Anisotropic Rashba splitting in Pt-based Janus monolayers PtXY (X,Y = S, Se, or Te)

Recent studies have demonstrated the feasibility of synthesizing two-dimensional (2D) Janus materials which possess intrinsic structural asymmetry. Hence, we performed a systematic first-principles study of 2D Janus transition metal dichalcogenide (TMD) monolayers based on PtXY (X,Y = S, Se, or Te). Our calculated formation energies show that these monolayer Janus structures retain the 1T phase. Furthermore, phonon spectral calculations confirm that these Janus TMD monolayers are thermodynamically stable. We found that PtSSe, PtSTe, and PtSeTe exhibit an insulating phase with indirect band gaps of 2.108, 1.335, and 1.221 eV, respectively, from hybrid functional calculations. Due to the breaking of centrosymmetry in the crystal structure, the spin–orbit coupling (SOC)-induced anisotropic Rashba splitting is observed around the M point. The calculated Rashba strengths from M to Γ (α(M–Γ)(R)) are 1.654, 1.103, and 0.435 eV Å(−1), while the calculated values from M to K (α(M–K)(R)) are 1.333, 1.244, and 0.746 eV Å(−1), respectively, for PtSSe, PtSTe, and PtSeTe. Interestingly, the spin textures reveal that the spin-splitting is mainly attributed to the Rashba effect. However, a Dresselhaus-like contribution also plays a secondary role. Finally, we found that the band gaps and the strength of the Rashba effect can be further tuned through biaxial strain. Our findings indeed show that Pt-based Janus TMDs demonstrate the potential for spintronics applications.