Abstract
Ferroic polarization in hybrid perovskites is crucial for enhancing photovoltaic performance and developing potential electronic applications. Controlling ferroic polarization with an optical field enables probing of ferroic polarization without the unwanted interface ionic effects caused by electronic contacts. This study employs ultrafast near-infrared photoexcitation to control dynamic structural transitions in soft single crystalline hybrid Cu (II) halide perovskites, achieving a long-lived polar state (beyond 104 s) at room temperature. We probe reversible long-lived polar domains under near-infrared photoexcitation using in-situ second harmonic generation microscopy. Theoretical calculation informs the polar lattice microstrain likely induced by anisotropic structure deformation in octahedral copper halide under near-infrared photoexcitation. The reversible slow structure deformation is further confirmed by in-situ photo-induced X-ray diffraction measurement. This work provides a material platform for understanding, controlling, and probing polarization under photoexcitation. Our methodology enables the identification of previously undiscovered polar phases in ferroelectric halide perovskites.
| Original language | English |
|---|---|
| Article number | 7230 |
| Journal | Nature Communications |
| Volume | 16 |
| Issue number | 1 |
| DOIs | |
| State | Published - Dec 2025 |
Funding
This work was supported by Virginia Tech’s Materials Characterization Facility under the Institute for Critical Technology and Applied Science, the Macromolecules Innovation Institute, and the Office of the Vice President for Research and Innovation. L.Q. acknowledges the support from the National Science Foundation under the Early CAREER Research Program 2440516. G.A.K. acknowledges the partial support by the Air Force Office of Scientific Research under award numbers FA9550-17-1-0341 and FA9550-24-1-0059, as well as the L.C. Hassinger Fellowship. Work performed at the Advanced Photon Source, U.S. Department of Energy Office (DOE) of Science User Facility, was supported by the U.S. DOE, Office of Basic Energy Sciences, under Contract No. DE-AC02-06CH11357. The purchase of the Xenocs Xeuss 3.0 SAXS/WAXS instrument used to obtain results included in this publication was supported by the National Science Foundation under the award DMR MRI 2018258. We thank the support of the National Science Foundation under CHE-1726077 for crystallography experiments. The DFT calculation work at the University of Toledo is supported as part of the Center for Hybrid Organic Inorganic Semiconductors for Energy (CHOISE) an Energy Frontier Research Center funded by the Office of Basic Energy Sciences, Office of Science within the US Department of Energy. The first-principles calculations were performed using computational resources sponsored by the Department of Energy’s Office of Energy Efficiency and Renewable Energy located at the National Renewable Energy Laboratory, and the resources of the National Energy Research Scientific Computing Center (NERSC), a US Department of Energy Office of Science User Facility located at Lawrence Berkeley National Laboratory, operated under contract DE-AC02-05CH11231 using NERSC awards BES-ERCAP0028897 and BES-ERCAP0032847. SHG Microscopy at the Molecular Foundry was supported by the Office of Science, Office of Basic Energy Sciences, of the U.S. Department of Energy under Contract No. DE-AC02-05CH11231. P.B. and R.R. acknowledge the support of the Army Research Office under the ETHOS MURI via cooperative agreement W911NF-21-2-0162. Work at the Molecular Foundry was supported by the Office of Science, Office of Basic Energy Sciences, of the U.S. Department of Energy under Contract No. DE-AC02-05CH11231. Y.D. acknowledges the support from Virginia Tech Presidential Postdoctoral Fellowship.