Roll‐to‐Roll Cohesive,Coated, Flexible,High‐Efficiency Polymer Light‐Emitting Diodes Utilizing ITO‐Free Polymer Anodes

This paper reports solution‐processed, high‐efficiency polymer light‐emitting diodes fabricated by a new type of roll‐to‐roll coating method under ambient air conditions. A noble roll‐to‐roll cohesive coating system utilizes only natural gravity and the surface tension of the solution to flow out from the capillary to the surface of the substrate. Because this mechanism uses a minimally cohesive solution, the roll‐to‐roll cohesive coating can effectively realize an ultra‐thin film thickness for the electron injection layer. In addition, the roll‐to‐roll cohesive coating enables the fabrication of a thicker polymer anode film more than 250 nm at one time by modification of the surface energy and without wasting the solution. It is observed that the standard sheet resistance deviation of the polymer anode is only 2.32 Ω/□ over 50 000 bending cycles. The standard sheet resistance deviation of the polymer anode in the different bending angles (0 to 180°) is 0.313 Ω/□, but the case of the ITO‐PET is 104.93 Ω/□. The average surface roughness of the polymer anode measured by atomic force microscopy is only 1.06 nm. Because the surface of the polymer anode has a better quality, the leakage current of the polymer light‐emitting diodes (PLEDs) using the polymer anode is much lower than that using the ITO‐PET substrate. The luminous power efficiency of the two devices is 4.13 lm/W for the polymer anode and 3.21 lm/W for the ITO‐PET. Consequently, the PLEDs made by using the polymer anode exhibited 28% enhanced performance because the polymer anode represents not only a higher transparency than the ITO‐PET in the wavelength of 560 nm but also greatly reduced roughness. The optimized the maximum current efficiency and power efficiency of the device show around 6.1 cd/A and 5.1 lm/W, respectively, which is comparable to the case of using the ITO‐glass.     

Phase‐Engineered Type‐II Multimetal–Selenide Heterostructures toward Low‐Power Consumption,Flexible, Transparent,and Wide‐Spectrum Photoresponse Photodetectors

Phase‐engineered type‐II metal–selenide heterostructures are demonstrated by directly selenizing indium‐tin oxide to form multimetal selenides in a single step. The utilization of a plasma system to assist the selenization facilitates a low‐temperature process, which results in large‐area films with high uniformity. Compared to single‐metal–selenide‐based photodetectors, the multimetal–selenide photodetectors exhibit obviously improved performance, which can be attributed to the Schottky contact at the interface for tuning the carrier transport, as well as the type‐II heterostructure that is beneficial for the separation of the electron–hole pairs. The multimetal–selenide photodetectors exhibit a response to light over a broad spectrum from UV to visible light with a high responsivity of 0.8 A W^?1 and an on/off current ratio of up to 10². Interestingly, all‐transparent photodetectors are successfully produced in this work. Moreover, the possibility of fabricating devices on flexible substrates is also demonstrated with sustainable performance, high strain tolerance, and high durability during bending tests.     

Writing,Self‐Healing,and Self‐Erasing on Conductive Pressure‐Sensitive Adhesives

A simple strategy for enabling conductive pressure sensitive adhesives (PSAs) to work as light‐responsive materials is reported. Direct laser‐writing of PSA substrates was achieved by means of a continuous‐wave He‐Ne laser focused through the objectives of an optical microscope. This approach takes advantage of cooperative interplay between viscoelastic properties of PSAs and enhanced thermal conductivity provided by an extra overlayer of gold. In particular, the thickness of the gold layer is a crucial parameter for tuning the substrate responsiveness. Self‐healing and self‐degradation processes can be exploited for controlling the lifetime of the written information, whereas additional protective coatings can be introduced to achieve permanent storage.     

High‐Performance,Room Temperature,Ultra‐Broadband Photodetectors Based on Air‐Stable PdSe2

Photodetection over a broad spectral range is crucial for optoelectronic applications such as sensing, imaging, and communication. Herein, a high‐performance ultra‐broadband photodetector based on PdSe₂ with unique pentagonal atomic structure is reported. The photodetector responds from visible to mid‐infrared range (up to ≈4.05 µm), and operates stably in ambient and at room temperature. It promises improved applications compared to conventional mid‐infrared photodetectors. The highest responsivity and external quantum efficiency achieved are 708 A W^?1 and 82 700%, respectively, at the wavelength of 1064 nm. Efficient optical absorption beyond 8 µm is observed, indicating that the photodetection range can extend to longer than 4.05 µm. Owing to the low crystalline symmetry of layered PdSe₂, anisotropic properties of the photodetectors are observed. This emerging material shows potential for future infrared optoelectronics and novel devices in which anisotropic properties are desirable.     

Three‐Layered Hollow Nanospheres Based Coatings with Ultrahigh‐Performance of Energy‐Saving,Antireflection, and Self‐Cleaning for Smart Windows

In this study, a well‐controlled interfacial engineering method for the synthesis of SiO₂/TiO₂/VO₂ three‐layered hollow nanospheres (TLHNs) and TLHNs‐based multifunctional coatings is reported. The as‐prepared coatings allow for an outstanding integration of thermochromism from the outer VO₂(M) layer, photocatalytic self‐cleaning capability from the middle TiO₂(A) layer, and antireflective property from internal SiO₂ HNs. The TLHNs coatings exhibit excellent optical performance with ultrahigh luminous transmittance (T_lum‐l = 74%) and an improved solar modulation ability (ΔT_sol = 12%). To the best knowledge, this integrated optical performance is the highest ever reported for TiO₂/VO₂‐based thermochromic coatings. An ingenious computation model is proposed, which allows the n_eff of nanostructured coatings to be rapidly obtained. The experimental and calculated results reveal that the unique three‐layered structure significantly reduces the refractive index (from 2.25 to 1.33 at 600 nm) and reflectance (Rave, from 22.3 to 5.3%) in the visible region as compared with dense coatings. Infrared thermal imaging characterization and self‐cleaning tests provide valid evidence of SiO₂/TiO₂/VO₂ TLHNs coatings' potential for energy‐saving and self‐cleaning smart windows. The exciting inexpensive and universal fabrication process for well‐defined structures may inspire various developments in processable and multifunctional devices.     

High‐Mobility Helical Tellurium Field‐Effect Transistors Enabled by Transfer‐Free,Low‐Temperature Direct Growth

The transfer‐free direct growth of high‐performance materials and devices can enable transformative new technologies. Here, room‐temperature field‐effect hole mobilities as high as 707 cm² V^?1 s^?1 are reported, achieved using transfer‐free, low‐temperature (≤120 °C) direct growth of helical tellurium (Te) nanostructure devices on SiO₂/Si. The Te nanostructures exhibit significantly higher device performance than other low‐temperature grown semiconductors, and it is demonstrated that through careful control of the growth process, high‐performance Te can be grown on other technologically relevant substrates including flexible plastics like polyethylene terephthalate and graphene in addition to amorphous oxides like SiO₂/Si and HfO₂. The morphology of the Te films can be tailored by the growth temperature, and different carrier scattering mechanisms are identified for films with different morphologies. The transfer‐free direct growth of high‐mobility Te devices can enable major technological breakthroughs, as the low‐temperature growth and fabrication is compatible with the severe thermal budget constraints of emerging applications. For example, vertical integration of novel devices atop a silicon complementary metal oxide semiconductor platform (thermal budget <450 °C) has been theoretically shown to provide a 10× systems level performance improvement, while flexible and wearable electronics (thermal budget <200 °C) can revolutionize defense and medical applications.     

A Mussel‐Inspired Persistent ROS‐Scavenging,Electroactive, and Osteoinductive Scaffold Based on Electrochemical‐Driven In Situ Nanoassembly

Conductive polymers are promising for bone regeneration because they can regulate cell behavior through electrical stimulation; moreover, they are antioxidative agents that can be used to protect cells and tissues from damage originating from reactive oxygen species (ROS). However, conductive polymers lack affinity to cells and osteoinductivity, which limits their application in tissue engineering. Herein, an electroactive, cell affinitive, persistent ROS‐scavenging, and osteoinductive porous Ti scaffold is prepared by the on‐surface in situ assembly of a polypyrrole‐polydopamine‐hydroxyapatite (PPy‐PDA‐HA) film through a layer‐by‐layer pulse electrodeposition (LBL‐PED) method. During LBL‐PED, the PPy‐PDA nanoparticles (NPs) and HA NPs are in situ synthesized and uniformly coated on a porous scaffold from inside to outside. PDA is entangled with and doped into PPy to enhance the ROS scavenging rate of the scaffold and realize repeatable, efficient ROS scavenging over a long period of time. HA and electrical stimulation synergistically promote osteogenic cell differentiation on PPy‐PDA‐HA films. Ultimately, the PPy‐PDA‐HA porous scaffold provides excellent bone regeneration through the synergistic effects of electroactivity, cell affinity, and antioxidative activity of the PPy‐PDA NPs and the osteoinductivity of HA NPs. This study provides a new strategy for functionalizing porous scaffolds that show great promise as implants for tissue regeneration.     

Bio‐Inspired,Self‐Toughening Polymers Enabled by Plasticizer‐Releasing Microcapsules

A new concept for the design of self‐toughening thermoplastic polymers is presented. The approach involves the incorporation of plasticizer‐filled microcapsules (MCs) in an intrinsically rigid and brittle matrix polymer. The intriguing adaptability that this simple tactic enables is demonstrated with composites composed of a poly(lactic acid) (PLA) matrix and 5–20% w/w poly(urea‐formaldehyde) (PUF) MCs that contained hexyl acetate as plasticizer. At low strain (<1.5%), the glassy PLA/MC composites remain rigid, although the intact MCs reduce the Young's modulus and tensile strength by up to 50%. While the neat PLA shows brittle failure at a strain of around 2.5%, the composites yield in this regime, because the MCs rupture and release their plasticizing cargo. This effect leads up to 25‐fold increase of the elongation at break and 20‐fold increase of the toughness vis‐à‐vis the neat PLA, while the impact on modulus and ultimate stress is much smaller. Ballistic impact tests show that the self‐toughening mechanism also works at much higher strain rates than applied in tensile tests and the operating mechanism is corroborated through systematic thermomechanical studies that involved dynamic mechanical testing and thermal analysis.