Control of structural domains in epitaxial thin films of functional materials is a fundamental technique to utilize their intrinsic physical and chemical properties in solid-state devices. In this study, we report on suppression of twisted-domain formation in thin-film growth of polar magnetic semiconductor $\mathrm{AgCrS}{\mathrm{e}}_2$ using pulsed-laser deposition. In exploring simultaneously optimized growth temperature and Ag/Cr composition ratio of supply, we find the critical growth temperature ($T_{\mathrm{sub}}$) for obtaining single ${60}^{\circ }$ domain in $c$-axis-oriented $\mathrm{AgCrS}{\mathrm{e}}_2$ thin film on a lattice-matched (111) plane of the yttria-stabilized zirconia substrate. At temperatures below and above the critical $T_{\mathrm{sub}}$, metastable $0^{\circ }$ domain in addition to the ${60}^{\circ }$ domain emerges, indicating delicate energy balance of thermodynamic stability for obtaining the single-domain structure. On the other hand, surface structural analysis using time-of-flight low-energy atom scattering spectroscopy reveals the presence of two polar orientations along +$Z$ and −$Z$ directions. These findings provide valuable insights into the thin-film growth mechanisms for a family of two-dimensional compounds with rhombohedral lattices.

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• Spintronics
• Multiferroics
• Thin films
• Crystal growth