Achieving ultrahigh-color-purity circularly polarized luminescence (CPL) in low-dimensional chiral perovskites is challenging due to strong electron-phonon coupling caused by lead halide octahedral distortion. Herein, the circularly polarized piezoluminescence behaviors of six novel chiral perovskites, (/-3-XPEA)PbBr (PEA = phenethylamine; X = F, Cl, Br), were systematically investigated. Upon compression, (/-3-ClPEA)PbBr exhibits significant piezofluorochromic behaviors, transforming from yellow CPL to ultrahigh-color-purity deep-blue CPL. At 2.5 GPa, the deep-blue CPL intensity increases by an order of magnitude and its luminescence asymmetry factors () are amplified from the initial ±0.03 to ±0.1. (/-3-BrPEA)PbBr presents a similar piezochromic response, realizing deep-blue CPL at 1.7 GPa, while (/-3-FPEA)PbBr retains a yellow CPL under high pressure. High-pressure structural characterization and theoretical calculations confirm that pressure-enhanced halogen bonds reduce the penetration depth of /-3-BrPEA and /-3-ClPEA into the [PbBr] frameworks, significantly suppressing electron-phonon coupling and increasing magnetic transition dipole moment in (/-3-BrPEA)PbBr and (/-3-ClPEA)PbBr, which are responsible for the ultrahigh-purity deep-blue CPL and chirality amplification, respectively.
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