ABSTRACT Low‐dimensional magnets, particularly 2D systems, offer a rich platform for realizing unconventional multiferroic mechanisms, especially when multiple polarization channels coexist. In the quasi‐2D antiferromagnet CrSbS 3 , which crystallizes in the centrosymmetric orthorhombic space group Pnma and orders magnetically at T N ≈ 90 K, two independent polarization mechanisms are uncovered. A weak spontaneous polarization (P 1 ) emerges near T E ≈ T N at zero field, driven by partial Cr charge transfer. Synchrotron XRD refinements reveal anomalies in bond valences and average Cr─S bond length, XAS detects subtle modifications in local electronic states, and Raman spectroscopy uncovers anomalous phonon softening, indicating a charge‐transfer‐driven reconstruction of the lattice and phonon. In addition, second‐harmonic generation (SHG) measurements exhibit a clear enhancement below T E , directly confirming inversion‐symmetry breaking and supporting the emergence of the spontaneous polarization P 1 . Further, neutron diffraction reveals a C‐type antiferromagnetic structure described by the magnetic space group Pnm'a , which breaks inversion symmetry and induces an additional polarization (P 2 ) under applied magnetic fields. Critical exponent analysis ( β ≈ 0.23(2)) highlights quasi‐2D magnetism. These results establish CrSbS 3 as a rare high‐ T c / T N (∼90 K) type‐II multiferroic, where charge, spin, lattice, and phonon degrees of freedom cooperatively produce robust ferroic responses in a 2D framework.
Wu et al. (Thu,) studied this question.