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Charge carrier dynamics of 2-dimensional photoelectrodes probed via ultrafast spectroelectrochemistry

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dc.contributor.authorAustin, Rachelle, author
dc.contributor.authorSambur, Justin, advisor
dc.contributor.authorKrummel, Amber, advisor
dc.contributor.authorRappe, Anthony, committee member
dc.contributor.authorPrieto, Amy, committee member
dc.contributor.authorMcNally, Andrew, committee member
dc.contributor.authorBrewer, Samuel, committee member
dc.date.accessioned2024-09-09T20:52:03Z
dc.date.available2025-08-16
dc.date.issued2024
dc.description.abstractThe integration of hot charge carrier-based energy conversion systems with two-dimensional (2D) semiconductors holds immense promise for enhancing the efficiency of solar energy technologies and enabling novel photochemical reactions. Current approaches, however, often rely on costly multijunction architectures. In this dissertation, I present research that combines spectroelectrochemical and in-operando transient absorption spectroscopy measurements to unveil ultrafast (<50 fs) hot exciton and free charge carrier extraction in a proof-of-concept photoelectrochemical solar cell constructed from earth-abundant monolayer (ML) MoS2. Theoretical analyses of exciton states reveal enhanced electronic coupling between hot exciton states and neighboring contacts, facilitating rapid charge transfer. Additionally, I discuss insights into the physical interpretation of transient absorption (TA) spectroscopy data in 2D semiconductors, comparing historical perspectives from physical chemistry and solid-state physics literature. My perspective encompasses various physical explanations for spectral features and experimental trends, particularly focusing on the contribution of trions to TA spectra. Furthermore, I examine how different physical interpretations and data analysis procedures can yield distinct timescales and mechanisms from the same experimental results, providing a comprehensive framework for understanding charge carrier dynamics in 2D semiconductor-based optoelectronic devices.
dc.format.mediumborn digital
dc.format.mediumdoctoral dissertations
dc.identifierAustin_colostate_0053A_18399.pdf
dc.identifier.urihttps://hdl.handle.net/10217/239210
dc.languageEnglish
dc.language.isoeng
dc.publisherColorado State University. Libraries
dc.relation.ispartof2020-
dc.rightsCopyright and other restrictions may apply. User is responsible for compliance with all applicable laws. For information about copyright law, please see https://libguides.colostate.edu/copyright.
dc.rights.accessEmbargo expires: 08/16/2025.
dc.subjectelectrochemistry
dc.subjectspectroelectrochemistry
dc.subjectultrafast spectroscopy
dc.subjectsolar
dc.subject2-dimensional materials
dc.subjectspectroscopy
dc.titleCharge carrier dynamics of 2-dimensional photoelectrodes probed via ultrafast spectroelectrochemistry
dc.typeText
dcterms.embargo.expires2025-08-16
dcterms.embargo.terms2025-08-16
dcterms.rights.dplaThis Item is protected by copyright and/or related rights (https://rightsstatements.org/vocab/InC/1.0/). You are free to use this Item in any way that is permitted by the copyright and related rights legislation that applies to your use. For other uses you need to obtain permission from the rights-holder(s).
thesis.degree.disciplineChemistry
thesis.degree.grantorColorado State University
thesis.degree.levelDoctoral
thesis.degree.nameDoctor of Philosophy (Ph.D.)

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