Programmable Jigsaw Puzzles of Soft Materials Enabled by Pixelated Holographic Surface Reliefs.

Manual intervention in the self-organization of soft matter to obtain a desired superstructure is a complex but significant project. Specifically, optical components made fully or partially from reconfigurable and stimuli-responsive soft materials, referred to as soft photonics, are poised to form versatile platforms in various areas; however, a limited scale, narrow spectral adaptability, and poor stability are still formidable challenges. Herein, a facile way is developed to program the optical jigsaw puzzle of nematic liquid crystals via pixelated holographic surface reliefs, leading to an era of manufacturing for programmable soft materials with tailored functions. Multiscale jigsaw puzzles are established and endowed with unprecedented stability and durability, further sketching a prospective framework toward customized adaptive photonic architectures. This work demonstrates a reliable and efficient approach for directly assembling soft matter, unlocking the long-sought full potential of stimuli-responsive soft systems, and providing opportunities to inspire the next generation of soft photonics and relevant areas.

Dynamically actuated soft heliconical architecture via frequency of electric fields.

Dynamic electric field frequency actuated helical and spiral structures enable a plethora of attributes for advanced photonics and engineering in the contemporary era. Nevertheless, leveraging the frequency responsiveness of adaptive devices and systems within a broad dynamic range and maintaining restrained high-frequency induced heating remain challenging. Herein, we establish a frequency-actuated heliconical soft architecture that is quite distinct from that of common frequency-responsive soft materials. We achieve reversible modulation of the photonic bandgap in a wide spectral range by delicately coupling the frequency-dependent thermal effect, field-induced dielectric torque and elastic equilibrium. Furthermore, an information encoder prototype without the aid of complicated algorithm design is established to analogize an information encoding and decoding process with a more convenient and less costly way. A technique for taming and tailoring the distribution of the pitch length is exploited and embodied in a prototype of a spatially controlled soft photonic cavity and laser emission. This work demonstrates a distinct frequency responsiveness in a heliconical soft system, which may not merely inspire the interest in field-assisted bottom-up molecular engineering of soft matter but also facilitate the practicality of adaptive photonics.

Stimulated transformation of soft helix among helicoidal, heliconical, and their inverse helices.

Dynamic modulation of soft helix in terms of the molecular organization, handedness, and pitch length could result in a sophisticated control over its functions, opening numerous possibilities toward the exploration of previously unidentified applications. Here, we report a dynamic and reversible transformation of a soft helical superstructure among the helicoidal (molecules orthogonal to helical axis), heliconical (molecules oblique to the helical axis, i.e., oblique helicoidal), and their inverse helices, together with a tunability on the helical pitch, by combining electrical and optical manipulations. This multistate transformation depends on a matching of the temperature, the strength of external stimuli, and the bend and twist elastic effects of the system. A laser emission with tunable wavelength and polarization, and prescribed micropatterns formed by any aforementioned architectures were achieved.

Light-Driven Reversible Transformation between Self-Organized Simple Cubic Lattice and Helical Superstructure Enabled by a Molecular Switch Functionalized Nanocage.

Self-organized stimuli-responsive smart materials with adjustable attributes are highly desirable for a plethora of device applications. Simple cubic lattice is quite uncommon in soft condensed matter due to its lower packing factor. Achieving a stable simple cubic soft lattice and endowing such a lattice with dynamic reconstruction capability solely by a facile light irradiation are of paramount significance for both fundamental studies and engineering explorations. Herein, an elegant stable self-organized simple cubic soft lattice, i.e., blue phase II, in a chiral liquid crystal (LC) system is disclosed, which is stable down to room temperature and exhibits both reversible lattice deformation and transformation to a helical superstructure, i.e., cholesteric LC, by light stimulation. Such an amazing trait is attained by doping a judiciously designed achiral photoresponsive molecular switch functionalized polyhedral oligomeric silsesquioxane nanocage into a chiral LC host. An unprecedented reversible collapse and reconstruction of such a high symmetric simple cubic blue phase II driven by light has been achieved. Furthermore, a well-defined conglomerate micropattern composed of simple cubic soft lattice and helical superstructure, which is challenging to fabricate in organic and inorganic crystalline materials, is produced using photomasking technology. Moreover, the promising photonic application based on such a micropattern is demonstrated.

Enhanced Low-temperature Electro-optical Kerr Effect of Stable Cubic Soft Superstructure Enabled by Fluorinated Polymer Stabilization.

An enhanced electro-optical Kerr effect of the stable self-organized cubic blue phase liquid crystal superstructure at a relatively low temperature down to -50 °C was achieved through a judiciously designed fluorinated polymer stabilization. The fluorinated sample exhibited not only a rather stable cubic structure, but the promoted electro-optical performances of low driving voltage, weak hysteresis and high contrast ratio at such a low-temperature, which were much distinct from the common non-fluorinated polymer stabilized blue phase liquid crystal without conspicuous low-temperature Kerr response behaviours. Kerr constant, which reflects the obviousness of Kerr effect, of the fluorinated sample at -50 °C indicated a spectacular enhancement of two orders of magnitude in contrast to the commonly material, thereby corroborating the high efficiency of polymer fluorination in enhancing low-temperature Kerr effect. Such an enhancement of Kerr effect was probably resulted from the decreasing of interfacial anchoring between liquid crystal and fluorinated polymer network. The fluorinated polymer stabilization not only ensures the stability of self-organized cubic structure of blue phase, but overcomes the challenge and bottleneck problem of low-temperature inapplicability of common blue phase liquid crystal and paves a brilliant and broad way for relevant materials to abundant perspective applications at low temperature.

Light-Patterned Crystallographic Direction of a Self-Organized 3D Soft Photonic Crystal.

Uniform and patterned orientation of a crystallographic direction of ordered materials is of fundamental significance and of great interest for electronic and photonic applications. However, such orientation control is generally complicated and challenging with regard to inorganic and organic crystalline materials due to the occurrence of uncontrollable dislocations or defects. Achieving uniform lattice orientation in frustrated liquid-crystalline phases, like cubic blue phases, is a formidable task. Taming and tailoring the ordering of such soft, cubic lattices along predetermined or desired directions, and even imparting a prescribed pattern on lattice orientation, are more challenging, due to the entropy-domination attribute of soft matter. Herein, we disclose a facile way to realize designed micropatterning of a crystallographic direction of a soft, cubic liquid-crystal superstructure, exhibiting an alternate uniform and random orientation of the lattice crystallographic direction enabled by a photoalignment technique. Because of the rewritable trait of the photoalignment film, the pattern can be erased and rewritten on-demand by light. Such an oriented soft lattice sensitively responds to various external stimuli such as temperature, electric field, and light irradiation. Furthermore, advanced reflective photonic applications are achieved based on the patterned crystallographic orientation of the cubic blue phase, soft lattice.