Coherent Light-Matter Coupling and Nonequilibrium Carrier Dynamics in Single-Chirality Carbon Nanotubes

dc.contributor.advisorKono, Junichiroen_US
dc.creatorCong, Kankanen_US
dc.date.accessioned2019-05-17T13:51:15Zen_US
dc.date.available2019-05-17T13:51:15Zen_US
dc.date.created2018-05en_US
dc.date.issued2018-03-02en_US
dc.date.submittedMay 2018en_US
dc.date.updated2019-05-17T13:51:16Zen_US
dc.description.abstractSingle-wall carbon nanotubes (SWCNTs) are unique one-dimensional (1D) condensed matter systems in which strongly enhanced Coulomb interactions are combined with unusual band structure. There are metallic and semiconducting SWCNTs, in both of which electron-electron interactions have significant impact on their electronic and optical properties. In this dissertation work, we used ultrafast optical pump-probe spectroscopy to investigate nonequilibrium dynamics of photogenerated electron-hole pairs, or excitons, in a sample in which a particular species, or chirality, of semiconducting SWCNTs was enriched. Specifically, we studied both an aqueous suspension and an aligned film of (6,5) SWCNTs. Depending on the pump photon energy, intensity, and polarization, different physical processes ensue after ultrafast pumping, including coherent light-matter interactions and incoherent relaxation of carriers/excitons. For example, under below-gap pumping, a transient blueshift of the exciton peak occurred, only during the pump pulse duration, a hallmark of the optical Stark effect. Under resonant pumping, transient splitting of the exciton peak was observed within the pulse duration, which is a manifestation of the Rabi doublet due to coherent light-matter interaction in the strong coupling regime. The Rabi doublet was observed only under resonant or near-resonant pumping conditions. In the case of a macroscopically aligned (6,5) SWCNT film sample, an anisotropic Rabi doublet of the exciton peak was observed under resonant pumping. In the case of above-gap excitation, incoherent relaxation processes dominated the dynamics of excitons. Analysis of these ultrafast, nonequilibrium, and strongly driven phenomena provided considerable new insight into the states and dynamics of electrons in the presence of extreme quantum confinement and strong many-body interactions.en_US
dc.format.mimetypeapplication/pdfen_US
dc.identifier.citationCong, Kankan. "Coherent Light-Matter Coupling and Nonequilibrium Carrier Dynamics in Single-Chirality Carbon Nanotubes." (2018) Diss., Rice University. <a href="https://hdl.handle.net/1911/105639">https://hdl.handle.net/1911/105639</a>.en_US
dc.identifier.urihttps://hdl.handle.net/1911/105639en_US
dc.language.isoengen_US
dc.rightsCopyright is held by the author, unless otherwise indicated. Permission to reuse, publish, or reproduce the work beyond the bounds of fair use or other exemptions to copyright law must be obtained from the copyright holder.en_US
dc.subjectUltrafast optical spectroscopyen_US
dc.subjectCarbon nanotubesen_US
dc.titleCoherent Light-Matter Coupling and Nonequilibrium Carrier Dynamics in Single-Chirality Carbon Nanotubesen_US
dc.typeThesisen_US
dc.type.materialTexten_US
thesis.degree.departmentApplied Physicsen_US
thesis.degree.disciplineNatural Sciencesen_US
thesis.degree.grantorRice Universityen_US
thesis.degree.levelDoctoralen_US
thesis.degree.majorApplied Physics/Electrical Engen_US
thesis.degree.nameDoctor of Philosophyen_US
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