Extended solids that combine unpaired electron spin and structural chirality can host unconventional magnetic behaviors with potential for electronic technologies. A versatile strategy for creating chiral solids is incorporation of chiral organic molecules into inorganic crystals. However, such hybrid organic-inorganic materials have so far been examined through the lens of absolute chirality, leaving enantiomeric excess (ee) underexplored as a tuning parameter. Here, we report two-dimensional (2D) intercalation compounds with controllable ee produced by cation exchange of MnPS3 with chiral organic molecules. We show that these materials' magnetism is determined by intercalant ee rather than absolute chirality. Moreover, low-ee materials display thermally activated dynamic magnetism absent from enantiopure analogs. These ee-dependent magnetic behaviors are explained by local ordering of Mn vacancies, directed by correlated vacancy-intercalant electrostatics and confined molecular packing. Together, these results demonstrate a distinctive tuning strategy for molecule-material hybrids and establish design principles for 2D chiral and magnetically dynamic materials.
@article{arxiv.2604.01317,
title = {Enantiopurity-Controlled Magnetism in a Two-Dimensional Organic-Inorganic Material},
author = {P. Garrett Hegel and Oscar Gonzalez and Mingrui Li and Shannon S. Fender and Harishankar Jayakumar and Archana Raja and Ariana Ray and Isaac M. Craig and D. Kwabena Bediako},
journal= {arXiv preprint arXiv:2604.01317},
year = {2026}
}