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arXiv · 2604.01317

Enantiopurity-Controlled Magnetism in a Two-Dimensional Organic-Inorganic Material

P. Garrett Hegel·Oscar Gonzalez·Mingrui Li·Shannon S. Fender·Harishankar Jayakumar·Archana Raja·Ariana Ray·Isaac M. Craig·D. Kwabena Bediako
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Abstract

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 MnPS$_3$ 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.

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P. Garrett Hegel, Oscar Gonzalez, Mingrui Li, Shannon S. Fender, Harishankar Jayakumar, Archana Raja, Ariana Ray, Isaac M. Craig, D. Kwabena Bediako. 2026-04-01. Enantiopurity-Controlled Magnetism in a Two-Dimensional Organic-Inorganic Material. https://arxiv.org/abs/2604.01317

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