Journal
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
Volume 60, Issue 11, Pages 5928-5935Publisher
WILEY-V C H VERLAG GMBH
DOI: 10.1002/anie.202013489
Keywords
energy landscape; inductive effect; metastability; phase transformation; stable undercooling
Categories
Funding
- Iowa State University
- NSF SBIR [1621910]
- Iowa regents innovation fund
- Directorate For Engineering
- Div Of Industrial Innovation & Partnersh [1621910] Funding Source: National Science Foundation
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Passivating oxide layers can protect the metal core and increase the activation energy needed for solidification, thus slowing down homogeneous nucleation of the metal. Research shows that the integrity of the oxide layer is crucial in stabilizing metal particles, and the influence of the passivating oxide may be more significant than size effects in undercooling.
Undercooling metals relies on frustration of liquid-solid transition mainly by an increase in activation energy. Passivating oxide layers are a way to isolate the core from heterogenous nucleants (physical barrier) while also raising the activation energy (thermodynamic/kinetic barrier) needed for solidification. The latter is due to composition gradients (speciation) that establishes a sharp chemical potential gradient across the thin (0.7-5 nm) oxide shell, slowing homogeneous nucleation. When this speciation is properly tuned, the oxide layer presents a previously unaccounted for interfacial tension in the overall energy landscape of the relaxing material. We demonstrate that 1) the integrity of the passivation oxide is critical in stabilizing undercooled particle, a key tenet in developing heat-free solders, 2) inductive effects play a critical role in undercooling, and 3) the magnitude of the influence of the passivating oxide can be larger than size effects in undercooling.
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