Dynamic heat and charge transports through double-quantum-dot-interferometer modulated by Majorana bound states and time-oscillating Aharonov-Bohm flux.

Dynamic properties of Majorana bound states (MBSs) coupled double-quantum-dot (DQD) interferometer threaded with ac magnetic flux are investigated, and the time-averaged thermal current formulas are derived. Photon-assisted local and nonlocal Andreev reflections contribute efficiently to the charge and heat transports. The modifications of source-drain electric, electric-thermal, thermal conductances (G,ξ,κe), Seebeck coefficient (Sc), and thermoelectric figure of merit (ZT) versus AB phase have been calculated numerically. These coefficients exhibit the shift of oscillation period from 2πto 4πdistinctly due to attaching MBSs. The applied ac flux enhances the magnitudes ofG,ξ,κeobviously, and the detailed enhancing behaviors are relevant to the energy levels of DQD. The enhancements ofScandZTare generated due to the coupling of MBSs, while the application of ac flux suppresses the resonant oscillations. The investigation provides a clue for detecting MBSs through measuring the photon-assistedScandZTversus AB phase oscillations.

Double Networks of Liquid-Crystalline Elastomers with Enhanced Mechanical Strength.

Liquid-crystalline elastomers (LCEs) are frequently used in soft actuator development. However, applications are limited because LCEs are prone to mechanical failure when subjected to heavy loads and high temperatures during the working cycle. A mechanically tough LCE system offers larger work capacity and lower failure rate for the actuators. Herein, we adopt the double-network strategy, starting with a siloxane-based exchangeable LCE and developing a series of double-network liquid-crystalline elastomers (DN-LCEs) that are mechanically tougher than the initial elastomer. We incorporate diacrylate reacting monomers to fabricate DN-LCEs, some of which have the breaking stress of 40 MPa. We incorporate thermoplastic polyurethane to fabricate a DN-LCE, achieving an enormous ductility of 90 MJ/m3. We have also attempted to utilize the aza-Michael chemistry to make a DN-LCE that retains high plasticity because of several bond-exchange mechanisms; however, it failed to produce a stable reprocessable LCE system using conventional ester-based reactive mesogens. Each of these DN-LCEs exhibits unique features and characteristics, which are compared and discussed.

Amine-Acrylate Liquid Single Crystal Elastomers Reinforced by Hydrogen Bonding.

Liquid crystalline elastomers (LCEs) have been considered one of the most promising material concepts for artificial muscles. However, accomplishing actuation of LCEs requires macroscopic alignment of the liquid-crystalline orientation in the rubbery network, which imposes challenges in the materials chemistry and processing. A two-stage curing strategy has been the dominating approach during last three decades. Despite its many successes, the method is difficult in practice and requires delicate experiential skills, dealing with intrinsic fragility of intermediate gels after the first crosslinking stage. Here, a robust fabrication method for monodomain LCE based on the amine-acrylate aza-Michael addition is developed, involving two readily commercially available components with no catalyst. The method is based on the large kinetic difference of hydrogen addition in primary amines to acrylates, which offers a sufficient gap separating two stages of curing and enabling versatile mechanical alignment techniques for manufacturing monodomain LCE in both liquid and gel states. Importantly, the mechanically robust network, helping processability at a partial-crosslinking stage, is facilitated by the chemically generated hydrogen bonding all through the process, as a by-product of hydrogen addition. Such a facile two-component kit-like fabrication should aid researchers from various fields in the search for a practical and reliable process of making soft actuators.

On demand shape memory polymer via light regulated topological defects in a dynamic covalent network.

The ability to undergo bond exchange in a dynamic covalent polymer network has brought many benefits not offered by classical thermoplastic and thermoset polymers. Despite the bond exchangeability, the overall network topologies for existing dynamic networks typically cannot be altered, limiting their potential expansion into unexplored territories. By harnessing topological defects inherent in any real polymer network, we show herein a general design that allows a dynamic network to undergo rearrangement to distinctive topologies. The use of a light triggered catalyst further allows spatio-temporal regulation of the network topology, leading to an unusual opportunity to program polymer properties. Applying this strategy to functional shape memory networks yields custom designable multi-shape and reversible shape memory characteristics. This molecular principle expands the design versatility for network polymers, with broad implications in many other areas including soft robotics, flexible electronics, and medical devices.

Light-triggered topological programmability in a dynamic covalent polymer network.

Dynamic covalent polymer networks exhibit unusual adaptability while maintaining the robustness of conventional covalent networks. Typically, their network topology is statistically nonchangeable, and their material properties are therefore nonprogrammable. By introducing topological heterogeneity, we demonstrate a concept of topology isomerizable network (TIN) that can be programmed into many topological states. Using a photo-latent catalyst that controls the isomerization reaction, spatiotemporal manipulation of the topology is realized. The overall result is that the network polymer can be programmed into numerous polymers with distinctive and spatially definable (thermo-) mechanical properties. Among many opportunities for practical applications, the unique attributes of TIN can be explored for use as shape-shifting structures, adaptive robotic arms, and fracture-resistant stretchable devices, showing a high degree of design versatility. The TIN concept enriches the design of polymers, with potential expansion into other materials with variations in dynamic covalent chemistries, isomerizable topologies, and programmable macroscopic properties.

Dynamic Covalent Polymer Networks: from Old Chemistry to Modern Day Innovations.

Dynamic covalent polymer networks have long been recognized. With the initial focus on the unintended impact of dynamic covalent linkages on the viscoelasticity of commercial rubbers, efforts in modern times have transitioned into designing dynamic covalent polymer networks with unique adaptive properties. Whereas self-healing and thermoset reprocessing have been the primary motivations for studying dynamic covalent polymer networks, the recent discovery of the vitrimeric rheological behavior and solid-state plasticity for this type of material have opened up new opportunities in material innovations. This, coupled with the revelation of the dynamic characteristics of commercially relevant polymer building blocks such as esters and urethanes, suggests a promising future for this class of materials.

Catalyst-Free Thermoset Polyurethane with Permanent Shape Reconfigurability and Highly Tunable Triple-Shape Memory Performance.

Thermoset shape memory polymer (SMP) with dynamic covalent bonds in the network is a new class of SMPs for which the permanent shape can be reconfigured via topological rearrangement (plasticity). Catalyzed transcarbamoylation has recently been established as an effective exchange reaction for plasticity in cross-linked polyurethane networks. However, ensuring the plasticity severely constrains the network design which adversely affects the ability to tune other classical shape memory properties for practical applications. Facing this new challenge, we design an amorphous polyurethane system for which the cross-linking density can be adjusted in a wide range. We discovered that the use of an aromatic diisocyanate in the synthesis of the polyurethanes facilitates achieving plasticity without requiring any catalyst. The overall network design leads to tunable recovery stress and shape memory transition temperatures without sacrificing the plasticity. The versatility of our polyurethane SMP is further reflected in its triple-shape memory performance. We anticipate that our tunable polyurethanes will benefit a variety of potential SMP device applications.

Thermoset Shape-Memory Polyurethane with Intrinsic Plasticity Enabled by Transcarbamoylation.

Thermoset polymers are known for their superior thermomechanical properties, but the chemical crosslinking typically leads to intractability. This is reflected in the great differences between thermoset and thermoplastic shape-memory polymers; the former exhibit a robust shape memory but are not capable of redefining the permanent shape. Contrary to current knowledge, we reveal here that a classical thermoset shape-memory polyurethane is readily capable of permanent reshaping (plasticity) after a topological network rearrangement that is induced by transcarbamoylation. By employing the Jianzhi technique (also known as kirigami), unexpected shape-shifting versatility was observed for this otherwise classical material. As the essential carbamate moiety in polyurethanes is one of the most common polymer building units, we anticipate that our finding will have significant benefits beyond shape shifting.

Shape memory polymer network with thermally distinct elasticity and plasticity.

Stimuli-responsive materials with sophisticated yet controllable shape-changing behaviors are highly desirable for real-world device applications. Among various shape-changing materials, the elastic nature of shape memory polymers allows fixation of temporary shapes that can recover on demand, whereas polymers with exchangeable bonds can undergo permanent shape change via plasticity. We integrate the elasticity and plasticity into a single polymer network. Rational molecular design allows these two opposite behaviors to be realized at different temperature ranges without any overlap. By exploring the cumulative nature of the plasticity, we demonstrate easy manipulation of highly complex shapes that is otherwise extremely challenging. The dynamic shape-changing behavior paves a new way for fabricating geometrically complex multifunctional devices.

Exploring Dynamic Equilibrium of Diels-Alder Reaction for Solid State Plasticity in Remoldable Shape Memory Polymer Network.

The reversible and click nature of Diels-Alder (DA) reactions has made them ideal candidates to design materials with nonconventional properties. Most commonly, the reversibility of DA is utilized for designing thermosets that can be liquefied for reprocessing and self-healing, yet the dynamic equilibrium nature has been largely neglected. In this work, shape memory polymers (SMP) containing DA moieties in the networks were synthesized. In addition to its remoldability at the liquid state at sufficiently high temperatures (above 110 °C), we show uniquely and surprisingly that such a network can undergo plastic deformation in its solid state at intermediate temperatures (60-100 °C) by taking advantage of its dynamic equilibrium for network topological rearrangement. The liquid state remoldability and solid state plasticity represent two distinct yet complementary mechanisms to manipulate the permanent shape of an SMP, leading to unprecedented versatility that can benefit a variety of applications in the future.