, emissions from automobiles and industry are quite small (<0.05 Tg (N)/y). The vertical structure of HCN and CH3CN indicated reduced mixing ratios in the MBL (Marine Boundary Layer). Using, a simple box model, the observed gradients across the top of the MBL are used to derive an oceanic flux of 6.7 x 10(exp -15) g (N) cm(exp -2)/s for HCN and 4.8 x 10(exp -15) g (N) cm(exp -2)/s for CH3CN. An air-sea exchange model is used to conclude that this flux can be maintained if the oceans are under-saturated in HCN and CH3CN by 23% and 17%, respectively. It is inferred that oceanic loss is a dominant sink for these nitrites, and they deposit some 1.3 Tg (N) of nitrogen annually to the oceans. Assuming reaction with OH radicals and loss to the oceans as the major removal processes, a mean atmospheric residence time of 4.7 months for HCN and 5.1 months for CH3CN is calculated. A global budget analysis shows that the sources and sinks of HCN and CH3CN are roughly in balance. There are indications that biogenic sources may also be present. Mechanisms involved in nitrate formation during combustion and removal in the oceans are poorly understood.

Singh, Hanwant B.

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

INTEX-NA: Intercontinental Chemical Transport Experiment - North America

INTEX-NA is an integrated atmospheric chemistry field experiment to be performed over North America using the NASA DC-8 and P-3B aircraft as its primary platforms. It seeks to understand the exchange of chemicals and aerosols between continents and the global troposphere. The constituents of interest are ozone and its precursors (hydrocarbons, NOX and HOX), aerosols, and the major greenhouse gases (CO2, CH4, N2O). INTEX-NA will provide the observational database needed to quantify inflow, outflow, and transformations of chemicals over North America. INTEX-NA is to be performed in two phases. Phase A will take place during the period of May-August 2004 and Phase B during March-June 2006. Phase A is in summer when photochemistry is most intense and climatic issues involving aerosols and carbon cycle are most pressing, and Phase B is in spring when Asian transport to North America is at its peak. INTEX-NA will coordinate its activities with concurrent measurement programs including satellites (e. g. Terra, Aura, Envisat), field activities undertaken by the North American Carbon Program (NACP), and other U.S. and international partners. However, it is being designed as a 'stand alone' mission such that its successful execution is not contingent on other programs. Synthesis of the ensemble of observation from surface, airborne, and space platforms, with the help of global/regional models is an important It is anticipated that approximately 175 flight hours for each of the aircraft (DC-8 and P-3B) will be required for each Phase. Principal operational sites are tentatively selected to be Bangor, ME; Wallops Island, VA; Seattle, WA; Rhinelander, WI; Lancaster, CA; and New Orleans, LA. These coastal and continental sites can support large missions and are suitable for INTEX-NA objectives. The experiment will be supported by forecasts from meteorological and chemical models, satellite observations, surface networks, and enhanced O3,-sonde releases. In addition to characterizing Atlantic-outflow and Pacific-inflow, INTEX-NA will characterize air masses transported between the U.S., Canada, and Mexico. INTEX-NA will be the first continental scale inflow, outflow, and transformation experiment to be performed over North America. It will provide the most comprehensive observational data set to date to understand the O3/NOX/HOX/aerosol photochemical system and the carbon cycle. One of the critical needs of the carbon cycle research is to obtain large-scale vertical and horizontal concentration gradients of CO2, throughout the troposphere over continental source/sink regions. INTEX-NA is ideally suited to perform this role. Coastal and continental operational sites will allow us to develop a curtain profile of greenhouse gases (e. g. CO2,) and other key pollutants across North America. Such information is central to our quantitative understanding of chemical budgets on the continental scale. We expect to provide a number of satellite under-flights over land and water to test and validate observations from the appropriate satellite platform (e. g. Aura). We plan to develop strong collaborations with other national and international observational programs. Results from INTEX-NA should directly benefit the development of environmental policy for air quality and climate change.

Singh, Hanwant B.

Airborne Sunphotometer Studies of Aerosol Properties and Effects, Including Closure Among Satellite, Suborbital Remote, and In situ Measurements

Airborne sunphotometry has been used to measure aerosols from North America, Europe, and Africa in coordination with satellite and in situ measurements in TARFOX (1996), ACE-2 (1997), PRIDE (2000), and SAFARI 2000. Similar coordinated measurements of Asian aerosols are being conducted this spring in ACE-Asia and are planned for North American aerosols this summer in CLAMS. This paper summarizes the approaches used, key results, and implications for aerosol properties and effects, such as single scattering albedo and regional radiative forcing. The approaches exploit the three-dimensional mobility of airborne sunphotometry to access satellite scenes over diverse surfaces (including open ocean with and without sunglint) and to match exactly the atmospheric layers sampled by airborne in situ measurements and other radiometers. These measurements permit tests of the consistency, or closure, among such diverse measurements as aerosol size-resolved chemical composition; number or mass concentration; light extinction, absorption, and scattering (total, hemispheric back and 180 deg.); and radiative fluxes. In this way the airborne sunphotometer measurements provide a key link between satellite and in situ measurements that helps to understand any discrepancies that are found. These comparisons have led to several characteristic results. Typically these include: (1) Better agreement among different types of remote measurements than between remote and in situ measurements. (2) More extinction derived from transmission measurements than from in situ measurements. (3) Larger aerosol absorption inferred from flux radiometry than from in situ measurements. Aerosol intensive properties derived from these closure studies have been combined with satellite-retrieved fields of optical depth to produce fields of regional radiative forcing. We show results for the North Atlantic derived from AVHRR optical depths and aerosol intensive properties from TARFOX and ACE-2. Companion papers show analogous, preliminary results for Asian-Pacific aerosols and results of SAFARI-2000 closure studies on African aerosols.

Russlee, Philip B.

Shortwave Radiative Fluxes, Solar-Beam Transmissions, and Aerosol Properties: TARFOX and ACE-2 Find More Absorption from Flux Radiometry than from Other Measurements

The Tropospheric Aerosol Radiative Forcing Observational Experiment (TARFOX) and the Second Aerosol Characterization Experiment (ACE-2) made simultaneous measurements of shortwave radiative fluxes, solar-beam transmissions, and the aerosols affecting those fluxes and transmissions. Besides the measured fluxes and transmissions, other obtained properties include aerosol scattering and absorption measured in situ at the surface and aloft; aerosol single scattering albedo retrieved from skylight radiances; and aerosol complex refractive index derived by combining profiles of backscatter, extinction, and size distribution. These measurements of North Atlantic boundary layer aerosols impacted by anthropogenic pollution revealed the following characteristic results: (1) Better agreement among different types of remote measurements of aerosols (e.g., optical depth, extinction, and backscattering from sunphotometers, satellites, and lidars) than between remote and in situ measurements; 2) More extinction derived from transmission measurements than from in situ measurements; (3) Larger aerosol absorption inferred from flux radiometry than from other measurements. When the measured relationships between downwelling flux and optical depth (or beam transmission) are used to derive best-fit single scattering albedos for the polluted boundary layer aerosol, both TARFOX and ACE-2 yield midvisible values of 0.90 +/- 0.04. The other techniques give larger single scattering albedos (i.e. less absorption) for the polluted boundary layer, with a typical result of 0.95 +/- 0.04. Although the flux-based results have the virtue of describing the column aerosol unperturbed by sampling, they are subject to questions about representativeness and other uncertainties (e.g., unknown gas absorption). Current uncertainties in aerosol single scattering albedo are large in terms of climate effects. They also have an important influence on aerosol optical depths retrieved from satellite radiances. More tests are needed of the consistency among different methods and of the effects of changing humidity on aerosol.

Russell, Philip B.

Satellite Observations of Tropospheric Chemistry

The troposphere is an essential component of the earth's life support system as well as the gateway for the exchange of chemicals between different geochemical reservoirs of the earth. The chemistry of the troposphere is sensitive to perturbation from a wide range of natural phenomena and human activities. The societal concern has been greatly enhanced in recent decades due to ever increasing pressures of population growth and industrialization. Chemical changes within the troposphere control a vast array of processes that impact human health, the biosphere, and climate. A main goal of tropospheric chemistry research is to measure and understand the response of atmospheric composition to natural and anthropogenic perturbations, and to develop the capability to predict future change. Atmospheric chemistry measurements are extremely challenging due to the low concentrations of critical species and the vast scales over which the observations must be made. Available tropospheric data are mainly from surface sites and aircraft missions. Because of the limited temporal extent of aircraft observations, we have very limited information on tropospheric composition above the surface. This situation can be contrasted to the stratosphere, where satellites have provided critical and detailed chemical data on the global distribution of key trace gases.

Singh, Hanwant B.

Solubility of methanol in low-temperature aqueous sulfuric acid and implications for atmospheric particle composition

Using traditional Knudsen cell techniques, we find well-behaved Henry's law uptake of methanol in aqueous 45 - 70 wt% H2SO4 solutions at temperatures between 197 and 231 K. Solubility of methanol increases with decreasing temperature and increasing acidity, with an effective Henry's law coefficient ranging from 10(exp 5) - 10(exp 8) M/atm. Equilibrium uptake of methanol into sulfuric acid aerosol particles in the upper troposphere and lower stratosphere will not appreciably alter gas-phase concentrations of methanol. The observed room temperature reaction between methanol and sulfuric acid is too slow to provide a sink for gaseous methanol at the temperatures of the upper troposphere and lower stratosphere. It is also too slow to produce sufficient quantities of soluble reaction products to explain the large amount of unidentified organic material seen in particles of the upper troposphere.

Iraci, Laura T.

The Colocation, or Lack Thereof, of Deep Convection and Cold Tropopause Temperatures in the Tropical Winter Western Pacific

Recent work has suggested that dehydration near the tropical tropopause during the northern hemisphere winter is separate in place and time from the actual transfer of mass from the troposphere to the stratosphere. In fact, some work suggests that dehydration takes place in an environment where the motion is downward, with such downward motion induced either by radiative cooling over cold cloud tops or turbulent heat flux divergence due to convection. Radiative heating and cooling rates at the tropical tropopause are quite small and very sensitive to the temperature profile and underlying cloudiness. Given this, the idea of downward motion in the region of coldest temperatures and dehydration implies that coldest temperatures and underlying cloudiness are colocated. This may not necessarily be the case. This paper attempts to explore, on a preliminary basis: (1) The sensitivity of radiative heating rates at the tropical tropopause to details of the temperature profile and underlying cloudiness and (2) the relative positions of high cold clouds and cold tropopause temperatures.

Pfister, Leonhard

Methanol Uptake by Low Temperature Aqueous Sulfuric Acid Solutions

The global methanol budget is currently unbalanced, with source terms significantly larger than the sinks terms. To evaluate possible losses of gaseous methanol to sulfate aerosols, the solubility and reactivity of methanol in aqueous sulfuric acid solutions representative of upper tropospheric and lower stratospheric aerosols is under investigation. Methanol will partition into sulfate aerosols according to its Henry's law solubility. Using standard uptake techniques in a Knudsen cell reactor, we have measured the effective Henry's law coefficient, H*, for cold (196 - 220 K) solutions ranging between 45 and 70 wt % H2SO4. We have found that methanol solubility ranges from approx. 10(exp 5) - 10(exp 7) M/atm for UT/LS conditions. Solubility increases with decreasing temperature and with increasing sulfuric acid content. Although methanol is slightly more soluble than are acetone and formaldehyde, current data indicate that uptake by clean aqueous sulfuric acid particles will not be a significant sink for methanol in the UT/LS. These solubility measurements include uptake due to physical solvation and any rapid equilibria which are established in solution. Reaction between primary alcohols and sulfuric acid does occur, leading to the production of alkyl sulfates. Literature values for the rate of this reaction suggest that formation of CH3OSO3H is not significant over our experimental time scale for solutions below 80 wt % H2SO4. To confirm this directly, results obtained using a complementary equilibrium measurement technique will also be presented.

Iraci, L. T.

Defining the Polar Vortex Edge Using an N2O: Potential Temperature Correlation Versus the Nash Criterion: A Comparison

A prerequisite to study phenomena in the winter stratospheric polar vortex is the separation of measurements inside and outside the dynamical barrier of the vortex edge. We describe a technique to accurately determine the inner edge of the vortex boundary region from measurements of potential temperature and a trace gas, such as N2O, and apply it to in situ aircraft and balloon measurements from the SOLVE/THESE02000 Arctic campaign. The method may be used to refine the Nash algorithm, which, due to the inherently coarser resolution of potential vorticity on which it is dependent, may misidentify the inner edge by up to 466 km, and omit the identification of small, extra-vortex filaments within the vortex.

Greenblatt, Jeffery B.