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- Creators: Darling, Kris A.
Description
Membrane proteins are a vital part of cellular structure. They are directly involved in many important cellular functions, such as uptake, signaling, respiration, and photosynthesis, among others. Despite their importance, however, less than 500 unique membrane protein structures have been determined to date. This is due to several difficulties with macromolecular crystallography, primarily the difficulty of growing large, well-ordered protein crystals. Since the first proof of concept for femtosecond nanocrystallography showing that diffraction patterns can be collected on extremely small crystals, thus negating the need to grow larger crystals, there have been many exciting advancements in the field. The technique has been proven to show high spatial resolution, thus making it a viable method for structural biology. However, due to the ultrafast nature of the technique, which allows for a lack of radiation damage in imaging, even more interesting experiments are possible, and the first temporal and spatial images of an undamaged structure could be acquired. This concept was denoted as time-resolved femtosecond nanocrystallography.
This dissertation presents on the first time-resolved data set of Photosystem II where structural changes can actually be seen without radiation damage. In order to accomplish this, new crystallization techniques had to be developed so that enough crystals could be made for the liquid jet to deliver a fully hydrated stream of crystals to the high-powered X-ray source. These changes are still in the preliminary stages due to the slightly lower resolution data obtained, but they are still a promising show of the power of this new technique. With further optimization of crystal growth methods and quality, injection technique, and continued development of data analysis software, it is only a matter of time before the ability to make movies of molecules in motion from X-ray diffraction snapshots in time exists. The work presented here is the first step in that process.
This dissertation presents on the first time-resolved data set of Photosystem II where structural changes can actually be seen without radiation damage. In order to accomplish this, new crystallization techniques had to be developed so that enough crystals could be made for the liquid jet to deliver a fully hydrated stream of crystals to the high-powered X-ray source. These changes are still in the preliminary stages due to the slightly lower resolution data obtained, but they are still a promising show of the power of this new technique. With further optimization of crystal growth methods and quality, injection technique, and continued development of data analysis software, it is only a matter of time before the ability to make movies of molecules in motion from X-ray diffraction snapshots in time exists. The work presented here is the first step in that process.
ContributorsKupitz, Christopher (Author) / Fromme, Petra (Thesis advisor) / Spence, John C. (Thesis advisor) / Redding, Kevin (Committee member) / Ros, Alexandra (Committee member) / Arizona State University (Publisher)
Created2014
Description
Nanocrystalline (NC) materials experience inherent microstructural instability when exposed to elevated temperature, deformation rates or loads over long periods of time which limits its applications as well as processing. The instability arises due to the predominance of grain boundary (GB) diffusional processes which hastens coarsening. This dissertation aims to provide a solution for the very first time, through the development and characterization of a bulk NC alloy system. The NC-Cu-Ta discussed here offers exceptional thermal stability in addition to superior strength and creep resistance. The systematic study of the behavior of this material will pave the way for future development of NC materials with a multitude of optimized properties for extreme applications.
In-situ and ex-situ TEM characterization, multiple strain-rate compression testing and atomistic modeling were employed to investigate the behavior of NC-Cu-Ta under intense heating, stress/strain-rate and creep conditions. Results reveal, that temperature influences the misfit strain, leading to a significant change in flow stress, despite which (strength) remains greater than all known NC metals. Further, this alloy was found to achieve and retain strengths which were over two orders of magnitude higher than most NC metals under elevated temperature conditions. Dislocation-based slip was found to predominate at elevated temperatures for both high- and low-strain rate testing whereas twinning was favored during low temperature high-strain rate testing. The solute concentration was also found to play a role in dictating the deformation where heterogeneous twinnability was found to decrease with an increase in Ta concentration.
A paradigm-shift in the creep response of NC-materials with unprecedented property combinations is also reported, i.e., high strength with extremely high temperature creep resistance (6-8 orders higher than other NC materials), in this NC-Cu-Ta-alloy. The unique combination of properties in these NC-alloys is achieved through a processing route that creates distinct GB-pinning nanoclusters of the solute that favor kinetic stability of grains.
Overall, this dissertation provides an understanding of the mechanical response of a stable alloy system to extreme conditions, which was previously unattainable, and a perspective on the design of a new class of NC alloys exhibiting a multitude of optimized high temperature properties.
In-situ and ex-situ TEM characterization, multiple strain-rate compression testing and atomistic modeling were employed to investigate the behavior of NC-Cu-Ta under intense heating, stress/strain-rate and creep conditions. Results reveal, that temperature influences the misfit strain, leading to a significant change in flow stress, despite which (strength) remains greater than all known NC metals. Further, this alloy was found to achieve and retain strengths which were over two orders of magnitude higher than most NC metals under elevated temperature conditions. Dislocation-based slip was found to predominate at elevated temperatures for both high- and low-strain rate testing whereas twinning was favored during low temperature high-strain rate testing. The solute concentration was also found to play a role in dictating the deformation where heterogeneous twinnability was found to decrease with an increase in Ta concentration.
A paradigm-shift in the creep response of NC-materials with unprecedented property combinations is also reported, i.e., high strength with extremely high temperature creep resistance (6-8 orders higher than other NC materials), in this NC-Cu-Ta-alloy. The unique combination of properties in these NC-alloys is achieved through a processing route that creates distinct GB-pinning nanoclusters of the solute that favor kinetic stability of grains.
Overall, this dissertation provides an understanding of the mechanical response of a stable alloy system to extreme conditions, which was previously unattainable, and a perspective on the design of a new class of NC alloys exhibiting a multitude of optimized high temperature properties.
ContributorsRajagopalan, Mansa (Author) / Solanki, Kiran N. (Thesis advisor) / Alford, Terry L. (Committee member) / Jiao, Yang (Committee member) / Darling, Kris A. (Committee member) / Arizona State University (Publisher)
Created2016