Phonons and Lattice Dielectric Properties of Zirconia

Abstract

We have performed a first-principles study of the structural and vibrational properties of the three low-pressure (cubic, tetragonal, and especially monoclinic) phases of ZrO2, with special attention to the computation of the zone-center phonon modes and related dielectric properties. The calculations have been carried out within the local-density approximation using ultrasoft pseudopotentials and a plane-wave basis. The fully relaxed structural parameters are found to be in excellent agreement with experimental data and with previous theoretical work. The total-energy calculations correctly reproduce the energetics of the ZrO2 phases, and the calculated zone-center phonon frequencies yield good agreement with the infrared and Raman experimental frequencies in the monoclinic phase. The Born effective charge tensors are computed and, together with the mode eigenvectors, used to decompose the lattice dielectric susceptibility tensor into contributions arising from individual infrared-active phonon modes. This work has been partially motivated by the potential for ZrO2 to replace SiO2 as the gate-dielectric material in modern integrated-circuit technology.

10 pages, with 4 postscript figures embedded. Uses REVTEX and epsf macros. Also available at http://www.physics.rutgers.edu/~dhv/preprints/zhao_zro2/index.html

Cited by in corpus (14)

• First-principles study of structural, vibrational and lattice dielectric properties of hafnium oxide
• Antiferroelectricity in thin film ZrO2 from first principles
• Structural, electronic, and optical properties of ZrO2 from ab initio calculations
• First-principles theoretical evaluation of crystalline zirconia and hafnia as gate oxides for Si microelectronics
• Structural and dielectric properties of amorphous ZrO2 and HfO2
• Amorphous ZrO2 from Ab-initio molecular dynamics: Structural, electronic and dielectric properties
• Structure and Dielectric Properties of Amorphous High-kappa Oxides: HfO2, ZrO2 and their alloys
• Structural and dielectric properties of Sr${}_2$TiO${}_4$ from first principles
• Magnetism and half-metallicity at the O surfaces of ceramic oxides
• Fatigue and retention in the growth window of ferroelectric Hf0.5Zr0.5O2 thin films
• Discovery prospects with the Dark-photons & Axion-Like particles Interferometer
• Growth Stress Induced Tunability of Dielectric Constant in Thin Films
• Theory of Ferroelectric ZrO${}_2$ Monolayers on Si
• Large thermal anisotropy in monoclinic niobium trisulfide: A thermal expansion tensor study