Structure, property and magneto-optical interaction of wide-band-gap layered magnetism near the Neel temperature with antiferromagnetic to paramagnetic transition

This work reports structural, optical, and vibrational behaviors, revealing the N ' eel ordering transformation of MnPS3 via temperature-dependent structure and optical measurements. In antiferromagnetic (AFM) state, MnPS3 exhibits high magnon-phonon coupling due to the ordered spin in the 3d orbital of the Mn2+ cation, which influences the intrinsic lattice and vibrational properties. The band-edge excitons of thin-layered MnPS3 were detected via micro-thermoreflectance (mu TR) measurements at 20-300 K. When below the Neel temperature (T-N = 78 K), MnPS3 exhibits two excitons, indicating the availability of a magnetic transition from the AFM to paramagnetic (PM) ordering. The direct-gap exciton of MnPS3 (E-1(OX)) is at similar to 2.632 eV at 300 K and it shifts to a higher energy of similar to 2.846 eV at 20 K. With T < T-N, an additional exciton (AMX) appeared at similar to 0.16 eV lower than E-1(OX). It shows stronger at 20 K. The E-1(OX) feature can be observed by mu TR, and it shows an anomalous temperatureintensity change with the maximum amplitude at T-N due to the spin-order transition from the AFM to the PM state. This work explores optical properties related to the magnetic transition of a wide-band-gap layered magnetism, which may be suitable for further magneto-optical device applications.

Automated summary

This work investigates the structural, optical, and vibrational behaviors of MnPS3 and discovers the N'eel ordering transformation through temperature-dependent structure and optical measurements. It is found that MnPS3 exhibits high magnon-phonon coupling in the antiferromagnetic state, which is influenced by the ordered spin in the 3d orbital of the Mn2+ cation. The study also detects band-edge excitons of thin-layered MnPS3 through micro-thermoreflectance measurements, revealing a magnetic transition from antiferromagnetic to paramagnetic ordering below the Neel temperature.