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We propose a novel design of thermoelectric (TE) effect-based soft temperature sensors for directly monitoring localized subtle temperature stimuli. This design integrates rheology-engineered three-dimensional (3D) printing of high-performance carbon-based TE materials and polymer-based viscoelastic materials with low thermal conductivity. Rheological engineering of carbon nanotube (CNT) TE inks ensures the 3D printing of highly sensitive TE sensing units on directly written 3D soft platforms. Additionally, we pre-dope CNT inks with p - and n -type organic dopants to achieve high sensitivity and a fast response to temperature changes. The introduced 3D soft platforms with low thermal conductivity lead to an efficient thermal gradient on TE sensing units in the out-of-plane direction. Furthermore, encapsulating the temperature sensor array with the same polymer-based materials as the 3D soft platforms facilitates independent detection of localized temperature stimuli by minimizing thermal interaction between sensing units, resulting in precise temperature mapping by localized detection. Our 3D-printed soft temperature sensors exhibit high sensitivity to relatively small temperature changes, with a minimum sensing resolution of 0.1 K within tens of milliseconds. Moreover, the temperature sensor array not only detects localized temperature stimuli by imaging the temperature distribution but also demonstrates remarkable mechanical reliability against repetitive deformation with high accuracy.

In this study, we examined how the regioregularity of poly(3-hexylthiophene) (P3HT) affects molecular packing, free volume, charge transport, and gas sensing properties. Our results showed that the presence of regular alkyl side chains on the polymer backbone promoted a high degree of structural order in regioregular P3HT molecules, leading to a compact packing density and reduced free volume. Consequently, it was more challenging for NO 2 molecules to interact with the hole charge carriers in the conductive channel. On the other hand, the regiorandom P3HT films displayed a larger free volume, attributed to the irregular side chains, which facilitated the gas-analyte interaction while impeding efficient charge transport. Thus, these films exhibited greater sensitivity to analyte gas molecules. The molecular order, packing density, and hardness of P3HT films were confirmed through the use of multiple techniques, including UV-vis spectroscopy, atomic force microscopy, and grazing-incidence X-ray diffraction. Additionally, the regiorandom P3HT films showed enhanced mechanical flexibility compared to the regioregular films. In conclusion, our findings emphasize that the regularity of polymer molecules plays a significant role in determining the charge carrier transport and gas adsorption characteristics.

Silent communication based on biosignals from facial muscle requires accurate detection of its directional movement and thus optimally positioning minimum numbers of sensors for higher accuracy of speech recognition with a minimal person-to-person variation. So far, previous approaches based on electromyogram or pressure sensors are ineffective in detecting the directional movement of facial muscles. Therefore, in this study, high-performance strain sensors are used for separately detecting x - and y -axis strain. Directional strain distribution data of facial muscle is obtained by applying three-dimensional digital image correlation. Deep learning analysis is utilized for identifying optimal positions of directional strain sensors. The recognition system with four directional strain sensors conformably attached to the face shows silent vowel recognition with 85.24% accuracy and even 76.95% for completely nonobserved subjects. These results show that detection of the directional strain distribution at the optimal facial points will be the key enabling technology for highly accurate silent speech recognition.

Microneedle (MN) patches enable simple self-administration of drugs via the skin. In this study, we sought to deliver drug-loaded microspheres (MSs) using MN patches and found that the poly(lactic- co -glycolic acid) (PLGA) MSs failed to localize in the MN tips during fabrication, thereby decreasing their delivered dose and delivery efficiency into skin. We determined that surface interactions between the hydrophobic MSs and the poly(dimethylsiloxane) (PDMS) mold caused MSs to adhere to the mold surface during casting in aqueous formulations, with hydrophobic interactions largely responsible for adhesion. Further studies with polystyrene MSs that similarly carry a negative charge like the PLGA MSs demonstrated both repulsive electrostatic interactions as well as adhesive hydrophobic interactions. Reducing hydrophobic interactions by addition of a surfactant or modifying mold surface properties increased MS loading into MN tips and delivery into porcine skin ex vivo by 3-fold. We conclude that surface interactions affect the loading of hydrophobic MSs into MN patches during aqueous fabrication procedures and that their modulation with the surfactant can increase loading and delivery efficiency.

The reinforcement of polymer nanocomposites can be achieved through alignment or percolation of cellulose nanocrystals (CNCs). Here, we compare the efficacy of these reinforcement mechanisms in thermoplastic polyurethane (PU) elastomer nanocomposites containing thermally stable cotton CNCs. CNC alignment was achieved by melt spinning nanocomposite fibers, while a percolating CNC network was generated by solvent casting nanocomposite films with CNC contents up to 20 wt %. While in films both the CNCs and the PU matrix were entirely isotropic at all concentrations as confirmed by wide-angle X-ray scattering and birefringence analysis, the CNCs in the fibers exhibited a preferential orientation, which improved with increasing CNC concentration. Increasing the CNC concentration in the fibers reduces, however, the alignment of the PU chains, resulting in an entirely isotropic PU matrix at high CNC contents. The mechanical properties of films and fibers were evaluated using stress-strain measurements. Nanocomposite fibers with low CNC content exhibited superior stiffness, extensibility, and strength compared to the films, while the films displayed superior mechanical properties at high CNC concentrations. These findings are rationalized using common semiempirical models describing the reinforcing effects of CNC alignment in fibers (Halpin-Tsai) and CNC percolation in films (percolation model). The formation of a percolating CNC network leads to a stronger reinforcement than CNC alignment, as the reinforcing effect of the latter is limited by the comparably low aspect ratio of CNCs extracted from cotton. As a consequence, above the percolation threshold for cotton CNCs, isotropic nanocomposite PU films show a higher stiffness than aligned nanocomposite PU fibers.

Despite the unique ability of lanthanide-doped upconversion nanoparticles (UCNPs) to convert near-infrared (NIR) light to high-energy UV-vis radiation, low quantum efficiency has rendered their application unpractical in biomedical fields. Here, we report anatase titania-coated plasmonic gold nanorods decorated with UCNPs (Au NR@aTiO 2 @UCNPs) for combinational photothermal and photodynamic therapy to treat cancer. Our novel architecture employs the incorporation of an anatase titanium dioxide (aTiO 2 ) photosensitizer as a spacer and exploits the localized surface plasmon resonance (LSPR) properties of the Au core. The LSPR-derived near-field enhancement induces a threefold boost of upconversion emissions, which are re-absorbed by neighboring aTiO 2 and Au nanocomponents. Photocatalytic experiments strongly infer that LSPR-induced hot electrons are injected into the conduction band of aTiO 2 , generating reactive oxygen species. As phototherapeutic agents, our hybrid nanostructures show remarkable in vitro anticancer effect under NIR light [28.0% cancer cell viability against Au NR@aTiO 2 (77.3%) and UCNP@aTiO 2 (98.8%)] ascribed to the efficient radical formation and LSPR-induced heat generation, with cancer cell death primarily following an apoptotic pathway. In vivo animal studies further confirm the tumor suppression ability of Au NR@aTiO 2 @UCNPs through combinatorial photothermal and photodynamic effect. Our hybrid nanomaterials emerge as excellent multifunctional phototherapy agents, providing a valuable addition to light-triggered cancer treatments in deep tissue.

In solution processing of thin films, the material layer is deposited from a solution composed of several solutes and solvents. The final morphology and hence the properties of the film often depend on the time needed for the evaporation of the solvents. This is typically the case for organic photoactive or electronic layers. Therefore, it is important to be able to predict the evaporation kinetics of such mixtures. We propose here a new phase-field model for the simulation of evaporating fluid mixtures and simulate their evaporation kinetics. Similar to the Hertz-Knudsen theory, the local liquid-vapor (LV) equilibrium is assumed to be reached at the film surface and evaporation is driven by diffusion away from this gas layer. In the situation where the evaporation is purely driven by the LV equilibrium, the simulations match the behavior expected theoretically from the free energy: for evaporation of pure solvents, the evaporation rate is constant and proportional to the vapor pressure. For mixtures, the evaporation rate is in general strongly time-dependent because of the changing composition of the film. Nevertheless, for highly nonideal mixtures, such as poorly compatible fluids or polymer solutions, the evaporation rate becomes almost constant in the limit of low Biot numbers. The results of the simulation have been successfully compared to experiments on a polystyrene-toluene mixture. The model allows to take into account deformations of the liquid-vapor interface and, therefore, to simulate film roughness or dewetting.

Any transition toward an era of flexible electronics will have to overcome the mechanical limitations of materials. Specifically, the attainment of both strength and flexibility, which are generally mutually exclusive, is required including glass-like wear resistance, plastic-like compliance, and a high level of strain. Here, we fabricate a urethane-methacrylate-siloxane hybrid (UMSH) material. It is found that UMSH, with molecule-level hybridization of urethane linkage and methacrylate-siloxane conetworks, demonstrates ceramic-like high strength (574 MPa), yet polymer-like low modulus (8.42 GPa), and even high strain (6.3%) at fracture with excellent optical transparency. This combination of high strength, flexibility, and optical transparency indicates that this is a suitable material for glass substitution and can be used as a transparent flexible cover window for foldable display.