Crystal growth, measurement and modeling of the optical activity of $\alpha$-GeO$_2$. Comparison with $\alpha$-SiO$_2$

TL;DR

This study successfully grew high-quality bulk $ ext{GeO}_2$ crystals, measured their optical activity across a spectrum, and developed an empirical model linking optical properties to structural features, with implications for optical materials.

Contribution

It is the first to grow large bulk $ ext{GeO}_2$ crystals and measure their optical activity, providing new data and an empirical model for optical behavior based on structure.

Findings

Achieved up to 90% growth yield of bulk $ ext{GeO}_2$ crystals.

Measured optical activity of $ ext{GeO}_2$ and $ ext{SiO}_2$ across 0.3-2 μm.

Developed an empirical model describing optical activity based on susceptibility and structural pitch.

Abstract

This work aimed first at growing high quality bulk $\alpha$-GeO$_2$ crystals in their Quartz iso-structural form ($\alpha$-SiO$_2$), using a high temperature flux method. By optimizing the flux composition and the geometry and orientation of the seeds, it has been possible to achieve growth yields up to 90 % leading for the first time to bulk single crystals up to 3.5 cm$^3$. Thanks to the optical quality and size of the obtained crystals, the second step of this study was the measurement of the optical activity of $\alpha$-GeO$_2$ between 0.3 and 2 $\mu$m. This gave access to the value of one of the independent components of the gyration tensor (g33) as a function of the wavelength. An $\alpha$-SiO$_2$ slab have been used to validate our methodology. Both crystals show a magnitude of optical activity of 3.4x10$^{-5}$ rad/$\mu$m in the near IR range and great variations where the higher values are 3.4x10$^{-3}$ rad/$\mu$m and 1.7x10$^{-3}$ rad/$\mu$m at 0.3 $\mu$m for $\alpha$-GeO$_2$ and $\alpha$-SiO$_2$, respectively. The measurements are perfectly described by an empirical model that we propose and which relies on the macroscopic first-order electrical susceptibility and on the pitch of the structural helix compared to the wavelength of light.