Tunable plasmonic resonances in highly porous nano-bamboo Si-Au superlattice-type thin films

We report on fabrication of spatially-coherent columnar plasmonic nanostructure superlattice-type thin films with high porosity and strong optical anisotropy using glancing angle deposition. Subsequent and repeated depositions of silicon and gold lead to nanometer-dimension subcolumns with controlled lengths. The superlattice-type columns resemble bamboo structures where smaller column sections of gold form junctions sandwiched between larger silicon column sections ("nano-bamboo"). We perform generalized spectroscopic ellipsometry measurements and finite element method computations to elucidate the strongly anisotropic optical properties of the highly-porous nano-bamboo structures. The occurrence of a strongly localized plasmonic mode with displacement pattern reminiscent of a dark quadrupole mode is observed in the vicinity of the gold subcolumns. We demonstrate tuning of this quadrupole-like mode frequency within the near-infrared spectral range by varying the geometry of the nano-bamboo structure. In addition, coupled-plasmon-like and inter-band transition-like modes occur in the visible and ultra-violet spectral regions, respectively. We elucidate an example for the potential use of the nano-bamboo structures as a highly porous plasmonic sensor with optical read out sensitivity to few parts-per-million solvent levels in water

Zinc Gallate Spinel Dielectric Function, Band-to-Band Transitions, and Γ-Point Effective Mass Parameters

We determine the dielectric function of the emerging ultrawide bandgap semiconductor ZnGa2O4 from the near-infrared (0.75 eV) into the vacuum ultraviolet (8.5 eV) spectral regions using spectroscopic ellipsometry on high quality single crystal substrates. We perform density functional theory calculations and discuss the band structure and the Brillouin zone Γ-point band-to-band transition energies, their transition matrix elements, and effective band mass parameters. We find an isotropic effective mass parameter (0.24me) at the bottom of the Γ-point conduction band, which equals the lowest valence band effective mass parameter at the top of the highly anisotropic and degenerate valence band (0.24me). Our calculated band structure indicates the spinel ZnGa2O4 is indirect, with the lowest direct transition at the Γ-point. We analyze the measured dielectric function using critical-point line shape functions for a three-dimensional, M0-type van Hove singularity, and we determine the direct bandgap with an energy of 5.27(3) eV. In our model, we also consider contributions from Wannier–Mott type excitons with an effective Rydberg energy of 14.8 meV. We determine the near-infrared index of refraction from extrapolation (1.91) in very good agreement with results from recent infrared ellipsometry measurements (√ε∞=1.94) [M. Stokey, Appl. Phys. Lett. 117, 052104 (2020)]

Brillouin Zone Center Phonon Modes in ZnGa\u3csub\u3e2\u3c/sub\u3eO\u3csub\u3e4\u3c/sub\u3e

Infrared-active lattice mode properties of melt-grown high-quality single bulk crystals of ZnGa2O4 are investigated by combined spectroscopic ellipsometry and density functional theory computation analysis. The normal spinel structure crystals are measured by spectroscopic ellipsometry at room temperature in the range of 100 cm–1–1200 cm–1. The complex-valued dielectric function is determined from a wavenumber-by-wavenumber approach, which is then analyzed by the four-parameter semi-quantum model dielectric function approach augmented by impurity mode contributions. We determine four infrared-active transverse and longitudinal optical mode pairs, five localized impurity mode pairs, and the high frequency dielectric constant. All four infrared-active transverse and longitudinal optical mode pairs are in excellent agreement with results from our density functional theory computations. With the Lyddane–Sachs–Teller relationship, we determine the static dielectric constant, which agrees well with electrical capacitance measurements performed on similarly grown samples. We also provide calculated parameters for all Raman-active and for all silent modes and, thereby, provide a complete set of all symmetry predicted Brillouin zone center modes

Tunable plasmonic resonances in Si-Au slanted columnar heterostructure thin films

We report on fabrication of spatially-coherent columnar plasmonic nanostructure superlattice-type thin films with high porosity and strong optical anisotropy using glancing angle deposition. Subsequent and repeated depositions of silicon and gold lead to nanometer-dimension subcolumns with controlled lengths. We perform generalized spectroscopic ellipsometry measurements and finite element method computations to elucidate the strongly anisotropic optical properties of the highly-porous Si-Au slanted columnar heterostructures. The occurrence of a strongly localized plasmonic mode with displacement pattern reminiscent of a dark quadrupole mode is observed in the vicinity of the gold subcolumns. We demonstrate tuning of this quadrupole-like mode frequency within the near-infrared spectral range by varying the geometry of Si-Au slanted columnar heterostructures. In addition, coupled-plasmon-like and inter-band transition-like modes occur in the visible and ultra-violet spectral regions, respectively. We elucidate an example for the potential use of Si-Au slanted columnar heterostructures as a highly porous plasmonic sensor with optical read out sensitivity to few parts-per-million solvent levels in water

Tunable plasmonic resonances in highly porous nano-bamboo Si-Au superlattice-type thin films

We report on fabrication of spatially-coherent columnar plasmonic nanostructure superlattice-type thin films with high porosity and strong optical anisotropy using glancing angle deposition. Subsequent and repeated depositions of silicon and gold lead to nanometer-dimension subcolumns with controlled lengths. The superlattice-type columns resemble bamboo structures where smaller column sections of gold form junctions sandwiched between larger silicon column sections (“nano-bamboo”). We perform generalized spectroscopic ellipsometry measurements and finite element method computations to elucidate the strongly anisotropic optical properties of the highly-porous nano-bamboo structures. The occurrence of a strongly localized plasmonic mode with displacement pattern reminiscent of a dark quadrupole mode is observed in the vicinity of the gold subcolumns. We demonstrate tuning of this quadrupole-like mode frequency within the near-infrared spectral range by varying the geometry of the nano-bamboo structure. In addition, coupled-plasmon-like and inter-band transition-like modes occur in the visible and ultra-violet spectral regions, respectively. We elucidate an example for the potential use of the nano-bamboo structures as a highly porous plasmonic sensor with optical read out sensitivity to few parts-per-million solvent levels in water

High-Frequency and Below Bandgap Anisotropic Dielectric Constants in \u3cem\u3eα\u3c/em\u3e-(Al\u3csub\u3ex\u3c/sub\u3eGa\u3csub\u3e1-x\u3c/sub\u3e)\u3csub\u3e2\u3c/sub\u3eO\u3csub\u3e3\u3c/sub\u3e (0≤x≤1)

A Mueller matrix spectroscopic ellipsometry approach was used to investigate the anisotropic dielectric constants of corundum α-(AlxGa1-x)2O3 thin films in their below bandgap spectral regions. The sample set was epitaxially grown using plasma-assisted molecular beam epitaxy on m-plane sapphire. The spectroscopic ellipsometry measurements were performed at multiple azimuthal angles to resolve the uniaxial dielectric properties. A Cauchy dispersion model was applied, and high-frequency dielectric constants are determined for polarization perpendicular (ε∞,⟂) and parallel (ε∞,∥) to the thin film c-axis. The optical birefringence is negative throughout the composition range, and the overall index of refraction substantially decreases upon incorporation of Al. We find small bowing parameters of the high-frequency dielectric constants with b⟂=0.386 and b∥=0.307

Anisotropic Dielectric Functions, Band-to-Band Transitions, and Critical Points in \u3cem\u3eα\u3c/em\u3e-Ga\u3csub\u3e2\u3c/sub\u3eO\u3csub\u3e3\u3c/sub\u3e

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

Dielectric Function Tensor (1.5 eV to 9.0 eV), Anisotropy, and Band to Band Transitions of Monoclinic \u3cem\u3eβ\u3c/em\u3e-(Al\u3cem\u3e\u3csub\u3ex\u3c/sub\u3e\u3c/em\u3eGa\u3csub\u3e1–\u3cem\u3ex\u3c/em\u3e\u3c/sub\u3e)\u3csub\u3e2\u3c/sub\u3eO\u3csub\u3e3\u3c/sub\u3e (x ≤ 0.21) Films

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

Optical Phonon Modes, Static and High-Frequency Dielectric Constants, and Effective Electron Mass Parameter in Cubic In\u3csub\u3e2\u3c/sub\u3eO\u3csub\u3e3\u3c/sub\u3e

A complete set of all optical phonon modes predicted by symmetry for bixbyite structure indium oxide is reported here from a combination of far-infrared and infrared spectroscopic ellipsometry, as well as first principles calculations. Dielectric function spectra measured on high quality, marginally electrically conductive melt grown single bulk crystals are obtained on a wavelength-by-wavelength (also known as point-by-point) basis and by numerical reduction of a subtle free charge carrier Drude model contribution. A four-parameter semi-quantum model is applied to determine all 16 pairs of infrared-active transverse and longitudinal optical phonon modes, including the high-frequency dielectric constant, ε∞=4.05±0.05. The Lyddane–Sachs–Teller relation then gives access to the static dielectric constant, εDC=10.55±0.07. All experimental results are in excellent agreement with our density functional theory calculations and with previously reported values, where existent. We also perform optical Hall effect measurements and determine for the unintentionally doped n-type sample a free electron density of n = (2.81±0.01)×1017 cm-3, a mobility of μ=(112±3) cm2/(Vs), and an effective mass parameter of (0.208±0.006)me. Density and mobility parameters compare very well with the results of electrical Hall effect measurements. Our effective mass parameter, which is measured independently of any other experimental technique, represents the bottom curvature of the Γ point in In2O3 in agreement with previous extrapolations. We use terahertz spectroscopic ellipsometry to measure the quasi-static response of In2O3, and our model validates the static dielectric constant obtained from the Lyddane–Sachs–Teller relation