Controlling Magnetism in the 2D van der Waals Antiferromagnet CrPS$_4$ via Ion Intercalation

Fuente: arXiv
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Main Authors: Ruiz, Alberto M., López-Alcalá, Diego, Rivero-Carracedo, Gonzalo, Shumilin, Andrei, Baldoví, José J.
Format: Preprint
Published: 2025
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author Ruiz, Alberto M.
López-Alcalá, Diego
Rivero-Carracedo, Gonzalo
Shumilin, Andrei
Baldoví, José J.
author_facet Ruiz, Alberto M.
López-Alcalá, Diego
Rivero-Carracedo, Gonzalo
Shumilin, Andrei
Baldoví, José J.
contents Two-dimensional van der Waals (vdW) magnetic materials are versatile platforms for tailoring electronic and magnetic properties, in which the insertion of chemical species into their interlayer gaps offers a powerful route to engineer magnetism. Here, we focus on the A-type antiferromagnetic semiconductor CrPS$_4$ (T$_N$ = 38 K) and investigate its electronic and magnetic properties upon intercalation of lithium (Li$^+$) and organic tetrabutylammonium (TBA$^+$) ions using first-principles calculations. Our results show that Li$^+$ incorporation induces a semiconductor-to-metal transition in CrPS$_4$ and selectively modifies its magnetic behaviour: switching from out-of-plane to in-plane antiferromagnetism, followed by an in-plane ferromagnetic ground state at higher intercalation levels. This is accompanied by a continuous increase of the ordering temperature, reaching a fivefold enhancement for Li$_{0.5}$CrPS$_4$. Similarly, TBA$^+$ intercalation expands the vdW gap, decoupling CrPS$_4$ layers and stabilising in-plane ferromagnetism with a T$_C$ above 100 K. Furthermore, it also modifies magnon propagation, leading to enhanced group velocities and a more isotropic magnon transport. This work highlights intercalation as a powerful and versatile approach for controlling magnetic behaviour and spin dynamics, paving the way for the design of tunable 2D layered magnetic materials for spintronic and magnonic applications.
format Preprint
id arxiv_https___arxiv_org_abs_2510_12371
institution arXiv
publishDate 2025
record_format arxiv
spellingShingle Controlling Magnetism in the 2D van der Waals Antiferromagnet CrPS$_4$ via Ion Intercalation
Ruiz, Alberto M.
López-Alcalá, Diego
Rivero-Carracedo, Gonzalo
Shumilin, Andrei
Baldoví, José J.
Materials Science
Mesoscale and Nanoscale Physics
Two-dimensional van der Waals (vdW) magnetic materials are versatile platforms for tailoring electronic and magnetic properties, in which the insertion of chemical species into their interlayer gaps offers a powerful route to engineer magnetism. Here, we focus on the A-type antiferromagnetic semiconductor CrPS$_4$ (T$_N$ = 38 K) and investigate its electronic and magnetic properties upon intercalation of lithium (Li$^+$) and organic tetrabutylammonium (TBA$^+$) ions using first-principles calculations. Our results show that Li$^+$ incorporation induces a semiconductor-to-metal transition in CrPS$_4$ and selectively modifies its magnetic behaviour: switching from out-of-plane to in-plane antiferromagnetism, followed by an in-plane ferromagnetic ground state at higher intercalation levels. This is accompanied by a continuous increase of the ordering temperature, reaching a fivefold enhancement for Li$_{0.5}$CrPS$_4$. Similarly, TBA$^+$ intercalation expands the vdW gap, decoupling CrPS$_4$ layers and stabilising in-plane ferromagnetism with a T$_C$ above 100 K. Furthermore, it also modifies magnon propagation, leading to enhanced group velocities and a more isotropic magnon transport. This work highlights intercalation as a powerful and versatile approach for controlling magnetic behaviour and spin dynamics, paving the way for the design of tunable 2D layered magnetic materials for spintronic and magnonic applications.
title Controlling Magnetism in the 2D van der Waals Antiferromagnet CrPS$_4$ via Ion Intercalation
topic Materials Science
Mesoscale and Nanoscale Physics
url https://arxiv.org/abs/2510.12371