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Article Abstract
We present a systematic high-pressure investigation of the chlorine-functionalized two-dimensional hybrid perovskite (ClPMA)PbI, integrating high-pressure synchrotron powder X-ray diffraction (HP-PXRD), photoluminescence spectroscopy (HP-PL), and first-principles density functional theory (DFT) calculations. Under hydrostatic compression up to 6.18 (±0.42) GPa, HP-PXRD reveals anisotropic lattice contraction (Δ = 4.06%, Δ = 3.00%, Δ = 8.66%) with a bulk modulus of 16.8 (±1.5) GPa ( = 34.1 TPa) and the onset of amorphization near 6.18 (±0.42) GPa. DFT-optimized structures corroborate progressive PbI octahedral flattening leading to reduced interlayer spacing and enhanced Cl···I, Cl···H, and I···H interactions. The full elastic tensor indicates moderate anisotropy ( = 2.1, = 2.63) yet large Poisson's ratios (-0.196 to 0.67), unveiling coexisting auxetic and elastic deformation pathways. HP-PL spectra exhibit a continuous red shift from 525.2 nm to ∼630.5 nm and intensity quenching, attributable to bond-contraction-induced bandgap narrowing and pressure-enhanced nonradiative recombination in the partially amorphous matrix. DFT band-structure calculations confirmed the pressure-dependent direct-gap evolution and maintaining k-space valence-band maximum and conduction-band minimum alignment. These findings elucidate the structural, mechanical, and optoelectronic tunability of (ClPMA)PbI, underscoring its promise for strain-engineered optoelectronic devices.
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