High-frequency/high-field electron paramagnetic resonance generalized spectroscopic ellipsometry characterization of Cr3+ in β-Ga2O3

Electron paramagnetic resonance of Cr3+ ions in beta-Ga2O3 is investigated using terahertz spectroscopic ellipsometry under magnetic field sweeping, a technique that enables the polarization resolving capabilities of ellipsometry for magnetic resonance measurements. We employed a single-crystal chromium-doped beta-Ga2O3 sample, grown by the Czochralski method, and performed ellipsometry measurements at magnetic field strengths ranging from 2 to 8 T, at frequencies from 82 to 125 and 190 to 230 GHz, and at a temperature of 15 K. Analysis of the frequency-field diagrams derived from all Mueller matrix elements allowed us to differentiate between the effects of electron spin Zeeman splitting and zero-field splitting and to accurately determine the anisotropic Zeeman splitting g-tensor and the zero-field splitting parameters. Our results confirm that Cr3+ ions predominantly substitute into octahedral gallium sites. Line shape analysis of Mueller matrix element spectra using the Bloch-Brillouin model provides the spin volume concentration of Cr3+ sites, showing very good agreement with results from chemical analysis by inductively coupled plasma-optical emission spectroscopy and suggesting minimal occupation of sites with inactive electron paramagnetic resonance. This study enhances our understanding of the magnetic and electronic properties of chromium-doped beta-Ga2O3 and demonstrates the effectiveness of high-frequency/high-field electron paramagnetic resonance generalized spectroscopic ellipsometry for characterizing defects in ultrawide-bandgap semiconductors.