Deformation
processing of immiscible systems is observed to disrupt
thermodynamic equilibrium, often resulting in nonequilibrium microstructures.
The microstructural changes including nanostructuring, hierarchical
distribution of phases, localized solute supersaturation, and oxygen
ingress result from high-strain extended deformation, causing a significant
change in mechanical properties. Because of the dynamic evolution
of the material under large strain shear load, a detailed understanding
of the transformation pathway has not been established. Additionally,
the influence of these microstructural changes on mechanical properties
is also not well characterized. Here, an immiscible Cu-4 at. % Nb
alloy is subjected to a high-strain shear deformation (∼200);
the deformation-induced changes in the morphology, crystal structure,
and composition of Cu and Nb phases as a function of total strain
are characterized using transmission electron microscopy and atom
probe tomography. Furthermore, a multimodal experiment-guided computational
approach is used to depict the initiation of deformation by an increase
in misorientation boundaries by crystal plasticity-based grain misorientation
modeling (strain ∼0.6). Then, co-deformation and nanolamination
of Cu and Nb are envisaged by a finite element method-based computational
fluid dynamic model with strain ranging from 10 to 200. Finally, the
experimentally observed amorphization of the severely sheared supersaturated
Cu–Nb–O phase was validated using the first principle-based
simulation using density functional theory while highlighting the
influence of oxygen ingress during deformation. Furthermore, the nanocrystalline
microstructure shows a >2-fold increase in hardness and compressive
yield strength of the alloy, elucidating the potential of deformation
processing to obtain high-strength low-alloyed metals. Our approach
presents a step-by-step evolution of a microstructure in an immiscible
alloy undergoing severe shear deformation, which is broadly applicable
to materials processing based on friction stir, extrusion, rolling,
and surface shear deformation under wear and can be directly applied
to understanding material behavior during these processes.