Planar Spin Glass with Topologically Protected Mazes in the Liquid Crystal Targeting for Reconfigurable Micro Security Media.

The planar spin glass pattern is widely known for its inherent randomness, resulting from the geometrical frustration. As such, developing physical unclonable functions (PUFs)-which operate with device randomness-with planar spin glass patterns is a promising candidate for an advanced security systems in the upcoming digitalized society. Despite their inherent randomness, traditional magnetic spin glass patterns pose considerable obstacles in detection, making it challenging to achieve authentication in security systems. This necessitates the development of facilely observable mimetic patterns with similar randomness to overcome these challenges. Here, a straightforward approach is introduced using a topologically protected maze pattern in the chiral liquid crystals (LCs). This maze exhibits a comparable level of randomness to magnetic spin glass and can be reliably identified through the combination of optical microscopy with machine learning-based object detection techniques. The "information" embedded in the maze can be reconstructed through thermal phase transitions of the LCs in tens of seconds. Furthermore, incorporating various elements can enhance the optical PUF, resulting in a multi-factor security medium. It is expected that this security medium, based on microscopically controlled and macroscopically uncontrolled topologically protected structures, may be utilized as a next-generation security system.

Synthesis of MAPbBr3 -Polymer Composite Films by Photolysis of DMF: Toward Transparent and Flexible Optical Physical Unclonable Functions (PUFs) with Hierarchical Multilevel Complexity.

Physical entities with inherent randomness have been investigated as anti-counterfeiting labels based on physical unclonable functions (PUFs). Herein, a transparent and flexible optical PUF label associated with multilevel complexity is demonstrated by taking advantage of the optical properties of hierarchical morphologies of the composite film composed of metal halide perovskite nanoparticles (MAPbBr3 NPs) and the intrinsic spinodal-decomposition-like phase separation of polymer blend (PMMA/PS blend). Due to the combinatorial effects of the photolysis synthesis of MAPbBr3 and the thermodynamic instability of the PMMA/PS blend, randomized patterns emerge at two-level scales. These patterns are intrinsically non-deterministic, and therefore, the PUF labels from the multilevel random patterns are challenging to replicate. This is mainly attributed to random spot patterns (higher-level patterns) confined within intricate bicontinuous patterns (lower-level patterns).

3D-Printed Sugar Scaffold for High-Precision and Highly Sensitive Active and Passive Wearable Sensors.

In this study, a pairing of a previously unidentified 3D printing technique and soft materials is introduced in order to achieve not only high-resolution printed features and flexibility of the 3D-printed materials, but also its light-weight and electrical conductivity. Using the developed technique and materials, high-precision and highly sensitive patient-specific wearable active or passive devices are fabricated for personalized health monitoring. The fabricated biosensors show low density and substantial flexibility because of 3D microcellular network-type interconnected conductive materials that are readily printed using an inkjet head. Using high-resolution 3D scanned body-shape data, on-demand personalized wearable sensors made of the 3D-printed soft and conductive materials are fabricated. These sensors successfully detect both actively changing body strain signals and passively changing signals such as electromyography (EMG), electrodermal activity (EDA), and electroencephalogram EEG. The accurately tailored subject-specific shape of the developed sensors exhibits higher sensitivity and faster real-time sensing performances in the monitoring of rapidly changing human body signals. The newly developed 3D printing technique and materials can be widely applied to various types of wearable, flexible, and light-weight biosensors for use in a variety of inexpensive on-demand and personalized point-of-care diagnostics.

Long-distance transmission of broadband near-infrared light guided by a semi-disordered 2D array of metal nanoparticles.

Near-infrared (NIR) waveguides are a key component of planar photonic devices such as optical communication couplers, image sensors, and spectroscopes for chemical or biological molecules. Conventional NIR waveguides used for signal transmission include silicon-on-insulator (SOI) waveguides and channel/ridge-type metal micro-strips. However, these waveguides usually have limitations of either signal delay or signal loss in optically integrated devices. In this study, a novel NIR waveguide composed of a semi-disordered array of metal nanoparticles (sDAMNPs) on Si substrate was proposed, fabricated, and tested. The disordered metallic nanoparticles array is geometrically localized in the form of 1D metal strips, thus replacing sDAMNPs with less lossy micro strip channel waveguides. From the measurements supported by various computational models, the fabricated waveguides operate effectively in the broadband NIR region (1100 to 1700 nm). The waveguide does not support signal transmission in the ultra violet-visible spectrum due to strong signal absorption, scattering, and localization effects inside the metal nanoparticles. Instead, it is capable of transmitting NIR over a distance longer than 100 µm (signal loss ∼3.85 dB per 100 µm for NIR from 1200 to 1600 nm), which is also sufficiently longer than the conventional surface plasmon polariton propagation distance at the metal-Si interface. Compared to a waveguide-free reference, the waveguide exhibited greatly improved signal transmission efficiency up to a factor of 7.42 × 104 at 1367 nm. It also exhibits a high deflection angle sensitivity of 1.89 dB per 0.01 rad, thus efficiently and straightly guiding the broadband NIR signal over a long distance.

On-Demand Drug Release from Gold Nanoturf for a Thermo- and Chemotherapeutic Esophageal Stent.

Stimuli-responsive delivery systems for cancer therapy have been increasingly used to promote the on-demand therapeutic efficacy of anticancer drugs and, in some cases, simultaneously generate heat in response to a stimulus, resulting in hyperthermia. However, their application is still limited due to the systemic drawbacks of intravenous delivery, such as rapid clearance from the bloodstream and the repeat injections required for sustained safe dosage, which can cause overdosing. Here, we propose a gold (Au)-coated nanoturf structure as an implantable therapeutic interface for near-infrared (NIR)-mediated on-demand hyperthermia chemotherapy. The Au nanoturf possessed long-lasting doxorubicin (DOX) duration, which helps facilitate drug release in a sustained and prolonged manner. Moreover, the Au-coated nanoturf provides reproducible hyperthermia induced by localized surface plasmon resonances under NIR irradiation. Simultaneously, the NIR-mediated temperature increase can promote on-demand drug release at desired time points. For in vivo analysis, the Au nanoturf structure was applied on an esophageal stent, which needs sustained anticancer treatment to prevent tumor recurrence on the implanted surface. This thermo- and chemo-esophageal stent induced significant cancer cell death with released drug and hyperthermia. These phenomena were also confirmed by theoretical analysis. The proposed strategy provides a solution to achieve enhanced thermo-/chemotherapy and has broad applications in sustained cancer treatments.

Long-term efficient organic photovoltaics based on quaternary bulk heterojunctions.

A major impediment to the commercialization of organic photovoltaics (OPVs) is attaining long-term morphological stability of the bulk heterojunction (BHJ) layer. To secure the stability while pursuing optimized performance, multi-component BHJ-based OPVs have been strategically explored. Here we demonstrate the use of quaternary BHJs (q-BHJs) composed of two conjugated polymer donors and two fullerene acceptors as a novel platform to produce high-efficiency and long-term durable OPVs. A q-BHJ OPV (q-OPV) with an experimentally optimized composition exhibits an enhanced efficiency and extended operational lifetime than does the binary reference OPV. The q-OPV would retain more than 72% of its initial efficiency (for example, 8.42-6.06%) after a 1-year operation at an elevated temperature of 65 °C. This is superior to those of the state-of-the-art BHJ-based OPVs. We attribute the enhanced stability to the significant suppression of domain growth and phase separation between the components via kinetic trapping effect.

Two-Dimensional Nanoparticle Supracrystals: A Model System for Two-Dimensional Melting.

In a Langmuir trough, successive compression cycles can drive a two-dimensional (2D) nanoparticle supracrystal (NPSC) closer to its equilibrium structure. Here, we show a series of equilibrated 2D NPSCs consisting of gold NPs of uniform size, varying solely in the length of their alkanethiol ligands. The ordering of the NPSC is governed by the ligand length, thus providing a model system to investigate the nature of 2D melting in a system of NPs. As the ligand length increases the supracrystal transitions from a crystalline to a liquid-like phase with evidence of a hexatic phase at an intermediate ligand length. The phase change is interpreted as an entropy-driven phenomenon associated with steric constraints between ligand shells. The density of topological defects scales with ligand length, suggesting an equivalence between ligand length and temperature in terms of melting behavior. On the basis of this equivalence, the experimental evidence indicates a two-stage 2D melting of NPSCs.

Upconversion luminescence enhancement in plasmonic architecture with random assembly of metal nanodomes.

We report an experimental study on the highly enhanced upconversion luminescence (UCL) of ß-NaYF4:Yb(3+)/Er(3+) nanocrystals (NCs) in a plasmonic architecture. For the architecture, we designed a thin film device composed of a thin layer of NCs capped with an upper layer of a plasmonic nanodome array (pNDA) and lower substrate of a back reflector (BR). Compared to the UCL intensity observed in a glass reference substrate, the designed plasmonic architecture exhibits distinctively strong luminescence enhanced by up to 800-fold. The intensity considerably exceeds the previously reported luminescence intensity regardless of the excitation power. We elucidated a mechanism explaining the large UCL enhancement, which quantitatively analyzes the combination of plasmonic effects as well as multiple large scattering. More importantly, we provided a detailed analysis of the Ag NDA-derived and BR-assisted plasmonic effects that contribute to an increase in the radiative decay rate and an enhancement of the absorption of incident light. The present study is expected to be beneficial for designing a thin film-based plasmonic structure with a randomized metal nanostructure for high-efficiency photovoltaic devices and infrared detectors.