Dynamic multifunctional devices enabled by ultrathin metal nanocoatings with optical/photothermal and morphological versatility.

Inspired by the intriguing adaptivity of natural life, such as squids and flowers, we propose a series of dynamic and responsive multifunctional devices based on multiscale structural design, which contain metal nanocoating layers overlaid with other micro-/nanoscale soft or rigid layers. Since the optical/photothermal properties of a metal nanocoating are thickness dependent, metal nanocoatings with different thicknesses were chosen to integrate with other structural design elements to achieve dynamic multistimuli responses. The resultant devices demonstrate 1) strain-regulated cracked and/or wrinkled topography with tunable light-scattering properties, 2) moisture/photothermal-responsive structural color coupled with wrinkled surface, and 3) mechanically controllable light-shielding properties attributed to the strain-dependent crack width of the nanocoating. These devices can adapt external stimuli, such as mechanical strain, moisture, light, and/or heat, into corresponding changes of optical signals, such as transparency, reflectance, and/or coloration. Therefore, these devices can be applied as multistimuli-responsive encryption devices, smart windows, moisture/photothermal-responsive dynamic optics, and smartphone app-assisted pressure-mapping sensors. All the devices exhibit high reversibility and rapid responsiveness. Thus, this hybrid system containing ultrathin metal nanocoatings holds a unique design flexibility and adaptivity and is promising for developing next-generation multifunctional devices with widespread application.

Dynamic Room Temperature Phosphorescence of Silane-Functionalized Carbon Dots Confining within Silica for Anti-Counterfeiting Applications.

Room temperature phosphorescent (RTP) materials with long-lived, excitation-dependent, and time-dependent phosphorescence are highly desirable but very hard to achieve. Herein, this work reports a rational strategy of multiple wavelength excitation and time-dependent dynamic RTP color by confining silane-functionalized carbon dots (CDs) in a silica matrix (Si-CDs@SiO2). The Si-CDs@SiO2 possesses unique green-light-excitation and a change in phosphorescence color from yellow to green. A slow-decaying phosphorescence at 500 nm with a lifetime of 1.28 s and a fast-decaying phosphorescence at 580 nm with a lifetime of 0.90 s are observed under 365 nm of irradiation, which originated from multiple surface triplet states of the Si-CDs@SiO2. Given the unique dynamic RTP properties, the Si-CDs@SiO2 are demonstrated for applications in fingerprint recognition and multidimensional dynamic information encryption. These findings will open an avenue to explore dynamic phosphorescent materials and significantly broaden their applications.

Tailoring the Growth of Nanosized α-Zirconium Phosphate.

Nanosized α-zirconium phosphate (α-ZrP), unlike microcrystalline α-ZrP, takes less time to prepare and is synthesized directly in organic solvents. During the synthesis of nanosized α-ZrP, the heating step is critical because during which the particle growth/aggregation is ongoing. In order to explore more details of this step, extra water molecules were intentionally introduced to the ethanol gel of nanosized α-ZrP so that the evaporation of the solvent was slowed. To heat the gels at 65 °C for different periods (1-6 days), one could control with ease the synthesized α-ZrP in size, from 63 to 155 nm, and in morphology, from amorphous to highly crystalline. Furthermore, the heating step also affects the intercalated solvent and the dangling propionate groups on the edge of the nanosized α-ZrP, which could be deduced from the intercalation/exfoliation behavior of the nanocrystals. This modified synthesis method of nanosized α-ZrP offers an alternate means to tune the size and morphology of the nanosized α-ZrP for broad applications.

Intensely phosphorescent block copolymer micelles containing gold(i) complexes.

The electrostatic combination of anionic block copolymers with cationic gold(i) complexes leads to the formation of spherical micelles, where gold(i)-containing ionic cores were formed with anionic blocks and further stabilized by neutral blocks of polystyrene or poly(ethylene oxide). This self-assembled strategy induces remarkable phosphorescence enhancement of the gold(i) complexes in solution. The emissive intensity increases unexpectedly with increasing molecular weight of the anionic block that is not coordinated onto the gold(i) complexes. The intensely phosphorescent micelles formed in water can be utilized as a luminescence bioimaging probe in living cells.

Interactive deformable electroluminescent devices enabled by an adaptable hydrogel system with optical/photothermal/mechanical tunability.

Deformable electroluminescent devices (DELDs) with mechanical adaptability are promising for new applications in smart soft electronics. However, current DELDs still present some limitations, including having stimuli-insensitive electroluminescence (EL), untunable mechanical properties, and a lack of versatile stimuli response properties. Herein, a facile approach for fabricating in situ interactive and multi-stimuli responsive DELDs with optical/photothermal/mechanical tunability was proposed. A polyvinyl alcohol (PVA)/polydopamine (PDA)/graphene oxide (GO) adaptable hydrogel exhibiting optical/photothermal/mechanical tunability was used as the top ionic conductor (TIC). The TIC can transform from a viscoelastic state to an elastic state via a special freezing-salting out-rehydration (FSR) process. Meanwhile, it endows the DELDs with a photothermal response and thickness-dependent light shielding properties, allowing them to dynamically demonstrate "on" or "off" or "gradually change" EL response to various mechanical/photothermal stimuli. Thereafter, the DELDs with a viscoelastic TIC can be utilized as pressure-responsive EL devices and laser-engravable EL devices. The DELDs with an elastic TIC can withstand both linear and out-of-plane deformation, enabling the designs of various interactive EL devices/sensors to monitor linear sliders, human finger bending, and pneumatically controllable bulging. This work offers new opportunities for developing next-generation EL-responsive devices with widespread application based on adaptable hydrogel systems.

Scalable self-assembly interfacial engineering for high-temperature dielectric energy storage.

Flexible polymer dielectrics which can function well at elevated temperatures continue to be significant in harsh condition energy storage. However, state-of-the-art high-temperature polymers traditionally designed with conjugated structures for better thermal stability have compromised bandgaps and charge injection barriers. Here, we demonstrate a self-assembled polyvinyl alcohol (PVA)/montmorillonite (MMT) coating to impede charge carriers injecting into the polyimide (PI) polymer film. The anisotropic conductivity of the 2D nanolayered coating further dissipates the energy of charges through tortuous injection pathways. With the coating, high field pre-breakdown conduction measurement and space-charge profiling of PI films reveal a clear shifting of the dominant mode of conduction from the bulk-limited hopping to Schottky-injection limited conduction. The coating thus imparts PI films with a significantly suppressed electrical conduction (∼10×), and substantially improved discharge efficiency (7×) and energy density (2.7×) at 150°C. The facile and scalable flow-induced fabrication unleash enormous applications for harsh condition electrification.

Reviving the "Schottky" Barrier for Flexible Polymer Dielectrics with a Superior 2D Nanoassembly Coating.

The organic insulator-metal interface is the most important junction in flexible electronics. The strong band offset of organic insulators over the Fermi level of electrodes should theoretically impart a sufficient impediment for charge injection known as the Schottky barrier. However, defect formation through Anderson localization due to topological disorder in polymers leads to reduced barriers and hence cumbersome devices. A facile nanocoating comprising hundreds of highly oriented organic/inorganic alternating nanolayers is self-coassembled on the surface of polymer films to revive the Schottky barrier. Carrier injection over the enhanced barrier is further shunted by anisotropic 2D conduction. This new interface engineering strategy allows a significant elevation of the operating field for organic insulators by 45% and a 7× improvement in discharge efficiency for Kapton at 150 °C. This superior 2D nanocoating thus provides a defect-tolerant approach for effective reviving of the Schottky barrier, one century after its discovery, broadly applicable for flexible electronics.