Thesis. 1977. M.S.--Massachusetts Institute of Technology. Dept. of Meteorology. / Microfiche copy available in Archives and Science. / Bibliography : leaves 99-101. / M.S.

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<div> <div> <div> <p>The mid-Miocene Climatic Optimum (MMCO), 17-14.50 million years ago, is studied using general circulation models (GCMs). This period of time is characterized by enhanced warming in the deep ocean and in the mid-to-high latitudes. Previous GCMs fail to accurately represent the warmer climate of the MMCO, providing evidence that other warming feedbacks are missing in the models. This study focuses on cloud feedbacks by modifying the Community Earth System Model (CESM 1.0) to explore the MMCO climate. We implement modifications in pre-industrial (284.7 ppm CO2) and modern slab ocean cases (367.0 ppm CO2, 400 ppm CO2, and 800 ppm CO2). One modified case showing the most potential implements an aerosol de- pendent ice nucleation mechanism and a theory based cloud phase separation. This modified case allows the model predicted aerosol concentrations to interact with the cloud microphysics and provide more realistic cloud water contents. The data shows an increase in surface temperature and increase in upper atmospheric cloud fraction when compared to the control case. Preliminary results suggest that this model is able to capture the mid-to-high latitude warming trends and weaker equator to pole temperature gradient. </p> </div> </div> </div>

Atmospheric aerosols are known to exert a significant influence on the Earth's climate system; however, the magnitude of this influence is highly uncertain because of the complex interaction between aerosols and water vapor to form clouds. Toward reducing this uncertainty, this dissertation outlines a series of laboratory and in-situ field measurements, instrument technique development, and model simulations designed to characterize the ability of aerosols to act as cloud condensation nuclei (CCN) and form cloud droplets. Specifically, we empirically quantify the mixing state and thermodynamic properties of organic aerosols (e.g., hygroscopicity and droplet condensational uptake coefficient) measured in polluted and non-polluted environments including Alaska, California, and Georgia. It is shown that organic aerosols comprise a substantial portion of the aerosol mass and are often water soluble. CCN measurements are compared to predictions from theory in order to determine the error associated with simplified composition and mixing state assumptions employed by current large-scale models, and these errors are used to constrain the uncertainty of global and regional cloud droplet number and albedo using a recently-developed cloud droplet parameterization adjoint coupled with the GMI chemical transport model. These sensitivities are important because they describe the main determinants of climate forcing. We also present two novel techniques for fast measurements of CCN concentrations with high size, supersaturation, and temporal resolution that substantially improve the state of the art by several orders of magnitude. Ultimately, this work represents a step toward better understanding how atmospheric aerosols influence cloud properties and Earth's climate.

This research focuses on aircraft observational studies of aerosol-cloud interactions in cumulus clouds. The data were collected in the summer of 2004, the spring of 2007 and the mid-winter and spring of 2008 in Texas, central Saudi Arabia and Istanbul, Turkey, respectively. A set of 24 pairs of sub-cloud aerosol and cloud penetration data are analyzed. Measurements of fine and coarse mode aerosol concentrations from 3 different instruments were combined and fitted with lognormal distributions. The fit parameters of the lognormal distributions are compared with cloud droplet effective radii retrieved from 260 cloud penetrations. Cloud condensation nuclei (CCN) measurements for a subset of 10 cases from the Istanbul region are compared with concentrations predicted from aerosol size distributions. Ammonium sulfate was assumed to represent the soluble component of aerosol with dry sizes smaller than 0.5 mm and sodium chloride for aerosol larger than 0.5 mm. The measured CCN spectrum was used to estimate the soluble fraction. The correlations of the measured CCN concentration with the predicted CCN concentration were strong (R2 > 0.89) for supersaturations of 0.2, 0.3 and 0.6%. The measured concentrations were typically consistent with an aerosol having a soluble fraction between roughly 0.5 and 1.0, suggesting a contribution of sulfate or some other similarly soluble inorganic compound. The predicted CCN were found to vary by +or-3.7% when the soluble fraction was varied by 0.1. Cumulative aerosol concentrations at cutoff dry diameters of 1.1, 0.1 and 0.06 mm were found to be correlated with cloud condensation nuclei concentrations but not with maximum cloud base droplet concentrations. It is also shown that in some cases the predominant mechanisms involved in the formation of precipitation were altered and modified by the aerosol properties. This study suggests that CCN-forced variations in cloud droplet number concentration can change the effective radius profile and the type of precipitation hydrometeors. These differences may have a major impact on the global hydrological cycle and energy budget.

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The feedbacks among aerosols, clouds, and radiation are important components for understanding Earth's climate system and quantifying human-induced climate change, yet the magnitude of these feedbacks remain highly uncertain. Since every cloud droplet in the atmosphere begins with water condensing on a pre-existing aerosol particle, characterizing the ability of aerosols to uptake water vapor and form cloud condensation nuclei (CCN) are key to understanding the microphysics behind cloud formation, as well as assess the impact aerosols have on the Earth system. Through a combination of controlled laboratory experiments and field measurements, this thesis characterizes the ability of atmospheric aerosols to uptake water vapor and become CCN at controlled levels of water vapor supersaturation. The origin of the particle water uptake, termed hygroscopicity, is also explored, being from either the presence of deliquescent soluble material and/or adsorption onto insoluble surfaces. The data collected and presented is comprehensive and includes (1) ground samples of volcanic ash, collected from six recent eruptions re-suspended in the laboratory for analysis, (2) laboratory chamber and flow-tube studies on the oxidation and uptake of surface active organic compounds, and (3) in-situ aircraft measurements of aerosols from the Arctic background, Canadian boreal forests, fresh and aged biomass burning, anthropogenic industrial pollution, and from within tropical cyclones in the Atlantic basin. Having a more thorough understanding of aerosol water uptake will enable more accurate representation of cloud droplet number concentrations in global models, which can have important implications on reducing the uncertainty of aerosol-cloud-climate interactions, as well as additional uncertainties in aerosol transport, atmospheric lifetime, and impact on storm dynamics.

The process of particle growth in a warm cloud caused by coalescence is studied. The purely probabilistic model introduced by Gillespie [J. Atmos. Sci. 29 (1972) 1496-1510j is used and solved exactly by the aid of the Monte Carlo algorithm developed by Gillespie [J. Atmos. Sci. 32 (1975) 1977-1989]. Another approach uses the kinetic coalescence equation which is solved numerically using finite difference methods. It is known that the stochastic completeness of the kinetic coalescence equation depends on the extent of correlations between particles. Our objective is to compare these two models and analyze the suitability of the kinetic coalescence equation to simulate the coalescence process using a Brownian diffusion collision kernel. The stochastic coalescence model introduced by Gillespie is discussed in detail. A description of Gillespie's Monte Carlo simulation procedure and the numerical code that implements this algorithm in Fortran are provided. This algorithm is applied to the coalescence kernel for Brownian diffusion and initial Poisson and uniform droplet size distributions. Numerical methods which can he applied to the continuous and the discrete forms of the kinetic equation are described. The discrete form of this equation is solved by using Euler's and the fourth order Runge-Kutta methods. Solutions from the two models at early and later times are examined and the effect of the number of droplets used in simulations is investigated. It is shown that solutions agree well for early and later times using large and relatively small number of droplets initially. The problem of the growth of a large particle as it settles through a monodisperse suspension of small elemental particles is considered. It is demonstrated that the solution to the stochastic equation predicts about twice the growth rate of a large particle than the kinetic model. To validate solutions obtained by the stochastic algorithm, the convergence of the solution to Poisson distribution as time increases is studied. It is shown that the normalized average concentration obtained from the initial uniform and Pois¬son distributions in the stochastic coalescence model can be approximated by the Marshall-Palmer distribution function well known in the cloud physics community. The results of numerical simulations of the coalescence process using Brownian diffusion suggest that the kinetic equation in general produces an average size spec-trum that well matches the stochastic average spectrum. However, in the case of poorly mixed suspensions when correlations between particles are more important, these two models predict different size distributions, which is expected.

<p>Urban meteorology has developed in parallel to other sub-fields in the science, but in many ways remains poorly described. In particular, the study of urban rainfall modification remains behind compared to other comparable features. Urban rainfall modification refers to the change of a precipitation feature as it crosses an urban area. Typically, this manifests as rainfall initiation, local suppression, local invigoration, and/or storm morphology changes. Research in the prior decades have shown urban rainfall modification to arise from a combination of land-atmosphere and aerosol-cloud interaction. Urban areas create a greater surface roughness, which produces local convergence and divergence, modifying local thunderstorm inflow and morphology. The land surface also generates vertical velocity perturbations which can act to initiate or modify existing convection. Urban aerosols act as CCN to perturb existing cloud and precipitation characteristics. Higher CCN narrows the cloud droplet distribution, creating more smaller cloud droplets, and initially reducing precipitation efficiency by keeping more liquid water in the cloud than what would form into rain. The CCN-cloud interaction eventually increasing heavy rainfall production as graupel riming is enhanced by the narrower cloud droplet distribution, leading to more larger raindrops and higher rain in areas.</p><p>This dissertation addresses the observation and modeling of urban thunderstorm interaction from both the land surface and aerosol perspective. It reassesses the original urban rainfall anomaly: The La Porte Anomaly. First analyzed in the late 1960s, the La Porte Anomaly was ultimately dismissed by 1980 as either a temporary, biased, or otherwise unexplainable observation, as the process level understanding had yet to be explained. The contemporary analysis utilizes all existing data and objective optimal interpolation to show that a rainfall anomaly downwind of Chicago has indeed existed at least since the 1930s. The current rainfall anomaly exists as a broad region of warm season rainfall downwind of Chicago that is 20-30% greater than the regional average. Using synoptic parameters, the rainfall anomaly is shown to be independent of wind direction and most closely associated with local land surface forcing. Weekdays, where local aerosol loading has been measured at 40% or more greater than weekends, have up to 50% more warm season rainfall than weekends. The analysis is able to show that there is a land surface and aerosol contribution to the rainfall anomaly, but cannot unambiguously separate them.</p><p>In order to separate the land surface and aerosol effects on urban rainfall distribution, a numerical model was improved to better handle urban weather interaction. The Regional Atmospheric Modeling System (RAMS 6.0) was chosen for its base land surface and cloud physics parameterization. The Town Energy Budget (TEB) urban canopy model was coupled to RAMS to handle the urban land surface. The Simple Photochemical Module (SPM) was coupled with the cloud physics to handle conversion of surface emissions to CCN. The model utilized an external traffic simulation to create a realistic diurnal and weekly cycle of surface emissions, based on human behavior. The new Urban RAMS was used to study the land surface sensitivity of city size and of aerosol loading in two studies using the Real Atmosphere Idealized Land surface (RAIL) method, by which all non-urban features of the land surface are removed to isolate the urban effects. The city size study determined that the land surface of a given city eventually has a maximum effect on thunderstorm modifying potential, and that rainfall does not continue to increase or decrease locally for cities larger than a certain size based on that storm’s own motion. The aerosol-cloud analysis corroborated previous observations on the non-linear effects of aerosol loading on clouds. It also demonstrated that understanding the aerosol effect in an urban environment requires high resolution observations of precipitation change. In a single thunderstorm, regions can be both impacted by local rainfall rate increases and decreases from urban aerosols, leading to little total change in precipitation. But the rainfall rate changes can significantly affect soil moisture and drought potential in and around urban areas.Following the idealized studies, the historical and current La Porte Anomaly was simulated to separate the land surface from the aerosol factors near the Chicago area. The Urban RAMS model was deployed on a real land surface with full model physics. Simulations with 1932, 1962, 1992, and 2012 land covers were run over an exceptionally wet Aug. 2007 to approximate the rain variability for an entire summer season. Surface emissions were also varied in the 2012 land cover for variable aerosol loading. The simulations successfully reproduced the location of the downwind rainfall anomaly in each land cover scenario: farther east toward La Porte in 1932, moving southwestward to its current location by 2012. Doubling surface emissions eliminated the downwind anomaly, as was observed during the highest pollution decade of the 1970s. Eliminating surface emissions also decreased the downwind anomaly. As the land cover at the upwind edge of Chicago became more connected from the 1932 to 2012 land cover scenarios, a local upwind rainfall anomaly developed, moving westward with urban expansion. The results of these simulations enabled the conclusions that a) at the upwind edge, the land surface dominates urban rainfall modification, b) the aerosol loading sustains and increases the locally downwind rainfall increase, and c) that the total modification distance is static on given day and given urban footprint. A more expansive city does not produce a rainfall anomaly more distantly downwind, but rather the distance of rainfall modification moves to where the upwind edge of the city begins.</p><p></p><p>The modeling work ends with a two-city simulation in the southeast United States, of a bow-echo forming near Memphis, TN and crossing Birmingham, AL before splitting. Simulations were performed on different surface emissions rates, land covers where Birmingham did not exist, and a novel approach with two inner emitting grids over both Birmingham and Memphis. A storm tracking algorithm enabled one-to-one comparisons of point simulated storm characteristics between scenarios. The results of most scenarios only corroborated previous research, showing how increased aerosol loading changes cloud and rainfall characteristics until the highest aerosol loading shuts down riming and rainfall enhancement. However, the two most accurate simulations, where the storm forms and splits over Birmingham, were a non-urban higher rural aerosol scenario and the scenario with Memphis also emitting pollution. In order to split the storm over Birmingham, the upwind cloud characteristics were primed by higher upwind aerosols, either from a realistic city upwind or unrealistically high rural aerosols. The conclusions produced by this study demonstrated the importance of aerosol cloud interaction, perhaps equal with land surface, but also the need for far upwind information for a storm in a given city. Memphis and Birmingham are separated by over 300km, far exceeding the threshold thought to connect two cities by mutual rainfall modification.</p><p>The overall conclusions of the research presented in this dissertation shows a more unified approach to the effects of urban rainfall modification. The upwind edge of a city is a fixed location, and a thunderstorm begins modifying at that point. The thunderstorm usually produces a local rainfall maximum at the upwind edge, due to the vertical velocity of the urban land surface. The urban aerosols proceed to narrow the cloud droplet distribution, locally reducing rainfall as the storm passes over the urban area. Eventually the enhanced rainfall from enhanced riming produces a maximum somewhere downwind. However, “downwind” is a location relative to the storm’s motion and could exist anywhere over the urban footprint or downwind in a rural region. The climatological location of increased rainfall is an average of every storm in a season and beyond. The results of each part of the study provide a way to continue the research presented here.</p><br>