Date of Award
Doctor of Philosophy (PhD)
Martin B. Forstner
Electroosmotic Flow, Nanomaterials, Self Assembly, Supported Lipid Bilayers
Physical Sciences and Mathematics
Materials that take advantage of the exceptional properties of nano-meter sized aggregates of atoms are poised to play an important role in future technologies. Prime examples for such nano-materials that have an extremely large surface to volume ratio and thus are physically determined by surface related effects are quantum dots (qdots) and carbon nanotubes (CNTs). The production of such manmade nano-objects has by now become routine and even commercialized. However, the controlled assembly of individual nano-sized building blocks into larger structures of higher geometric and functional complexity has proven to be much more challenging. Yet, this is exactly what is required for many applications that have transformative potential for new technologies. If the tedious procedure to sequentially position individual nano-objects is to be forgone, the assembly of such objects into larger structures needs to be implicitly encoded and many ways to bestow such self-assembly abilities onto nano objects are being developed. Yet, as overall size and complexity of such self-assembled structures increases, kinetic and geometric frustration begin to prevent the system to achieve the desired configuration. In nature, this problem is solved by relying on guided or forced variants of the self-assembly approach. To translate such concepts into the realm of man-made nano-technology, ways to dynamically manipulate nano-materials need to be devised.
Thus, in the first part of this work, I provide a proof of concept that supported lipid bilayers (SLBs) that exhibit free lateral diffusion of their constituents can be utilized as a two-dimensional platform for active nano-material manipulation. We used streptavidin coated quantum dots (Q-dots) as a model nano-building-block. Q-dots are 0-dimensional nanomaterials engineered to be fluorescent based solely on their diameter making visualization convenient. Biotinylated lipids were used to tether Q-dots to a SLB and we observed that the 2-dimensional fluidity of the bilayer was translated to the quantum dots as they freely diffused. The quantum dots were visualized using wide-field fluorescent microscopy and single particle tracking techniques were employed to analyze their dynamic behavior. Next, an electric field was applied to the system to induce electroosmotic flow (EOF) which creates a bulk flow of the buffer solution. The quantum dots were again tracked and ballistic motion was observed in the particle tracks due to the electroosmosis in the system. This proved that SLBs could be used as a two-dimensional fluid platform for nanomaterials and electroosmosis can be used to manipulate the motion of the Q-dots once they are tethered to the membrane.
Next, we set out to employ the same technique to carbon nanotubes (CNTs), which are known for their highly versatile mechanical and electrical properties. However, carbon nanotubes are extremely hydrophobic and tend to aggregate in aqueous solutions which negatively impacts the viability of tethering the CNTs to the bilayer, fluorescently staining and then imaging them. First, we had to solubilize the CNTs such that they were monodisperse and characterize the CNT-detergent solutions. We were able to create monodisperse solutions of CNTs such that the detergent levels were low enough that the integrity of the bilayer was intact. We were also able to fluorescently label the CNTs in order to visualize them, and tether them to a SLB using a peptide sequence. Future directions of this project would include employing EOF to mobilize the CNTs and use a more sophisticated single particle tracking software to track individual CNTs and analyze their motion.
Kelly, Kathleen, "TWO-DIMENSIONAL FLUIDIZATION OF NANOMATERIALS VIA BIOMIMETIC MEMBRANES TOWARDS ASSISTED SELF-ASSEMBLY" (2017). Dissertations - ALL. 754.