Designing broadband enhanced chirality is of strong interest to the emerging fields of chiral chemistry and sensing, or to control the spin orbital momentum of photons in recently introduced nanophotonic chiral quantum and classical optical applications. However, chiral light‐matter interactions have an extremely weak nature, are difficult to control and enhance, and cannot be made tunable or broadband. In addition, planar ultrathin nanophotonic structures to achieve strong, broadband, and tunable chirality at the technologically important visible to ultraviolet spectrum still remain elusive. Here, these important problems are tackled by experimentally demonstrating and theoretically verifying spectrally tunable, extremely large, and broadband chiroptical response by nanohelical metamaterials. The reported new designs of all‐dielectric and dielectric‐metallic (hybrid) plasmonic metamaterials permit the largest and broadest ever measured chiral Kuhn's dissymmetry factor achieved by a large‐scale nanophotonic structure. In addition, the strong circular dichroism of the presented bottom‐up fabricated optical metamaterials can be tuned by varying their dimensions and proportions between their dielectric and plasmonic helical subsections. The currently demonstrated ultrathin optical metamaterials are expected to provide a substantial boost to the developing field of chiroptics leading to significantly enhanced and broadband chiral light‐matter interactions at the nanoscale.

We use a combined generalized spectroscopic ellipsometry and density functional theory approach to determine and analyze the anisotropic dielectric functions of an α-Ga2O3 thin film. The sample is grown epitaxially by plasma-assisted molecular beam epitaxy on m-plane sapphire. Generalized spectroscopic ellipsometry data from multiple sample azimuths in the spectral range from 0.73 eV to 8.75 eV are simultaneously analyzed. Density functional theory is used to calculate the valence and conduction band structure. We identify, for the indirect-bandgap material, two direct band-to-band transitions with M0-type van Hove singularities for polarization perpendicular to the c axis, E0,⊥=5.46(6) eV and E0,⊥=6.04(1) eV, and one direct band-to-band transition with M1-type van Hove singularity for polarization parallel to E0,||=5.44(2) eV. We further identify excitonic contributions with a small binding energy of 7 meV associated with the lowest ordinary transition and a hyperbolic exciton at the M1-type critical point with a large binding energy of 178 meV.

Mueller matrix spectroscopic ellipsometry is applied to determine anisotropic optical properties for a set of single-crystal rhombohedral structure α-(Al xGa1− x)2O3 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-Ga2O3 and α-Al2O3, respectively, and we identify a switch in band order where the lowest band-to-band transition occurs with polarization perpendicular to c in α-Ga2O3 whereas for α-Al2O3 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 M1 type in α-Ga2O3 to M0 type van Hove singularity in α-Al2O3.

We determine the composition dependence of the transverse and longitudinal optical infrared-active phonon modes in rhombohedral α-(Al xGa1− x)2O3 alloys by far-infrared and infrared generalized spectroscopic ellipsometry. Single-crystalline high quality undoped thin-films grown on m-plane oriented α-Al2O3 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-Ga2O3 and α-Al2O3. The optical phonon modes and static dielectric constants will become useful for device design and free charge carrier characterization using optical techniques.

A set of monoclinic β-(AlxGa1–x)2O3 films coherently grown by plasma-assisted molecular beam epitaxy onto (010)-oriented β-Ga2O3 substrates for compositions x ≤ 0.21 is investigated by generalized spectroscopic ellipsometry at room temperature in the spectral range of 1.5 eV–9.0 eV. We present the composition dependence of the excitonic and band to band transition energy parameters using a previously described eigendielectric summation approach for β-Ga2O3 from the study by Mock et al. All energies shift to a shorter wavelength with the increasing Al content in accordance with the much larger fundamental band to band transition energies of Al2O3 regardless of crystal symmetry. The observed increase in the lowest band to band transition energy is in excellent agreement with recent theoretical predictions. The most important observation is that charge confinement in heterostructures will strongly depend on the growth condition due to the strongly anisotropic properties of the band to band transitions.