Clever, Caleb
(2024)
Charge and Spin Transport in Organic Systems:
From Molecules to Materials.
Doctoral Dissertation, University of Pittsburgh.
(Unpublished)
This is the latest version of this item.
Abstract
The nature of charge transport and the interplay between spin and chirality, manifested by the chiral induced spin selectivity (CISS) effect, are of prime importance to deepen our understanding of biochemical redox processes, as well as facilitate progress in fields such as spintronics and enantioseparation. In this dissertation, fundamental factors affecting charge and spin transport through biomolecules are investigated. The first study examines the pathways of charge transport through nucleic acids. It is determined that the electron transport occurs primarily through the base pair stack as opposed to the backbone. In the second study, we examine the transport of electrons through nucleic acids with a peptide backbone (PNA). The high conductivity of the basepair sequence GnCn indicates a coherent transport mechanism, and differences in conductance between DNA and PNA are seen to arise from differences in cross-strand electronic coupling between the GnCn segments. In the third study, an examination of the chiral induced spin selectivity (CISS) effect on small biomolecules are presented. A strong emphasis is also placed on establishing a robust terminology which can facilitate meaningful comparisons across experimental techniques. The fourth study presents preliminary data aimed at assessing the impact of spin control on different reaction mechanisms for the hydrogen evolution reaction, as determined by the choice of catalyst. The findings of these studies serve to advance the understanding of electron transport pathways and will aid in future studies of the interplay between charge, spin, and chirality.
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Details
| Item Type: |
University of Pittsburgh ETD
|
| Status: |
Unpublished |
| Creators/Authors: |
|
| ETD Committee: |
|
| Date: |
8 January 2024 |
| Date Type: |
Publication |
| Defense Date: |
10 August 2023 |
| Approval Date: |
8 January 2024 |
| Submission Date: |
26 June 2023 |
| Access Restriction: |
No restriction; Release the ETD for access worldwide immediately. |
| Number of Pages: |
206 |
| Institution: |
University of Pittsburgh |
| Schools and Programs: |
Dietrich School of Arts and Sciences > Chemistry |
| Degree: |
PhD - Doctor of Philosophy |
| Thesis Type: |
Doctoral Dissertation |
| Refereed: |
Yes |
| Uncontrolled Keywords: |
CISS, chiral induced spin selectivity, single molecule conductance, STM-BJ, peptide nucleic acid (PNA), Hall effect |
| Date Deposited: |
08 Jan 2024 17:41 |
| Last Modified: |
08 Jan 2024 17:41 |
| URI: |
http://d-scholarship.pitt.edu/id/eprint/45361 |
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Charge and Spin Transport in Organic Systems:
From Molecules to Materials. (deposited 08 Jan 2024 17:41)
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