Effect of Confinement and Heterogeneity on Phase Behavior: A Density Functional Approach

Persistent Link:
http://hdl.handle.net/10150/196124
Title:
Effect of Confinement and Heterogeneity on Phase Behavior: A Density Functional Approach
Author:
Husowitz, Barry Charles
Issue Date:
2007
Publisher:
The University of Arizona.
Rights:
Copyright © is held by the author. Digital access to this material is made possible by the University Libraries, University of Arizona. Further transmission, reproduction or presentation (such as public display or performance) of protected items is prohibited except with permission of the author.
Abstract:
Density functional theory of statistical mechanics in a square gradient approximation was used to study nucleation in confined systems such as a cylindrical pore and in-between two cylindrical disks. This approximation was further applied to study the evaporation and condensation in nanopores with finite lengths. Confinement effects induced nucleation phenomena that are not observed in more open systems. Density functional theory was also used to explore the solvation properties of a spherical solute immersed in a supercritical diatomic fluid. The solute was modeled as a hard core Yukawa particle surrounded by a diatomic Lennard-Jones fluid represented by two fused tangent spheres using an interaction site approximation. The results of this study indicate that local density augmentation and the solvation free energies are particularly sensitive to changes in solute and solvent particle geometry and solute/solvent anisotropic interactions. Density functional theory allowed us to systematically study the effect of a variety of geometric and interaction parameters on the properties and behavior of all the systems. Although more sophisticated, but computationally more demanding, theoretical approaches can be used, our results provide fundamental physical insights into the behavior of real systems and create a solid basis for the development of more realistic models.
Type:
text; Electronic Dissertation
Keywords:
DFT; Nucleation; Statistical Mechanics
Degree Name:
Ph.D.
Degree Level:
doctoral
Degree Program:
Chemistry; Graduate College
Degree Grantor:
University of Arizona
Advisor:
Talanquer, Vicente A.
Committee Chair:
Talanquer, Vicente A.

Full metadata record

DC FieldValue Language
dc.language.isoenen_US
dc.titleEffect of Confinement and Heterogeneity on Phase Behavior: A Density Functional Approachen_US
dc.creatorHusowitz, Barry Charlesen_US
dc.contributor.authorHusowitz, Barry Charlesen_US
dc.date.issued2007en_US
dc.publisherThe University of Arizona.en_US
dc.rightsCopyright © is held by the author. Digital access to this material is made possible by the University Libraries, University of Arizona. Further transmission, reproduction or presentation (such as public display or performance) of protected items is prohibited except with permission of the author.en_US
dc.description.abstractDensity functional theory of statistical mechanics in a square gradient approximation was used to study nucleation in confined systems such as a cylindrical pore and in-between two cylindrical disks. This approximation was further applied to study the evaporation and condensation in nanopores with finite lengths. Confinement effects induced nucleation phenomena that are not observed in more open systems. Density functional theory was also used to explore the solvation properties of a spherical solute immersed in a supercritical diatomic fluid. The solute was modeled as a hard core Yukawa particle surrounded by a diatomic Lennard-Jones fluid represented by two fused tangent spheres using an interaction site approximation. The results of this study indicate that local density augmentation and the solvation free energies are particularly sensitive to changes in solute and solvent particle geometry and solute/solvent anisotropic interactions. Density functional theory allowed us to systematically study the effect of a variety of geometric and interaction parameters on the properties and behavior of all the systems. Although more sophisticated, but computationally more demanding, theoretical approaches can be used, our results provide fundamental physical insights into the behavior of real systems and create a solid basis for the development of more realistic models.en_US
dc.typetexten_US
dc.typeElectronic Dissertationen_US
dc.subjectDFTen_US
dc.subjectNucleationen_US
dc.subjectStatistical Mechanicsen_US
thesis.degree.namePh.D.en_US
thesis.degree.leveldoctoralen_US
thesis.degree.disciplineChemistryen_US
thesis.degree.disciplineGraduate Collegeen_US
thesis.degree.grantorUniversity of Arizonaen_US
dc.contributor.advisorTalanquer, Vicente A.en_US
dc.contributor.chairTalanquer, Vicente A.en_US
dc.contributor.committeememberSalzman, W. Ronen_US
dc.contributor.committeememberSanov, Andreien_US
dc.contributor.committeememberArmstrong, Neal R.en_US
dc.contributor.committeememberPemberton, Jeanne E.en_US
dc.identifier.proquest2087en_US
dc.identifier.oclc659747292en_US
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