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            A generalized approach derived from Bloch's equation of motion of nuclear magnetic moments is presented to model the frequency, magnetic field, spin density, and temperature dependencies in the electromagnetic permeability tensor for materials with magnetic resonances. The resulting tensor model predicts characteristic polarization signatures which can be observed, for example, in Mueller matrix element spectra measured. When augmented with thermodynamic considerations and suitable Hamiltonian description of the magnetic eigenvalue spectrum, important parameters such as density, spectral amplitude distribution, relaxation time constants, and geometrical orientation parameters of the magnetic moments can be obtained from comparing the generalized model approach to experimental data. We demonstrate our approach by comparing model calculations with full Mueller matrix element spectra measured at an oblique angle of incidence in the terahertz spectral range, across electron spin resonance quintuplet transitions observed in wurtzite-structure GaN doped with iron. Our model correctly predicts the complexity of the polarization signatures observed in the 15 independent elements of the normalized Mueller matrix for both positive and negative magnetic fields and will become useful for future analysis of frequency and magnetic field-dependent magnetic resonance measurements. Published by the American Physical Society2024more » « less
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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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            AlxGa1−xN/GaN high-electron-mobility transistor (HEMT) structures are key components in electronic devices operating at gigahertz or higher frequencies. In order to optimize such HEMT structures, understanding their electronic response at high frequencies and room temperature is required. Here, we present a study of the room temperature free charge carrier properties of the two-dimensional electron gas (2DEG) in HEMT structures with varying Al content in the AlxGa1−xN barrier layers between x=0.07 and x=0.42. We discuss and compare 2DEG sheet density, mobility, effective mass, sheet resistance, and scattering times, which are determined by theoretical calculations, contactless Hall effect, capacitance-voltage, Eddy current, and cavity-enhanced terahertz optical Hall effect (THz-OHE) measurements using a low-field permanent magnet (0.6 T). From our THz-OHE results, we observe that the measured mobility reduction from x=0.13 to x=0.42 is driven by the decrease in 2DEG scattering time, and not the change in effective mass. For x<0.42, the 2DEG effective mass is found to be larger than for electrons in bulk GaN, which in turn, contributes to a decrease in the principally achievable mobility. From our theoretical calculations, we find that values close to 0.3m0 can be explained by the combined effects of conduction band nonparabolicity, polarons, and hybridization of the electron wavefunction through penetration into the barrier layer.more » « 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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            The hot-wall metalorganic chemical vapor deposition (MOCVD) concept, previously shown to enable superior material quality and high performance devices based on wide bandgap semiconductors, such as Ga(Al)N and SiC, has been applied to the epitaxial growth of β-Ga 2 O 3 . Epitaxial β-Ga 2 O 3 layers at high growth rates (above 1 μm/h), at low reagent flows, and at reduced growth temperatures (740 °C) are demonstrated. A high crystalline quality epitaxial material on a c-plane sapphire substrate is attained as corroborated by a combination of x-ray diffraction, high-resolution scanning transmission electron microscopy, and spectroscopic ellipsometry measurements. The hot-wall MOCVD process is transferred to homoepitaxy, and single-crystalline homoepitaxial β-Ga 2 O 3 layers are demonstrated with a [Formula: see text]01 rocking curve width of 118 arc sec, which is comparable to those of the edge-defined film-fed grown ([Formula: see text]01) β-Ga 2 O 3 substrates, indicative of similar dislocation densities for epilayers and substrates. Hence, hot-wall MOCVD is proposed as a prospective growth method to be further explored for the fabrication of β-Ga 2 O 3 .more » « less
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            Zmuidzinas, Jonas; Gao, Jian-Rong (Ed.)
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