Revealing the free energy landscape of halide perovskites: Metastability and transition characters in CsPbBr_3 and MAPbI_3
arxiv(2023)
摘要
Halide perovskites have emerged as a promising class of materials for
photovoltaic applications. A challenge in these applications is how to prevent
the crystal structure from degradation to photovoltaically inactive phases,
which requires an understanding of the free energy landscape of these
materials. Here, we uncover the free energy landscape of two prototypical
halide perovskites, CsPbBr_3 and MAPbI_3 via atomic scale simulations using
umbrella sampling and machine-learned potentials. For CsPbBr_3 we find very
small free energy differences and barriers close to the transition temperatures
for both the tetragonal-to-cubic and the orthorhombic-to-tetragonal transition.
For MAPbI_3, however, the situation is more intricate. In particular the
orthorhombic-to-tetragonal transition exhibits a large free energy barrier and
there are several competing tetragonal phases. Using large-scale molecular
dynamics simulations we explore the character of these transition and observe
latent heat and a discrete change in structural parameters for the
tetragonal-to-cubic phase transition in both CsPbBr_3 and MAPbI_3
indicating first-order transitions. We find that in MAPbI_3 the orthorhombic
phase has an extended metastability range and furthermore identify a second
metastable tetragonal phase. Finally, we compile a phase diagram for MAPbI_3
that includes potential metastable phases.
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