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At least 19 records
All sourcesNASA NTRSDOE OSTI
NASA NTRS2000

Structure, Hydrodynamics, and Phase Transition of Freely Suspended Liquid Crystals

Smectic liquid crystals are phases of rod shaped molecules organized into one dimensionally (1D) periodic arrays of layers, each layer being between one and two molecular lengths thick. In the least ordered smectic phases, the smectics A and C, each layer is a two dimensional (2D) liquid. Additionally there are a variety of more ordered smectic phases having hexatic short range translational order or 2D crystalline quasi long range translational order within the layers. The inherent fluid-layer structure and low vapor pressure of smectic liquid crystals enable the long term stabilization of freely suspended, single component, layered fluid films as thin as 30A, a single molecular layer. The layering forces the films to be an integral number of smectic layers thick, quantizing their thickness in layer units and forcing a film of a particular number of layers to be physically homogeneous with respect to its layer structure over its entire area. Optical reflectivity enables the precise determination of the number of layers. These ultrathin freely suspended liquid crystal films are structures of fundamental interest in condensed matter and fluid physics. They are the thinnest known stable condensed phase fluid structures and have the largest surface-to-volume ratio of any stable fluid preparation, making them ideal for the study of the effects of reduced dimensionality on phase behavior and on fluctuation and interface phenomena. Their low vapor pressure and quantized thickness enable the effective use of microgravity to extend the study of basic capillary phenomena to ultrathin fluid films. Freely suspended films have been a wellspring of new liquid crystal physics. They have been used to provide unique experimental conditions for the study of condensed phase transitions in two dimensions. They are the only system in which the hexatic has been unambiguously identified as a phase of matter, and the only physical system in which fluctuations of a 2D XY system and Kosterlitz Thouless phase transition has been observed and 2D XY quasi long range order verified. Smectic films have enabled the precise determination of smectic layer electron density and positional fluctuation profile and have been used to show that the interlayer interactions in anti-ferroelectric tilted smectics do not extend significantly beyond nearest neighbors. The interactions which are operative in liquid crystals are generally weak in comparison to those in crystalline phases, leading to the facile manipulation of the order in liquid crystals by external agents such as applied fields and surfaces. Effects arising from weak ordering are significantly enhanced in ultrathin free films and filaments wherein the intermolecular coupling is effectively reduced by loss of neighbors. Over the past four years this research, which we now detail, has produced a host of exciting new discoveries and unexpected results, maintaining the position of the study of freely suspended liquid crystal structures as one of most exciting and fruitful areas of complex fluid physics. In addition, several potentially interesting microgravity free film experiments have been identified.

Clark, Noel A.↗
NASA NTRS2004

Structure and Dynamics of Freely Suspended Liquid Crystals

Smectic liquid crystals are phases of rod shaped molecules organized into one dimensionally (1 D) periodic arrays of layers, each layer being between one and two molecular lengths thick. In the least ordered smectic phases, the smectics A and C, each layer is a two dimensional (2D) liquid. Additionally there are a variety of more ordered smectic phases having hexatic short range translational order or 2D crystalline or quasi long range translational order within the layers. The inherent fluid-layer structure and low vapor pressure of smectic liquid crystals enables the long term stabilization of freely suspended, single component, layered fluid films as thin as 30A, a single molecular layer. The layering forces the films to be an integral number of smectic layers thick, quantizing their thickness in layer units and forcing a film of a particular number of layers to be physically homogeneous with respect to its layer structure over its entire area. Optical reflectivity enables the precise determination of the number of layers. These ultrathin freely suspended liquid crystal films are structures of fundamental interest in condensed matter and fluid physics. They are the thinnest known stable fluid structures and have the largest surface-to-volume ratio of any stable fluid preparation, making them ideal for the study of the effects of reduced dimensionality on phase behavior and on fluctuation and interface phenomena. Their low vapor pressure and quantized thickness enable the effective use of microgravity to extend the study of basic capillary phenomena to ultrathin fluid films. Freely suspended films have been a wellspring of new LC physics. They have been used to provide unique experimental conditions for the study of condensed phase transitions in two dimensions. They are the only system in which the hexatic has been unambiguously identified as a phase of matter, and the only physical system in which fluctuations of a 2D XY system and Kosterlitz Thouless phase transition has been observed and 2D XY quasi long range order verified. Smectic films have enabled the precise determination of smectic layer electron density and positional fluctuation profiles and have been used to show that the interlayer interactions in antiferroelectric tilted smectics do not extend significantly beyond nearest neighbors. Freely suspended films played a pivotal role in the recent discovery of macroscopic chiral-polar ordering in fluids of achiral molecules. The interactions which are operative in liquid crystals are generally weak in comparison to those in crystalline phases, leading to the facile manipulation of the order in liquid crystals by external agents such as applied fields and surfaces. Effects arising from weak ordering are significantly enhanced in ultrathin free films and filaments, in which the intermolecular coupling is effectively further reduced by loss of neighbors. Over the past four years this research, which we now detail, has produced a host of exciting new discoveries and unexpected results, maintaining the study of freely suspended liquid crystal structures as one of most exciting and fruitful areas of complex fluid physics. In addition, a class of experiments on the behavior of 1D interfaces in 2D films have been pursued with results that point to potentially quite interesting effects in microgravity.

Clark, Noel A.↗
NASA NTRS2017

Interfacial and Hydrodynamic Behavior of Thin Spherical Bubbles of Smectic Liquid Crystal in Microgravity

The Observation and Analysis of Smectic Islands in Space (OASIS) project comprises a series of experiments that probe the interfacial and hydrodynamic behavior of thin spherical bubbles of smectic liquid crystal in microgravity. Smectic films are the thinnest known structures formed of condensed phases, making them ideal for studies of two-dimensional (2D) coarsening dynamics and thermocapillary phenomena. The OASIS flight hardware was launched on SpaceX-6 in April 2015 and experiments were carried out on the International Space Station using four different smectic A and C liquid crystal materials in separate sample chambers. We will describe the behavior of collective island dynamics on the bubbles, including temperature-gradient-induced thermomigration, 2D Rayleigh-Plateau Instability, Oswald ripening dynamics, the single and multiple island diffusion on the curved surface and coalescence-driven coarsening dynamics of island emulsions in microgravity. On Earth, such island emulsions would rapidly sediment to the bottom of the bubble and coalesce, but in microgravity, coarsening of the emulsion can be observed free of gravitational effects.

liquid crystal↗
DOE OSTI2021

Mono- and bilayer smectic liquid crystal ordering in dense solutions of “gapped” DNA duplexes

Significance Liquid crystalline behavior of DNA has been studied for decades, yet only recently has one of the most fundamental liquid crystal phases—the smectic phase in which rod-like objects assemble into stacks of fluid layers—been demonstrated in this system. Here, we describe distinct bilayer and monolayer smectic phases in solutions of “gapped” DNA (GDNA), consisting of two DNA duplexes connected by a single strand. The smectic order is amphotropic (sensitive to temperature as well as concentration), and the layer structure is stable against significant perturbations of the GDNA construct (e.g., “gap” length variation and asymmetry in duplex lengths). The temperature sensitivity may provide a means to compare end-to-end interaction strengths between DNA duplexes at biologically relevant concentrations.

36 MATERIALS SCIENCE↗
NASA NTRS2002

Studies of Islands on Freely Suspended Bubbles of Smectic Liquid Crystal

We have constructed an optical system for observing the internal structure of freely suspended smectic liquid crystal bubbles using a reflected light microscope. Liquid crystal bubbles can have thicker circular regions (islands) which can easily be generated by shrinking the bubble diameter. The diameter of these islands is approximately 10 microns and they are typically up to five times thicker than the surrounding liquid crystal film (500 angstroms). In the Laboratory, the location of the islands is strongly influenced by gravity, which causes the majority of islands to migrate to the bottom half of the bubble. We will describe the size and thickness distributions of islands and their time evolution, and also discuss two-dimensional hydrodynamics and turbulence of smectic bubbles, the shapes of islands and holes affected by bubble vibrations, and the interactions between islands, which we have probed using optical tweezers.

Pattanaporkratana, A.↗
DOE OSTI2026

Alignment switching in 3D-printed smectic liquid crystal elastomers

Extrusion-based additive manufacturing has emerged as a powerful platform for designing shape-morphing materials through controlled orientation. However, existing approaches primarily rely on a single mode of flow-induced alignment, limiting orientation programmability. Herein, we present a direct-ink-writing approach for smectic liquid crystal elastics that exploits two distinct alignment modes within a single ink. The smectic ink exhibits shear- and temperature-dependent orientation switching, enabling molecular alignment either perpendicular or parallel to the print direction. Combined rheological, X-ray, and molecular dynamics analyses reveal that this alignment inversion arises from the preservation or collapse of smectic layers under flow. This reversible switching encodes both contractile and elongational actuation within individual filaments, greatly expanding the design freedom of printed liquid crystal elastomers. We demonstrate 2D and 3D structures with diverse programmed shape transformations, highlighting the potential of this platform for adaptive soft actuators and architected functional materials.

Lee, Jin Hyeong [Pusan National University, Busan,↗
DOE OSTI2020

Cell alignment by smectic liquid crystal elastomer coatings with nanogrooves

Control of cells behavior through topography of substrates is a vital theme in biomedical applications. Among many materials used as substrates, polymers show advantages since they can be tailored by chemical functionalization. Fabrication of polymer substrates with nano- and microscale topography requires processing by lithography, microprinting, etching, etc. In this work, we present a different approach based on anisotropic elastic properties of polymerized smectic A (SmA) liquid crystal elastomer (LCE). When the SmA liquid crystal coating is deposited onto a substrate with planar alignment of the molecules, it develops nanogrooves at its free surface. After photopolymerization, these nanogrooves show an excellent ability to align human dermal fibroblasts (hDFs) over large areas. The alignment quality is good for both bare SmA LCE substrates and for substrates coated with fibronectin. The SmA LCE nano-topographies show a high potential for tissue engineering.

36 MATERIALS SCIENCE↗
NASA NTRS1972

Electron paramagnetic resonance study of two smectic A liquid crystals.

Study of the molecular ordering in two smectic A liquid crystals using vanadyl acetylacetonate as a paramagnetic probe. The average hyperfine splitting of the spectrum in the smectic A mesophase is measured as a function of the orientation relative to the dc magnetic field of the spectrometer after alignment of the molecules of the liquid crystal.

Fryburg, G. C.↗
NASA NTRS1972

Electron paramagnetic resonance study of alinement induced by magnetic fields in two smectic-A liquid crystals not exhibiting nematic phases

Using vanadyl acetylacetonate (VAAC) as a paramagnetic probe, the molecular ordering in two smectic-A liquid crystals that do not display nematic phases were studied. Reproducible alinement was attained by slow cooling throughout the isotropic smectic-A transition in dc magnetic fields of 1.1 and 2.15 teslas. The degree of order attained is small for a smectic-A liquid crystal. Measurements were made of the variation of the average hyperfine splitting of the alined samples as a function of orientation relative to the dc magnetic field of the spectrometer. This functional dependence is in agreement with the theoretical prediction except where the viscosity of the liquid crystal becomes large enough to slow the tumbling of the VAAC, as indicated by asymmetry in the end lines of the spectrum.

Fryburg, G. C.↗
DOE OSTI2023

Helfrich-Hurault elastic instabilities driven by geometrical frustration

Here, the Helfrich-Hurault (HH) elastic instability is a well-known mechanism behind patterns that form as a result of strain upon liquid crystal systems with periodic ground states. In the HH model, layered structures undulate and buckle in response to local, geometric incompatibilities in order to maintain the preferred layer spacing. Classic HH systems include cholesteric liquid crystals under electromagnetic field distortions and smectic liquid crystals under mechanical strains, where both materials are confined between rigid substrates. However, richer phenomena are observed when undulation instabilities occur in the presence of deformable interfaces and variable boundary conditions. Understanding how the HH instability is affected by deformable surfaces is imperative for applying the instability to a broader range of materials. In this review, the HH mechanism is reexamined and special focus is given to how the boundary conditions influence the response of lamellar systems to geometrical frustration. Lamellar liquid crystals confined within a spherical shell geometry are used as the model system. Made possible by the relatively recent advances in microfluidics within the past 15 years, liquid crystal shells are composed entirely of fluid interfaces and have boundary conditions that can be dynamically controlled at will. Past and recent work that exemplifies how topological constraints, molecular anchoring conditions, and boundary curvature can trigger the HH mechanism in liquid crystals with periodic ground states is examined. The review ends by identifying similar phenomena across a wide variety of materials, both biological and synthetic. The fact that the HH mechanism is a generic and often overlooked response of periodic materials to geometrical frustration is highlighted.

42 ENGINEERING↗
DOE OSTI2021

Synchrotron Microbeam Diffraction Studies on the Alignment within 3D-Printed Smectic-A Liquid Crystal Elastomer Filaments during Extrusion

3D printing of novel and smart materials has received considerable attention due to its applications within biological and medical fields, mostly as they can be used to print complex architectures and particular designs. However, the internal structure during 3D printing can be problematic to resolve. We present here how time-resolved synchrotron microbeam Small-Angle X-ray Diffraction (μ-SAXD) allows us to elucidate the local orientational structure of a liquid crystal elastomer-based printed scaffold. Most reported 3D-printed liquid crystal elastomers are mainly nematic; here, we present a Smectic-A 3D-printed liquid crystal elastomer that has previously been reported to promote cell proliferation and alignment. The data obtained on the 3D-printed filaments will provide insights into the internal structure of the liquid crystal elastomer for the future fabrication of liquid crystal elastomers as responsive and anisotropic 3D cell scaffolds.

36 MATERIALS SCIENCE↗
NASA NTRS1988

Static and dynamic properties of incommensurate smectic-A(IC) liquid crystals

The elasticity, topological defects, and hydrodynamics of the incommensurate smectic A(IC) phase liquid crystals are studied. The phase is characterized by two colinear mass density waves of incommensurate spatial frequency. The elastic free energy is formulated in terms of a displacement field and a phason field. It is found that the topological defects of the system are dislocations with a nonzero phason field and phason field components. A two-dimensional Burgers lattice for these dislocations is introduced. It is shown that the hydrodynamic modes of the phase include first- and second-sound modes whose direction-dependent velocities are identical to those in ordinary smectics.

Lubensky, T. C.↗
DOE OSTI2021

Solvent-Free Coating of Organic Semiconductor Membranes with Centimetric Crystalline Domains

Organic semiconductors (OSCs) have shown great promise in a variety of applications. Although solution processing of OSCs has resulted in high-quality films, exquisite control of structural development to minimize defect formation during large-scale fabrication remains formidable. Compounding this challenge is the use of halogenated organic solvents, which poses significant health and environmental hazards. However, the solvent-free techniques introduced thus far impose additional limitations on solidification kinetics; the resulting OSC thin films are often more defective than those processed from solution. Here, a solvent-free technique is reported to prepare OSC membranes with centimetric crystalline domains. Leveraging the tendency for liquid crystalline materials to preferentially orient, OSCs are “prealigned” by depositing them from the melt over a metal frame to form a freely suspended membrane. Additionally, crystallization from this prealigned phase affords membranes with unprecedented structural order across macroscopic distances. Field-effect transistors comprising membranes of dioctyl[1]-benzothieno[3,2-b][1]benzothiophene (C8BTBT) and didodecyl[1]-benzothieno[3,2-b][1]benzothiophene (C12BTBT) having centimeter-sized domains as active layers exhibit a hole mobility of ≈8.6 cm2 V -1 s -1 , superseding the mobility of any transistors whose active layers are deposited from melt. This technique is scalable to yield membranes with large crystalline domains over wafer dimensions, making it amenable for broad applications in large-area organic electronics.

36 MATERIALS SCIENCE↗