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As nanotechnology continues to advance, the need for smaller, structurally complex materials has grown. However, these microscopic (10⁶) and nanoscopic (10⁹) structures often display unexpected changes in mechanical properties as compared to their macroscopic counterparts. Nanomechanical studies investigating size-effects in stiffness, strength, recoverability, ductility, and fracture, reveal an intimate interplay between the breakdown in continuum behavior and the energetic landscape of microstructural mechanisms. Additive manufacturing opens new opportunities to explore this microstructure-mechanics relationship as it enables the micro- and nano-scale production of novel materials and microstructures. While existing studies on structural and functional materials highlight the unique size-scale behavior, a large gap remains in our understanding of the complex relationship between microstructure and material performance. This work investigates the interactions and mechanisms that give rise to emergent nanoscale phenomena. With microstructural characterizations, we demonstrate the role of boundaries and interfaces on mechanical and mechanically-coupled behavior in (1) dense nanowire arrays, (2) nano-architected nanocrystalline zinc oxide, and (3) highly-twinned additively manufactured metallic systems. This work provides critical insights into the mechanisms underlying the observed emergent phenomena and further opens our fundamental intuition for microstructure-mechanics relationships in materials at the nanoscale.

Ultralow-k materials used in high voltage devices require mechanical resilience and electrical and dielectric stability even when subjected to mechanical loads. Existing devices with organic polymers suffer from low thermal and mechanical stability while those with inorganic porous structures struggle with poor mechanical integrity. Recently, 3D hollow-beam nanolattices have emerged as promising candidates that satisfy these requirements. However, their properties are maintained for only five stress cycles at strains below 25%. Here, we demonstrate that alumina nanolattices with different relative density distributions across their height elicit a deterministic mechanical response concomitant with a 1.5–3.3 times higher electrical breakdown strength than nanolattices with uniform density. These density-variant nanolattices exhibit an ultralow-k of ≈1.2, accompanied by complete electric and dielectric stability and mechanical recoverability over 100 cyclic compressions to 62.5% strain. We explain the enhanced insulation and long-term cyclical stability by the bi-phase deformation where the lower-density region protects the higher-density region as it is compressed before the higher-density region, allowing to simultaneously possess high strength and ductility like composites. This study highlights the superior electrical performance of the bi-phase nanolattice with a single interface in providing stable conduction and maximum breakdown strength.

Thesis: S.B., Massachusetts Institute of Technology, Department of Materials Science and Engineering, 2017., This electronic version was submitted by the student author. The certified thesis is available in the Institute Archives and Special Collections., Cataloged from student-submitted PDF version of thesis., Includes bibliographical references (page 31)., Both biological and synthetic materials crosslinked via metal coordinate dynamic chemistry display interesting advanced behavior. In particular, coordinate networks have been shown to form self-healing, self-assembling, and stimuli-responsive behaviors through its tunable optical and mechanical properties as well as its ability to for dynamic networks. However, while the majority of research has focused on characterization of bulk coordinate networks, coordinate complexes have also been shown to be useful in molecular film formation [1 and 2]. This study investigates the mechanical and optical properties of tannic acid and 4 arm catechol polyethylene glycol based coordinate network films. It shows that these films can contribute to energy dissipation and undergo pH-induced optical shifts when used as coatings on soft hydrogels. It also provides evidence that the molecular architecture of the network formers may have considerable effect on the properties and behavior of coordinate network films. Ultimately this work lays the foundation for further investigation of the underlying mechanisms and engineering potential of coordinate network based films., by Rebecca Anne Gallivan., S.B.