Controlling Magnetism in the 2D van der Waals Antiferromagnet CrPS<sub>4</sub> via Ion Intercalation.

Ruiz, Alberto M; López-Alcalá, Diego; Rivero-Carracedo, Gonzalo; Shumilin, Andrei; Baldoví, José J · Nano Lett · 2026

basic_science · Level V

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Abstract

Two-dimensional (2D) van der Waals (vdW) magnetic materials are platforms in which inserting chemical species into their interlayer gaps offers a powerful route to engineer magnetism. Here, we focus on the A-type antiferromagnetic semiconductor CrPS<sub>4</sub> (<i>T</i><sub>N</sub> = 38 K) and investigate its electronic and magnetic properties upon intercalation of lithium (Li<sup>+</sup>) and organic tetrabutylammonium (TBA<sup>+</sup>) ions using first-principles calculations. Li<sup>+</sup> incorporation induces a semiconductor-to-metal transition in CrPS<sub>4</sub> and triggers a switching from an out-of-plane antiferromagnetism state to an in-plane ferromagnetic state. This is accompanied by an increase of the ordering temperature, reaching a 5-fold enhancement for Li<sub>0.5</sub>CrPS<sub>4</sub>. TBA<sup>+</sup> intercalation expands the vdW gap, decoupling CrPS<sub>4</sub> layers and stabilizing in-plane ferromagnetism with <i>T</i><sub>C</sub> > 100 K. Furthermore, it enhances magnon group velocities and yields more isotropic magnon transport. This work highlights intercalation as a powerful approach for tailoring magnetism, paving the way for tunable 2D-layered magnetic materials for spintronic and magnonic applications.