Halogen-Driven Tunability in Cubic KZnX(3) (X = F-I) Halide Perovskites: A First-Principles Study

卤素驱动的立方KZnX(3) (X = FI)卤化物钙钛矿的可调谐性:第一性原理研究

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Abstract

This paper systematically studied the structural, mechanical, electronic, and optical characteristics of cubic KZnX(3) (X = F, Cl, Br, and I) perovskites through the density functional theory (DFT) in the Quantum Espresso framework. Structural optimization and stability analyses confirm that all compounds crystallize in the cubic Pm-3m phase and are thermodynamically, mechanically, and dynamically stable. Elastic constants indicate that the materials are anisotropic and ductile in nature. Calculations of Debye temperatures show a systematic decrease of 402 K (KZnF(3)) to 158 K (KZnI(3)), which is related to the increasing mass of halogen and its impact on the rigidity of the lattice. Electronic structure calculations show that all compounds are indirect bandgap semiconductors, with bandgaps systematically decreasing from 4.24 eV (KZnF(3)) to 0.86 eV (KZnI(3)) at the HSE06 level, enabling tunable semiconducting characteristics for optoelectronic applications. The analysis of the density of states and charge density indicates that the bonding between Zn and X is mixed ionic and covalent and that the bonding between K and X is mostly ionic. Calculations of optical properties show an increase in polarizability, absorption, refractive index and plasmonic response when heavier halogen is used, highlighting the potential of KZnX(3) perovskites for photovoltaic and optoelectronic devices. Overall, halogen substitution in KZnX(3) provides an effective strategy for tailoring electronic and optical properties.

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