Thesis (Ph. D.)--University of Washington, 2003. / Vita. Includes bibliographical references (p. 100-107).

This dissertation discusses, in brief, the production and transport property characterization of films made from the extrusion and biaxial stretching of [beta] nucleated isotactic polypropylene and the extrusion of PEBAX block copolymers. Multilayered films for modified atmosphere packaging applications were also produced by coextrusion and biaxial stretching of these two materials and similarly characterized. Current membranes for packaging applications are generally produced by coating a porous support with a polymeric solution to deposit an active layer for separation. The goal of this project is to displace membranes produced by solvent-based processes, which are environmentally hazardous and thus costly, with equivalent or superior materials produced using melt extrusion. / text

Large uncertainties exist in estimations of aerosol direct radiative forcing and indirect radiative forcing, and the values derived from globalmodeling differ substantially with satellite-based calculations. Following the approach of Quaas et al. (2008; hereafter named Quaas2008),we reassess satellite-based clear- and cloudy-sky radiative forcings and their seasonal variations by employing updated satellite products from 2004 to 2011 in combination with the anthropogenic aerosol optical depth (AOD) fraction obtained frommodel simulations using the Goddard Earth Observing System-Chemistry-Advanced ParticleMicrophysics (GEOS-Chem-APM). Our derived annual mean aerosol clear-sky forcing (-0.59 W m-2) is lower, while the cloudy-sky forcing (-0.34 W m-2) is higher than the corresponding results (-0.9Wm-2 and -0.2W m-2, respectively) reported in Quaas2008. Our study indicates that the derived forcings are sensitive to the anthropogenic AOD fraction and its spatial distribution but insensitive to the temporal resolution used to obtain the regression coefficients, i.e.,monthly or seasonal based. The forcing efficiency (i.e., the magnitude per anthropogenic AOD) for the clear-sky forcing based on this study is 19.9Wm-2, which is about 5% smaller than Quaas2008’s value of 21.1Wm-2. In contrast, the efficiency for the cloudy-sky forcing of this study (11 W m-2) is more than a factor of 2 larger than Quaas2008’s value of 4.7 W m-2. Uncertainties tests indicate that anthropogenic fraction of AOD strongly affects the computed forcings while using aerosol index instead of AOD from satellite data as aerosol proxy does not appear to cause any significant differences in regression slopes and derived forcings.

A simple way to diagnose fractional cloud cover in general circulation models is to relate it to the simulated relative humidity, and allowing for fractional cloud cover above a “critical relative humidity” of less than 100%. In the formulation chosen here, this is equivalent to assuming a uniform “top-hat” distribution of subgrid-scale total water content with a variance related to saturation. Critical relative humidity has frequently been treated as a “tunable” constant, yet it is an observable. Here, this parameter, and its spatial distribution, is examined from Atmospheric Infrared Sounder (AIRS) satellite retrievals, and from a combination of relative humidity from the ECMWF Re-Analyses (ERA-Interim) and cloud fraction obtained from CALIPSO lidar satellite data. These observational data are used to evaluate results from different simulations with the ECHAM general circulation model (GCM). In sensitivity studies, a cloud feedback parameter is analyzed from simulations applying the original parameter choice, and applying parameter choices guided by the satellite data. Model sensitivity studies applying parameters adjusted to match the observations show larger positive cloud-climate feedbacks, increasing by up to 30% compared to the standard simulation.

In this study we examine the performance of 31 global model radiative transfer schemes in cloudfree conditions with prescribed gaseous absorbers and no aerosols (Rayleigh atmosphere), with prescribed scatteringonly aerosols, and with more absorbing aerosols. Results are compared to benchmark results from high-resolution, multiangular line-by-line radiation models. For purely scattering aerosols, model bias relative to the line-by-line models in the top-of-the atmosphere aerosol radiative forcing ranges from roughly −10 to 20 %, with over- and underestimates of radiative cooling at lower and higher solar zenith angle, respectively. Inter-model diversity (relative standard deviation) increases from ~ 10 to 15% as solar zenith angle decreases. Inter-model diversity in atmospheric and surface forcing decreases with increased aerosol absorption, indicating that the treatment of multiple-scattering is more variable than aerosol absorption in the models considered. Aerosol radiative forcing results from multi-stream models are generally in better agreement with the line-by-line results than the simpler two-stream schemes. Considering radiative fluxes, model performance is generally the same or slightly better than results from previous radiation scheme intercomparisons. However, the inter-model diversity in aerosol radiative forcing remains large, primarily as a result of the treatment of multiple-scattering. Results indicate that global models that estimate aerosol radiative forcing with two-stream radiation schemes may be subject to persistent biases introduced by these schemes, particularly for regional aerosol forcing.

The formation of cloud droplets on aerosol particles, technically known as the activation of cloud condensation nuclei (CCN), is the fundamental process driving the interactions of aerosols with clouds and precipitation. Knowledge of these interactions is foundational to our understanding of weather and climate. The Intergovernmental Panel on Climate Change (IPCC) and the Decadal Survey (NRC 2007) indicate that the uncertainty in how clouds adjust to aerosol perturbations dominates the uncertainty in the overall quantification of the radiative forcing attributable to human activities. The Clouds, Hazards, and Aerosols Survey for Earth Researchers (CHASER) satellite mission concept responds to the IPCC and Decadal Survey concerns by studying the activation of CCN and their interactions with clouds and storms. The CHASER satellite mission was developed to remotely sense quantities necessary for determining the interactions of aerosols with clouds and storms. The links between the Decadal Survey recommendations and the CHASER goals, science objectives, measurements, and instruments are described in Table 1. Measurements by current satellites allow a rough determination of profiles of cloud particle size but not of the activated CCN that seed them. CHASER will use an innovative technique (Freud et al. 2011; Freud and Rosenfeld 2012; Rosenfeld et al. 2012) and high-heritage (flown in a previous spaceflight mission) instruments to produce satellite-based remotely sensed observations of activated CCN and the properties of the clouds associated with them. CHASER will estimate updraft velocities at cloud base to calculate the number density of activated CCN as a function of the water vapor supersaturation. CHASER will determine the CCN concentration and cloud thermodynamic forcing (i.e., forcing caused by changes in the temperature and humidity of the boundary layer air) simultaneously, allowing their effects to be distinguished. Changes in the behavior of a group of weather systems in which only one of the quantities varies (a partial derivative of the intensity of the weather system with respect to the desirable quantity) will allow the determination of each effect statistically.

The Advanced Very High Resolution Radiometer (AVHRR) instruments onboard the series of National Oceanic and Atmospheric Administration (NOAA) satellites offer the longest available meteorological data records from space. These satellites have drifted in orbit resulting in shifts in the local time sampling during the life span of the sensors onboard. Depending upon the amplitude of the diurnal cycle of the geophysical parameters derived, orbital drift may cause spurious trends in their time series. We investigate tropical deep convective clouds, which show pronounced diurnal cycle amplitude, to estimate an upper bound of the impact of orbital drift on their time series. We carry out a rotated empirical orthogonal function analysis (REOF) and show that the REOFs are useful in delineating orbital drift signal and, more importantly, in subtracting this signal in the time series of convective cloud amount. These results will help facilitate the derivation of homogenized data series of cloud amount from NOAA satellite sensors and ultimately analyzing trends from them. However, we suggest detailed comparison of various methods and rigorous testing thereof applying final orbital drift corrections.

A process-oriented climate model evaluation is presented, applying the International Satellite Cloud Climatology Project (ISCCP) simulator to pinpoint deficiencies related to the cloud processes in the ECHAM5general circulation model.ALagrangian trajectory analysis is performed to track the transitions of anvil cirrus originating from deep convective detrainment to cirrostratus and thin cirrus, comparing ISCCP observations and the ECHAM5 model. Trajectories of cloudy air parcels originating from deep convection are computed for both, the ISCCP observations and the model, over which the ISCCP joint histograms are used for analyzing the cirrus life cycle over 5 days. The cirrostratus and cirrus clouds originate from detrainment from deep convection decay and gradually thin out after the convective event over 3–4 days. The effect of the convection–cirrus transitions in a warmer climate is analyzed in order to understand the climate feedbacks due to deep convective cloud transitions. An idealized climate change simulation is performed using a+2-K sea surface temperature (SST) perturbation. The Lagrangian trajectory analysis over perturbed climate suggests that more and thicker cirrostratus and cirrus clouds occur in the warmer climate compared to the present-day climate. Stronger convection is noticed in the perturbed climate, which leads to an increased precipitation, especially on day -2 and -3 after the individual convective events. The shortwave and the longwave cloud forcings both increase in the warmer climate, with an increase of net cloud radiative forcing (NCRF), leading to an overall positive feedback of the increased cirrostratus and cirrus clouds from a Lagrangian transition perspective.

In this study, we employ the global aerosol-climate model ECHAM-HAM to globally assess aerosol indirect effects (AIEs) resulting from shipping emissions of aerosols and aerosol precursor gases. We implement shipping emissions of sulphur dioxide (SO2), black carbon (BC) and particulate organic matter (POM) for the year 2000 into the model and quantify the model’s sensitivity towards uncertainties associated with the emission parameterisation as well as with the shipping emissions themselves. Sensitivity experiments are designed to investigate (i) the uncertainty in the size distribution of emitted particles, (ii) the uncertainty associated with the total amount of emissions, and (iii) the impact of reducing carbonaceous emissions from ships. We use the results from one sensitivity experiment for a detailed discussion of shipping-induced changes in the global aerosol system as well as the resulting impact on cloud properties. From all sensitivity experiments, we find AIEs from shipping emissions to range from −0.32±0.01Wm−2 to −0.07±0.01Wm−2 (global mean value and inter-annual variability as a standard deviation). The magnitude of the AIEs depends much more on the assumed emission size distribution and subsequent aerosol microphysical interactions than on the magnitude of the emissions themselves. It is important to note that although the strongest estimate of AIEs from shipping emissions in this study is relatively large, still much larger estimates have been reported in the literature before on the basis of modelling studies. We find that omitting just carbonaceous particle emissions from ships favours new particle formation in the boundary layer. These newly formed particles contribute just about as much to the CCN budget as the carbonaceous particles would, leaving the globally averaged AIEs nearly unaltered compared to a simulation including carbonaceous particle emissions from ships.

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