Author ORCID Identifier

https://orcid.org/0000-0002-5485-4496

Date of Award

2026

Document Type

Thesis (Ph.D.)

Department or Program

Chemistry

First Advisor

Wenlin Zhang

Abstract

Predicting the emergence of molecular assembly in solution requires bridging phenomena that span significant time and length scales. The non-covalent interactions that govern these processes require an atomistic level of understanding, yet predicting the resulting macroscale structure requires careful extrapolation across scales. In this dissertation, I utilize computational methods to understand the assembly of the eco-corona that envelopes micro- and nanoplastics in the environment, and model the assembly of polypseudorotaxane and polyrotaxane hydrogels that are utilized in three-dimensional (3D) printing.

Through the use of all-atom (AA) molecular dynamics (MD) simulations and advanced sampling methods, I identify the driving force governing surface adsorption at the polymer-water interface and quantify the thermodynamics of host-guest complex formation. By incorporating the reaction rates associated with host-guest formation, I develop a framework for predicting the kinetics of polypseudorotaxane self-assembly. I then employ coarse-grained (CG) simulations to predict the morphology and material properties of polyrotaxane hydrogels, elucidating the mechanism responsible for their observed softening after printing and explaining why covalently crosslinked hydrogels exhibit self-strengthening following uniaxial training.

This dissertation reports my work on applying microscopic insights that connect molecular interactions to emergent structure and material properties. I present key insights into the driving forces of self-assembly and propose future research directions that can guide the rational design of functional materials and understand their environmental fate.

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Available for download on Friday, August 11, 2028

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