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Uncovering Multiple Intrinsic Chiral Phases in (PEA)2PbI4 Halide Perovskites

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JOURNAL OF PHYSICAL CHEMISTRY LETTERS
卷 14, 期 21, 页码 4901-4907

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AMER CHEMICAL SOC
DOI: 10.1021/acs.jpclett.3c00685

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In this work, the anharmonic ground state of the (PEA)(2)PbI4 compound was thoroughly investigated using low-temperature X-ray diffraction and photoluminescence spectroscopy, supported by density functional theory calculations. It was found that the ground state has two coexisting chiral sublattices and uneven anharmonicity, where the state population can be tuned by surface effects. These findings uncover a disordered ground state that may induce intrinsic grain boundaries, which are important in practical applications.
Two-dimensional (2D) halide perovskitesoffer a uniqueplatformfor investigating the ground state of materials possessing significantanharmonicity. In contrast to three-dimensional perovskites, their2D counterparts offer substantially fewer degrees of freedom, resultingin multiple well-defined crystal structures. In this work, we thoroughlyinvestigate the anharmonic ground state of the benchmark (PEA)(2)PbI4 compound, using complementary informationfrom low-temperature X-ray diffraction (XRD) and photoluminescencespectroscopy, supported by density functional theory calculations.We extrapolate four crystallographic configurations from low-temperatureXRD. These configurations imply that the ground state has an intrinsicdisorder stemming from two coexisting chiral sublattices, each witha bioriented organic spacer molecule. We further show evidence thatthese chiral structures form unevenly populated ground states, portrayinguneven anharmonicity, where the state population may be tuned by surfaceeffects. Our results uncover a disordered ground state that may induceintrinsic grain boundaries, which cannot be ignored in practical applications.

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