Abstract
The mechanisms governing pressure-induced amorphization and its reversibility in halide perovskites are not yet fully understood, particularly the contribution of local disorder. We performed high-pressure synchrotron total X-ray scattering and reverse Monte Carlo (RMC) big-box modeling using CsPbBr3 as a model system to investigate short-range structural evolution in both the ordered and partially amorphous phases. While diffraction data indicate that long-range order persists up to 2 GPa, pair distribution function (PDF) analysis reveals significant local distortions, including PbBr6 octahedral tilting and Cs displacement, which influence the bandgap through a complex interplay between bond compression and angular tilting. Beyond 2 GPa, CsPbBr3 undergoes partial amorphization, with significant disordering of Cs and Br, while the Pb sublattice remains preserved, allowing for structural recovery upon decompression. Our work, accounting for both short- and long-range structural evolution through RMC modeling, successfully captures how disorder shapes the structural response of halide perovskites under pressure.
| Original language | English |
|---|---|
| Article number | 7631 |
| Journal | Nature Communications |
| Volume | 16 |
| Issue number | 1 |
| DOIs | |
| State | Published - Dec 2025 |
Funding
This work was supported by the Department of Energy (DOE), Office of Science, Basic Energy Sciences, Materials Sciences and Engineering Division under Contract No. DE-AC02-76SF00515 (H.I.K., W.L.M., Y.L.). This research used resources of the Advanced Photon Source, a U.S. DOE Office of Science User Facility operated by Argonne National Laboratory under contract no. DE-AC02-06CH11357. This research used resources at the Spallation Neutron Source, a DOE Office of Science User Facility operated by the Oak Ridge National Laboratory. C.R.D. acknowledges a Stanford Center for Molecular Analysis and Design Fellowship and N.R.W. acknowledges a Stanford Interdisciplinary Graduate Fellowship. The authors thank Olaf Borkiewicz and Leighanne Gallington for assistance with PDF measurements. The mail-in program at Beamline 11-ID-B of the Advanced Photon Source contributed to the data. The authors thank Zhenxian Liu for assistance with high-pressure absorption measurements, which used beamline 22-IR-1 of the National Synchrotron Light Source II, a U.S. DOE Office of Science User Facility operated by the Brookhaven National Laboratory (DE-AC98- 06CH10886). Use of the 22-IR-1 beamline is supported by the National Science Foundation Division of Earth Sciences (EAR) SEES: Synchrotron Earth and Environmental Science (EAR-2223273) and Chicago/DOE Alliance Center (CDAC) DENA-0004153.