Date of Award

Fall 12-2022

Degree Type

Dissertation

Degree Name

Doctor of Philosophy (PhD)

School

Polymer Science and Engineering

Committee Chair

Dr. Jason D. Azoulay

Committee Chair School

Polymer Science and Engineering

Committee Member 2

Dr. Sergei I. Nazarenko

Committee Member 2 School

Polymer Science and Engineering

Committee Member 3

Dr. Derek L. Patton

Committee Member 3 School

Polymer Science and Engineering

Committee Member 4

Dr. Jeffrey S. Wiggins

Committee Member 4 School

Polymer Science and Engineering

Committee Member 5

Dr. Xiaodan Gu

Abstract

Donor-acceptor (DA) conjugated polymer (CPs) represent the forefront of research for achieving new and improved functionality and capability within current and next-generation (opto)electronic devices. Critical features include narrow bandgaps, open-shell (diradical) properties, and a narrow singlet-triplet energy gap collectively giving rise to rich features. These features have historically been exclusive to metals and enable their use in semiconducting applications, infrared (IR) photodetection, and quantum computing. However, the complex structural and electronic heterogeneities that define these materials also complicate control over the electronic structure. Compounding this, the results of computational studies that explicitly focus on DA CPs are only emerging and have not yet established clear guidelines for appropriately modeling these polymers. Despite advancements of recent, connections that link topology, exchange interactions, and functionality are nascent and incomplete. There remains a fundamental necessity for uncovering essential parameters that influence open-shell properties and performance. To this end, we developed a DA CP framework that allows facile tuning of the chemical structure of the monomer. These efforts enable atomistic-level modifications that can be used in isolation or in concert to exercise fine control over the electronic structure, the diradical properties, singlet-triplet energy gap, and electronic quantum phenomena and facilitate comparisons at the computational theoretical level.

ORCID ID

0000-0002-9041-6506

Available for download on Wednesday, January 01, 2070

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