Crystal Alignment Research Articles

Rapid Meniscus-Assisted Solution Printing of Large-Area Stripe Arrays of Highly Oriented Conjugated Polymers for Field-Effect Transistors.

The ability to pattern semiconducting conjugated polymers (CPs) and concurrently enable their highly oriented chains represents an important endeavor to render their high charge mobility for electronic devices. However, simple yet generalizable routes to CPs with such desirable characteristics are limited. Herein, we report a robust meniscus-assisted solution printing (MASP) strategy to craft arrays of donor-acceptor CP stripes and scrutinize the correlation between different stripes and their charge transport attributes. Specifically, the MASP constrains the CP solution to evaporate between two nearly parallel plates with a stationary upper plate and a mobile lower plate containing periodic photoresist (PR) microchannels. Orchestrating the MASP speed comparable to the CP crystal growth rate yields CP stripe arrays with highly aligned CP crystals, resulting in the highest carrier mobility. Notably, our MASP technique can conveniently pattern other CPs of interest. It stands out as a simple strategy to impart large-scale production of functional materials for a wide range of applications in optics, electronics, sensors, etc.

Liquid Piezoelectric Materials: Linear Electromechanical Effect in Fluid Ferroelectric Nematic Liquid Crystals

AbstractThe first demonstration of converse piezoelectricity in 3D fluids is presented by measuring a linear electromechanical effect in ferroelectric nematic liquid crystals. The observed piezoelectric coupling constant below 6 kHz electric field is larger than 1 nC/N, comparable to, or better than, values for the strongest solid piezoelectric materials. Symmetry considerations indicate that the alignment of the ferroelectric nematic liquid crystal in the experimental study is not optimized, so the observed signal is likely only a fraction of the theoretically achievable signal. Understanding the electromechanical response of ferroelectric nematics will enable mechanical energy harvesting and open up a new avenue for developing fluid actuators, micro positioners, and electrically tunable optical lenses.

Synthesis and characterization of strontium substituted monetite coatings via mild phosphate chemical conversion

Strontium (Sr) substitution into calcium phosphate (CaP) materials has gained acceptance in research into the enhancement of physiochemical and osteogenic potential. Conventional synthesis of metal cationic substitution into CaP coatings on metal substrate usually takes relatively high temperature (﹥100 °C) and hours of processing time. Herein, a mild phosphate chemical conversion method was developed for preparing Sr-substituted CaP coatings on surface of titanium (Ti) in the presence of increasing amount of Sr (40–60 mol%). The results indicated that the complete and even coatings could be produced on the whole surface of Ti only within 50–60 % Sr and the coatings represented a unique lamellar texture in micro/nano-scale. As Sr concentration increased, the phases of coatings were predominantly indexed to monetite and SrHPO4, which presented a highly oriented crystal alignment. With high content of Sr, monetite, instead of brushite, was deposited in the coatings. The possible mechanism of coating formation was proposed that α-SrHPO4 and α-monetite were co-deposited in the acidic phosphating solution and finally a compound of (CaxSr1-x)HPO4 was produced on surface of Ti. Results revealed that coatings formed at high degree of Sr substitution exhibited relative improved mechanical and electrochemical properties. The coatings enhanced the cell focal adhesion and proliferation of BMSCs compared with that of the bare Ti.

Improved optical quality of heteroepitaxially grown metal-organic framework thin films by modulating the crystal growth.

Fabricating high-quality thin films of metal-organic frameworks (MOFs) is important for integrating MOFs in various applications. Specifically, optical/electrical devices require MOF thin films that are crystallographically oriented, with closely packed crystals and smooth surfaces. Although the heteroepitaxial growth approach of MOFs on metal hydroxides has been demonstrated to control the orientation of the three crystallographic axes, the fabrication of MOF thin films with both three-dimensional crystallographic orientation and smooth surfaces remains a challenge. In this study, we report the fabrication of high-quality thin films of MOFs with closely packed MOF crystals, smooth surfaces, optical transparency, and crystal alignment by modulating the crystal growth of MOFs using the heteroepitaxial growth approach. High-quality thin films of Cu-paddlewheel-based pillar-layered MOFs are fabricated on oriented Cu(OH)2 thin films via epitaxial growth using acetate ions as modulators to control the crystal morphology. Increasing the modulator concentration results in a uniform crystal shape with a relatively long one-dimensional pore direction and uniform heterogeneous nucleation over the entire film. The MOF thin films fabricated using the modulator exhibit high optical transparency. High-quality MOF thin films with dense and flat surfaces will pave the way for integrating MOFs into sophisticated optical and electrical devices.

Exploring the interplay of liquid crystal orientation and spherical elastic shell deformation in spatial confinement.

The application of liquid crystal technology typically relies on the precise control of molecular orientation at a surface or interface. This control can be achieved through a combination of morphological and chemical methods. Consequently, variations in constrained boundary flexibility can result in a diverse range of phase behaviors. In this study, we delve into the self-assembly of liquid crystals within elastic spatial confinement by using the Gay-Berne model with the aid of molecular dynamics simulations. Our findings reveal that a spherical elastic shell promotes a more regular and orderly alignment of liquid crystals compared to a hard shell. Moreover, during the cooling process, the hard-shell confined system undergoes an isotropic-smectic phase transition. In contrast, the phase behavior within the spherical elastic shell closely mirrors the isotropic-nematic-smectic phase transition observed in bulk systems. This indicates that the orientational arrangement of liquid crystals and the deformations induced by a flexible interface engage in a competitive interplay during the self-assembly process. Importantly, we found that phase behavior could be manipulated by altering the flexibility of the confined boundaries. This insight offers a fresh perspective for the design of innovative materials, particularly in the realm of liquid crystal/polymer composites.

Dielectric Meta-Atoms with Liquid Crystal Alignment Effect for Electrically Tunable Metasurface

Dielectric metasurfaces with tunable functions are increasingly appealing to both the academia and industrial communities. Among the many tuning mechanisms reported so far, metasurface immersed in liquid crystal (LC) stands out as one of the most viable approaches for industrial applications such as Lidar and 3D sensing. However, as with traditional LC devices, alignment processes are necessary for LC-based tunable metasurfaces, leading to additional costs in terms of time and materials. In this paper, we present a novel LC-based tunable metasurface, wherein the alignment of LC is provided by the metasurface structures. LC serves as the dielectric environment for the metasurface with an electrically tunable refractive index. Simultaneously, purposely engineered metasurface induces alignment effects within the LC. The alignment effect of the metasurface on the LC was quantitatively characterized using crossed polarizers. A marked transmission contrast was observed, indicating the high-quality alignment provided solely by the metasurface. Electrical tunability was also measured, recording a maximum modulation depth in transmission amplitude of 94% at near-infrared telecommunication wavelengths. This work highlights the remarkable advantages of LC-based tunable metasurface devices, making them highly valuable for next-generation metasurface-integrated LC on silicon devices.

Cost-effective photolithography-based dual liquid crystal alignment for versatile electro-optic applications

Nematic liquid crystals (NLCs) containing rod-shaped molecules exhibit remarkable birefringence and tunability. Therefore, they are of high interest for numerous electro-optic applications. Uniform molecular orientation is of utmost importance for their effective use. Current techniques for LC alignment, such as mechanical rubbing or photo-alignment, have limitations in creating specifically complex LC orientation patterns. To address this issue, we have developed a cost-effective photolithography-based technique for dual LC alignment which combines planar and vertical alignments. Our process involves inexpensive exposure systems and a lift-off process and employs commercially-available alignment materials, thereby reducing production costs. We utilized this process to generate a tunable phase grating with diffraction efficiencies which can be varied through voltage application, thus demonstrating the potential of dual alignment. Furthermore, we investigated smart windows that are insensitive to polarization, utilizing a two-dimensional grating structure, achieving high haze values and dynamic shading without relying on incident polarization.

Spontaneously homogeneous alignment of liquid crystals on self-assembly organic rubrene

A novel spontaneously homogeneous liquid crystal (LC) alignment with self-assembled organic rubrene layer on the substrate surface has been reported. The spontaneous alignment technique without surface pre-treatment results in low cost, short processing time, and the room-temperature processing extends application to plastic device. The rubrene-nematic LC mixture is used to fabricate the LC cell. During the capillary filling, the LC molecules align in the flow direction. Meanwhile, the flow-induced LC alignment enforces the tetracene of the rubrene dopants along the flow direction because of the van der Waals and π–π interactions between the rubrene and LC molecules. Afterwards, the rubrene dopants spontaneously migrate onto substrate surface and self-assemble as the triclinic crystalline rubrene (TCR) with ribbon morphology. The LC alignment on TCR has a low pretilt angle, thereby providing a homogeneous LC alignment spontaneously. LC alignment on TCR shows a higher thermal stability compared to conventional polyimide due to the strong interactions of the rubrene and LC molecules. Moreover, the rubrene molecules remain in the bulk suppress the free-ions, decrease the rotational viscosity of LCs and hence shortening the response time of cell. The suppressed free-ions also decrease the screening effect on the substrate surfaces and hence the operation voltage of cell. The TCR structure on the substrate surface and the residual rubrene molecules dispersed in the bulk simultaneously contribute to the enhancement in electro-optical performance of the LC cell.

CLASS Observations of Atmospheric Cloud Polarization at millimeter Wavelengths

The dynamic atmosphere imposes challenges to ground-based cosmic microwave background observation, especially for measurements on large angular scales. The hydrometeors in the atmosphere, mostly in the form of clouds, scatter the ambient thermal radiation and are known to be the main linearly polarized source in the atmosphere. This scattering-induced polarization is significantly enhanced for ice clouds due to the alignment of ice crystals under gravity, which are also the most common clouds seen at the millimeter-astronomy sites at high altitudes. This work presents a multifrequency study of cloud polarization observed by the Cosmology Large Angular Scale Surveyor experiment on Cerro Toco in the Atacama Desert of northern Chile, from 2016–2022, at the frequency bands centered around 40, 90, 150, and 220 GHz. Using a machine-learning-assisted cloud classifier, we made connections between the transient polarized emission found in all four frequencies with the clouds imaged by monitoring cameras at the observing site. The polarization angles of the cloud events are found to be mostly 90° from the local meridian, which is consistent with the presence of horizontally aligned ice crystals. The 90 and 150 GHz polarization data are consistent with a power law with a spectral index of 3.90 ± 0.06, while an excess/deficit of polarization amplitude is found at 40/220 GHz compared with a Rayleigh scattering spectrum. These results are consistent with Rayleigh-scattering-dominated cloud polarization, with possible effects from supercooled water absorption and/or Mie scattering from a population of large cloud particles that contribute to the 220 GHz polarization.

Bismuth-magnesium-oxide-based graphene oxide hybrid film for liquid crystal device application

Hybrid films containing bismuth magnesium oxide (BiMgO) and graphene oxide (GO) are investigated in this study. Solution-processed brush coating is used to fabricate the hybrid films, with the graphene oxide weight ratios adjusted to 0, 5, and 15%. The hybrid films show more stable and higher optical transmittances than the pure BiMgO film. A directional micro/nanogroove structure is observed on the hybrid film surface, which is derived from the shear stress during the brush-coating process; this anisotropic structure is used as a uniform liquid crystal (LC) alignment layer. Uniform and homogeneous LC alignment is then demonstrated via polarized optical microscopy and pretilt angle analyses, along with perfect light-control performance. Enhanced LC polar anchoring energy and hysteresis-free characteristics are observed for the brush-coated hybrid film as the GO-doping concentration is increased. Based on this perspective, the BiMgO-based GO hybrid film achieved via brush coating has potential for applications in next-generation LC systems.

Dynamic propagation of an Airy beam in metasurface-enabled gradiently-aligned liquid crystals

Abstract Due to the unique self-acceleration, self-healing, and non-diffraction properties, Airy beams have been explored extensively and found applications in various fields. It has been proven as an essential aspect to tune the trajectory of Airy beams for extensive applications. In this paper, we propose a method based on liquid crystal (LC) alignment with metasurfaces, which enables dynamic tuning of the trajectory of Airy beams. Benefiting from both the tunable property of LCs and the compact alignment of metasurfaces, we achieve a sizeable linear potential in a short distance, which leads to the effective tuning of the trajectory of Airy beams dynamically. The introduction of metasurfaces into the alignment of LCs provides a promising method to manipulate the planar optical field.

Graphene-oxide-doped oriented nickel oxide film achieved through brush coating for liquid crystal system

Hybrid films containing nickel oxide and graphene oxide are introduced in this work. The hybrid films are fabricated through a one-step brush-coating process, and the weight ratios of graphene oxide are controlled to 0, 5, and 15 %. The fabricated hybrid films show oriented nano/microgroove structures on their surfaces by directional shear stress, which originates from the brush hair movements during the solution-processed brush-coating process. The hybrid film formation is confirmed using X-ray photoelectron spectroscopy. The films also demonstrate high optical transmittance with amorphous structures. The hybrid films are then used to form liquid crystal (LC) alignment layers, and uniform as well as homogeneous LC alignment is confirmed via polarized optical microscopy and pretilt angle analyses. Compared to the pure nickel-oxide film, the hybrid film with graphene oxide enhances LC alignment stability by increasing the polar anchoring energy of the surface LC molecules. From these observations, the hybrid film containing metal oxide and graphene oxide is expected to be a promising alternative for functional LC systems.

Surface confinement of vertically aligned liquid crystals between flexible silver nanoparticles hybridized polyimide thin layers

Alignment of liquid crystals (LCs) has emerged as an essentially fundamental approach for exploring the electro-optical performance and fabricating novel LC devices. Growing evidence suggests that the surface wettability of the alignment layer plays a key role in tuning the tilt angles of LCs. In this work, silver (Ag) nanoparticles (d ≤ 100 nm) are blended in polyimide (PI) by a wide range of concentration from 0.1% to 1.0% to tune surface wettability and align LCs. Ag nanoparticles agglomerate and result in a bumpy surface topology and somewhat reduce the transparency of hybrid thin layer to 85.1% by 1.0% doping because of their shielding effect. Nevertheless, Ag nanoparticle agglomerates change the thickness of hybrid thin layers less, and the hybrid thin layers are ∼96 nm thick like a pure PI thin layer. LCs are vertically aligned on hybrid thin layers after rubbing. Benefit from the declined anchoring energy and the outstanding surface plasmon polariton (SPP) of Ag nanoparticles, the external electric field to switch LCs is substantial boosted, and hence remarkably diminish the operating voltage and likewise notably shorten the response time. In particular, LCs that vertically aligned between PI hybrid alignment layers by 0.5% doping could be electrically switched to become planner at 3.38 V and go back to their original vertical alignment state within 73.21 ms. Ag nanoparticles agglomerates in hybrid thin layers also fairly hinder the drift of LCs when cells are mechanically bent with various radii. The hybrid alignment layers cell that blended with 0.5% Ag nanoparticles could be bent under 1500 mm without any new evident light leakages and fluctuating electro-optical characteristics. These results indicate the promising applications of PI hybrid thin layers blended with Ag nanoparticles for flexible LC devices.

Ferroelectric liquid crystal array driven by a two‐layer electrode with a 1 × 1 μm pixel pitch for light modulation in electro‐holography

AbstractWe clarified that a ferroelectric liquid crystal (FLC) has high resolution display capability as small as 1 × 1 μm pixel pitch using an FLC pixel array with a two‐layer electrode, which has a 1 × 1‐μm‐checkered apertured electrode and a plane electrode separated by an insulation layer. By applying +2 V to the apertured electrode and −10 V to the plane electrode in the two‐layer electrode and 0 V to the transparent common electrode, a checkered pattern was clearly observed, which indicates the successful individual pixel driving with a pixel pitch of 1 × 1 μm. When fabricating 1 × 2‐μm‐pitch rectangular FLC pixels, we elucidated that the liquid crystal alignment direction should be along the shorter side of the pixels to avoid asymmetric transmittance distribution in each pixel. Moreover, we successfully reconstructed a 3D holographic image using 10 × 10 k FLC pixel array with a pitch of 1 × 1 μm driven by the two‐layer electrode with hologram‐patterned apertures. We showed that FLC is a strong candidate material for realizing spatial light modulator with extremely small pixel pitches, which is essential for holographic displays with wide‐viewing‐zone angles.

Effect of Azo Dye on Electro-Optic and Optical Band Gap Characteristics in ZnO Nanoparticles Induced Vertically Aligned Liquid Crystal Cells

Alignment of liquid crystal (LC) molecules in vertical direction is the most promising and interesting aspect for display devices in view of scientific and technological growth. Moreover, in accordance with the photovoltaic device applications, liquid crystals (LCs) show numerous applications. In the present work, the impact of dye as dopant with appropriate amount, over the electro-optic (E-O) and band gap properties as well as phase behaviour of vertically aligned liquid crystals (VALCs) has been studied and discussed. Initially, zinc oxide (ZnO) nanoparticles (NPs) were mixed to induce the vertical alignment (VA) in confined cell. Then, to prepare the dye doped LC sample, 0.125% of azo dye as dopant was uniformly mixed in the host sample. The results showed enhanced E-O characteristics with reduction in optical band gap as calculated using UV Visible study in 0.125% dye doped cell as compared to host sample cell.

How do carbon dots with amine terminals help perovskite solar cells perform better?

Lead halide perovskite solar cells can be significantly improved with multifunctional additives such as carbon dots (CDs) with amine terminals via defect passivation and band alignment. Here, we determine rational guidelines for the usage of such quantum dots in perovskite solar cells by systematically studying their effects on crystal quality and carrier transport. The amine-terminated CDs homogeneously dispersed in precursors improve the crystal quality of perovskite films, but they reduce the hole mobility hampering hole extraction. In contrast, CDs deposited between the electron transport layer and active layer could promote spin-coated film quality and electron’s extraction efficiently. So, the approaches of the carbon dots in device alters semiconductor properties and energy level structure. Interface engineering achieve better crystal quality and energy level alignment, which in turn affects charge collection, thereby increasing current density and power conversion efficiency. According to the findings of this study, when considering defect passivation by additives, the energy band alignment of the device should also be considered, since this could change carrier dynamics and device performance differently.

Parameters Affecting Interfacial Assembly and Alignment of Nanotubes.

Tangential flow interfacial self-assembly (TaFISA) is a promising scalable technique enabling uniformly aligned carbon nanotubes for high-performance semiconductor electronics. In this process, flow is utilized to induce global alignment in two-dimensional nematic carbon nanotube assemblies trapped at a liquid/liquid interface, and these assemblies are subsequently deposited on target substrates. Here, we present an observational study of experimental parameters that affect the interfacial assembly and subsequent aligned nanotube deposition. We specifically study the water contact angle (WCA) of the substrate, nanotube ink composition, and water subphase and examine their effects on liquid crystal defects, overall and local alignment, and nanotube bunching or crowding. By varying the substrate chemical functionalization, we determine that highly aligned, densely packed, individualized nanotubes deposit only at relatively small WCA between 35 and 65°. At WCA (< 10°), high nanotube bunching or crowding occurs, and the film is nonuniform, while aligned deposition ceases to occur at higher WCA (>65°). We find that the best alignment, with minimal liquid crystal defects, occurs when the polymer-wrapped nanotubes are dispersed in chloroform at a low (0.6:1) wrapper polymer to nanotube ratio. We also demonstrate that modifying the water subphase through the addition of glycerol not only improves overall alignment and reduces liquid crystal defects but also increases local nanotube bunching. These observations provide important guidance for the implementation of TaFISA and its use toward creating technologies based on aligned semiconducting carbon nanotubes.

Nanoantenna induced liquid crystal alignment for high performance tunable metasurface

Abstract Liquid crystal (LC) based spatial light modulators (SLMs) are a type of versatile device capable of arbitrarily reconfiguring the wavefront of light. For current commercial LC-SLM devices, the large pixel size limits their application to diffractive optics and 3D holographic displays. Pixel miniaturization of these devices is challenging due to emerging inter-pixel crosstalk, ultimately linked to the thick LC layer necessary for full phase (or amplitude) control. Integration of metasurfaces, i.e., 2D arrangements of resonant nanoantennas, with thin LC has emerged as a promising platform to boost light modulation, enabling realization of sub-wavelength pixel size SLMs with full phase (or amplitude) control. In most devices realized so far, however, the presence of an alignment layer, necessary to induce a preferential initial LC orientation, increases the voltage requirement for resonance tuning and reduces the efficiency of light modulation, something that accentuates for an ultra-thin (e.g., submicron) metasurface-LC cell. Here, we present an alternative strategy by which the LC molecular alignment is purely controlled by the periodicity and geometry of the nanoantenna without any additional alignment layer. The nanoantennas are specifically designed for the double purpose of sustaining optical resonances that are used for light modulation and to, simultaneously, induce the required LC pre-alignment. The proposed device structure allows lower voltage and reduced switching times (sub-millisecond) compared to devices including the alignment layer. This novel strategy thus helps to improve the performance of these miniaturized-pixel devices, which have emerged as one of the potential candidates for the next generation of products in a wide range of applications, from virtual/augmented reality (VR/AR) and solid-state light detection and ranging (LiDAR), to 3D holographic displays and beyond.

Alignment of Breathing Metal-Organic Framework Particles for Enhanced Water-Driven Actuation.

As the majority of known metal-organic frameworks (MOFs) possess anisotropic crystal lattices and thus anisotropic physicochemical properties, a pressing practical challenge in MOF research is the establishment of robust and simple processing methods to fully harness the anisotropic properties of the MOFs in various applications. We address this challenge by applying an E-field to precisely align MIL-88A microcrystals and generate MIL-88A@polymer films. Thereafter, we demonstrate the impact of MOF crystal alignment on the actuation properties of the films as a proof of concept. We investigate how different anisotropies of the MIL-88A@polymer films, specifically, crystal anisotropy, particle alignment, and film composition, can lead to the synergetic enhancement of the film actuation upon water exposure. Moreover, we explore how the directionality in application of the external stimuli (dry/humid air stream, water/air interface) affects the direction and the extent of the MIL-88A@polymer film movement. Apart from the superior water-driven actuation properties of the developed films, we demonstrate by dynamometer measurements the higher degree of mechanical work performed by the aligned MIL-88A@polymer films with the preserved anisotropies compared to the unaligned films. The insights provided by this work into anisotropic properties displayed by aligned MIL-88A@polymer films promise to translate crystal performance benefits measured in laboratories into real-world applications. We anticipate that our work is a starting point to utilize the full potential of anisotropic properties of MOFs.

Effect of the Correction of Bilateral Differences in Masseter Muscle Functional Pressure on the Mandible of Growing Rats.

The objective of this study is to clarify the effect of restoring the lowered masticatory muscle functional pressure and correcting bilateral differences in masticatory muscle functional pressure on jawbone growth during growth and development with a quantitative evaluation of the changes in the micro/nanostructural characteristics of entheses. Male Wistar rats aged 4 weeks were divided into an experimental group injected with a botulinum toxin serotype A (BoNT/A) formulation to reduce muscle function (BTX group) and a control group (CTRL group). They were euthanised after 6, 8, 10, 12, and 16 weeks after measuring the difference between the midline of the upper and lower incisors. The mandibles were harvested for histological examination, second harmonic generation imaging, and the quantitative evaluation of biological apatite (BAp) crystal alignment. The midline difference decreased with age in weeks. In rats from 6 weeks after BoNT/A administration to 12 weeks after administration, the collagen fibre bundle diameter was significantly smaller in the BTX group; the difference between the two groups decreased with increasing age. BAp crystal alignment was significantly different on the x-axis and the y-axis on the BTX group from 6 weeks after BoNT/A administration to 10 weeks after administration. Asymmetry of mandibular bone formation caused by load imbalance during growth could be corrected by the adjustment of the function of the masseter muscle on either side.