A Comparative Study of A(2)SiF(6) (A = Cs, K) Phosphor Host Matrices: Linear Combination of Atomic Orbital Hybrid Density Functional Theory Calculations

A(2)SiF(6) (A = Cs, K) 磷光体基质的比较研究:原子轨道杂化密度泛函理论计算的线性组合

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Abstract

Cesium hexafluorosilicate (Cs(2)SiF(6), CSF) and potassium hexafluorosilicate (K(2)SiF(6), KSF) compounds are suitable hosts for luminescent impurities. In this work, the results of first-principle calculations of the basic properties of both these compounds are discussed and compared with the available experimental and theoretical data. The simulations were performed using the CRYSTAL23 computer code within the linear combination of atomic orbitals (LCAO) method of the density functional theory (DFT) and the advanced hybrid DFT-HF exchange-correlation B1WC functional. A comparative study of the structural, electronic, and elastic properties of the two materials is presented, along with a study of the dependence of properties on external pressure in the range of 0-20 GPa. In particular, the electronic properties with an emphasis on the effective atomic charges (by means of Mulliken analysis) and the chemical bonding properties (by means of crystal orbital overlap population (COOP) analysis) were addressed, with regards to the pressure effects. The structure of the valence bands at 0 and 20 GPa was compared. The vibrational properties of CSF and KSF were calculated, including the simulation of the one-phonon IR and Raman spectra. The calculated Raman spectra exhibit excellent agreement with the experimental ones. The pressure dependences of sound speeds and the Debye temperature are evaluated.

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