Search for: All records

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. 

We demonstrate detection and measurement of electron paramagnetic spin resonances (EPR) of iron defects in $\beta \text{−}{\mathrm{Ga}}_2{\mathrm{O}}_3$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 ${45}^{\circ }$and magnetic fields between 3 and 7 T. In contrast with low-field, low-frequency EPR measurements, we observe all five transitions of the $s=5/2$high-spin state ${\mathrm{Fe}}^{3+}$simultaneously. We confirm that ferric ${\mathrm{Fe}}^{3+}$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 Society2024 

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. 

Abstract A unique class of advanced materials—quantum composites based on polymers with fillers composed of a van der Waals quantum material that reveals multiple charge‐density‐wave quantum condensate phases—is demonstrated. Materials that exhibit quantum phenomena are typically crystalline, pure, and have few defects because disorder destroys the coherence of the electrons and phonons, leading to collapse of the quantum states. The macroscopic charge‐density‐wave phases of filler particles after multiple composite processing steps are successfully preserved in this work. The prepared composites display strong charge‐density‐wave phenomena even above room temperature. The dielectric constant experiences more than two orders of magnitude enhancement while the material maintains its electrically insulating properties, opening a venue for advanced applications in energy storage and electronics. The results present a conceptually different approach for engineering the properties of materials, extending the application domain for van der Waals materials. 

Abstract Polar dielectrics are key materials of interest for infrared (IR) nanophotonic applications due to their ability to host phonon‐polaritons (PhPs) that allow for low‐loss, subdiffractional control of light. The properties of phonon‐polaritons are limited by the characteristics of optical phonons, which are nominally fixed for most “bulk” materials. Superlattices composed of alternating atomically‐thin materials offer control over crystal anisotropy through changes in composition, optical phonon confinement, and the emergence of new modes. In particular, the modified optical phonons in superlattices offer the potential for so‐called crystalline hybrids whose IR properties cannot be described as a simple mixture of the bulk constituents. To date, however, studies have primarily focused on identifying the presence of new or modified optical phonon modes rather than assessing their impact on the IR response. This study focuses on assessing the impact of confined optical phonon modes on the hybrid IR dielectric function in superlattices of GaSb and AlSb. Using a combination of first principles theory, Raman, FTIR, and spectroscopic ellipsometry, the hybrid dielectric function is found to track with the confinement of optical phonons, leading to optical phonon spectral shifts of up to 20 cm⁻¹. These results provide an alternative pathway towards designer IR optical materials. This article is protected by copyright. All rights reserved 

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 . 

We report on terahertz (THz) electron paramagnetic resonance generalized spectroscopic ellipsometry (THz-EPR-GSE). Measurements of field and frequency dependencies of magnetic response due to spin transitions associated with nitrogen defects in 4H-SiC are shown as an example. THz-EPR-GSE dispenses with the need of a cavity, permits independently scanning field and frequency parameters, and does not require field or frequency modulation. We investigate spin transitions of hexagonal ( h) and cubic ( k) coordinated nitrogen including coupling with its nuclear spin (I = 1), and we propose a model approach for the magnetic susceptibility to account for the spin transitions. From the THz-EPR-GSE measurements, we can fully determine polarization properties of the spin transitions, and we can obtain the k coordinated nitrogen g and hyperfine splitting parameters using magnetic field and frequency dependent Lorentzian oscillator line shape functions. Magnetic-field line broadening presently obscures access to h parameters. We show that measurements of THz-EPR-GSE at positive and negative fields differ fundamentally and hence provide additional information. We propose frequency-scanning THz-EPR-GSE as a versatile method to study properties of spins in solid state materials. 

We report the elevated temperature (22 °C [Formula: see text]  T [Formula: see text] 600 °C) dielectric function properties of melt grown single crystal ZnGa 2 O 4 using a spectroscopic ellipsometry approach. A temperature dependent Cauchy dispersion analysis was applied across the transparent spectrum to determine the high-frequency index of refraction yielding a temperature dependent slope of 3.885(2) × 10 −5  K −1 . A model dielectric function critical point analysis was applied to examine the dielectric function and critical point transitions for each temperature. The lowest energy M 0 -type critical point associated with the direct bandgap transition in ZnGa 2 O 4 is shown to red-shift linearly as the temperature is increased with a subsequent slope of −0.72(4) meV K −1 . Furthermore, increasing the temperature results in a reduction of the excitonic amplitude and increase in the exciton broadening akin to exciton evaporation and lifetime shortening. This matches current theoretical understanding of excitonic behavior and critically provides justification for an anharmonic broadened Lorentz oscillator to be applied for model analysis of excitonic contributions. 

We determine the composition dependence of the transverse and longitudinal optical infrared-active phonon modes in rhombohedral α-(Al x Ga 1− x ) 2 O 3 alloys by far-infrared and infrared generalized spectroscopic ellipsometry. Single-crystalline high quality undoped thin-films grown on m-plane oriented α-Al 2 O 3 substrates with x =  0.18, 0.37, and 0.54 were investigated. A single mode behavior is observed for all phonon modes, i.e., their frequencies shift gradually between the equivalent phonon modes of the isostructural binary parent compounds. We also provide physical model line shape functions for the anisotropic dielectric functions. We use the anisotropic high-frequency dielectric constants for polarizations parallel and perpendicular to the lattice c axis measured recently by Hilfiker et al. [Appl. Phys. Lett. 119, 092103 (2021)], and we determine the anisotropic static dielectric constants using the Lyddane–Sachs–Teller relation. The static dielectric constants can be approximated by linear relationships between those of α-Ga 2 O 3 and α-Al 2 O 3 . The optical phonon modes and static dielectric constants will become useful for device design and free charge carrier characterization using optical techniques.