Multimode interactive displays utilizing more than two stimulus-responsive light manipulation schemes have attracted considerable attention. However, sensing displays with asynchronous light control—where two responsive optical phenomena are complementary, thereby minimizing interference between two optical modes—have seldom been demonstrated. Here we report a novel self-assembled material exhibiting asynchronous fluorescence (FL) and structural color (SC), which enables multilevel optical sensing and encryption. Asynchronous FL and SC was achieved by chemically doping aggregation-induced emission luminogens (AIEgens) into one-dimensional block copolymer (BCP) photonic crystals (PCs) comprising alternating lamellae of two dielectric components. The AIEgen-derived FL of a nonswollen BCP PC with no visible SC was deactivated when it was swollen in a solvent, consequently exhibiting fully visible SC. The complementary FL and SC manipulation through reversible molecular (aggregation vs. separation) and structural (nonswollen vs. swollen) alteration aided in developing a multimode sensing display, which could detect temperature and/or nitroaromatic gas in FL mode as well as the pH of a solution in SC mode. The AIEgen-doped BCP PC exhibiting asynchronous FL and SC assisted in constructing a novel write-once-read-many optical encryption system with multilevel security where three levels of quaternary code-type passwords were encrypted with SC, FL, and pH-matched SC.

We investigated the thermal expansion of amorphous polystyrene (PS) and poly(methyl methacrylate) (PMMA) homopolymers using the temperature dependence of spatial electron-density correlations. The strong and broad X-ray interference maxima arising from inter- and intramolecular correlation distances were distinct, maintaining their shape during the heating of the samples to 250 degrees C. Three maxima characteristic of electron density correlations between the backbones, substituents along the chain, and repeat-units were observed. A remarkable temperature dependence was identified in the largest correlation distances arising from the intermolecular interactions. Based on the temperature dependence of the correlation distances, the coefficients of molecular expansion were very close to the coefficients of thermal expansion. This study provides a simple yet accurate way to correlate macroscopic volume expansions with the molecular expansion obtained from wide-angle X-ray scattering (WAXS) data.

Despite significant progress in developing artificial synapses to emulate the human nervous system for bio-signal transmission, synapses with thermo-adaptive coloration and soft actuators driven by temperature change have seldom been reported. Herein, a photonic neuro-actuating synaptic skin is presented enabling thermoresponsive synaptic signal transmission, color variation, and actuation. First, a thermoresponsive display synapse is developed based on a 3-terminal ion-gel transistor with a poly (3,4-ethylene dioxythiophene):poly (styrene sulfonate) (PEDOT:PSS) semiconducting channel mixed with 2D titanium carbide (Ti3C2Tx) MXene and a thermo-adaptive 1D block copolymer (BCP) photonic crystal (PC) gate insulator. Temperature-dependent synaptic behavior is successfully observed in the ion-gel transistor with the corresponding structural colors, leading to a thermo-adaptive display synapse. The 3 × 3 arrays of thermo-adaptive display synapses with Joule heaters show that each pixel is controlled by the thermoresponsive structural color and synaptic output. The synaptic output current from the MXene ion-gel transistor can be converted and amplified to a voltage signal, which powers a soft actuator connected to the ion-gel display synapse and triggers temperature-dependent actuation related to the thermoresponsive synaptic performance. This study showcases a thermo-adaptive photonic neuro-actuating artificial skin that emulates muscle-combined neuronal human skin with visualization capability.

AbstractA block copolymer (BCP) with specific monomer structures of fluoroacrylate polymers was designed by exploiting the inorganic superhydrophobicity and low glass transition temperature of polydimethylsiloxane (PDMS). With the use of a fluorine-containing block providing a surface tension as low as that of PDMS (19.9 < $$\gamma$$ γ < 21.5 mN/m), PDMS-b-poly(2,2,3,3,3-pentafluoropropyl acrylate) (PDMS-b-PPeFPA) copolymer was synthesized to create a volume-symmetric lamellar structure. The compositional randomness of the BCP chains adsorbed onto the substrates provided well-balanced interfacial interactions toward the overlaid PDMS-b-PPeFPA ($$\gamma$$ γ PDMS-ads ≈ $$\gamma$$ γ PPeFPA-ads). Under this symmetric confinement with simultaneous dual neutral interfaces, lamellar microdomains with a sub-10 nm half-pitch feature size were successfully oriented perpendicular to the interfaces at room temperature. We showed the response of the BCP films to a lateral electric field, demonstrating that the perpendicular lamellae were adaptively aligned along the electric vector within a short treatment period. Furthermore, the PDMS-b-PPeFPA system exhibited a remarkable etch contrast for O2 reactive ion etching, yielding unidirectionally aligned air–inorganic nanoarrays emanating from the perpendicular lamellae between the electrodes. This study reports a system engineering approach for conceiving highly immiscible, silicon- and fluorine-containing BCP whose components exhibit identical surface tensions ($$\gamma$$ γ PDMS ≈ $$\gamma$$ γ PPeFPA) and for generating perpendicularly oriented lamellar microdomains due to substrate neutrality.

Unique sphere-packing mesophases such as Frank-Kasper (FK) phases have emerged from the viable design of intermolecular interactions in supramolecular assemblies. Herein, a series of Cn-G2-CONH2 dendrons possessing an identical core wedge are investigated to elucidate the impact of peripheral alkyl chain lengths (Cn) on the formation of the close-packed structures. The C18 and C14 dendrons, of which the contour lengths of the periphery Lp are longer than the wedge length Lw, assemble into a uniform sphere-packing phase such as body-centred cubic (BCC), whereas the C8 dendron with short (Lp < Lw) corona environment forms the FK A15 phase. Particularly in the intermediate C12 and C10 dendrons (Lp ≈ Lw), cooling the samples from an isotropic state leads to cooling-rate-dependent phase behaviours. The C12 dendron produces two structures of hexagonal columnar and sphere-packing phases (BCC and A15), while the C10 dendron generates the A15 and σ phases by the fast- and slow-cooling processes, respectively. Our results show the impact of peripheral alkyl chain lengths on the formation of mesocrystal phases, where the energy landscape of the dendrons at Lp/Lw ≈ 1 must be more complex and delicate than those with either longer or shorter peripheral alkyl chains.