Infrared dielectric functions and Brillouin zone center phonons of $\alpha$-Ga$_2$O$_3$ compared to $\alpha$-Al$_2$O$_3$

TL;DR

This study combines experimental and computational methods to determine the dielectric functions and phonon properties of $oldsymbol{ extit{ extalpha}}$-Ga$_2$O$_3$, compares them with $oldsymbol{ extit{ extalpha}}$-Al$_2$O$_3$, and explores implications for alloy systems.

Contribution

It provides comprehensive experimental and theoretical data on phonon modes and dielectric properties of $ extit{ extalpha}$-Ga$_2$O$_3$ and $ extit{ extalpha}$-Al$_2$O$_3$, including mode shifts and eigenvector overlaps.

Findings

Excellent agreement between experiment and theory.

Computed phonon mode shifts between Ga$_2$O$_3$ and Al$_2$O$_3$.

Discussed mode evolution in ternary alloys.

Abstract

We determine the anisotropic dielectric functions of rhombohedral $\alpha$-Ga$_2$O$_3$ by far-infrared and infrared generalized spectroscopic ellipsometry and derive all transverse optical and longitudinal optical phonon mode frequencies and broadening parameters. We also determine the high frequency and static dielectric constants. We perform density functional theory computations and determine the phonon dispersion for all branches in the Brillouin zone, and we derive all phonon mode parameters at the Brillouin zone center including Raman-active, infrared-active, and silent modes. Excellent agreement is obtained between our experimental and computation results as well as among all previously reported partial information from experiment and theory. We also compute the same information for $\alpha$-Al$_2$O$_3$, the binary parent compound for the emerging alloy of $\alpha$-(Al$_{x}$Ga$_{1-x}$)$_2$O$_3$, and use results from previous investigations [Schubert, Tiwald, and Herzinger, Phys. Rev. B 61, 8187 (2000)] to compare all properties among the two isostructural compounds. From both experimental and theoretical investigations we compute the frequency shifts of all modes between the two compounds. Additionally, we calculate overlap parameters between phonon mode eigenvectors and discuss the possible evolution of all phonon modes into the ternary alloy system and whether modes may form single mode or more complex mode behaviors.