Author ORCID Identifier

https://orcid.org/0009-0009-7548-7611

Semester

Summer

Date of Graduation

2025

Document Type

Dissertation

Degree Type

PhD

College

Eberly College of Arts and Sciences

Department

Chemistry

Committee Chair

Mark Tinsley

Committee Co-Chair

Kenneth Showalter

Committee Member

Terry Gullion

Committee Member

Fabien Goulay

Committee Member

Adam Halasz

Abstract

Cell-like model chemical systems are powerful tools that can be used to explore the role of intercellular coupling on population level behaviors in communities of biological cells. Firstly, we present a new method for fabricating such micro-reactors using the photosensitive Belousov–Zhabotinsky (BZ) reaction system employed in silica microparticles. These BZ micro-reactors have a tunable response to photochemical coupling, varying from a fully excitatory response to a fully inhibitory response. Their response can be tuned through variations in either the reactive mixture or, on an individual micro-reactor level, by changes in the synthesis temperature used during the fabrication of the silica micro-reactors. We observe fully inhibitory behavior for micro-reactors synthesized at 22 °C and fully excitatory behavior for micro-reactors synthesized at temperatures ≥ 40 °C. A five-variable photosensitive Oregonator model is used to explore the physicochemical properties of the microparticles that lead to their tunable behavior.

We then investigate collective behaviors associated with coupling inhibitory and excitatory micro-reactor networks using light. In this work we utilize the inhibitory properties of MOs synthesized at 22 °C and excitatory properties of MOs synthesized at 40 °C. Bi-stable synchronization and cluster states are observed with small networks consisting of two and three globally coupled oscillator networks. The dimensionless three-variable Zhabotinsky-Buchholtz-Kiyatin-Epstein (ZBKE) model of the BZ chemical system is used in simulations.

Finally, we investigate the effect of temperature on the photochemistry of the BZ reaction. We demonstrate a change in the phase response as the BZ reaction temperature is increased. For BZ mixtures which show excitatory and mixed behavior at 0 °C, a change to close to inhibitory behavior is observed when the BZ reaction temperature is changed to 20 °C.

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