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Abstract The Rashba effect enables control over the spin degree of freedom, particularly in polar materials where the polar symmetry couples to Rashba‐type spin splitting. The exploration of this effect, however, has been hindered by the scarcity of polar materials exhibiting the bulk‐Rashba effect and rapid spin‐relaxation effects dictated by the D'yakonov–Perel mechanism. Here, a polar LiNbO₃‐typeR3cphase of Bi_1‐xIn_1+xO₃withx≈0.15–0.24 is stabilized via epitaxial growth, which exhibits a bulk‐Rashba effect with suppressed spin relaxation as a result of its unidirectional spin texture. As compared to the previously observed non‐polarPnmaphase, this polar phase exhibits higher conductivity, reduced bandgap, and enhanced dielectric and piezoelectric responses. Combining first‐principles calculations and multimodal magnetotransport measurements, which reveal weak (anti)localization, anisotropic magnetoresistance, planar‐Hall effect, and nonreciprocal charge transport, a bulk‐Rashba effect without rapid spin relaxation is demonstrated. These findings offer insights into spin‐orbit coupling physics within polar oxides and suggest potential spintronic applications. 

Abstract The hafnate perovskites PbHfO₃(antiferroelectric) and SrHfO₃(“potential” ferroelectric) are studied as epitaxial thin films on SrTiO₃(001) substrates with the added opportunity of observing a morphotropic phase boundary (MPB) in the Pb_1−xSr_xHfO₃system. The resulting (240)‐oriented PbHfO₃(Pba2) films exhibited antiferroelectric switching with a saturation polarization ≈53 µC cm⁻²at 1.6 MV cm⁻¹, weak‐field dielectric constant ≈186 at 298 K, and an antiferroelectric‐to‐paraelectric phase transition at ≈518 K. (002)‐oriented SrHfO₃films exhibited neither ferroelectric behavior nor evidence of a polarP4mmphase . Instead, the SrHfO₃films exhibited a weak‐field dielectric constant ≈25 at 298 K and no signs of a structural transition to a polar phase as a function of temperature (77–623 K) and electric field (–3 to 3 MV cm⁻¹). While the lack of ferroelectric order in SrHfO₃removes the potential for MPB, structural and property evolution of the Pb_1−xSr_xHfO₃(0 ≤x < 1) system is explored. Strontium alloying increased the electric‐breakdown strength (E_B) and decreased hysteresis loss, thus enhancing the capacitive energy storage density (U_r) and efficiency (η). The composition, Pb_0.5Sr_0.5HfO₃produced the best combination ofE_B = 5.12 ± 0.5 MV cm⁻¹,U_r = 77 ± 5 J cm⁻³, and η = 97 ± 2%, well out‐performing PbHfO₃and other antiferroelectric oxides.