Anisotropy and phonon modes from analysis of the dielectric function tensor and inverse dielectric function tensor of monoclinic yttrium orthosilicate

TL;DR

This study characterizes the dielectric tensor and phonon modes of monoclinic Y$_2$SiO$_5$ using advanced spectroscopic ellipsometry and density functional theory, revealing detailed phonon properties and validating a generalized Lyddane-Sachs-Teller relation.

Contribution

It introduces a novel eigendielectric displacement loss vector summation approach with anharmonic broadening for monoclinic materials and compares experimental results with DFT calculations.

Findings

Excellent agreement between measured and modeled dielectric tensor elements.

Identification of 23 A$_{ ext{u}}$ and 22 B$_{ ext{u}}$ phonon modes and their orientations.

Validation of a generalized Lyddane-Sachs-Teller relation for monoclinic materials.

Abstract

We determine the frequency dependence of the four independent Cartesian tensor elements of the dielectric function for monoclinic symmetry Y$_2$SiO$_5$ using generalized spectroscopic ellipsometry from 40-1200 cm$^{-1}$. Three different crystal cuts, each perpendicular to a principle axis, are investigated. We apply our recently described augmentation of lattice anharmonicity onto the eigendielectric displacement vector summation approach [A. Mock et al., Phys. Rev. B 95, 165202 (2017)], and we present and demonstrate the application of an eigendielectric displacement loss vector summation approach with anharmonic broadening. We obtain excellent match between all measured and model calculated dielectric function tensor elements and all dielectric loss function tensor elements. We obtain 23 A$_{\mathrm{u}}$ and 22 B$_{\mathrm{u}}$ symmetry long wavelength active transverse and longitudinal optical mode parameters including their eigenvector orientation within the monoclinic lattice. We perform density functional theory calculations and obtain 23 A$_{\mathrm{u}}$ symmetry and 22 B$_{\mathrm{u}}$ transverse and longitudinal optical mode parameters and their orientation within the monoclincic lattice. We compare our results from ellipsometry and density functional theory and find excellent agreement. We also determine the static and above reststrahlen spectral range dielectric tensor values and find a recently derived generalization of the Lyddane-Sachs-Teller relation for polar phonons in monoclinic symmetry materials satisfied [M. Schubert, Phys. Rev. Lett. 117, 215502 (2016)].