Tailoring spin waves in 2D transition metal phosphorus trichalcogenides via atomic-layer substitution

Abstract: The family of two-dimensional (2D) van der Waals transition metal phosphorus trichalcogenides has received a renewed interest due to their intrinsic 2D antiferromagnetism, which proves them as unprecedented and highly tunable building blocks for spintronics and magnonics at the single-layer limit. Herein, motivated by the exciting potential of atomic-substitution demonstrated in Janus transition metal dichalcogenides, we investigate the crystal, electronic and magnetic structure of selenized Janus monolayers based on MnPS$3$ and NiPS$_3$ from first-principles. In addition, we calculate the magnon dispersion and perform real-time real-space atomistic dynamic simulations to explore the propagation of spin waves in MnPS$_3$, NiPS$_3$, MnPS${1.5}$Se${1.5}$ and NiPS${1.5}$Se$_{1.5}$. Our calculations predict a drastic enhancement of magnetic anisotropy and the emergence of large Dzyaloshinskii-Moriya interactions, which arises from the induced broken inversion symmetry in the 2D Janus layers. These results pave the way to the development of Janus 2D transition metal phosphorus trichalcogenides and highlight their potential for magnonic applications.