Abstract
In the quest toward rational design of materials, establishing direct links between the attributes of microscopic building blocks and the macroscopic performance limits of the bulk structures they comprise is essential. Building blocks of concern to the field of crystallization are the impurities, foreign ingredients that are either deliberately added to or naturally present in the growth medium. While the role of impurities has been studied extensively in various materials systems, the inherent complexity of eutectic crystallization in the presence of trace, often metallic impurities (‘eutectic modification’) remains poorly understood. In particular, the origins behind the drastic microstructural changes observed upon modification are elusive. Herein, we employ an integrated imaging approach to shed light on the influence of trace metal impurities during the growth of an irregular (faceted–non-faceted) eutectic. Our dynamic and 3D synchrotron-based X-ray imaging results reveal the markedly different microstructural and, for the first time, topological properties of the eutectic constituents that arise upon modification, not fully predicted by the existing theories. Together with ex situ crystallographic characterization of the fully-solidified specimen, our multi-modal study provides a unified picture of eutectic modification: The impurities selectively alter the stacking sequence of the faceted phase, thereby inhibiting its steady-state growth. Consequently, the non-faceted phase advances deeper into the melt, eventually engulfing the faceted phase in its wake. We present a quantitative topological framework to rationalize these experimental observations.
Highlights
In the quest toward rational design of materials, establishing direct links between the attributes of microscopic building blocks and the macroscopic performance limits of the bulk structures they comprise is essential
The synchrotron experiment was guided by the equilibrium phase diagram of the unmodified a ductile matrix (Al)-Ge eutectic, with the anticipation that chemical modification leads to higher nucleation undercooling[21,28]
Direct interrogation of the time-resolved 3D results demonstrate uniquely that chemical modification brings about significant changes in the topology of the eutectic constituents, the reasons for which are discussed in detail below
Summary
In the quest toward rational design of materials, establishing direct links between the attributes of microscopic building blocks and the macroscopic performance limits of the bulk structures they comprise is essential. Impurities, whether intentionally introduced to modify a product or unavoidably present in the growth medium, have been shown to play important roles during all stages of solidification in areas as diverse as pharmaceutical and protein crystallization[1,2], semiconductor and polymer processing[3,4], single crystal production[5], and process metallurgy[6] including additive manufacturing[7,8,9] In the latter case, it has been demonstrated recently that chemical modification of the feedstock alloy by impurities can vastly expand the range of compatible metallic materials that can be processed[7], which could lead to landscape-changing advances across multiple sectors such as aerospace, automotive, and biomedical. We note that while quenching in the absence of modifying agents can produce fibrous, as opposed to flake-like, Si in Al-Si alloys, it does not change the twin density of Si23
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