Persistent Link:
http://hdl.handle.net/10150/265338
Title:
Photophysics of C60 Colloids
Author:
Clements, Andrew Franklin
Issue Date:
2012
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:
The goal of this dissertation is to study the photophysics of suspensions of colloidal C₆₀ particles to determine if their nonlinear optical (NLO) response is superior in any way to benchmark NLO materials such as molecular solutions of C₆₀ and carbon black suspensions (CBS). C₆₀ in molecular form is known to exhibit strong reverse saturable absorption (RSA) and it is posited that colloidal particles composed of many C₆₀ molecules would maintain some degree of RSA behavior upon association, although some quenching is to be expected. CBS is known to have an NLO response that is dominated by nonlinear scattering resulting from a phase change due to heating of the carbon black particles by absorbed energy. Colloidal C₆₀ particles that are many nanometers in diameter are similar to CBS, so it is posited that they would also have a nonlinear scattering mechanism contributing to their NLO response. Three samples of C₆₀ colloids are characterized by several techniques, along with two carbon black suspensions and one molecular solution of C₆₀. Transmission electron microscopy is used to determine morphology. Femtosecond pump-probe spectroscopy is used to determine the absorption spectrum and the relaxation kinetics of the first excited singlet state. Nanosecond laser flash photolysis is used to determine the absorption spectrum and the relaxation kinetics of the first excited triplet state. Z-scan is used to determine triplet-triplet absorption cross-sections. An experiment is performed to determine the percentage of the input energy that is transmitted, scattered, or absorbed by each sample. Computer modeling is performed to compare the experimental results to theory. Results show that all materials that exhibit nonlinear scattering have a constant extinction coefficient in the nonlinear regime, implying a characteristic size for the scattering centers that is independent of input energy. Quenching processes in C₆₀ colloids are found to be morphology dependent, with more crystalline structures resulting in stronger quenching and less RSA. C₆₀ colloids with stronger RSA are found to result in less nonlinear scattering than strongly quenched colloids. Highly crystalline C₆₀ colloids were shown to have a stronger NLO response than the benchmark materials at medium to high energies.
Type:
text; Electronic Dissertation
Keywords:
nonlinear scattering; reverse saturable absorption; total scattering; Optical Sciences; Buckminsterfullerene; C₆₀
Degree Name:
Ph.D.
Degree Level:
doctoral
Degree Program:
Graduate College; Optical Sciences
Degree Grantor:
University of Arizona
Advisor:
Kost, Alan

Full metadata record

DC FieldValue Language
dc.language.isoenen_US
dc.titlePhotophysics of C60 Colloidsen_US
dc.creatorClements, Andrew Franklinen_US
dc.contributor.authorClements, Andrew Franklinen_US
dc.date.issued2012-
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.abstractThe goal of this dissertation is to study the photophysics of suspensions of colloidal C₆₀ particles to determine if their nonlinear optical (NLO) response is superior in any way to benchmark NLO materials such as molecular solutions of C₆₀ and carbon black suspensions (CBS). C₆₀ in molecular form is known to exhibit strong reverse saturable absorption (RSA) and it is posited that colloidal particles composed of many C₆₀ molecules would maintain some degree of RSA behavior upon association, although some quenching is to be expected. CBS is known to have an NLO response that is dominated by nonlinear scattering resulting from a phase change due to heating of the carbon black particles by absorbed energy. Colloidal C₆₀ particles that are many nanometers in diameter are similar to CBS, so it is posited that they would also have a nonlinear scattering mechanism contributing to their NLO response. Three samples of C₆₀ colloids are characterized by several techniques, along with two carbon black suspensions and one molecular solution of C₆₀. Transmission electron microscopy is used to determine morphology. Femtosecond pump-probe spectroscopy is used to determine the absorption spectrum and the relaxation kinetics of the first excited singlet state. Nanosecond laser flash photolysis is used to determine the absorption spectrum and the relaxation kinetics of the first excited triplet state. Z-scan is used to determine triplet-triplet absorption cross-sections. An experiment is performed to determine the percentage of the input energy that is transmitted, scattered, or absorbed by each sample. Computer modeling is performed to compare the experimental results to theory. Results show that all materials that exhibit nonlinear scattering have a constant extinction coefficient in the nonlinear regime, implying a characteristic size for the scattering centers that is independent of input energy. Quenching processes in C₆₀ colloids are found to be morphology dependent, with more crystalline structures resulting in stronger quenching and less RSA. C₆₀ colloids with stronger RSA are found to result in less nonlinear scattering than strongly quenched colloids. Highly crystalline C₆₀ colloids were shown to have a stronger NLO response than the benchmark materials at medium to high energies.en_US
dc.typetexten_US
dc.typeElectronic Dissertationen_US
dc.subjectnonlinear scatteringen_US
dc.subjectreverse saturable absorptionen_US
dc.subjecttotal scatteringen_US
dc.subjectOptical Sciencesen_US
dc.subjectBuckminsterfullereneen_US
dc.subjectC₆₀en_US
thesis.degree.namePh.D.en_US
thesis.degree.leveldoctoralen_US
thesis.degree.disciplineGraduate Collegeen_US
thesis.degree.disciplineOptical Sciencesen_US
thesis.degree.grantorUniversity of Arizonaen_US
dc.contributor.advisorKost, Alanen_US
dc.contributor.committeememberDereniak, Eustaceen_US
dc.contributor.committeememberChipman, Russellen_US
dc.contributor.committeememberKost, Alanen_US
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