Ln(2)(SeO(3))(2)(SO(4))(H(2)O)(2) (Ln=Sm, Dy, Yb): A Mixed‐Ligand Pathway to New Lanthanide(III) Multifunctional Materials Featuring Nonlinear Optical and Magnetic Anisotropy Properties

Bottom‐up assembly of optically nonlinear and magnetically anisotropic lanthanide materials involving precisely placed spin carriers and optimized metal‐ligand coordination offers a potential route to developing electronic architectures for coherent radiation generation and spin‐based technologies, but the chemical design historically has been extremely hard to achieve. To address this, we developed a worthwhile avenue for creating new noncentrosymmetric chiral Ln(3+) materials Ln(2)(SeO(3))(2)(SO(4))(H(2)O)(2) (Ln=Sm, Dy, Yb) by mixed‐ligand design. The materials exhibit phase‐matching nonlinear optical responses, elucidating the feasibility of the heteroanionic strategy. Ln(2)(SeO(3))(2)(SO(4))(H(2)O)(2) displays paramagnetic property with strong magnetic anisotropy facilitated by large spin‐orbit coupling. This study demonstrates a new chemical pathway for creating previously unknown polar chiral magnets with multiple functionalities.