Remarkable advances have been made since rapid solidification was first introduced to the field of materials science and technology. New types of materials such as amorphous alloys and nanostructure materials have been developed as a result of rapid solidification techniques. While these advances are, in many respects, ground breaking, much remains to be discerned concerning the fundamental relationships that exist between a liquid and a rapidly solidified solid.;The scope of the current dissertation involves an extensive set of experimental, analytical, and computational studies designed to increase the overall understanding of morphological selection, phase competition, and structural hierarchy that occurs under far-from equilibrium conditions. High pressure gas atomization and Cu-block melt-spinning are the two different rapid solidification techniques applied in this study. The research is mainly focused on Al-Si and Al-Sm alloy systems. Silicon and samarium produce different, yet favorable, systems for exploration when alloyed with aluminum under far-from equilibrium conditions. One of the main differences comes from the positions of their respective T0 curves, which makes Al-Si a good candidate for solubility extension while the plunging T0 line in Al-Sm promotes glass formation.;The rapidly solidified gas-atomized Al-Si powders within a composition range of 15 to 50 wt% Si are examined using scanning and transmission electron microscopy. The non-equilibrium partitioning and morphological selection observed by examining powders at different size classes are described via a microstructure map. The interface velocities and the amount of undercooling present in the powders are estimated from measured eutectic spacings based on Jackson-Hunt (JH) and Trivedi-Magnin-Kurz (TMK) models, which permit a direct comparison of theoretical predictions. For an average particle size of 10 microm with a Peclet number of ~0.2, JH and TMK deviate from each other. This deviation indicates an adiabatic type solidification path where heat of fusion is reabsorbed. It is interesting that this particle size range is also consistent with the appearance of a microcellular growth. While no glass formation is observed within this system, the smallest size powders appear to consist of a mixture of nanocrystalline Si and Al.;Al-Sm alloys have been investigated within a composition range of 34 to 42 wt% Sm. Gas atomized powders of Al-Sm are investigated to explore the morphological and structural hierarchy that correlates with different degrees of departure from full equilibrium conditions. The resultant powders show a variety of structural selection with respect to amount of undercooling, with an amorphous structure appearing at the highest cooling rates. Because of the chaotic nature of gas atomization, Cu-block melt-spinning is used to produce a homogeneous amorphous structure. The as-quenched structure within Al-34 to 42 wt% Sm consists of nanocrystalline fcc-Al (on the order of 5 nm) embedded in an amorphous matrix. The nucleation density of fcc-Al after initial crystallization is on the order of 1022-1023 m-3, which is 105-106 orders of magnitude higher than what classical nucleation theory predicts. Detailed analysis of liquid and as-quenched structures using high energy synchrotron X-ray diffraction, high energy transmission electron microscopy, and atom probe tomography techniques revealed an Al-Sm network similar in appearance to a medium range order (MRO) structure. A model whereby these MRO clusters promote the observed high nucleation density of fcc-Al nanocrystals is proposed. The devitrification path was identified using high temperature, in-situ, high energy synchrotron X-ray diffraction techniques and the crystallization kinetics were described using an analytical Johnson-Mehl-Avrami (JMA) approach.
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