Exploring the magnetic ordering in atomically thin antiferromagnetic MnPSe3 by Raman spectroscopy

Magnetic ground state in the two-dimensional (2D) limit is fundamental issue and essential building block for next-generation nano-spintronic devices. Here, we report the observation of antiferromagnetic ordering in 2D MnPSe3 by Raman spectroscopy. Thickness and temperature-dependent Raman spectroscopy confirms the antiferromagnetic ordering in MnPSe3 down to atomically thin layers with trivial thickness-dependent Néel temperature from multiple evidence: the enhanced phonon Raman intensities, significant deviations from the anharmonic contribution of phonon frequencies due to spin-phonon coupling, and the occurrence of one-magnon Raman peak below the Néel temperature. The Raman vibration mode evolution studies reveal that the magnetic ion d-electron transfer is mediated by the nonmagnetic clusters of [P2Se6]4-. Our work motivates the explorations of intriguing spin dynamics in 2D antiferromagnet and promotes the development of novel spintronic devices.