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At least 37 records · Page 2

Optical functions of crystalline and amorphous TeO2

The optical functions of crystalline paratellurite (α-TeO2) and amorphous TeO2 were determined using several optical techniques: (1) standard spectroscopic two-modulator generalized ellipsometry (2-MGE) of paratellurite (200–850 nm, 6.2–1.46 eV), (2) near-normal-incidence two-modulator generalized ellipsometry microscopy (2-MGEM) of paratellurite (577 nm, 2.15 eV), (3) Mueller matrix transmission of paratellurite (320–798 nm, 3.87–1.55 eV), and (4) polarized transmission of paratellurite (323.6–334.3 nm, 3.83–3.71 eV). The 2-MGE measurements yielded highly accurate values of the dielectric functions and error estimates from 1.46 to 6.2 eV for both paratellurite and amorphous TeO2, whereas the polarization-dependent transmission yielded more accurate values of the absorption coefficient below the band edge of paratellurite. The 2-MGEM measured the diattenuation of paratellurite, which is related to the birefringence. Mueller matrix transmission measurements of paratellurite of a (001) cut crystal as a function of angle of incidence were used to determine both the birefringence and the rotary power as a function of photon energy.

Jellison Jr, Gerald [ORNL]↗

A Comparison of the Measured Scattering Matrix Elements of Polydisperse Systems of Irregular Particles with the Matrix Elements Calculated for Spheres that Have the Same Distribution of Projected Areas

The elements of the scattering or Mueller Matrix for three polydisperse systems of irregular, randomly-oriented particles have been measured in absolute terms as a function of scattering angle for several visible wavelengths. The samples consisted of commercially available silicon dioxide particles that fit three distinct lognormal size distributions. The measured matrix elements were compared with the matrix elements calculated for spheres that had the same refractive index and fitted the same distribution of projected areas. Correlations and discrepancies between the two sets of matrix elements will be discussed.

Holland, A. C.↗

Polarimetric signatures of a canopy of dielectric cylinders based on first and second order vector radiative transfer theory

Complete polarimetric signatures of a canopy of dielectric cylinders overlying a homogeneous half space are studied with the first and second order solutions of the vector radiative transfer theory. The vector radiative transfer equations contain a general nondiagonal extinction matrix and a phase matrix. The energy conservation issue is addressed by calculating the elements of the extinction matrix and the elements of the phase matrix in a manner that is consistent with energy conservation. Two methods are used. In the first method, the surface fields and the internal fields of the dielectric cylinder are calculated by using the fields of an infinite cylinder. The phase matrix is calculated and the extinction matrix is calculated by summing the absorption and scattering to ensure energy conservation. In the second method, the method of moments is used to calculate the elements of the extinction and phase matrices. The Mueller matrix based on the first order and second order multiple scattering solutions of the vector radiative transfer equation are calculated. Results from the two methods are compared. The vector radiative transfer equations, combined with the solution based on method of moments, obey both energy conservation and reciprocity. The polarimetric signatures, copolarized and depolarized return, degree of polarization, and phase differences are studied as a function of the orientation, sizes, and dielectric properties of the cylinders. It is shown that second order scattering is generally important for vegetation canopy at C band and can be important at L band for some cases.

Tsang, Leung↗

Polarized optical scattering by inhomogeneities and surface roughness in an anisotropic thin film

We extend the theory for scattering by oblique columnar structure thin films to include the induced form birefringence and the propagation of radiation in those films. We generalize the 4 × 4 matrix theory to include arbitrary sources in the layer, which are necessary to determine the Green function for the inhomogeneous wave equation. We further extend first-order vector perturbation theory for scattering by roughness in the smooth surface limit, when the layer is anisotropic. Scattering by an inhomogeneous medium is approximated by a distorted Born approximation, where effective medium theory is used to determine the effective properties of the medium and strong fluctuation theory is used to determine the inhomogeneous sources. In this manner, we develop a model for scattering by inhomogeneous films, with anisotropic correlation functions. Here, the results are compared to Mueller matrix bidirectional scattering distribution function measurements for a glancing-angle deposition (GLAD) film. While the results are applied to the GLAD film example, the development of the theory is general enough that it can guide simulations for scattering in other anisotropic thin films.

36 MATERIALS SCIENCE↗

Twisted Crystalline Organic Semiconductor Photodetectors

Optoelectronic properties of anisotropic crystals vary with direction requiring that the orientation of molecular organic semiconductor crystals is controlled in optoelectronic device active layers to achieve optimal performance. Here, in this work, a generalizable strategy to introduce periodic variations in the out-of-plane orientations of 5,11-bis(triisopropylsilylethynyl)anthradithiophene (TIPS ADT) crystals is presented. TIPS ADT crystallized from the melt in the presence of 16 wt.% polyethylene (PE) forms banded spherulites of crystalline fibrils that twist in concert about the radial growth direction. These spherulites exhibit band-dependent light absorption, photoluminescence, and Raman scattering depending on the local orientation of crystals. Mueller matrix imaging reveals strong circular extinction (CE), with TIPS ADT banded spherulites exhibiting domains of positive or negative CE signal depending on the crystal twisting sense. Furthermore, orientation-dependent enhancement in charge injection and extraction in films of twisted TIPS ADT crystals compared to films of straight crystals is visualized in local conductive atomic force microscopy maps. This enhancement leads to 3.3- and 6.2-times larger photocurrents and external quantum efficiencies, respectively, in photodetectors comprising twisted crystals than those comprising straight crystals.

36 MATERIALS SCIENCE↗

Charge Transport in Twisted Organic Semiconductor Crystals of Modulated Pitch

Many molecular crystals (approximately one third) grow as twisted, helicoidal ribbons from the melt, and this preponderance is even higher in restricted classes of materials, for instance, charge-transfer complexes. Previously, twisted crystallites of such complexes present an increase in carrier mobilities. In this paper, the effect of twisting on charge mobility is better analyzed for a monocomponent organic semiconductor, 2,5-bis(3-dodecyl-2-thienyl)-thiazolo[5,4-d]thiazole (BDT), that forms twisted crystals with varied helicoidal pitches and makes possible a correlation of twist strength with carrier mobility. Films are analyzed by X-ray scattering and Mueller matrix polarimetry to characterize the microscale organization of the polycrystalline ensembles. Carrier mobilities of organic field-effect transistors are five times higher when the crystals are grown with the smallest pitches (most twisted), compared to those with the largest pitches, along the fiber elongation direction. A tenfold increase is observed along the perpendicular direction. Simulation of electrical potential based on scanning electron microscopy images and density functional theory suggests that the twisting-enhanced mobility is mainly controlled by the fiber organization in the film. A greater number of tightly packed twisted fibers separated by numerous smaller gaps permit better charge transport over the film surface compared to fewer big crystallites separated by larger gaps.

36 MATERIALS SCIENCE↗

Anisotropic Optical and Frictional Properties of Langmuir–Blodgett Film Consisting of Uniaxially-Aligned Rod-Shaped Cellulose Nanocrystals

Langmuir–Blodgett (LB) film deposition gives an opportunity to control the packing density and orientation of anisotropic nanoparticles at a monolayer level, allowing accurate characterization of their anisotropic material properties. Additionally, the uniaxial deposition of rod-shaped cellulose nanocrystals (CNCs) over a macroscopically large area is achieved by aligning the long axis of CNCs on the LB trough with the direction of the maximum drag force within the meniscus during the vertical pulling of the substrate from the LB trough. On the uniaxially-aligned LB films, anisotropic linear and non-linear optical properties of CNCs are obtained using Mueller matrix spectroscopy and sum frequency generation spectroscopy, respectively, and explained with time-dependent density functional theory calculations. Also, the frictional anisotropy of the LB film is measured using atomic force microscopy and explained theoretically. The findings of this study will be valuable for preparation of anisotropic nanoparticle thin films with uniform arrangements and utilization of their anisotropic material properties.

36 MATERIALS SCIENCE↗

Two–Photon Printing of Shape–Memory Microstructures and Metasurfaces via Radical–Mediated Thiol–Vinyl Hydrothiolation

Shape-memory resists capable of high-resolution curing into arbitrarily designed structures are increasingly demanded for soft robotics, optical sensors, microscale manufacturing, and biomedicine. Amorphous, shape-memory thiol-vinyl networks were printed using two-photon polymerization (2PP) curing of a simple resin formulated with commercially available reagents. The ability to print high-resolution feature sizes down to 200 nm is attributed to the use of radicalmediated, thiol-vinyl step-growth polymerization that quickly crosslinks the resin, limiting diffusive transport. The thermomechanical behavior of the 2PP-cured material analyzed in compression, tension and three-point bending is similar to the behavior of the UV-polymerized samples. To demonstrate the ability to design, field, and test 4D responsive microstructures, an array of nine springs with coil diameters of 330 μm was printed. Following compressive shapefixing, printed arrays can release 11 μJ of stored elastic strain energy when reheated. Further, a new concept of dichroic-memory of a metamaterial device is demonstrated by printing a twisted woodpile structure with circular dichroism as characterized by Mueller Matrix ellipsometry. Furthermore, our results demonstrate how combining high-resolution 2PP curing with stimuli-responsive molecular architectures can further the engineering of responsive microstructures and metamaterials.

36 MATERIALS SCIENCE↗

Strong Induced Circular Dichroism in a Hybrid Lead‐Halide Semiconductor Using Chiral Amino Acids for Crystallite Surface Functionalization

Abstract Chirality is a desired property in functional semiconductors for optoelectronic, catalytic, and spintronic applications. Here, introducing enantiomerically‐pure 3‐aminobutyric acid (3‐ABA) into thin films of the 1D semiconductor dimethylammonium lead iodide (DMAPbI 3 ) is found to result in strong circular dichroism (CD) in the optical absorption. X‐ray diffraction and grazing incidence small angle X‐ray scattering (GISAXS) are applied to gain molecular‐scale insights into the chirality transfer mechanism, which is attributed to a chiral surface modification of DMAPbI 3 crystallites. This study demonstrates that the CD signal strength can be controlled by the amino‐acid content relative to the crystallite surface area. The CD intensity is tuned by the composition of the precursor solution and the spin‐coating time, thereby achieving anisotropy factors ( g abs ) as high as 1.75 × 10 –2 . Grazing incidence wide angle scattering reveals strong preferential ordering that can be suppressed via tailored synthesis conditions. Different contributions to the chiroptical properties are resolved by a detailed analysis of the CD signal utilizing an approach based on the Mueller matrix model. This report of a novel class of chiral hybrid semiconductors with precise control over their optical activity presents a promising approach for the design of circularly polarized light detectors and emitters.

36 MATERIALS SCIENCE↗

A 2D chiral microcavity based on apparent circular dichroism

Abstract Engineering asymmetric transmission between left-handed and right-handed circularly polarized light in planar Fabry–Pérot (FP) microcavities would enable a variety of chiral light-matter phenomena, with applications in spintronics, polaritonics, and chiral lasing. Such symmetry breaking, however, generally requires Faraday rotators or nanofabricated polarization-preserving mirrors. We present a simple solution requiring no nanofabrication to induce asymmetric transmission in FP microcavities, preserving low mode volumes by embedding organic thin films exhibiting apparent circular dichroism (ACD); an optical phenomenon based on 2D chirality. Importantly, ACD interactions are opposite for counter-propagating light. Consequently, we demonstrated asymmetric transmission of cavity modes over an order of magnitude larger than that of the isolated thin film. Through circular dichroism spectroscopy, Mueller matrix ellipsometry, and simulation using theoretical scattering matrix methods, we characterize the spatial, spectral, and angular chiroptical responses of this 2D chiral microcavity.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Invited Article: An integrated mid-infrared, far-infrared, and terahertz optical Hall effect instrument

We report on the development of the first integrated mid-infrared, far-infrared, and terahertz optical Hall effect instrument, covering an ultra wide spectral range from 3 cm{sup −1} to 7000 cm{sup −1} (0.1–210 THz or 0.4–870 meV). The instrument comprises four sub-systems, where the magneto-cryostat-transfer sub-system enables the usage of the magneto-cryostat sub-system with the mid-infrared ellipsometer sub-system, and the far-infrared/terahertz ellipsometer sub-system. Both ellipsometer sub-systems can be used as variable angle-of-incidence spectroscopic ellipsometers in reflection or transmission mode, and are equipped with multiple light sources and detectors. The ellipsometer sub-systems are operated in polarizer-sample-rotating-analyzer configuration granting access to the upper left 3 × 3 block of the normalized 4 × 4 Mueller matrix. The closed cycle magneto-cryostat sub-system provides sample temperatures between room temperature and 1.4 K and magnetic fields up to 8 T, enabling the detection of transverse and longitudinal magnetic field-induced birefringence. We discuss theoretical background and practical realization of the integrated mid-infrared, far-infrared, and terahertz optical Hall effect instrument, as well as acquisition of optical Hall effect data and the corresponding model analysis procedures. Exemplarily, epitaxial graphene grown on 6H-SiC, a tellurium doped bulk GaAs sample and an AlGaN/GaN high electron mobility transistor structure are investigated. The selected experimental datasets display the full spectral, magnetic field and temperature range of the instrument and demonstrate data analysis strategies. Effects from free charge carriers in two dimensional confinement and in a volume material, as well as quantum mechanical effects (inter-Landau-level transitions) are observed and discussed exemplarily.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

Optical functions of uniaxial rutile and anatase (TiO 2 ) revisited

In this study, the optical functions of uniaxial rutile and anatase (TiO2) were determined from 200 to 850 nm (6.2 to 1.46 eV) using several of four optical techniques: (1) standard spectroscopic two-modulator generalized ellipsometry (2-MGE), (2) near-normal-incidence two-modulator generalized ellipsometry microscopy (2-MGEM), (3) Mueller matrix transmission of rutile, and (4) polarized transmission of rutile. The 2-MGE measurements yielded highly accurate values of the dielectric functions and error estimates from 1.46 to 6.2 eV, whereas the polarization-dependent transmission yielded more accurate values of the absorption coefficient below the band edge of rutile. The 2-MGEM also measured the diattenuation, which is related to the birefringence, and other parameters but at near-normal incidence at a single wavelength (577 nm).

36 MATERIALS SCIENCE↗

Cross-polarization systematics due to Mizuguchi-Dragone condition breaking by a continuously rotating half-wave plate at prime focus in the Huan Tran telescope

Polarization modulation using a continuously rotating half-wave plate (HWP) is a promising technique to reduce both low-frequency noise and instrumental systematics for Cosmic Microwave Background (CMB) polarization measurements targeting in ationary B-modes. Although a HWP is best placed sky-side of the telescope optics in order to minimize systematics, >0.5 meter aperture class telescopes must put the HWP elsewhere in the optics chain due to current fabrication limitations in the available HWP size. Polarbear is a ground-based CMB experiment installed on the 2.5m aperture off-axis Gregorian-Dragone type Huan Tran Telescope (HTT) designed to satisfy the Mizuguchi-Dragone condition. Polarbear-2 is a receiver that will be installed on a second HTT in 2018. Polarbear-2 is designed to have a larger field-of-view (FOV) and vastly increased sensitivity to the polarized CMB compared to Polarbear. From the third season of observations, Polarbear has installed a continuously rotating HWP at the spatially localized focus plane between the HTT primary and secondary re ectors which is an optimal location for minimizing the HWP diameter. The HWP's polarization angle re ection with respect to its birefringent axis will theoretically break the Mizuguchi-Dragone condition when placed between the two reflectors and increase cross-polarization systematics. In this study, we analyze how the Mizuguchi-Dragone condition is violated due to a HWP at this location. We then estimate the crosspolarization systematics of the HTT using physical optics simulations. We model an ideal HWP at various angles to estimate the effects of demodulation. We evaluate the increased cross-polarization as the Stokes Q-U mixing term using the Mueller Matrix formalism. It is calculated that this term creates a varying dipole beam pattern whose amplitude ranges from 1% at the center to 10% at the edge FOV pixels for Polarbear and potentially up to 20% for Polarbear-2. We also estimate the leakage of the E-mode into the B-mode angular power spectrum measurements due to this cross-polarization. We show that the cross-polarization systematic error leakage is sufficiently lower than the Polarbear-2 statistical uncertainty thanks to mitigations such as focal plane averaging and sky rotation. Currently for Polarbear-2 we are planning to place the HWP at Gregorian focus, but keeping the HWP at prime focus as a back-up solution in case that there are unforeseen telescope spatial and HWP material size constraints. Through this study we find that even though a HWP between the two reflectors will violate the Mizuguchi-Dragone condition, this HWP at prime focus will still have sufficiently low cross-polarization for Polarbear-2. The prime focus HWP is a potential configuration that can be applied to similar off-axis Gregorian-Dragone telescopes in order to minimize the required HWP diameter.

Takakura, Satoru↗

The San Fernando Observatory video Stokes polarimeter

A study was conducted to determine the suitability of the San Fernando Observatory's 61 cm (24 inch) aperture vacuum solar telescope and 3 m (118 inch) focal length vacuum spectroheliograph for Stokes Polarimetry measurements. The polarization characteristics of these two instruments was measured by determining their Mueller matrices as a function of telescope orientation, field angle, wavelength, grating type, and position of the measuring beam in the telescope entrance window. In general, the polarizing and depolarizing properties are small so that inversion of the system Mueller matrix will permit the accurate measurement of Stokes profiles for vector magnetic field determination. A proposed polarimeter design based on the use of a TV camera system to simultaneously scan six different polarization components of a given line profile is described. This design, which uses no rotating optics or electronic modulators and makes efficient use of the available irradiance, promises to yield high quality vector magnetograms.

Richter, P. H.↗

Radar scene generation for tactical decision aids

The Mueller matrix and polarization covariance matrix for polarimetric radar systems was studied. The clutter was modeled by a layer of random permittivity, described by a three-dimensional correlation function, with variance, and horizontal and vertical correlation lengths. This model was applied, using the wave theory with Born approximations carried to the second order, to find the backscattering elements of the polarimetric matrices. Theoretical predictions are matched with experimental data for vegetation fields. The strong fluctuation theory was used to derive the backscattering cross sections. A two-layer anisotropic random medium model was developed for the active and passive microwave remote sensing of ice fields. A three-layer random medium model was adopted to study the volume scattering effects for the active and passive microwave remote sensing of snow-covered ice fields.

Kong, J. A.↗

Radar scene generation for tactical decision aids

The Mueller matrix and polarization covariance matrix for polarimetric radar systems was studied. The clutter is modeled by a layer of random permittivity, described by a three-dimensional correlation function, with variance, and horizontal and vertical correlation lengths. A general mixing formula was derived for discrete scatters immersed in a host medium. The results are applicable to general multiphase mixtures. The strong fluctuation theory was used to derive the backscattering cross sections, and was further extended to include higher order co-polarized and cross-polarized moments. A two-layer anisotropic random medium model was developed for the active and passive remote sensing of ice fields. A three-layer random medium model was adopted to study the volume scattering effects for the active and passive microwave remote sensing of snow-covered ice fields. The snow layer was simulated by an isotropic random medium and the ice layer by an anisotropic random medium. The vegetation canopy and snow-covered ice field were studied with a three-layer model, an isotropic random medium layer overlying an anisotropic random medium. The dyadic Green's function of the three-layer medium and the scattered electromagnetic intensities with Born approximation were calculated.

Kong, J. A.↗