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At least 19 records

Development of a spectroscopic Mueller matrix imaging ellipsometer for nanostructure metrology

In this paper, we describe the development of a spectroscopic Mueller matrix imaging ellipsometer (MMIE), which combines the great power of Mueller matrix ellipsometry with the high spatial resolution of optical microscopy. A dual rotating-compensator configuration is adopted to collect the full 4 × 4 imaging Mueller matrix in a single measurement. The light wavelengths are scanned in the range of 400–700 nm by a monochromator. The instrument has measurement accuracy and precision better than 0.01 for all the Mueller matrix elements in both the whole image and the whole spectral range. The instrument was then applied for the measurement of nanostructures combined with an inverse diffraction problem solving technique. The experiment performed on a photoresist grating sample has demonstrated the great potential of MMIE for accurate grating reconstruction from spectral data collected by a single pixel of the camera and for efficient quantification of geometrical profile of the grating structure over a large area with pixel resolution. It is expected that MMIE will be a powerful tool for nanostructure metrology in future high-volume nanomanufacturing.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

Mueller-matrix mapping of biological tissues in differential diagnosis of optical anisotropy mechanisms of protein networks

We report a model of Mueller-matrix description of optical anisotropy of protein networks in biological tissues with allowance for the linear birefringence and dichroism. The model is used to construct the reconstruction algorithms of coordinate distributions of phase shifts and the linear dichroism coefficient. In the statistical analysis of such distributions, we have found the objective criteria of differentiation between benign and malignant tissues of the female reproductive system. From the standpoint of evidence-based medicine, we have determined the operating characteristics (sensitivity, specificity and accuracy) of the Mueller-matrix reconstruction method of optical anisotropy parameters and demonstrated its effectiveness in the differentiation of benign and malignant tumours. (laser applications and other topics in quantum electronics)

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

Mueller matrix ellipsometric detection of profile asymmetry in nanoimprinted grating structures

Mueller matrix ellipsometry (MME) is applied to detect foot-like asymmetry encountered in nanoimprint lithography (NIL) processes. We present both theoretical and experimental results which show that MME has good sensitivity to both the magnitude and direction of asymmetric profiles. The physics behind the use of MME for asymmetry detection is the breaking of electromagnetic reciprocity theorem for the zeroth-order diffraction of asymmetric gratings. We demonstrate that accurate characterization of asymmetric nanoimprinted gratings can be achieved by performing MME measurements in a conical mounting with the plane of incidence parallel to grating lines and meanwhile incorporating depolarization effects into the optical model. The comparison of MME-extracted asymmetric profile with the measurement by cross-sectional scanning electron microscopy also reveals the strong potential of this technique for in-line monitoring NIL processes, where symmetric structures are desired.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

Fluorescent Mueller matrix analysis of a highly scattering turbid media

We report the fluorescent Mueller matrix analysis of a highly scattering, inhomogeneous, and low quantum yield polymeric nanoparticle system. Both the ground and the excited state anisotropy of this turbid system were measured. The excited state anisotropy was found to be higher than ground state anisotropy by inverse polar decomposition analysis. The depolarization coefficients of these polythiophene nanoparticles were experimentally determined by recording Mueller matrices from this complex random medium. This approach provides an alternative method of determining optical characteristics of low quantum efficiency turbid system like fluorescently leveled tissue phantom.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

Mueller-matrix mapping of optically anisotropic fluorophores of biological tissues in the diagnosis of cancer

We report the results of studying the polarisation manifestations of laser autofluorescence of optically anisotropic structures in biological tissues. A Mueller-matrix model is proposed to describe their complex anisotropy (linear and circular birefringence, linear and circular dichroism). The relationship is established between the mechanisms of optical anisotropy and polarisation manifestations of laser autofluorescence of histological sections of rectal tissue biopsy in different spectral regions. The ranges of changes in the statistical moments of the 1st-to-4th orders, which describe the distribution of the azimuth-invariant elements of Mueller matrices of rectal tissue autofluorescence, are found. Effectiveness of laser autofluorescence polarimetry is determined and the histological sections of biopsy of benign (polyp) and malignant (adenocarcinoma) tumours of the rectal wall are differentiated for the first time. (laser biophotonics)

62 RADIOLOGY AND NUCLEAR MEDICINE↗

Metasurface‐Based Mueller Matrix Microscope

In conventional optical microscopes, image contrast of objects mainly results from the differences in light intensity and/or color. Muller matrix optical microscopes (MMMs), on the other hand, can provide significantly enhanced image contrast and rich information about objects by analyzing their interactions with polarized light. However, state-of-the-art MMMs are fundamentally limited by bulky and slow polarization state generators and analyzers. Here, the study demonstrates a metasurface-based MMM, i.e., Meta-MMM, which is equipped with a chip-integrated, single-shot metasurface polarization state analyzer (Meta-PSA). The Meta-MMM is featured with high-speed measurement (≈2s per Muller matrix (MM) image), superior operation stability, dual-color operation, and high measurement accuracy (measurement error 1–2%) for MM imaging. The Meta-MMM is applied to nanostructure characterization, surface morphology analysis, and discovering birefringent structures in honeybee wings. As a result, the Meta-MMMs hold the promise to revolutionize various applications from biological imaging, medical diagnosis, and material characterization to industry inspection and space exploration.

36 MATERIALS SCIENCE↗

Exact relativistic expressions for polarization of incoherent Thomson scattering

We present a derivation of the degree of polarization for incoherent Thomson scattering (TS) using Mueller matrix formalism. An exact analytic solution is obtained for spectrum-integrated matrix elements. The solution is valid for the full range of incident polarizations, scattering angles, and electron thermal motion from non-relativistic to ultra-relativistic. It is based on a newly developed theoretical model, a finite transit time (FTT) correction to previous theoretical work on TS polarization. The Mueller matrix elements are substantially different from previous calculations without the FTT correction, even to the lowest linear order in T e =m e c 2 <<1. Mathematically, the derivation is a unique example of fully analytical integration of the 3D scattering operator over a relativistic Maxwellian distribution function; experimentally, the results have application to the use of the polarization properties of Thomson scattered light as a method of electron temperature measurement. The results can also be used as a reliable tool for benchmarking and verification of numerical codes for frequency resolved properties of TS polarization.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗

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]↗

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↗