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We demonstrate detection and measurement of electron paramagnetic spin resonances (EPR) of iron defects in utilizing generalized ellipsometry at frequencies between 110 and 170 GHz. The experiments are performed on an Fe-doped single crystal in a free-beam configuration in reflection at and magnetic fields between 3 and 7 T. In contrast with low-field, low-frequency EPR measurements, we observe all five transitions of the high-spin state simultaneously. We confirm that ferric is predominantly found at octahedrally coordinated Ga sites. We obtain the full set of fourth-order monoclinic zero-field splitting parameters for both octahedrally and tetrahedrally coordinated sites by employing measurements at multiple sample azimuth rotations. The capability of high-field EPR allows us to demonstrate that simplified second-order orthorhombic spin Hamiltonians are insufficient, and fourth-order terms as well as consideration of the monoclinic symmetry are needed. These findings are supported by computational approaches based on density-functional theory for second-order and on ligand-field theory for fourth-order parameters of the spin Hamiltonian. Terahertz ellipsometry is a way to measure spin resonances in a cavity-free setup. Its possibility of varying the probe frequency arbitrarily without otherwise changing the experimental setup offers unique means of truly disentangling different components of highly anisotropic spin Hamiltonians. Published by the American Physical Society2024more » « less
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The anisotropic permittivity parameters of monoclinic single crystal lutetium oxyorthosilicate, Lu2SiO5 (LSO), have been determined in the terahertz spectral range. Using terahertz generalized spectroscopic ellipsometry (THz-GSE), we obtained the THz permittivities along the a, b, and c⋆ crystal directions, which correspond to the εa, εb, and εc⋆ on-diagonal tensor elements. The associated off diagonal tensor element εac⋆ was also determined experimentally, which is required to describe LSO's optical response in the monoclinic a–c crystallographic plane. From the four tensor elements obtained in the model fit, we calculate the direction of the principal dielectric axes in the a–c plane. We find good agreement when comparing THz-GSE permittivities to the static permittivity tensors from previous infrared and density functional theory studies.more » « less
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Electron effective mass is a fundamental material parameter defining the free charge carrier transport properties, but it is very challenging to be experimentally determined at high temperatures relevant to device operation. In this work, we obtain the electron effective mass parameters in a Si-doped GaN bulk substrate and epitaxial layers from terahertz (THz) and mid-infrared (MIR) optical Hall effect (OHE) measurements in the temperature range of 38–340 K. The OHE data are analyzed using the well-accepted Drude model to account for the free charge carrier contributions. A strong temperature dependence of the electron effective mass parameter in both bulk and epitaxial GaN with values ranging from (0.18 ± 0.02) m0 to (0.34 ± 0.01) m0 at a low temperature (38 K) and room temperature, respectively, is obtained from the THz OHE analysis. The observed effective mass enhancement with temperature is evaluated and discussed in view of conduction band nonparabolicity, polaron effect, strain, and deviations from the classical Drude behavior. On the other hand, the electron effective mass parameter determined by MIR OHE is found to be temperature independent with a value of (0.200 ± 0.002) m0. A possible explanation for the different findings from THz OHE and MIR OHE is proposed.more » « less
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Mueller matrix spectroscopic ellipsometry is applied to determine anisotropic optical properties for a set of single-crystal rhombohedral structure α-(Al x Ga 1− x ) 2 O 3 thin films (0 [Formula: see text] x [Formula: see text] 1). Samples are grown by plasma-assisted molecular beam epitaxy on m-plane sapphire. A critical-point model is used to render a spectroscopic model dielectric function tensor and to determine direct electronic band-to-band transition parameters, including the direction dependent two lowest-photon energy band-to-band transitions associated with the anisotropic bandgap. We obtain the composition dependence of the direction dependent two lowest band-to-band transitions with separate bandgap bowing parameters associated with the perpendicular ([Formula: see text] = 1.31 eV) and parallel ([Formula: see text] = 1.61 eV) electric field polarization to the lattice c direction. Our density functional theory calculations indicate a transition from indirect to direct characteristics between α-Ga 2 O 3 and α-Al 2 O 3 , respectively, and we identify a switch in band order where the lowest band-to-band transition occurs with polarization perpendicular to c in α-Ga 2 O 3 whereas for α-Al 2 O 3 the lowest transition occurs with polarization parallel to c. We estimate that the change in band order occurs at approximately 40% Al content. Additionally, the characteristic of the lowest energy critical point transition for polarization parallel to c changes from M 1 type in α-Ga 2 O 3 to M 0 type van Hove singularity in α-Al 2 O 3 .more » « less
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