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The Intercoupling of Thermal Transport and Mechanical Properties in Colloidal Nanocrystal Assemblies
Description
Colloidal nanocrystals (NCs) are promising candidates for a wide range of applications (electronics, optoelectronics, photovoltaics, thermoelectrics, etc.). Mechanical and thermal transport property play very important roles in all of these applications. On one hand, mechanical robustness and high thermal conductivity are desired in electronics, optoelectronics, and photovoltaics. This improves thermomechanical stability and minimizes the temperature rise during the device operation. On the other hand, low thermal conductivity is desired for higher thermoelectric figure of merit (ZT). This dissertation demonstrates that ligand structure and nanocrystal ordering are the primary determining factors for thermal transport and mechanical properties in colloidal nanocrystal assemblies. To eliminate the mechanics and thermal transport barrier, I first propose a ligand crosslinking method to improve the thermal transport across the ligand-ligand interface and thus increasing the overall thermal conductivity of NC assemblies. Young’s modulus of nanocrystal solids also increases simultaneously upon ligand crosslinking. My thermal transport measurements show that the thermal conductivity of the iron oxide NC solids increases by a factor of 2-3 upon ligand crosslinking. Further, I demonstrate that, though with same composition, long-range ordered nanocrystal superlattices possess higher mechanical and thermal transport properties than disordered nanocrystal thin films. Experimental measurements along with theoretical modeling indicate that stronger ligand-ligand interaction in NC superlattice accounts for the improved mechanics and thermal transport. This suggests that NC/ligand arranging order also plays important roles in determining mechanics and thermal transport properties of NC assemblies. Lastly, I show that inorganic ligand functionalization could lead to tremendous mechanical enhancement (a factor of ~60) in NC solids. After ligand exchange and drying, the short inorganic Sn2S64- ligands dissociate into a few atomic layers of amorphous SnS2 at room temperature and interconnects the neighboring NCs. I observe a reverse Hall-Petch relation as the size of NC decreases. Both atomistic simulations and analytical phase mixture modeling identify the grain boundaries and their activities as the mechanic bottleneck.
ContributorsWang, Zhongyong (Author) / Wang, Robert RW (Thesis advisor) / Wang, Liping LW (Committee member) / Newman, Nathan NN (Committee member) / Arizona State University (Publisher)
Created2021
Description
Over the past few years, research into the use of doped diamond in electronics has seen an exponential growth. In the course of finding ways to reduce the contact resistivity, nanocarbon materials have been an interesting focus. In this work, the transfer length method (TLM) was used to investigate Ohmic contact properties using the tri-layer stack Ti/Pt/Au on nitrogen-doped n-type conducting nano-carbon (nanoC) layers grown on (100) diamond substrates. The nanocarbon material was characterized using Secondary Ion Mass Spectrometry (SIMS), Scanning electron Microscopy (SEM) X-ray diffraction (XRD), Raman scattering and Hall effect measurements to probe the materials characteristics. Room temperature electrical measurements were taken, and samples were annealed to observe changes in electrical conductivity. Low specific contact resistivity values of 8 x 10^-5 Ωcm^2 were achieved, which was almost two orders of magnitude lower than previously reported values. The results were attributed to the increased nitrogen incorporation, and the presence of electrically active defects which leads to an increase in conduction in the nanocarbon. Further a study of light phosphorus doped layers using similar methods with Ti/Pt/Au contacts again yielded a low contact resistivity of about 9.88 x 10^-2 Ωcm^2 which is an interesting prospect among lightly doped diamond films for applications in devices such as transistors. In addition, for the first time, hafnium was substituted for Ti in the contact stack (Hf/Pt/Au) and studied on nitrogen doped nanocarbon films, which resulted in low contact resistivity values on the order of 10^-2 Ωcm^2. The implications of the results were discussed, and recommendations for improving the experimental process was outlined. Lastly, a method for the selective area growth of nanocarbon was developed and studied and the results provided an insight into how different characterizations can be used to confirm the presence of the nanocrystalline diamond material, the limitations due to the film thickness was explored and ideas for future work was proposed.
ContributorsAmonoo, Evangeline Abena (Author) / Thornton, Trevor (Thesis advisor) / Alford, Terry L (Thesis advisor) / Anwar, Shahriar (Committee member) / Theodore, David (Committee member) / Arizona State University (Publisher)
Created2023
Description
Integrating advanced materials with innovative manufacturing techniques has propelled the field of additive manufacturing into new frontiers. This study explores the rapid 3D printing of reduced graphene oxide/polymer composites using Micro-Continuous Liquid Interface Production (μCLIP), a cutting-edge technology known for its speed and precision. A printable ink is formulated with reduced graphene oxide for μCLIP-based 3D printing. The research focuses on optimizing μCLIP parameters to fabricate reduced graphene composites efficiently. The study encompasses material synthesis, ink formulation and explores the resulting material's structural and electrical properties. The marriage of graphene's unique attributes with the rapid prototyping capabilities of μCLIP opens new avenues for scalable and rapid production in applications such as energy storage, sensors, and lightweight structural components. This work contributes to the evolving landscape of advanced materials and additive manufacturing, offering insights into the synthesis, characterization, and potential applications of 3D printed reduced graphene oxide/polymercomposites.
ContributorsRavishankar, Chayaank Bangalore (Author) / Chen, Xiangfan (Thesis advisor) / Bhate, Dhruv (Committee member) / Azeredo, Bruno (Committee member) / Arizona State University (Publisher)
Created2024
Description
Engineering polymers are critical for contemporary high-performance applications where toughness, thermal stability, and density are at a premium. These materials often demand high-energy processing conditions or highly reactive monomers that hold negative impacts on human and environmental health. Thus, this work serves to remediate the negative impacts of engineering polymer synthesis by addressing toxicity and processing at the monomer level, while maintaining or exceeding previous thermomechanical and stimuli-responsive performance. Polyurethanes (PUs) represent a class of engineering polymers that possess highly modular properties due to the diverse monomer selection available for their synthesis. The efficient reaction between isocyanates and hydroxyls impart stellar properties and flexible processing modalities, however recent scrutiny regarding the toxicity of the isocyanate precursors has driven the search for non-isocyanate polyurethane (NIPU) pathways. The advancement of bis-carbonylimidazolide (BCI) monomers for the synthesis of NIPU thermoplastics and foams is thoroughly investigated in this work. Remarkably, a novel decarboxylation pathway for BCI monomers controlled by catalyst loading enabled in-situ CO2 generation during crosslinking with trifunctional amines, and resulted in a facile synthetic route for NIPU foams. Further explorations into catalyst considerations revealed Dabco® 33-LV as a suitable mechanism for controlling reaction times and careful selection of surfactant concentration provided control over pore size and geometry. This led to a library of flexible and rigid NIPU foams that displayed a wide range of thermomechanical properties. Furthermore, sequestration of the imidazole byproduct through an efficient Michael reaction identified maleimide and acrylate additives as a viable pathway to eliminate post-processing steps resulting in NIPU foam synthesis that is amenable to current industrial standards. This route held advantages over the isocyanate route, as condensate removal drove molecular weight increase and ultimately achieved the first reported phase separation behavior of a NIPU thermoplastic containing a poly(ethylene glycol) soft segment. Furthermore, sustainable considerations for engineering polymers were explored with the introduction of a novel cyclobutane bisimide monomer that readily installs into various polymeric systems. Direct installation of this monomer, CBDA-AP-I, into a polysulfone backbone enabled controlled photo-cleavage, while further hydroxy ethyl functionalization allowed for incorporation into PU systems for photo-cleavable high-performance adhesive applications.
ContributorsSintas, Jose Ignacio (Author) / Long, Timothy E (Thesis advisor) / Sample, Caitlin S. (Committee member) / Jin, Kailong (Committee member) / Arizona State University (Publisher)
Created2024