This work identifies alloy terminal freezing range, columnar growth, grain coarsening, liquid availability towards the terminal stage of solidification, and segregation towards boundaries as primary factors affecting the hot-cracking susceptibility of fusion-based additive manufacturing (F-BAM) processed alloys. Additionally, an integrated computational materials engineering (ICME)-based approach has been formulated to design novel Al alloys, and high entropy alloys for F-BAM processing. The ICME-based approach has led to heterogeneous nucleation-induced grain refinement, terminal eutectic solidification-enabled liquid availability, and segregation-induced coalescence of solidification boundaries during laser-powder bed fusion (L-PBF) processing. In addition to exhibiting a wide crack-free L-PBF processing window, the designed alloys exhibited microstructural heterogeneity and hierarchy (MHH), and thus could leverage the unique process dynamics of L-PBF to produce a fine-tunable MHH and mechanical behavior. Furthermore, alloy chemistry-based fine tuning of the stacking fault energy has led to transformative damage tolerant alloys. Such alloys can shield defects stemming from the stochastic powder bed in L-PBF, and consequently can prevent catastrophic failure despite the solidification defects. A modified materials systems approach that explicitly includes alloy chemistry as a means to modify the printability, properties and performance with F-BAM is also presented. Overall, this work is expected to facilitate application specific manufacture with F-BAM and eventually facilitate widespread adoption of F-BAM in structural application.

The recent emphasis on magnesium alloys can be appreciated by following the research push from several agencies, universities and editorial efforts. With a density equal to two-thirds of Al and one-thirds of steel, Mg provides the best opportunity for lightweighting of metallic components. However, one key bottleneck restricting its insertion into industrial applications is low strength values. In this respect, Mg-Y-Nd alloys have been promising due to their ability to form strengthening precipitates on the prismatic plane. However, if the strength is compared to Al alloys, these alloys are not attractive. The primary reason for low structural performance in Mg is related to low alloying and microstructural efficiency. In this dissertation, these terminologies are discussed in detail. A simple calculation showed that the microstructural efficiency in Mg-4Y-3Nd alloy is 30% of its maximum potential. Guided by the definitions of alloying and microstructural efficiency, the two prime objectives of this thesis were to: (i) to use thermomechanical processing routes to tailor the microstructure and achieve high strength in an Mg-4Y-3Nd alloy, and (ii) optimize the alloy chemistry of the Mg-rare earth alloy and design a novel rare—earth free Mg alloy by Calphad approach to achieve a strength of 500 MPa. Experimental, theoretical and computational approaches have been used to establish the process-structure-property relationships in an Mg-4Y-3Nd alloy. For example, increase in strength was observed after post aging of the friction stir processed/additive manufactured microstructure. This was attributed to the dissolution of Mg2Y particles which increased the alloying and microstructural efficiency. Further quantification by numerical modeling showed that the effective diffusivity during friction stir processing and friction stir welding is 60 times faster than in the absence of concurrent deformation leading to the dissolution of thermally stable particles. In addition, the investigation on the interaction between dislocations and strengthening precipitate revealed that, specific defects like the I1 fault aid in the accelerated precipitation of the strengthening precipitate in an Mg-4Y-3Nd alloy. Also, the effect of external field (ultrasonic waves) was studied in detail and showed accelerated age hardening response in Mg-4Y-3Nd alloy by a factor of 24. As the bottleneck of low strength is addressed, the answers to the following questions are discussed in this dissertation: What are the fundamental micro-mechanisms governing second phase evolution in an Mg-4Y-3Nd alloy? What is the mechanical response of different microstructural states obtained by hot rolling, friction stir processing and friction stir additive manufacturing? Is defect engineering critical to achieve high strength Mg alloys? Can application of an external field influence the age hardening response in an Mg-4Y-3Nd alloy? Can a combination of innovative processing for tailoring microstructures and computational alloy design lead to new and effective paths for application of magnesium alloys?