Atom-Based Computer Simulation Studies of Gas-to-Liquid Nucleation in Atmospherically Relevant Systems: Clarifying Discrepancies and Elucidating Mechanisms

For over a century, nucleation for all systems was thought simplistically to be a process that advances through the formation of critical clusters with a well-defined composition. Our results show intriguing nucleation mechanisms that challenge the aforementioned notion. We employed the simple TraPPE-UA (transferable potential for phase equilibria – united atom) force field and the AVUS-HR approach (a combination of aggregation-volume-bias Monte Carlo, umbrella sampling, and histogram reweighting), to investigate the homogeneous vapor-to-liquid nucleation of various nucleating systems. We found out that these systems could nucleate through a variety of unique non-ideal mechanisms. Alongside existing experimental investigations, this dissertation presents pioneering works on the computer simulation of nucleation in multicomponent systems. Our results are very relevant to atmospheric aerosol formations but may also find its applications in drug encapsulations and the design of nanomaterials as well as in sorting out experimental and theoretical discrepancies. This dissertation outlines the results of a series of nucleation investigations involving unary, binary, and ternary nucleating systems. Introductory and background information regarding nucleation, computer simulations, the classical nucleation theory and the AVUS – HR approach are provided in Chapters 1 and 2. The major findings of this work are given in Chapters 3, 4, 5, and 6. They are presented here in order of increasing complexity. Chapter 3 is on unary nucleation of 1-pentanol. Chapter 4 is on the investigation of the n-Nonane/1-Alcohol binary series. Finally, our pioneering works on the various ternary nucleation studies are discussed in Chapters 5 and 6.

Name thesis:degree_name

Doctor of Philosophy (PhD)

Level thesis:degree_level

Dissertation

Discipline thesis:degree_discipline

Chemistry

Grantor

Chemistry

Year dc:date.available

2009

Author dc:creator

• Nellas, Ricky Bendanillo

• umbrella sampling
• histogram reweighting
• CNT
• nonane
• 1-alcohol
• water
• Mars
• 4D
• ternary nucleation
• binary nucleation
• AVUS-HR
• Monte Carlo
• avbmc

Statement dc:rights

• withheld
• Secure the entire work for patent and/or proprietary purposes for a period of one year. Student has submitted appropriate documentation which states: During this period the copyright owner also agrees not to exercise her/his ownership rights, including public use in works, without prior authorization from LSU. At the end of the one year period, either we or LSU may request an automatic extension for one additional year. At the end of the one year secure period (or its extension, if such is requested), the work will be released for access worldwide.

Identifier

etd-01122010-163908
https://repository.lsu.edu/gradschool_dissertations/930

OAI identifier oai:identifier

oai:repository.lsu.edu:gradschool_dissertations-1929