  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 Ln3+ materials Ln2(SeO3)2(SO4)(H2O)2 (Ln = Sm, Dy,
Yb) by mixed-ligand design. The materials exhibit phase-matching nonlinear
optical responses, elucidating the feasibility of the heteroanionic strategy.
Ln2(SeO3)2(SO4)(H2O)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.
