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Abstract Ferro-rotational magnet RbFe(SO₄)₂has attracted attention for its stable ferro-rotational phase and electric-field-controlled magnetic chirality. This work presents the multiferroic properties andH–Tphase diagram of RbFe(SO₄)₂, which have been underexplored. Our measurements of magnetic susceptibility, ferroelectric polarization, and dielectric constant under various magnetic fields reveal four distinct phases: (I) a ferroelectric and helical magnetic phase below 4 K and 6 T, (II) a paraelectric and collinear magnetic phase below 4 K and above 6 T, (III) a paraelectric and non-collinear magnetic phase below 4 K and above 9 T, and (IV) a paraelectric and paramagnetic above 4 K. This study clarifies the multiferroic behavior andH–Tphase diagram of RbFe(SO₄)₂, providing valuable insights into ferro-rotational magnets. 

Abstract Ferro‐rotational (FR) materials, renowned for their distinctive material functionalities, present challenges in the growth of homo‐FR crystals (i.e., single FR domain). This study explores a cost‐effective approach to growing homo‐FR helimagnetic RbFe(SO₄)₂(RFSO) crystals by lowering the crystal growth temperature below theT_FRthreshold using the high‐pressure hydrothermal method. Through polarized neutron diffraction experiments, it is observed that nearly 86% of RFSO crystals consist of a homo‐FR domain. Notably, RFSO displays remarkable stability in the FR phase, with an exceptionally highT_FRof ≈573 K. Furthermore, RFSO exhibits a chiral helical magnetic structure with switchable ferroelectric polarization below 4 K. Importantly, external electric fields can induce a single magnetic domain state and manipulate its magnetic chirality. The findings suggest that the search for new FR magnets with outstanding material properties should consider magnetic sulfates as promising candidates.