Abstract
We report a spin reorientation from Γ4(Gx, Ay, Fz) to Γ1(Ax, Gy, Cz) magnetic configuration near room temperature and a re-entrant transition from Γ1(Ax, Gy, Cz) to Γ4(Gx, Ay, Fz) at low temperature in TbFe1−xMnxO3 single crystals by performing both magnetization and neutron diffraction measurements. The Γ4 − Γ1 spin reorientation temperature can be enhanced to room temperature when x is around 0.5 ~ 0.6. These new transitions are distinct from the well-known Γ4 − Γ2 transition observed in TbFeO3, and the sinusoidal antiferromagnetism to complex spiral magnetism transition observed in multiferroic TbMnO3. We further study the evolution of magnetic entropy change (−ΔSM) versus Mn concentration to reveal the mechanism of the re-entrant spin reorientation behavior and the complex magnetic phase at low temperature. The variation of −ΔSM between a and c axes indicates the significant change of magnetocrystalline anisotropy energy in the TbFe1−xMnxO3 system. Furthermore, as Jahn-Teller inactive Fe3+ ions coexist with Jahn-Teller active Mn3+ ions, various anisotropy interactions, compete with each other, giving rise to a rich magnetic phase diagram. The large magnetocaloric effect reveals that the studied material could be a potential magnetic refrigerant. These findings expand our knowledge of spin reorientation phenomena and offer the alternative realization of spin-switching devices at room temperature in the rare-earth orthoferrites.
Highlights
New magnetic phase and reveal the mechanism of new spin reorientation in TbFe1−xMnxO3 system, from which some remarkable behaviors expected to be found due to competitive magnetic phases that do not exist in both
We demonstrate that the phase transition of Γ4 →Γ1 →Γ4 exists in TbFe0.75Mn0.25O3 single crystal, rather than the common transition of Γ4 →Γ2 as observed in TbFeO3 and other orthoferrites
We speculate that the magnetic structure transforms from the canted antiferromagnetism with weak ferromagnetism along the c axis (Gx, Ay, Fz) to the major G-type antiferromagnetic vector along the b axis (Ax, Gy, Cz)
Summary
New magnetic phase and reveal the mechanism of new spin reorientation in TbFe1−xMnxO3 system, from which some remarkable behaviors expected to be found due to competitive magnetic phases that do not exist in both. We synthesized a series of TbFe1−xMnxO3 and reported their special magnetic phase transitions by performing magnetization and neutron powder diffraction (NPD) measurements. We demonstrate that the phase transition of Γ4 →Γ1 →Γ4 exists in TbFe0.75Mn0.25O3 single crystal, rather than the common transition of Γ4 →Γ2 as observed in TbFeO3 and other orthoferrites. From a practical point of view, Γ4 →Γ1 (weak magnetic moment to zero net moment) transition may find use even with -obtained polycrystalline samples whereas we need to grow single crystals to observe Γ4 →Γ2 (weak magnetic moment along c to a direction) transition. The evolution of entropy change versus Mn doping are presented and discussed with in the scenario of
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