Single crystals on a macroscopic scale exhibit microscopic periodicity on an atomic level, which enables us to investigate their intrinsic physical properties and to optimize their functional properties. We have grown various kinds of magnetic single crystals of intermetallic compounds for fundamental research and for applications. In this, much effort has been focused on the growth conditions to satisfy the different requirements, especially for crystals that are hard to grow. In this paper, we review some selected results on various single crystals grown in our institute and illustrate the importance of single‐crystal growth for research and application. Several intrinsic magnetic properties, including magnetocrystallographic anisotropy, spin reorientations, and magnetostriction have been investigated in detail on single crystals of rare‐earth intermetallic compounds. The internal stress induced in crystals of magnetic shape‐memory alloys is utilized to reorient the martensitic microstructure for maximizing the output strain. Combining the self‐flux method with magnetic elevating Czochraski cold‐crucible growth technology, a deeply undercooled environment was achieved to enable (Tb,Dy)Fe2 single crystals to be grown. Some research works on crystal growth, such as solidifying theories, growth dynamics, and phase diagrams, are also discussed.

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