MnPS3, a novel ternary-layered material, has
attracted
extensive attention in materials, physics, and chemistry owing to
its excellent electrical transport and photoelectric properties. Pressure
is a useful technique to explore unprecedented phenomena and properties
in condensed matter. In this study, combining high-pressure Raman
spectroscopy, high-pressure absorption spectroscopy measurements,
and first-principles calculations, the pressure-induced lattice and
electronic structural evolutions of multilayer MnPS3 were
uncovered. A pressure-induced lifted symmetry (layer sliding) of multilayer
MnPS3 from the C2/m-staggered
P-dimer phase (phase I) to P3̅1m aligned P-dimer phase (phase II) at 6.7 GPa was demonstrated, evidenced
by the overlap of Eg5 and A1g3 modes under high pressure and further first-principles calculations.
Meanwhile, the linearly decreased optical band gap with pressure indicated
that the charge-transfer excitations that define the gap were confined
in intra-slab in nature regardless of the interlayer sliding. Further
calculated band gap structure also suggested that no obvious electronic
structural phase transition occurred in multilayer MnPS3 during the pressure-induced phase transition of multilayer MnPS3 except from a decreased band gap with pressure. In addition,
both the results of absorption spectroscopy measurements and first-principles
calculation demonstrated that multilayer MnPS3 remained
to be a direct band gap semiconductor up to 21.8 GPa. Our findings
are of great significance in expanding the application of compressive
MnPS3 in photoelectric devices.