Engineering topics

White, Timothy J.

Publications and source records attributed to White, Timothy J..

6 records

DOE OSTI2024

Digital Light Process 3D Printing of Magnetically Aligned Liquid Crystalline Elastomer Free–forms

Liquid crystalline elastomers (LCEs) are anisotropic soft materials capable of large dimensional changes when subjected to a stimulus. The magnitude and directionality of the stimuli-induced thermomechanical response is associated with the alignment of the LCE. Recent reports detail the preparation of LCEs by additive manufacturing (AM) techniques, predominately using direct ink write printing. Another AM technique, digital light process (DLP) 3D printing, has generated significant interest as it affords LCE free-forms with high fidelity and resolution. However, one challenge of printing LCEs using vat polymerization methods such as DLP is enforcing alignment. Here, we document the preparation of aligned, main-chain LCEs via DLP 3D printing using a 100 mT magnetic field. Systematic examination isolates the contribution of magnetic field strength, alignment time, and build layer thickness on the degree of orientation in 3D printed LCEs. Informed by this fundamental understanding, DLP is used to print complex LCE free-forms with through-thickness variation in both spatial orientations. Further, the hierarchical variation in spatial orientation within LCE free-forms is used to produce objects that exhibit mechanical instabilities upon heating. DLP printing of aligned LCEs opens new opportunities to fabricate stimuli-responsive materials in form factors optimized for functional use in soft robotics and energy absorption.

36 MATERIALS SCIENCE↗

DOE OSTI2024

Stiffness anisotropy coordinates supracellular contractility driving long-range myotube-ECM alignment

The ability of cells to organize into tissues with proper structure and function requires the effective coordination of proliferation, migration, polarization, and differentiation across length scales. Skeletal muscle is innately anisotropic; however, few biomaterials can emulate mechanical anisotropy to determine its influence on tissue patterning without introducing confounding topography. Here, we demonstrate that substrate stiffness anisotropy coordinates contractility-driven collective cellular dynamics resulting in C2C12 myotube alignment over millimeter-scale distances. When cultured on mechanically anisotropic liquid crystalline polymer networks (LCNs) lacking topography, C2C12 myoblasts collectively polarize in the stiffest direction. Cellular coordination is amplified through reciprocal cell-ECM dynamics that emerge during fusion, driving global myotube-ECM ordering. Conversely, myotube alignment was restricted to small local domains with no directional preference on mechanically isotropic LCNs of the same chemical formulation. These findings provide valuable insights for designing biomaterials that mimic anisotropic microenvironments and underscore the importance of stiffness anisotropy in orchestrating tissue morphogenesis.

59 BASIC BIOLOGICAL SCIENCES↗

DOE OSTI2024

The association of structural chirality and liquid crystal anchoring in polymer stabilized cholesteric liquid crystals

Polymer stabilized cholesteric liquid crystals (PSCLCs) are electrically reconfigurable reflective elements. Prior studies have hypothesized and indirectly confirmed that the electro-optic response of these composites is associated with the electrically mediated distortion of the stabilizing polymer network. The proposed mechanism is based on the retention of structural chirality in the polymer stabilizing network, which upon deformation is spatially distorted, which accordingly affects the pitch of the surrounding low molar-mass liquid crystal host. Here, we utilize fluorescent confocal polarized microscopy to directly assess the electro-optic response of PSCLCs. By utilizing dual fluorescent probes, sequential imaging experiments confirm that the periodicity of the polymer stabilizing network matches that of the low molar-mass liquid crystal host. Further, we isolate distinct ion-polymer interactions that manifest in certain photopolymerization conditions.

Radka, Brian P.↗

DOE OSTI2023

Millimeter-Thick Liquid Crystalline Elastomer Actuators Prepared by-Surface-Enforced Alignment

Here, liquid crystalline elastomers (LCE) are thermally cyclable, compliant actuators with compelling mechanical properties. The large and programmable deformation of LCE has led to numerous functional examinations spanning optics, medical devices, and robotics. A well-established method to prepare complex LCE actuators is to utilize surface-enforced photoalignment. Herein, a facile and scalable approach is reported to circumvent the physical limits of surface-enforced alignment (e.g., samples that are 50 µm or less) to amplify the achievable force output in LCE. Applying an approach termed direct layering, the thermomechanical response of LCE elements prepared with +1 disclination patterns in a range of compositions and thicknesses is contrasted. The design and preparation of +1 disclination patterns and arrays is explored to assess the contribution of sample geometry and overlap to deformation and force output. The methodology detailed in this contribution allows for the preparation of elements ≈1 mm in thickness that are capable of actuating large objects. Furthermore, the fabrication of these elements uniquely enables the realization of mechanical instabilities to hasten the actuation rate in response to thermal change and to enable leaping.

36 MATERIALS SCIENCE↗

DOE OSTI2022

Variable Temperature Behaviour of the Hybrid Double Perovskite MA 2 KBiCl 6

Perovskite-related materials show very promising properties in many fields. Pb-free perovskites are particularly interesting, because of the toxicity of Pb. In this study, hybrid double perovskite MA 2 KBiCl 6 (MA = methylammonium cation) was found to have interesting variable temperature behaviours. Both variable temperature single crystal X-ray diffraction, synchrotron powder diffraction, and Raman spectroscopy were conducted to reveal a rhombohedral to cubic phase transition at around 330 K and an order to disorder transition for inorganic cage below 210 K.

36 MATERIALS SCIENCE↗

DOE OSTI2022

Surface‐Enforced Alignment of Reprogrammable Liquid Crystalline Elastomers

Abstract Liquid crystalline elastomers (LCEs) are stimuli‐responsive materials capable of undergoing large deformations. The thermomechanical response of LCEs is attributable to the coupling of polymer network properties and disruption of order between liquid crystalline mesogens. Complex deformations have been realized in LCEs by either programming the nematic director via surface‐enforced alignment or localized mechanical deformation in materials incorporating dynamic covalent chemistries. Here, the preparation of LCEs via thiol‐Michael addition reaction is reported that are amenable to surface‐enforced alignment. Afforded by the thiol‐Michael addition reaction, dynamic covalent bonds are uniquely incorporated in chemistries subject to surface‐enforce alignment. Accordingly, LCEs prepared with complex director profiles are able to be programmed and reprogrammed by (re)activating the dynamic covalent chemistry to realize distinctive shape transformations.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗