Janus Engineering of Polar Magnetism and Valley Splitting in CuCrP2X6 (X: S, Se) Monolayers

Voloshina, Elena; Dedkov, Yuriy (2026) Janus Engineering of Polar Magnetism and Valley Splitting in CuCrP2X6 (X: S, Se) Monolayers. The Journal of Physical Chemistry Letters, 17 (25). pp. 7020-7027. ISSN 1948-7185

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Abstract

We investigate the interplay of multiferroicity and structural asymmetry in two-dimensional CuCrP2X6 (X: S, Se) and the Janus CuCrP2S3Se3 monolayer using density functional theory. While pristine CuCrP2S6 exhibits an antiferroelectric ground state with in-plane magnetic anisotropy, complete or partial substitution of S by Se fundamentally alters both lattice polarity and magnetic behavior. In particular, the Janus CuCrP2S3Se3 structure stabilizes a ferroelectric phase with a finite out-of-plane dipole moment arising from asymmetric Cu+ displacement. This polarity, combined with enhanced spin–orbit coupling, drives a transition to robust out-of-plane magnetic anisotropy and induces sizable spontaneous valley splitting at the K and K′ points. All studied monolayers are predicted to be ferromagnetic semiconductors with composition-dependent band gaps and exchange interactions. The coupling between ferroelectric polarization and magnetic order in the Janus system suggests a route toward electric-field control of magnetism in a single-phase material. These findings highlight Janus engineering of transition metal phosphorus trichalcogenides as an effective strategy to realize intrinsically coupled ferroic and valleytronic functionalities for next-generation (opto)spintronic applications.

Item Type:	Article
Additional Information:	"This document is the Accepted Manuscript version of a Published Article that appeared in final form in The Journal of Physical Chemistry Letters, Copyright © 2026 American Chemical Society. To access the final published article, see ACS Articles on Request."
Uncontrolled Keywords:	MPX3; Monolayers; Janus Engineering
Subjects:	NATURAL SCIENCES > Physics > Condensed Matter Physics
Divisions:	Theoretical Physics Division
Depositing User:	Elena Voloshina
Date Deposited:	07 Jul 2026 06:09
URI:	https://fulir.irb.hr:/id/eprint/12028
DOI:	10.1021/acs.jpclett.6c01517

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