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  1. High-field/high-frequency electron spin resonances of Fe-doped β Ga 2 O 3 by terahertz generalized ellipsometry: Monoclinic symmetry effects

    We demonstrate detection and measurement of electron paramagnetic spin resonances (EPR) of iron defects in β Ga 2 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 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 Fe 3more » + simultaneously. We confirm that ferric 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 Society 2024« less
  2. Quantum Composites with Charge-Density-Wave Fillers

    Here, 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 whilemore » 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.« less
  3. Remote surface optical phonon scattering in ferroelectric Ba0.6Sr0.4TiO3 gated graphene

    We report the effect of remote surface optical (RSO) phonon scattering on carrier mobility in monolayer graphene gated by ferroelectric oxide. We fabricate monolayer graphene transistors back-gated by epitaxial (001) Ba0.6Sr0.4TiO3 films, with field effect mobility up to 23 000 cm2 V–1 s–1 achieved. Switching ferroelectric polarization induces nonvolatile modulation of resistance and quantum Hall effect in graphene at low temperatures. Ellipsometry spectroscopy studies reveal four pairs of optical phonon modes in Ba0.6Sr0.4TiO3, from which we extract RSO phonon frequencies. The temperature dependence of resistivity in graphene can be well accounted for by considering the scattering from the intrinsic longitudinalmore » acoustic phonon and the RSO phonon, with the latter dominated by the mode at 35.8 meV. Furthermore, our study reveals the room temperature mobility limit of ferroelectric-gated graphene transistors imposed by RSO phonon scattering.« less
  4. Infrared-active phonon modes in single-crystal thorium dioxide and uranium dioxide

    The infrared-active phonon modes, in single-crystal samples of thorium dioxide (ThO 2 ) and uranium dioxide (UO 2 ), were investigated using spectroscopic ellipsometry and compared with density functional theory. Both ThO 2 and UO 2 are found to have one infrared-active phonon mode pair [consisting of one transverse optic (TO) and one associated longitudinal optic (LO) mode], which is responsible for the dominant features in the ellipsometric data. Furthermore, at room temperature, our results for the mode pair’s resonant frequencies andmore » broadening parameters are comparable with previous reflectance spectroscopy characterizations and density functional theory predictions. For ThO 2 , our ellipsometry and density function theory results both show that the LO mode broadening parameter is larger than the TO mode broadening. This signifies mode anharmonicity, which can be attributed to the intrinsic phonon–phonon interaction. In addition to the main mode pair, a broad low-amplitude impurity-like vibrational mode pair is detected within the reststrahlen band for both ThO 2 and UO 2 . Elevated temperature measurements were performed for ThO 2 in order to study the mechanisms by which the phonon parameters evolve with increased heat. The observed change in the TO resonant frequency is in excellent agreement with previous density functional calculations, which only consider volume expansion of the crystal lattice. This suggests that the temperature-dependent change in the TO frequency is primarily due to volume expansion. The change in the main mode pair’s broadening parameters is nearly linear within the temperature range of this study, which indicates the intrinsic anharmonic scattering (via cubic anharmonicities) as the main decay mechanism.« less
  5. Band-to-band transitions and critical points in the near-infrared to vacuum ultraviolet dielectric functions of single crystal urania and thoria

    Band-to-band transition energy parameters for single-crystal actinide samples of uranium oxide and thorium oxide were determined and compared using spectroscopic ellipsometry and critical-point dielectric function analyses. Spectroscopic ellipsometry measurements from the near-infrared to the vacuum ultraviolet spectral region were used to determine the dielectric functions of uranium oxide and thorium oxide. Furthermore, the critical-point structure is similar between UO2 and ThO2 but strongly blue shifted for ThO2. We find bandgap energies of 2.1 eV and 5.4 eV for UO2 and ThO2, respectively.

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