1. |
- Kilic, Ufuk, et al.
(author)
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Broadband Enhanced Chirality with Tunable Response in Hybrid Plasmonic Helical Metamaterials
- 2021
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In: Advanced Functional Materials. - : WILEY-V C H VERLAG GMBH. - 1616-301X .- 1616-3028. ; 31:20
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Journal article (peer-reviewed)abstract
- 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 Kuhns 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.
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2. |
- Kilic, Ufuk, et al.
(author)
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Controlling the broadband enhanced light chirality with L-shaped dielectric metamaterials
- 2024
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In: Nature Communications. - 2041-1723. ; 15:1
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Journal article (peer-reviewed)abstract
- The inherently weak chiroptical responses of natural materials limit their usage for controlling and enhancing chiral light-matter interactions. Recently, several nanostructures with subwavelength scale dimensions were demonstrated, mainly due to the advent of nanofabrication technologies, as a potential alternative to efficiently enhance chirality. However, the intrinsic lossy nature of metals and the inherent narrowband response of dielectric planar thin films or metasurface structures pose severe limitations toward the practical realization of broadband and tailorable chiral systems. Here, we tackle these problems by designing all-dielectric silicon-based L-shaped optical metamaterials based on tilted nanopillars that exhibit broadband and enhanced chiroptical response in transmission operation. We use an emerging bottom-up fabrication approach, named glancing angle deposition, to assemble these dielectric metamaterials on a wafer scale. The reported strong chirality and optical anisotropic properties are controllable in terms of both amplitude and operating frequency by simply varying the shape and dimensions of the nanopillars. The presented nanostructures can be used in a plethora of emerging nanophotonic applications, such as chiral sensors, polarization filters, and spin-locked nanowaveguides.
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3. |
- Richter, Steffen, et al.
(author)
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High-field/high-frequency electron spin resonances of Fe-doped β-Ga2 O3 by terahertz generalized ellipsometry : Monoclinic symmetry effects
- 2024
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In: Physical Review B. - 2469-9950. ; 109:21
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Journal article (peer-reviewed)abstract
- We demonstrate detection and measurement of electron paramagnetic spin resonances (EPR) of iron defects in β-Ga2O3 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 Fe3+ simultaneously. We confirm that ferric Fe3+ 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.
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4. |
- Rindert, Viktor, et al.
(author)
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Bloch equations in terahertz magnetic-resonance ellipsometry
- 2024
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In: Physical Review B. - 2469-9950. ; 110:5
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Journal article (peer-reviewed)abstract
- A generalized approach derived from Bloch's 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 Mueller matrix element spectra measured. When augmented with thermodynamic considerations and suitable Hamiltonian description of the magnetic eigenvalue spectrum, important parameters such as density, spectral amplitude distribution, relaxation time constants, and geometrical orientation parameters of the magnetic moments 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 an oblique angle of incidence in the terahertz spectral range, across electron spin resonance quintuplet transitions observed in wurtzite-structure GaN doped with iron. 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 and will become useful for future analysis of frequency and magnetic field-dependent magnetic resonance measurements.
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5. |
- Ruder, Alexander, et al.
(author)
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Mueller matrix ellipsometer using dual continuously rotating anisotropic mirrors
- 2020
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In: Optics Letters. - : OPTICAL SOC AMER. - 0146-9592 .- 1539-4794. ; 45:13, s. 3541-3544
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Journal article (peer-reviewed)abstract
- We demonstrate calibration and operation of a single wavelength (660 nm) Mueller matrix ellipsometer in normal transmission configuration using dual continuously rotating anisotropic mirrors. The mirrors contain highly spatially coherent nanostructure slanted columnar titanium thin films deposited onto optically thick gold layers on glass substrates. Upon rotation around the mirror normal axis, sufficient modulation of the Stokes parameters of light reflected at oblique angle of incidence is achieved. Thereby, the mirrors can be used as a polarization state generator and polarization state analyzer in a generalized ellipsometry instrument. A Fourier expansion approach is found sufficient to render and calibrate the effects of the mirror rotations onto the polarized light train within the ellipsometer. The Mueller matrix elements of a set of anisotropic samples consisting of a linear polarizer and a linear retarder are measured and compared with model data, and very good agreement is observed. (C) 2020 Optical Society of America
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6. |
- Ruder, Alexander, et al.
(author)
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Mueller matrix imaging microscope using dual continuously rotating anisotropic mirrors
- 2021
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In: Optics Express. - : Optical Society of America. - 1094-4087. ; 29:18, s. 28704-28724
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Journal article (peer-reviewed)abstract
- We demonstrate calibration and operation of a Mueller matrix imaging microscope using dual continuously rotating anisotropic mirrors for polarization state generation and analysis. The mirrors contain highly spatially coherent nanostructure slanted columnar titanium thin films deposited onto optically thick titanium layers on quartz substrates. The first mirror acts as polarization state image generator and the second mirror acts as polarization state image detector. The instrument is calibrated using samples consisting of laterally homogeneous properties such as straight-through-air, a clear aperture linear polarizer, and a clear aperture linear retarder waveplate. Mueller matrix images are determined for spatially varying anisotropic samples consisting of a commercially available (Thorlabs) birefringent resolution target and a spatially patterned titanium slanted columnar thin film deposited onto a glass substrate. Calibration and operation are demonstrated at a single wavelength (530 nm) only, while, in principle, the instrument can operate regardless of wavelength. We refer to this imaging ellipsometry configuration as rotating-anisotropic-mirror-sample-rotating-anisotropic-mirror ellipsometry (RAM-S-RAM-E). (C) 2021 Optical Society of America under the terms of the OSA Open Access Publishing Agreement
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7. |
- Schubert, Mathias, et al.
(author)
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Terahertz electron paramagnetic resonance generalized spectroscopic ellipsometry: The magnetic response of the nitrogen defect in 4H-SiC
- 2022
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In: Applied Physics Letters. - : AIP Publishing. - 0003-6951 .- 1077-3118. ; 120:10
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Journal article (peer-reviewed)abstract
- 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.
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8. |
- Stokey, Megan, et al.
(author)
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Optical phonon modes, static and high-frequency dielectric constants, and effective electron mass parameter in cubic In2O3
- 2021
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In: Journal of Applied Physics. - : AMER INST PHYSICS. - 0021-8979 .- 1089-7550. ; 129:22
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Journal article (peer-reviewed)abstract
- 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, epsilon(infinity) = 4.05 +/- 0.05. The Lyddane-Sachs-Teller relation then gives access to the static dielectric constant, epsilon(DC) = 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) x 10(17) cm(-3), a mobility of mu = (112 +/- 3) cm(2)/(Vs), and an effective mass parameter of (0.208 +/- 0.006)m(e). 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 Gamma 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. Published under an exclusive license by AIP Publishing.
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