Spin-Phonon Coupling and High Pressure Phase Transitions of RMnO3 (R= Ca and Pr): An Inelastic Neutron Scattering and First Principle Studies

TL;DR

This study combines inelastic neutron scattering and first-principles calculations to investigate spin-phonon coupling, phase transitions, and pressure effects in RMnO3 (R=Ca, Pr), revealing pressure-induced insulator-metal transition and Jahn-Teller distortion suppression.

Contribution

It provides new insights into the pressure-dependent structural and magnetic properties of RMnO3, highlighting differences between CaMnO3 and PrMnO3 and challenging previous reports on phase stability.

Findings

Pressure induces insulator-metal transition in PrMnO3.

CaMnO3 remains stable up to 60 GPa without phase transition.

Jahn-Teller distortion is suppressed under pressure in PrMnO3.

Abstract

We report inelastic neutron scattering measurements over 7-1251 K in CaMnO3 covering various phase transitions, and over 6-150 K in PrMnO3 covering the magnetic transition. The excitations around 20 meV in CaMnO3 and at 17 meV in PrMnO3 are found to be associated with magnetic origin. In spite of similarity of the structure of the two compounds, the neutron inelastic spectrum of PrMnO3 exhibits broad features at 150 K unlike well-defined peaks in the spectrum of CaMnO3. This might result from the difference in nature of interactions in the two compounds (magnetic and Jahn-Teller distortion). The interpretation and analysis of the observed phonon spectra have been performed using ab-initio phonon calculations. We also discuss the effect of pressure on the structural distortions in the orthorhombic phase of CaMnO3 and PrMnO3. On application of pressure, we found that the variations of Mn-O distances are isotropic for CaMnO3 and highly anisotropic for PrMnO3. The calculated structure as a function of pressure in PrMnO3 shows that suppression of Jahn-Teller distortion and insulator to metal transition occurs simultaneously. Our calculations show that this transition may not be associated with the occurrence of the tetragonal phase above 20 GPa as reported in the literature, since the tetragonal phase is found to be dynamically unstable although it is found to be energetically favored over the orthorhombic phase above 20 GPa. CaMnO3 does not show any phase transition up to 60 GPa.