Rewritable Photoluminescence and Structural Color Display for Dual-Responsive Optical Encryption.

Optical encryption using coloration and photoluminescent (PL) materials can provide highly secure data protection with direct and intuitive identification of encrypted information. Encryption capable of independently controlling wavelength-tunable coloration as well as variable light intensity PL is not adequately demonstrated yet. Herein, a rewritable PL and structural color (SC) display suitable for dual-responsive optical encryption developed with a stimuli-responsive SC of a block copolymer (BCP) photonic crystal (PC) with alternating in-plane lamellae, of which a variety of 3D and 2D perovskite nanocrystals is preferentially self-assembled with characteristic PL, is presented. The SC of a BCP PC is controlled in the visible range with different perovskite precursor doping times. The perovskite nanocrystals developed in the BCP PC are highly luminescent, with a PL quantum yield of ≈33.7%, yielding environmentally stable SC and PL dual-mode displays. The independently programmed SC and PL information is erasable and rewritable. Dual-responsive optical encryption is demonstrated, in which true Morse code information is deciphered only when the information encoded by SCs is properly combined with PL information. Numerous combinations of SC and PL realize high security level of data anticounterfeiting. This dual-mode encryption display offers novel optical encryption with high information security and anti-counterfeiting.

Dual-light emitting 3D encryption with printable fluorescent-phosphorescent metal-organic frameworks.

Optical encryption technologies based on room-temperature light-emitting materials are of considerable interest. Herein, we present three-dimensional (3D) printable dual-light-emitting materials for high-performance optical pattern encryption. These are based on fluorescent perovskite nanocrystals (NCs) embedded in metal-organic frameworks (MOFs) designed for phosphorescent host-guest interactions. Notably, perovskite-containing MOFs emit a highly efficient blue phosphorescence, and perovskite NCs embedded in the MOFs emit characteristic green or red fluorescence under ultraviolet (UV) irradiation. Such dual-light-emitting MOFs with independent fluorescence and phosphorescence emissions are employed in pochoir pattern encryption, wherein actual information with transient phosphorescence is efficiently concealed behind fake information with fluorescence under UV exposure. Moreover, a 3D cubic skeleton is developed with the dual-light-emitting MOF powder dispersed in 3D-printable polymer filaments for 3D dual-pattern encryption. This article outlines a universal principle for developing MOF-based room-temperature multi-light-emitting materials and a strategy for multidimensional information encryption with enhanced capacity and security.

Room-Temperature, Homogeneous, Single-Step, and Large-Scale Synthesis of Perovskite Nanoplatelets for Blue Light-Emitting Diodes.

Inorganic perovskite nanocrystals (IPNCs) have attracted considerable attention due to their excellent optoelectronic properties. However, problems arise from anion migration during the preparation of a blue light-emitting diode (LED), and only small-scale syntheses have been conducted on a laboratory scale. By using only Br as the anion here, CsPbBr3 was synthesized in the form of nanoplatelets to eliminate the effects of anion migration and to prepare an inorganic perovskite nanoplatelet (IPNPL) emitting blue light. In addition, the synthesis was performed under ambient conditions at room temperature, and the synthetic process was shortened to enable large-scale synthesis. We used a 1 L bottle for large-scale synthesis, and a photoluminescence quantum yield (PLQY) of 78% was observed at 460 nm. We fabricated LEDs by using IPNPLs, and we observed an electroluminescence peak at 461 nm. The developed synthetic method is expected to pave the way for commercialization of IPNCs and the next-generation display market.

Sub-30 nm 2D Perovskites Patterns via Block Copolymer Guided Self-Assembly for Color Conversion Optical Polarizer.

Despite the remarkable advances made in the development of 2D perovskites suitable for various high-performance devices, the development of sub-30 nm nanopatterns of 2D perovskites with anisotropic photoelectronic properties remains challenging. Herein, a simple but robust route for fabricating sub-30 nm 1D nanopatterns of 2D perovskites over a large area is presented. This method is based on nanoimprinting a thin precursor film of a 2D perovskite with a topographically pre-patterned hard poly(dimethylsiloxane) mold replicated from a block copolymer nanopattern consisting of guided self-assembled monolayered in-plane cylinders. 1D nanopatterns of various 2D perovskites (A'2 MAn -1 Pbn X3 n +1 ,A' = BA, PEA, X = Br, I) are developed; their enhanced photoluminescence (PL) quantum yields are approximately four times greater than those of the corresponding control flat films. Anisotropic photocurrent is observed because 2D perovskite nanocrystals are embedded in a topological 1D nanopattern. Furthermore, this 1D metal-coated nanopattern of a 2D perovskite is employed as a color conversion optical polarizer, in which polarized PL is developed. This is due to its capability of polarization of an incident light arising from the sub-30 nm line pattern, as well as the PL of the confined 2D perovskite nanocrystals in the pattern.

Humidity-Tolerant Moisture-Driven Energy Generator with MXene Aerogel-Organohydrogel Bilayer.

Free-standing and film-type moisture-driven energy generators (MEGs) that harness the preferential interaction of ionized moisture with hydrophilic materials are interesting because of their wearability and portability without needing a water container. However, most such MEGs work in limited humidity conditions, which provide a substantial moisture gradient. Herein, we present a high-performance MEG with sustainable power-production capability in a wide range of environments. The bilayer-based device comprises a negatively surface-charged, hydrophilic MXene (Ti3C2Tx) aerogel and polyacrylamide (PAM) ionic hydrogel. The preferential selection on the MXene aerogel of positive charges supplied from the salts and water in the hydrogel is predicted by the first-principle simulation, which results in a high electric output in a wide relative humidity range from 20% to 95%. Furthermore, by replacing the hydrogel with an organohydrogel of PAM that has excellent water retention and structural stability, a device with long-term electricity generation is realized for more than 15 days in a broad temperature range (from -20 to 80 °C). Our MXene aerogel MEGs connected in series supply sufficient power for commercial electronic components in various outdoor environments. Moreover, an MXene aerogel MEG works as a self-powered sensor for recognizing finger bending and facial expression.

Flexible and Transparent Electrode of Hybrid Ti3C2TX MXene-Silver Nanowires for High-Performance Quantum Dot Light-Emitting Diodes.

The development of electrodes with high conductivity, optical transparency, and reliable mechanical flexibility and stability is important for numerous solution-processed photoelectronic applications. Although transparent Ti3C2TX MXene electrodes with high conductivity are promising, their suitability for displays remains limited because of the high sheet resistance, which is caused by undesirable flake junctions and surface roughness. Herein, a flexible and transparent electrode has been fabricated that is suitable for a full-solution-processed quantum dot light-emitting diode (QLED). An MXene-silver nanowire (AgNW) hybrid electrode (MXAg) consists of a highly conductive AgNW network mixed with solution-processed MXene flakes. Efficient welding of wire-to-wire junctions with MXene flakes yields an electrode with a low sheet resistance and a high transparency of approximately 13.9 Ω sq-1 and 83.8%, respectively. By employing a thin polymer buffer layer of poly(methyl methacrylate) (PMMA), followed by mild thermal treatment, a hybrid PMMA-based MXene-AgNW (MXAg@PMMA) electrode in which the work function of an MXAg hybrid FTE physically embedded in PMMA (MXAg@PMMA) can be tuned by controlling the amount of MXene in the hybrid film facilitates the development of a high-performance solution-processed QLED that exhibits maximum external quantum and current efficiencies of approximately 9.88% and 25.8 cd/A, respectively, with excellent bending stability. This work function-tunable flexible transparent electrode based on solution-processed nanoconductors provides a way to develop emerging high-performance, wearable, cost-effective, and soft electroluminescent devices.

Halide Perovskite Nanocrystal-Enabled Stabilization of Transition Metal Dichalcogenide Nanosheets.

Transition metal dichalcogenide (TMD) nanosheets exfoliated in the liquid phase are of significant interest owing to their potential for scalable and flexible photoelectronic applications. Although various dispersants such as surfactants, oligomers, and polymers are used to obtain highly exfoliated TMD nanosheets, most of them are electrically insulating and need to be removed; otherwise, the photoelectric properties of the TMD nanosheets degrade. Here, inorganic halide perovskite nanocrystals (NCs) of CsPbX3  (X = Cl, Br, or I) are presented as non-destructive dispersants capable of dispersing TMD nanosheets in the liquid phase and enhancing the photodetection properties of the nanosheets, thus eliminating the need to remove the dispersant. MoSe2 nanosheets dispersed in the liquid phase are adsorbed with CsPbCl3  NCs. The CsPbCl3 nanocrystals on MoSe2 efficiently withdraw electrons from the nanosheets, and suppress the dark current of the MoSe2 nanosheets, leading to flexible near-infrared MoSe2  photodetectors with a high ON/OFF photocurrent ratio and detectivity. Moreover, lanthanide ion-doped CsPbCl3  NCs enhance the ON/OFF current ratio to >106 . Meanwhile, the dispersion stability of the MoSe2  nanosheets exfoliated with the perovskite NCs is sufficiently high.