Macroscopic Orientation Research Articles

Peculiarities of polarised light scattering in nematic liquid crystals with large-scale director perturbations

ABSTRACT We examine light scattering in a birefringent material, namely uniaxial nematic liquid crystal possessing macroscopic orientation perturbations (variations of director in planar alignment). Our theoretical analysis and direct experiments proved that the polarisation state of the scattered speckle-field is uniform and elliptical (in a common case). The polarisation ellipse azimuth of scattered waves is mirror reflected to one of the directly transmitted waves relative to the optical axis.

Characterization of quantum dot-like emitters in programmable arrays of nanowrinkles of 1L-WSe2

When combined with nanostructured substrates, two-dimensional semiconductors can be engineered with strain to tailor light–matter interactions on the nanoscale. Recently, room-temperature nanoscale exciton localization with controllable wrinkling in 1L-WSe2 was achieved using arrays of gold nanocones. Here, the characterization of quantum dot-like states and single-photon emitters in the 1L-WSe2/nanocone system is reported. The nanocones induce a wide range of strains, and as a result, a diverse ensemble of narrowband, potential single-photon emitters is observed. The distribution of emitter energies reveals that most reside in two spectrally isolated bands, leaving a less populated intermediate band that is spectrally isolated from the ensembles. The spectral isolation is advantageous for high-purity quantum light emitters, and anti-bunched emission from one of these states is confirmed up to 25 K. Although the spatial distribution of strain is expected to influence the orientation of the transition dipoles of the emitters, multimodal emission polarization anisotropy and atomic force microscopy reveal that the macroscopic orientation of the wrinkles is not a good predictor of dipole orientation. Finally, the emission is found to change with thermal cycling from 4 to 290 K and back to 4 K, highlighting the need to control factors such as temperature-induced strain to enhance the robustness of this quantum emitter platform. The initial characterization here shows that controlled nanowrinkles of 1L-WSe2 generate quantum light in addition to uncovering potential challenges that need to be addressed for their adoption into quantum photonic technologies.

Grain-level effects on in-situ deformation-induced phase transformations in a complex-phase steel using 3DXRD and EBSD

A novel complex-phase steel alloy is conceived with a deliberately unstable austenite, γ, phase that enables the deformation-induced martensitic transformations (DIMT) to be explored at low levels of plastic strain. The DIMT was thus explored, in-situ and non-destructively, using both far-field Three-Dimensional X-ray Diffraction (3DXRD) and Electron Back-Scatter Diffraction (EBSD). Substantial α′ martensite formation was observed under 10% applied strain with EBSD, and many ɛ grain formation events were captured with 3DXRD, indicative of the indirect transformation of martensite via the reaction γ→ɛ→α′. Using ɛ grain formation as a direct measurement of γ grain stability, the influence of several microstructural properties, such as grain size, orientation and neighbourhood configuration, on γ stability have been identified. Larger γ grains were found to be less stable than smaller grains. Any γ grains oriented with {100} parallel to the loading direction preferentially transformed with lower stresses. Parent ɛ-forming γ grains possessed a neighbourhood with increased ferritic/martensitic volume fraction. This finding shows, unambiguously, that the nearby presence of α and α′ promotes ɛ formation in neighbouring grains. The minimum strain work criterion model for ɛ variant prediction was also evaluated, which worked well for most grains. However, ɛ-forming grains with a lower stress were less well predicted by the model, indicating crystal-level behaviour must be considered for accurate ɛ formation. The findings from this work are considered key for the future design of alloys where the deformation response can be controlled by tailoring microstructure and local or macroscopic crystal orientations.

Injection-induced fault slip and associated seismicity in the lab: Insights from source mechanisms, local stress states and fault geometry

Probing source mechanisms of natural and induced earthquakes is a powerful tool to unveil associated rupture kinematics. The source processes of failure and slip instability driven by stress loading are affected by fault geometry, but the source ruptures of injection-induced seismicity in relation to fault structures and local stress states remain poorly understood. We have conducted a series of fault reactivation and slip experiments on sandstone samples containing faults with different surface roughness (smooth saw-cut fault and fractured rough fault). We impose progressive fluid injection to induce fault slip, and simultaneously monitor the associated acoustic emission (AE) activity. Using high-resolution AE recordings, we perform full moment tensor inversion of all located AE sources, and investigate the changes of AE source characteristics associated with induced fault slip and their relation to fault roughness. For the complex and rough fault, we observe significant non-double-couple components of AE sources and a high degree of focal mechanism heterogeneity. The temporal changes of AE mechanisms associated with injection-induced fault slip on the smooth fault reveal increasing proportions of double-couple components and decreasing variability of AE focal mechanisms when approaching the onset of slip events. The observed inconsistency between the nodal planes of AE sources and the macroscopic fault plane orientation is attributed to the development of secondary fracture networks surrounding the principal slip surface. We analyze changes in the magnitude-frequency characteristics and source mechanisms of AEs with fault-normal distance, showing that for the smooth (mature) fault, Gutenberg–Richter b-value of on-fault seismicity is lower and focal mechanisms are less heterogeneous, compared to off-fault seismicity. Our results emphasize the important role of roughness-related changes in local fault geometry and associated stress heterogeneity for source mechanisms and rupture kinematics of injection-induced seismicity.

Macroscopic Orientation and Local Mobility of PI during Shear Alignment of ISI and SIIS Triblock Copolymers Investigated by SAXS and Rheo-Dielectric Spectroscopy

Macroscopic Orientation and Local Mobility of PI during Shear Alignment of ISI and SIIS Triblock Copolymers Investigated by SAXS and Rheo-Dielectric Spectroscopy

Comparative 3D inversion of magnetotelluric phase tensors and impedances reveals electrically anisotropic base of Gawler Craton, South Australia

Isotropic three-dimensional (3-D) inversion has become a standard tool in the interpretation of magnetotelluric (MT) data. 3-D anisotropic inversion codes are under development, yet the number of unknowns increases by a factor of 6 rendering the problem extremely ill-posed. The presence of anisotropy is usually inferred from (i) spurious sequences of conductive and resistive bodies or (ii) comparison with two-dimensional anisotropic modelling approaches. Here, we investigate the 3-D structure of the Gawler Craton down to ∼250 km depth using 282 sites of the AusLAMP array located in the southern half of South Australia. Inversions of the MT impedance as phase tensors and real and imaginary parts result in diverging structures at depths > 70 km. We demonstrate that a unifying model that explains all data types similarly well is suggestive of an anisotropic resistivity structure at the base of the Gawler Craton lithosphere at depths of 120–210 km. Depth location and orientation of the anisotropy agree well with results from the analysis of seismic receiver functions. We suggest that electric anisotropy in the Gawler Craton is a result of lattice-preferred orientation of olivine crystals and metasomatic processes with macroscopic preferential orientation. Our results illustrate that inversion of phase tensor data is superior for the direct imaging of anisotropic resistivity contrasts in otherwise isotropic resistivity models; inversion models obtained with impedances may miss such structures. “Comparable” overall RMS misfits are often meaningless when comparing inversion results for various data types since sensitivities differ between data types. Reliable inversion results consistent with the entire data set can only be recovered if data fits are assessed systematically for all data representations. We also discuss the influence of error settings for phase tensors on the inversion. Our study also revealed that, if persistent across large areas, (i) parallel orientation of phase tensor major axes, (ii) constantly high phase tensor maximum phases or (iii) diverging directions of phase tensor major axes and induction arrows are suggestive of anisotropic structures and corresponding hypotheses should be evaluated.

Linear Dichroism Measurements for the Study of Protein-DNA Interactions.

Linear dichroism (LD) is a differential polarized light absorption spectroscopy used for studying filamentous molecules such as DNA and protein filaments. In this study, we review the applications of LD for the analysis of DNA-protein interactions. LD signals can be measured in a solution by aligning the sample using flow-induced shear force or a strong electric field. The signal generated is related to the local orientation of chromophores, such as DNA bases, relative to the filament axis. LD can thus assess the tilt and roll of DNA bases and distinguish intercalating from groove-binding ligands. The intensity of the LD signal depends upon the degree of macroscopic orientation. Therefore, DNA shortening and bending can be detected by a decrease in LD signal intensity. As examples of LD applications, we present a kinetic study of DNA digestion by restriction enzymes and structural analyses of homologous recombination intermediates, i.e., RecA and Rad51 recombinase complexes with single-stranded DNA. LD shows that the DNA bases in these complexes are preferentially oriented perpendicular to the filament axis only in the presence of activators, suggesting the importance of organized base orientation for the reaction. LD measurements detect DNA bending by the CRP transcription activator protein, as well as by the UvrB DNA repair protein. LD can thus provide information about the structures of protein-DNA complexes under various conditions and in real time.

Macroscopic Nematic Orientation Dictated by an Orientationally Frustrated Random-Field Surface: Equilibrium Structure and Kinetics

Macroscopic Nematic Orientation Dictated by an Orientationally Frustrated Random-Field Surface: Equilibrium Structure and Kinetics

Prediction of slip activity of crystal grains around semi-circular and semi-elliptical notches in thin-sheet specimens of pure titanium using formulated macroscopic stress distribution and crystal orientation

Thin metal sheets and wires are important materials for various devices used in electrical, mechanical, and medical fields. With the downsizing of these devices, demand for thinner sheets and wires has increased. Amongst the many metals available, pure titanium has been attracting much attention for use in medical and dental devices because of its good biocompatibility in addition to its light weight and high corrosion resistance. However, thin metal sheets and wires are usually polycrystalline materials and, with the downsizing of materials, there is a loss of homogeneity during deformations. Inhomogeneous deformation becomes significant in thin sheets and wires, owing to the different crystal orientations and geometries of crystal grains. Furthermore, the shapes of such devices are not uniform, unlike, say, a simple rod. Therefore, macroscopic stress and strain concentrations should be taken into consideration when designing these devices as they affect the localization of deformation and the resultant fracture. In this study, semi-circular and semi-elliptical notched specimens made of thin-sheet polycrystalline pure titanium are subjected to tensile testing. Inhomogeneous deformation caused by crystallographic slip is observed near the notch root. Analysis of the crystal orientation and observation of the slip line show that the slip initiation in crystal grains is affected by the macroscopic stress distribution and can be predicted from the slip activity calculated from both the critical resolved shear stress on the slip systems and the resolved shear stress acting on prospective slip planes obtained from the macroscopic multiaxial stress distribution.

Flexible piezoelectric generator based on PLLA/ZnO oriented fibers for wearable self-powered sensing

Herein, PLLA/ZnO oriented fibers were prepared via orientation electrospinning towards a piezoelectric generator, omitting polarization and stretching postprocesses. The composite fibers achieved macroscopic orientation and molecular alignment, as well as higher crystallinity and more polar phase for PLLA. Collectively, the resulting generator exhibited dramatic and stable piezoelectric signals over 1000 s, boosting the open-circuit voltage to 7.9 V, nearly 4.6 times larger than that of the random neat device. With the same changing tendency, the simulated results confirmed oriented fibers and ZnO induced stress concentration, imparting better piezoelectricity. Furthermore, the generated electricity from the generator with a short-circuit current of 286nA and an output power density of 1.25 mW cm−3 charged a 10 μF capacitor up to 2 V at 210 s then illuminated a LED. Encouragingly, high flexibility and sensitivity allowed this device to function as a wearable self-powered sensor for differentiating human movement and monitoring human health.

Triple and double twin interfaces in magnesium—the role of disconnections and facets

Twin boundaries have been shown to deviate from the twinning planes in hcp metals, and facets have often been observed in twin interfaces. This study presents a twinning disconnection-based model for faceting in single, double and triple twin boundaries in magnesium. Primary twinning disconnections predicted via symmetry arguments are shown to produce commensurate facets in single twin boundaries, which are then transformed into commensurate facets in double twin boundaries via the action of secondary twinning disconnections. In contrast, it is shown that for triple twin boundaries with tension-compression-tension twinning sequence, no commensurate facets can be produced by the action of tertiary twinning disconnections. The effect of facets on the macroscopic orientation of twin interfaces is discussed. Theoretical findings are validated by a transmission electron microscopy study of a hot rolled Mg-1.18wt%Al-1.77wt%Nd alloy. Single and double twins are observed, as well as rare triple twins, and the interface between the matrix and a triple twin is captured for the first time. Facets consistent with theoretical predictions are imaged via high-resolution TEM and macroscopic deviations of the boundaries from the primary twinning planes are measured.

Bioinspired Liquid Crystalline Spinning Enables Scalable Fabrication of High-Performing Fibrous Artificial Muscles.

Leveraging liquid crystal elastomers (LCEs) to realize scalable fabrication of high-performing fibrous artificial muscles is of particular interest because these active soft materials can provide large, reversible, programmable deformations upon environmental stimuli. High-performing fibrous LCEs require the used processing technology to enable shaping LCEs into micro-scale fine fibers as thin as possible while achieving macroscopic LC orientation, which however remains a daunting challenge. Here, a bioinspired spinning technology is reported that allows for continuous, high-speed production (fabrication speed up to 8400mh-1 ) of thin and aligned LCE microfibers combined with rapid deformation (actuation strain rate up to 810% s-1 ), powerful actuation (actuation stress up to 5.3MPa), high response frequency (50Hz), and long cycle life (250 000 cycles without obvious fatigue). Inspired by liquid crystalline spinning of spiders that takes advantage of multiple drawdowns to thin and align their dragline silks, internal drawdown via tapered-wall-induced-shearing and external drawdown via mechanical stretching are employed to shape LCEs into long, thin, aligned microfibers with the desirable actuation performances, which few processing technologies can achieve. This bioinspired processing technology capable of scalable production of high-performing fibrous LCEs would benefit the development of smart fabrics, intelligent wearable devices, humanoid robotics, and other areas.

Design of N-Type Textured Bi2 Te3 with Robust Mechanical Properties for Thermoelectric Micro-Refrigeration Application.

Thermoelectric refrigeration is one of the mature techniques used for cooling applications, with the great advantage of miniaturization over traditional compression refrigeration. Due to the anisotropic thermoelectric properties of n-type bismuth telluride (Bi2 Te3 ) alloys, these two common methods, including the liquid phase hot deformation (LPHD) and traditional hot forging (HF) methods, are of considerable importance for texture engineering to enhance performance. However, their effects on thermoelectric and mechanical properties are still controversial and not clear yet. Moreover, there has been little documentation of mechanical properties related to micro-refrigeration applications. In this work, the above-mentioned methods are separately employed to control the macroscopic grain orientation for bulk n-type Bi2 Te3 samples. The HF method enabled the stabilization of both composition and carrier concentration, therefore yielding a higher quality factor to compare with that of LPHD samples, supported by DFT calculations. In addition to superior thermoelectric performance, the HF sample also exhibited robust mechanical properties due to the presence of nano-scale distortion and dense dislocation, which is the prerequisite for realizing ultra-precision machining. This work helps to pave the way for the utilization of n-type Bi2 Te3 for commercial micro-refrigeration applications.

GLOBAL REGULARITY TO THE 2D INHOMOGENEOUS LIQUID CRYSTAL FLOWS WITH LARGE INITIAL DATA AND VACUUM

We study the 2D incompressible nematic liquid crystal equations in a smooth bounded domain, where the velocity u and macroscopic molecular orientation d admit the Dirichlet and Neumann boundary condition, respectively. Under a geometric condition for the initial orientation field, we establish the global existence of strong solutions with large initial data. In particular, the initial density can be allowed to vanish. Furthermore, this result extends the corresponding results of J. Li (2015) and X. Li (2017) to the Neumann boundary condition and removes the smallness conditions on the initial data.

Discharge of elongated grains in silos under rotational shear.

The discharge of elongated particles from a silo with rotating bottom is investigated numerically. The introduction of a slight transverse shear reduces the flow rate Q by up to 70% compared with stationary bottom, but the flow rate shows a modest increase by further increasing the external shear. Focusing on the dependency of flow rate Q on orifice diameter D, the spheres and rods show two distinct trends. For rods, in the small-aperture limit Q seems to follow an exponential trend, deviating from the classical power-law dependence. These macroscopic observations are in good agreement with our earlier experimental findings [Phys. Rev. E 103, 062905 (2021)2470-004510.1103/PhysRevE.103.062905]. With the help of the coarse-graining methodology we obtain the spatial distribution of the macroscopic density, velocity, kinetic pressure, and orientation fields. This allows us detecting a transition from funnel to mass flow pattern caused by the external shear. Additionally, averaging these fields in the region of the orifice reveals that the strong initial decrease in Q is mostly attributed to changes in the flow velocity, while the weakly increasing trend at higher rotation rates is related to increasing packing fraction. Similar analysis of the grain orientation at the orifice suggests a correlation of the flow rate magnitude with the vertical orientation and the packing fraction at the orifice with the order of the grains. Lastly, the vertical profile of mean acceleration at the center of the silo denotes that the region where the acceleration is not negligible shrinks significantly due to the strong perturbation induced by the moving wall.

Alignment of Organic Conjugated Molecules for High-Performance Device Applications.

High-performance organic semiconductor materials as the electroactive components of optoelectronic devices have attracted much attention and made them ideal candidates for solution-processable, large-area, and low-cost flexible electronics. Especially, organic field-effect transistors (OFETs) based on conjugated semiconductor materials have experienced stunning progress in device performance. To make these materials economically viable, comprehensive knowledge of charge transport mechanisms is required. The alignment of organic conjugated molecules in the active layer is vital to charge transport properties of devices. The present review highlights the recent progress of processing-structure-transport correlations that allow the precise and uniform alignment of organic conjugated molecules over large areas for multiple electronic applications, including OFETs, organic thermoelectric devices (OTEs), and organic phototransistors (OPTs). Different strategies for regulating crystallinity and macroscopic orientation of conjugated molecules are introduced to correlate the molecular packing, the device performance, and charge transport anisotropy in multiple organic electronic devices.

Electrically Switchable Anisometric Carbon Quantum Dots Exhibiting Linearly Polarized Photoluminescence: Syntheses, Anisotropic Properties, and Facile Control of Uniaxial Orientation.

Carbon quantum dots (CQDs) have been extensively explored in diverse fields because of their exceptional features. The nanometric particles with photoluminescence (PL) benefit various optical and photonic applications. However, the majority of previous reports have mainly focused on either unpolarized or circular-polarized (CP) PL. Linearly polarized (LP) emission of CQDs is limited mainly because of their isometric shape and difficulties in macroscopic orientation control. Herein, we report syntheses of anisometric CQDs and facile control of the uniaxial orientation on a macroscopic scale, which results in linearly polarized photoluminescence (LP-PL). The anisometric CQDs are synthesized from rigid-rod-shaped precursors and evenly dispersed in the rod-like liquid crystal (LC) host. As-synthesized CQDs exhibit a PL quantum yield as high as 35% in chloroform. In addition to uniform alignment, facile directional switching of the elongated CQD is established by employing the electrical responsiveness of the CQD and host LC. Therefore, the dichroic photophysical properties of anisometric CQDs have been beneficially adopted for fabrications of polarization-sensitive and electrically switchable PL devices. Also, anisometric CQDs are embedded in polymer films with molecular orientational patterns and clearly recognized by LP-PL.

Liquid Crystalline Elastomers Based on Click Chemistry.

Liquid crystalline elastomers (LCEs) have emerged as an important class of functional materials that are suitable for a wide range of applications, such as sensors, actuators, and soft robotics. The unique properties of LCEs originate from the combination between liquid crystal and elastomeric network. The control of macroscopic liquid crystalline orientation and network structure is crucial to realizing the useful functionalities of LCEs. A variety of chemistries have been developed to fabricate LCEs, including hydrosilylation, free radical polymerization of acrylate, and polyaddition of epoxy and carboxylic acid. Over the past few years, the use of click chemistry has become a more robust and energy-efficient way to construct LCEs with desired structures. This article provides an overview of emerging LCEs based on click chemistries, including aza-Michael addition between amine and acrylate, radical-mediated thiol-ene and thiol-yne reactions, base-catalyzed thiol-acrylate and thiol-epoxy reactions, copper-catalyzed azide-alkyne cycloaddition, and Diels-Alder cycloaddition. The similarities and differences of these reactions are discussed, with particular attention focused on the strengths and limitations of each reaction for the preparation of LCEs with controlled structures and orientations. The compatibility of these reactions with the traditional and emerging processing techniques, such as surface alignment and additive manufacturing, are surveyed. Finally, the challenges and opportunities of using click chemistry for the design of LCEs with advanced functionalities and applications are discussed.

力を可視化できるキラル液晶エラストマーの動的挙動制御

Strain sensors are a key for the development of next-generation soft robots. For such applications, the electronic sensing using flexible electronic materials are continuing to be at the forefront of the sensing technology. Recently, optical-sensing technology have attracted much attention because of high spatiotemporal resolution, high sensitivity and noninvasively. Especially, chiral-nematic liquid-crystalline elastomers have much attention to be applied to optical strain sensors because of the change of selective reflection wavelength in response to the strain. Here, we introduce our recent research on optical strain sensors using chiral-nematic liquid-crystalline elastomers. There is remarkable maturity in the development of numerous stimuli-responsive liquid-crystalline elastomers. However, the control of the recovery process after the removal of the stimuli has remained difficult. Interestingly, our simple materials design concept of “layering the elastomers with other materials” allows us to arbitrary control the recovery process in both macroscopic deformation and microscopic molecular orientation. Based on the concept, we have succeeded to fabricate a mechano-optical sensor with high sensitivity and high spatiotemporal resolution. This concept would open a pathway to control the recovery process in various stimuli-responsive liquid-crystalline elastomers.

Polarization Spectroscopy of Anisotropic Plasmons in Self‐Oriented Nanoclusters of Gold on Monolayer of Nitrogen Atoms Chemisorbed at GaAs(001) Surface

Herein, the formation of Au nanoclusters on nitridized GaAs(001) surface is described, as well as the structure diagnostics and spectroscopic studies which reveal a strong anisotropy of the plasmons localized on the clusters. Principal aspects of the work are the following. Technologically, structures of Au/N/GaAs are fabricated with a monolayer of nitrogen atoms chemisorbed preliminary onto GaAs substrate to prevent its reaction with subsequently deposited Au film. Annealing of the structures Au/N/GaAs results in the appearance of anisotropic nanoclusters of chemically clean gold on GaAs surface. Experimentally, the existence of in‐surface anisotropy of Au clusters is verified with the atomic force microscopy and it is investigated with the resonant optical spectroscopies of anisotropy reflectance and polarized reflection. All the methods are applied jointly for the detailed study of anisotropic plasmons revealed in gold nanocluster arrays. Theoretically, the plasmon‐conditioned features observed in optical polarized spectra are interpreted using an optical model of in‐surface anisotropic plasmons in Au nanospheroids. As a result, the macroscopic anisotropy and orientation of gold nanoclusters and their plasmons relative to the crystallographic axes of GaAs substrate are unambiguously established and reliably specified.