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A generalized approach derived from Blochs 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 fully polarization-resolved Mueller matrix element spectra measured across magnetic resonances as a function of frequency, magnetic field, magnetic moment density, and temperature. When augmented with thermodynamic considerations and suitable Hamiltonian description of the magnetic eigenvalue spectrum, important parameters such as zero-frequency magnetization, spectral amplitude distribution, relaxation time constants, and geometrical orientation parameters of the magnetic moment density 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 oblique angle of incidence in the terahertz spectral range, across electron spin resonance quintuplet transitions observed in wurtzite-structure GaN doped with iron. Measurements were performed by ellipsometry, using a superconducting cryostat magnet at magnetic fields of 7.23 T and at temperatures of 20 K and 30 K. We detail the occurrence of linear and circular birefringence and dichroism associated with each of the zero-field split spin transitions in the S = 5/2 defect system. We derive the spectral dependence of the magnetic susceptibility function and obtain the temperature and magnetic field dependence of the spin Hamiltonian. 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.

We report on terahertz (THz) electron paramagnetic resonance generalized spectroscopic ellipsometry (THz-EPR-GSE). Measurements of the field and frequency dependencies of the magnetic response due to the spin transitions associated with the nitrogen defect 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 the polarization properties of the spin transitions and we obtain $g$ and hyperfine splitting parameters using magnetic field and frequency dependent Lorentzian oscillator lineshape functions. We propose frequency-scanning THz-EPR-GSE as a new and versatile method to study properties of spins in solid state materials., Comment: 6 pages, 5 figures

Presented here is the development and demonstration of a tunable cavity-enhanced terahertz frequency-domain optical Hall effect technique. The cavity consists of at least one fixed and one tunable Fabry-P\'erot resonator. The approach is suitable for enhancement of the optical signatures produced by the optical Hall effect in semi-transparent conductive layer structures with plane parallel interfaces. The physical principle is the constructive interference of electric field components that undergo multiple optical Hall effect induced polarization rotations upon multiple light passages through the conductive layer stack. Tuning one of the cavity parameters, such as the external cavity thickness, permits shifting of the frequencies of the constructive interference, and enhancement of the optical signatures produced by the optical Hall effect can be obtained over large spectral regions. A cavity-tuning optical stage and gas flow cell are used as examples of instruments that exploit tuning an external cavity to enhance polarization changes in a reflected terahertz beam. Permanent magnets are used to provide the necessary external magnetic field. Conveniently, the highly reflective surface of a permanent magnet can be used to create the tunable external cavity. The signal enhancement allows the extraction of the free charge carrier properties of thin films, and can eliminate the need for expensive super-conducting magnets. Furthermore, the thickness of the external cavity establishes an additional independent measurement condition, similar to, for example, the magnetic field strength, terahertz frequency, and angle of incidence. A high electron mobility transistor structure and epitaxial graphene are studied as examples. We discuss the theoretical background, instrument design, data acquisition, and data analysis procedures., Comment: 12 pages, 8 figures

Polymer based stereolithographic additive manufacturing has been established for the rapid and low-cost fabrication of THz optical components due to its ability to construct complex 3D geometries with high resolution. For polymer based or integrated optics, thermal annealing processes are often used to optimize material properties. However, despite the growing interest in THz optics fabricated using stereolithography, the effects of thermal annealing on the THz dielectric properties of polymethacrylates compatible with stereolithography has not been studied yet. In this manuscript we report on the THz ellipsometric response of thermally annealed polymethacrylates prepared using UV polymerization. Our findings indicate that the investigated polymethacrylate maintain a stable optical response in THz spectral range from 650 to 950 GHz after thermal annealing at temperatures up to 70 degrees C for several hours.

Metal nanostructures are key elements in nanooptics owing to their strong resonant interaction with light through local plasmonic charge oscillations. Their ability to shape light at the nanoscale have made them important across a multitude of areas, including biosensing, energy conversion and ultrathin flat metaoptics. Yet another dimension of avenues is foreseen for dynamic nanoantennas, ranging from tuneable metalenses for miniaturized medical devices to adaptable windows that control radiation flows in and out of buildings. However, enabling nano-optical antennas to be dynamically controllable remains highly challenging and particularly so for traditional metals with fixed permittivity. Here we present state-of-the-art conductive polymers as a new class of organic plasmonic materials for redox-tuneable nano-optics. Through experiments and simulations, we show that nanodisks of highly conductive polymers can provide clear optical extinction peaks via excitation of dipolar localised surface plasmon resonances. Resonance frequencies redshift with increasing nanodisk aspect ratio, in agreement with analytical calculations based on dipolar polarizability theory. We furthermore demonstrate complete switching of the optical response of the organic nanoantennas by chemical tuning of the polymer's redox state, which effectively modulates the material permittivity between plasmonic and non-plasmonic regimes. Our results thereby show that conductive polymer nanostructures can act as redox-tuneable plasmonic nanoantennas, based on bipolaronic charge carriers rather than electrons as in conventional metals. Future directions may investigate different polymers and geometries to further widen the plasmonic spectral range (here around 0.8 to 3.6 {\mu}m) as well as different ways of tuning.

We present a terahertz (THz) frequency-domain spectroscopic (FDS) ellipsometer design which suppresses formation of standing waves by use of stealth technology approaches. The strategy to suppress standing waves consists of three elements \textit{geometry}, \textit{coating} and \textit{modulation}. The instrument is based on the rotating analyzer ellipsometer principle and can incorporate various sample compartments, such as a superconducting magnet, \textit{in-situ} gas cells or resonant sample cavities, for example. A backward wave oscillator and three detectors are employed, which permit operation in the spectral range of 0.1--1~THz (3.3--33~cm$^{-1}$ or 0.4--4~meV). The THz frequency-domain ellipsometer allows for standard and generalized ellipsometry at variable angles of incidence in both reflection and transmission configurations. The methods used to suppress standing waves and strategies for an accurate frequency calibration are presented. Experimental results from dielectric constant determination in anisotropic materials, and free charge carrier determination in optical Hall effect, resonant-cavity enhanced optical Hall effect and \textit{in-situ} optical Hall effect experiments are discussed. Examples include silicon and sapphire optical constants, free charge carrier properties of two dimensional electron gas in group-III nitride high electron mobility transistor structure, and ambient effects on free electron mobility and density in epitaxial graphene.

Mid-infrared optical Hall effect measurements are used to determine the free charge carrier parameters of an unintentionally doped wurtzite-structure $c$-plane oriented In$_{0.33}$Ga$_{0.67}$N epitaxial layer. Room temperature electron effective mass parameters of $m^{*}_{\bot}=(0.205 \pm 0.013)~m_0$ and $m^{*}_{\parallel}=(0.204 \pm 0.016)~m_0$ for polarization perpendicular and parallel to the $c$-axis, respectively, were determined. The free electron concentration was obtained as $(1.7 \pm 0.2)\times 10^{19}~$cm$^{-3}$. Within our uncertainty limits we detect no anisotropy for the electron effective mass parameter and we estimate the upper limit of the possible effective mass anisotropy is 7$\%$. We discuss the influence of band nonparabolicity on the electron effective mass parameter as a function of In content. The effective mass parameter is consistent with a linear interpolation scheme between the conduction band mass parameters in GaN and InN when the strong nonparabolicity in InN is included. The In$_{0.33}$Ga$_{0.67}$N electron mobility parameters were found to be anisotropic supporting previous experimental findings for wurtzite-structure GaN, InN, and Al$_{x}$Ga$_{1-x}$N epitaxial layers with $c$-plane growth orientation., Comment: 5 pages, 3 figures, 1 table

We present a comprehensive study of the band structure of two- and three-dimensional hexagonal layered materials using Landau Level optical Hall effect spectroscopy investigations, employing graphene and graphite as model systems. We study inter-Landau-level transitions in highly oriented pyrolytic graphite and a stack of multilayer graphene on C-face 6\textit{H}-SiC, using data from reflection-type optical Hall effect measurements in the mid-infrared spectral range at sample temperatures of $T=1.5$~K and magnetic fields up to $B=8$~T. We describe a comprehensive dielectric polarizability model for inter-Landau-level transitions, which permits analysis of the optical Hall effect data. From their magnetic field dependence we identify sets of H- and K-point inter-Landau-level transitions in graphite and sets of inter-Landau-level transition from decoupled graphene single, and coupled graphene bi-, tri-, and quad-layer for the multilayer graphene stack. For inter-Landau-level transitions in decoupled graphene single-layers and H-point transitions in graphite we observe polarization mode preserving behavior, requiring symmetric magneto-optical contributions to the corresponding dielectric tensors. Inter-Landau-level transitions in coupled graphene layers as well as K-point transitions in graphite exhibit polarization mode mixing behavior, requiring antisymmetric magneto-optical contributions to the corresponding dielectric tensors. From the circular-polarization-averaged inter-Landau-level transition energies and the energy splitting between right- and left-handed circular polarized inter-Landau-level transitions we determine the model parameters in the Slonczewski-Weiss-McClure band structure approximation for two- and three-dimensional hexagonal layered materials, with graphene and graphite as examples.