First-Principles-Based Strain and Temperature Dependent Ferroic Phase Diagram of SrMnO$_3$

TL;DR

This study uses first-principles calculations to map the strain and temperature-dependent ferroic phases of SrMnO$_3$, revealing tunable magnetic and ferroelectric properties with potential for electric field control.

Contribution

It provides the first comprehensive phase diagram of SrMnO$_3$ based on parameter-free density functional theory and simulations, highlighting strain-induced magnetic and ferroelectric transitions.

Findings

Ferroelectric Curie temperature increases with strain and crosses magnetic transition temperature.

Multiple magnetic transitions occur under tensile strain with moderate critical temperature variation.

Coexistence of ferroelectric and ferromagnetic order observed above 4% strain.

Abstract

Perovskite structure SrMnO$_3$ is a rare example of a multiferroic material where strain-tuning and/or cation substitution could lead to coinciding magnetic and ferroelectric ordering temperatures, which would then promise strong magnetoelectric coupling effects. Here, we establish the temperature and strain dependent ferroic phase diagram of SrMnO$_3$ using first-principles-based effective Hamiltonians. All parameters of these Hamiltonians are calculated using density functional theory, i.e., no fitting to experimental data is required. Temperature dependent properties are then obtained from Monte Carlo and molecular dynamics simulations. We observe a sequence of several magnetic transitions under increasing tensile strain, with a moderate variation of the corresponding critical temperatures. In contrast, the ferroelectric Curie temperature increases strongly after its onset around 2.5\,\% strain, and indeed crosses the magnetic transition temperature just above 3\,\% strain. Our results indicate pronounced magnetoelectric coupling, manifested in dramatic changes of the magnetic ordering temperatures and different magnetic ground states as function of the ferroelectric distortion. In addition, coexisting ferroelectric and ferromagnetic order is obtained for strains above 4\,\%. Our calculated phase diagram suggests the possibility to control the magnetic properties of SrMnO$_3$ through an applied electric field, significantly altering the magnetic transition temperatures, or even inducing transitions between different magnetic states.