Advances in Carbon Nanotechnology: Non-Equilibrium Graphene Synthesis and the Control of Cell Signaling with Molecular Machines

dc.contributor.advisorTour, James
dc.contributor.advisorPasquali, Matteo
dc.creatorBeckham, Jacob Lee
dc.date.accessioned2023-09-01T19:40:10Z
dc.date.available2023-09-01T19:40:10Z
dc.date.created2023-08
dc.date.issued2023-08-11
dc.date.submittedAugust 2023
dc.date.updated2023-09-01T19:40:11Z
dc.description.abstractCarbon, known as the "element of life," has long fascinated researchers due to its exceptional versatility as a molecular building block. With its ability to form a wide range of molecular structures and exhibit diverse bonding configurations, carbon has become the cornerstone of countless organic compounds. In recent years, this inherent versatility has taken on a new dimension with the emergence of carbon nanomaterials, including carbon nanotubes, graphene, and, indeed, even buckminsterfullerenes. These materials hold immense promise for the advancement of both science and industry. This thesis presents several major advances in the field of carbon nanotechnology. First, various investigations of non-equilibrium graphene synthesis techniques are discussed. Second, the use of carbon-based molecular nanomotors to control cell signaling is explored. In the first several chapters, explorations using different non-equilibrium synthesis techniques to generate graphene are presented. Chapter 1 explores the conversion of positive photoresist into laser-induced graphene, demonstrating that a combination of lasing and photolithography allows the patterning of graphene at high resolution. Chapter 2 presents machine learning models trained to predict the extent of crystallization in beds of amorphous carbon treated with an electrothermal discharge. This work comprised a major thrust in our lab’s research program on flash Joule heating and revealed several key factors for the design of Joule heating reactors. This work also presented software programs capable of learning to synthesize graphene from scrap rubber tires with no human oversight using Bayesian meta-learning. Chapter 3 represents a pivot in my PhD where I began exploring the biomedical applications of carbon nanomaterials. In the Tour lab, we explore the use of carbon-based molecular motors for various applications in biology. These molecular motors convert incident photons into mechanical work through a series of photochemical and thermal steps. Our previous work has shown that the actuation of fast molecular motors causes the permeabilization of lipid bilayers. Chapter 3 is a perspective discussing the potential applications of these motors, laying out foundational standards for the literature. This chapter discusses how to differentiate the light-driven effects of molecular actuation and potential confounding factors, including photothermal and photodynamic effects. Chapter 4 then demonstrates the use of these molecular motors for the treatment of fungal infections. This work involved extensive microscopy and fundamental studies showing how our motors are processed by eukaryotes, and what that might imply for their basic mechanism-of-action. Chapter 5 explores the use of these molecular motors to control cell signaling. When they are mechanically perturbed, cells participate in mechanosensitive signaling phenomena known as intercellular calcium waves. Thirty years ago, cell biologists used to study calcium waves initiated by poking cells with a micropipette. My work showed that the same responses could be achieved using a fast, unidirectional molecular motor. This work represents the first demonstration that a cell signaling cascade could be initiated by the mechanical force administered by a small molecule, opening the door for the design of new drugs that work based on mechanical, rather than chemical, forces. Chapter 6 explores the dependence of motor performance on the functionalization chemistry used in the motor. Our findings indicate that surface charge and polarity are critical factors that drive motor effectiveness for killing bacteria, killing fungi, and initiating calcium waves. We found substantial overlap in motor performance across all three tasks. Finally, Chapter 7 explores the use of molecular motors to control endocrine signaling. This chapter shows that light-activated motors can potentiate the release of insulin from pancreatic beta cells through the modulation of intracellular calcium, a finding with substantial implications for the design of new drugs to treat diabetes.
dc.format.mimetypeapplication/pdf
dc.identifier.citationBeckham, Jacob Lee. "Advances in Carbon Nanotechnology: Non-Equilibrium Graphene Synthesis and the Control of Cell Signaling with Molecular Machines." (2023) Diss., Rice University. https://hdl.handle.net/1911/115236.
dc.identifier.urihttps://hdl.handle.net/1911/115236
dc.language.isoeng
dc.rightsCopyright is held by the author, unless otherwise indicated. Permission to reuse, publish, or reproduce the work beyond the bounds of fair use or other exemptions to copyright law must be obtained from the copyright holder.
dc.subjectCarbon nanotechnology
dc.subjectmachine learning
dc.subjectmolecular machines
dc.subjectmotors
dc.subjectcalcium waves
dc.titleAdvances in Carbon Nanotechnology: Non-Equilibrium Graphene Synthesis and the Control of Cell Signaling with Molecular Machines
dc.typeThesis
dc.type.materialText
thesis.degree.departmentChemistry
thesis.degree.disciplineNatural Sciences
thesis.degree.grantorRice University
thesis.degree.levelDoctoral
thesis.degree.nameDoctor of Philosophy
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