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 materials Ln (SeO ) (SO )(H O) (Ln=Sm, Dy, Yb) by mixed-ligand design. The materials exhibit phase-matching nonlinear optical responses, elucidating the feasibility of the heteroanionic strategy. Ln (SeO ) (SO )(H O) 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.