Nanoscale Structures for Synthetic Implementations of Biologically-Inspired Transport
PublicThis thesis describes the relationships between nanoscale structure and particle transport in two systems: i) the transport and conversion of excitons in colloidal quantum dot (QD) assemblies and ii) the transport of carriers in flashing electron ratchets. One major crux in the creation of efficient photocatalytic systems is the low photon flux of sunlight, where the absorption of light and transport of the photochemical potential to the catalytic centers is the rate-limiting step. Natural photosynthetic systems overcome the limitations of photon flux through energy transfer, which enables spatial migration of excitons to the catalytic centers. However, energy-transfer based photosensitization schemes have not been previously explored in photocatalytic systems. Quantum dots (QDs) are proven to be viable photocatalysts, and the usage of QDs in photocatalysis is advantageous due to their easily tunable optoelectronic properties and surface chemistry. This research experimentally realizes and computationally models the spatial control of excitons within QD assemblies for enhancing the efficiency of photocatalytic reactions—proving the viability of energy-transfer based sensitization in photocatalytic systems. Molecular motors utilize asymmetry to obtain directional transport of particles from non-directional chemical energy in noisy, damped environments through a mechanism called “ratcheting”. This research examines the ratcheting of carriers in the noisy, damped environment of a poly(3-hexyl-thiophene-2,5-diyl) (P3HT) transport layer in relation to the microscopic properties of the transport layer and electric potential.
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Kodaimati_northwestern_0163D_14764.pdf | 2020-02-12 | Public |
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