Wimpled thin films via multiple motions of a bubble decorated with surface-active molecules.

HYPOTHESIS: Thin liquid films play a crucial role in various systems and applications. Understanding the mechanisms that regulate their morphology is a scientific challenge with obvious implications for application optimization. Thin liquid films trapped between bubbles and air-liquid interface can show various configurations influenced by their deformation history and system characteristics. EXPERIMENTS: The morphology of thin liquid films formed in the presence of surface-active molecules is here studied with interferometric techniques. Three different systems with varying interfacial properties are investigated to understand their influence on film morphology. Specific deformation histories are applied to the films to generate complex film structures. FINDINGS: We achieve the creation of a rather stable wimple by implementing controlled bubble motions against the air-liquid interface. We provide a criterion for wimple formation based on lubrication theory. The long-term stability of the wimple is also investigated, and more complex multi-wimple structures are experimentally produced building upon the achieved wimple stability.

Fabrication of PHFPO Surface-Modified Conductive AgNWs/PNAGA Hydrogels with Enhanced Water Retention Capacity toward Highly Sensitive Strain Sensors.

Conductive hydrogels, characterized by their unique features of flexibility, biocompatibility, electrical conductivity, and responsiveness to environmental stimuli, have emerged as promising materials for sensitive strain sensors. In this study, a facile strategy to prepare highly conductive hydrogels is reported. Through rational structural and synthetic design, silver nanowires (AgNWs) are incorporated into poly(N-acryloyl glycinamide) (PNAGA) hydrogels, achieving high electrical conductivity (up to 0.88 S m-1), significantly enhanced mechanical properties, and elevated deformative sensitivity. Furthermore, surface modification with polyhexafluoropropylene oxide (PHFPO) has substantially improved the water retention capacity and dressing comfort of this hydrogel material. Based on the above merits, these hydrogels are employed to fabricate highly sensitive wearable strain sensors which can detect and interpret subtle hand and finger movements and enable precise control of machine interfaces. The AgNWs/PNAGA based strain sensors can effectively sense finger motion, enabling the control of robotic fingers to replicate the human hand's gestures. In addition, the high deformative sensitivity and elevated water retention performance of the hydrogels makes them suitable for flow sensing. These conceptual applications demonstrate the potential of this conductive hydrogel in high-performance strain sensors in the future.

Comparison of user interfaces for measuring the matrix sentence test on a smartphone.

OBJECTIVE: Smartphone-based self-testing could facilitate large-scale data collection and remote diagnostics. For this purpose, the matrix sentence test (MST) is an ideal candidate due to its repeatability and accuracy. In clinical practice, the MST requires professional audiological equipment and supervision, which is infeasible for smartphone-based self-testing. Therefore, it is crucial to investigate the feasibility of self-administering the MST on smartphones, including the development of an appropriate user interface for the small screen size. DESIGN: We compared the traditional closed matrix user interface (10 × 5 matrix) to three alternative, newly-developed interfaces (slide, type, wheel) regarding SRT consistency, user preference, and completion time. STUDY SAMPLE: We included 15 younger normal hearing and 14 older hearing-impaired participants in our study. RESULTS: The slide interface is most suitable for mobile implementation, providing consistent and fast SRTs and enabling all participants to perform the tasks effectively. While the traditional matrix interface works well for most participants, some participants experienced difficulties due to its small size on the screen. CONCLUSIONS: We propose the newly-introduced slide interface as a plausible alternative for smartphone screens. This might be more attractive for elderly patients that may exhibit more challenges with dexterity and vision than our test subjects employed here.

Potential of plasmonics and nanoscale light-matter interactions for the next generation of optical neural interfaces.

Within the realm of optical neural interfaces, the exploration of plasmonic resonances to interact with neural cells has captured increasing attention among the neuroscience community. The interplay of light with conduction electrons in nanometer-sized metallic nanostructures can induce plasmonic resonances, showcasing a versatile capability to both sense and trigger cellular events. We describe the perspective of generating propagating or localized surface plasmon polaritons on the tip of an optical neural implant, widening the possibility for neuroscience labs to explore the potential of plasmonic neural interfaces.

Real-Time Observation of Protein Aggregation at Liquid-Liquid Interfaces in a Microfluidic Device.

A droplet microfluidic device to capture in real-time protein aggregation at liquid-liquid interfaces is described. In contrast to conventional methods, typically characterized by a lag time between the application of interfacial stress and the measurement of protein aggregation, here protein adsorption, the formation of a viscoelastic protein layer, aggregation, and shedding of protein particles into solution is simultaneously monitored. The device is applied to analyze the stability of antibody formulations over a wide range of concentrations (1-180 mg mL-1) at the silicone oil (SO)-water interface under controlled mechanical deformation. The adsorption onto oil droplets induces the formation of a viscoelastic protein layer on a subsecond timescale, which progressively restricts the relaxation of the droplets within the chip. Upon mechanical rupture, the protein layer releases particles in solution. The rate of particle formation increases strongly with concentration, similar to the bulk viscosity. Concentrations above 120 mg mL-1 lead to aggregation in seconds and drastically decrease the mechanical perturbations required to shed protein particles in solution. These results are important for the development of formulations at high-protein concentrations (>100 mg mL-1) and indicate that particular attention should be given to interface-induced particle formation in this concentration range. In this context, low-volume microfluidic platforms allow the assessment of protein physical instabilities early in development and represent attractive tools to optimize antibody stability and formulation design consuming limited amounts of material.

Molecular-Resolution Imaging of Ionic Liquid/Alkali Halide Interfaces with Varied Surface Charge Densities via Atomic Force Microscopy.

When in contact with charged solid surfaces, ionic liquids (ILs) are known to form solvation structures consisting of alternating cation and anion layers. This phenomenon is considered to originate from the adsorption layer of counterions overcompensating the surface charge, so-called overscreening. However, the response of these layers to surfaces with near-zero or extremely high surface charge density (σ) remains inadequately understood. Here, we probe the solvation structure of ILs on alkali halide surfaces with varied surface orientations: nearly zero-charged RbI(100) and highly charged RbI(111), by employing frequency modulation atomic force microscopy with atomic resolution. Two commonly used ILs are examined in this study: 1-methyl-1-propylpyrrolidinium bis(trifluoromethylsulfonyl)imide ([C3mpyr][NTf2]) and 1-ethyl-3-methylimidazolium bis(trifluoromethylsulfonyl)imide ([C2mim][NTf2]). On RbI(100) surfaces with near zero σ, we observe alternating cation and anion layers, diverging from the previously proposed monolayer model for IL/alkali halide(100) interfaces. These results support the argument that overscreening occurs under low σ, even approaching zero, and reconcile conflicting experimental conclusions about low σ systems. On RbI(111) surfaces with high σ, we identify solvation structures consisting of two consecutive counterion layers. This structure aligns with the theoretically predicted crowding; a phenomenon rarely observed in commonly used ILs due to typically unreachable σ in electrochemical IL/electrode systems. Our findings indicate that alkali halide(111) surfaces are potentially valuable for exploring the crowding phenomenon in ILs, addressing the current scarcity of experimental observations.

Decoding working-memory load during n-Back task performance from high channel fNIRS data.

OBJECTIVE: Functional near-infrared spectroscopy (fNIRS) can measure neural activity through blood oxygenation changes in the brain in a wearable form factor, enabling unique applications for research in and outside the lab and in practical occupational settings. fNIRS has proven capable of measuring cognitive states such as mental workload, often using machine learning (ML) based brain-computer interfaces (BCIs). To date, this research has largely relied on probes with channel counts from under ten to several hundred, although recently a new class of wearable NIRS devices featuring thousands of channels has emerged. This poses unique challenges for ML classification, as fNIRS is typically limited by few training trials, which results in severely under-determined estimation problems. So far, it is not well understood how such high-resolution data is best leveraged in practical BCIs and whether state-of-the-art or better performance can be achieved. APPROACH: To address these questions, we propose an ML strategy to classify working-memory load that relies on spatio-temporal regularization and transfer learning from other subjects in a combination that, to our knowledge, has not been used in previous fNIRS BCIs. The approach can be interpreted as an end-to-end generalized linear model and allows for a high degree of interpretability using channel-level or cortical imaging approaches. MAIN RESULTS: We show that using the proposed methodology, it is possible to achieve state-of-the-art decoding performance with high-resolution fNIRS data. We also replicated several state-of-the-art approaches on our dataset of 43 participants wearing a 3198 dual-channel NIRS device while performing the n-Back task and show that these existing methodologies struggle in the high-channel regime and are largely outperformed by the proposed pipeline. SIGNIFICANCE: Our approach helps establish high-channel NIRS devices as a viable platform for state-of-the-art BCI and opens new applications using this class of headset while also enabling high-resolution model imaging and interpretation.

Enhancing the Efficiency and Stability of Perovskite Solar Cells Using Chemical Bath Deposition of SnO2 Electron Transport Layers and 3D/2D Heterojunctions.

Chemical bath deposition (CBD) is an effective technique used to produce high-quality SnO2 electron transport layers (ETLs) employed in perovskite solar cells (PSCs). By optimizing the CBD process, high-quality SnO2 films are obtained with minimal oxygen vacancies and close energy level alignment with the perovskite layer. In addition, the 3D perovskite layers are passivated with n-butylammonium iodide (BAI), iso-pentylammonium iodide (PNAI), or 2-methoxyethylammonium iodide (MOAI) to form 3D/2D heterojunctions, resulting in defect passivation, suppressing ion migration and improving charge carrier extraction. As a result of these heterojunctions, the power conversion efficiency (PCE) of the PSCs increased from 21.39% for the reference device to 23.70% for the device containing the MOAI-passivated film. The 2D perovskite layer also provides a hydrophobic barrier, thus enhancing stability to humidity. Notably, the PNAI-based device exhibited remarkable stability, retaining approximately 95% of its initial efficiency after undergoing 1000-h testing in an N2 environment at room temperature.

In-Situ Polymerized High-Voltage Solid-State Lithium Metal Batteries with Dual-Reinforced Stable Interfaces.

Solid polymer electrolytes (SPEs) represent a pivotal advance toward high-energy solid-state lithium metal batteries. However, inadequate interfacial contact remains a significant bottleneck, impeding scalability and application. Inadequate interfacial contact remains a significant bottleneck, impeding scalability and application. Recent efforts have focused on transforming liquid/solid interfaces into solid/solid ones through in situ polymerization, which shows potential especially in reducing interface impedance. Here, we designed high-voltage SSLMBs with dual-reinforced stable interfaces by combining interface modification with an in situ polymerization technology inspired by targeted effects in medicine. Theoretical calculations and time-of-flight secondary ion mass spectrometry (TOF-SIMS) analysis demonstrate that tetramethylene sulfone (TMS) and bis(2,2,2-trifluoromethyl) carbonate (TFEC) exhibit selective adsorption at the interface of the LiNi0.8Co0.1Mn0.1O2 (NCM) cathode and Li anode, respectively. These compounds further decompose to form a stable cathode-electrolyte interface (CEI) film and a solid electrolyte interface (SEI) film, thereby simultaneously achieving a superior interface between the SPE and both the Li anode and NCM cathode. The developed Li||SPE||Li cell sustained cycling for more than 1000 h at 0.3 mA cm-2, and the NCM||SPE||Li cell also demonstrated an excellent capacity retention of 86.8% after 1000 cycles at 1 °C. This work will provide valuable insights for the rational design of high-voltage SSLMBs with stable interfaces, leveraging in situ polymerization as a cornerstone technology.

Prelude to a Compositional Systems Biology.

Composition is a powerful principle for systems biology, focused on the interfaces, interconnections, and orchestration of distributed processes. Whereas most systems biology models focus on the structure or dynamics of specific subsystems in controlled conditions, compositional systems biology aims to connect such models into integrative multiscale simulations. This emphasizes the space between models-a compositional perspective asks what variables should be exposed through a submodel's interface? How do coupled models connect and translate across scales? How can we connect domain-specific models across biological and physical research areas to drive the synthesis of new knowledge? What is required of software that integrates diverse datasets and submodels into unified multiscale simulations? How can the resulting integrative models be accessed, flexibly recombined into new forms, and iteratively refined by a community of researchers? This essay offers a high-level overview of the key components for compositional systems biology, including: 1) a conceptual framework and corresponding graphical framework to represent interfaces, composition patterns, and orchestration patterns; 2) standardized composition schemas that offer consistent formats for composable data types and models, fostering robust infrastructure for a registry of simulation modules that can be flexibly assembled; 3) a foundational set of biological templates-schemas for cellular and molecular interfaces, which can be filled with detailed submodels and datasets, and are designed to integrate knowledge that sheds light on the molecular emergence of cells; and 4) scientific collaboration facilitated by user-friendly interfaces for connecting researchers with datasets and models, and which allows a community of researchers to effectively build integrative multiscale models of cellular systems.

Impact of interface traps on charge noise and low-density transport properties in Ge/SiGe heterostructures.

Hole spins in Ge/SiGe heterostructures have emerged as an interesting qubit platform with favourable properties such as fast electrical control and noise-resilient operation at sweet spots. However, commonly observed gate-induced electrostatic disorder, drifts, and hysteresis hinder reproducible tune-up of SiGe-based quantum dot arrays. Here, we study Hall bar and quantum dot devices fabricated on Ge/SiGe heterostructures and present a consistent model for the origin of gate hysteresis and its impact on transport metrics and charge noise. As we push the accumulation voltages more negative, we observe non-monotonous changes in the low-density transport metrics, attributed to the induced gradual filling of a spatially varying density of charge traps at the SiGe-oxide interface. With each gate voltage push, we find local activation of a transient low-frequency charge noise component that completely vanishes again after 30 hours. Our results highlight the resilience of the SiGe material platform to interface-trap-induced disorder and noise and pave the way for reproducible tuning of larger multi-dot systems.

Boron-doped diamond composites for durable oxygen evolution.

The urgent need to develop efficient, durable, and cost-effective oxygen evolution reaction (OER) catalysts for energy conversion and storage has prompted extensive research. Currently available commercial noble metal-based OER catalysts are expensive and exhibit limited long-term stability. In this study, boron-doped diamond composites (BDDCs) consisting of CoFe and CoFe2C nanoparticles supported by boron-doped diamond (BDD) particles have been prepared. The BDDC catalyst, prepared through a straightforward annealing process, exhibits exceptional durability (up to 72 h at 10 mA cm-2), a low overpotential (306 mV at 10 mA cm-2), and modest Tafel slope (58 mV dec-1). The coherent interfaces between CoFe/CoFe2C nanoparticles and the BDD substrate are essential for enhancing the OER performance. The fabrication method and composite structures presented in this study may facilitate the design and production of promising catalysts.

Materials, Structure, and Interface of Stretchable Interconnects for Wearable Bioelectronics.

Since wearable technologies for telemedicine have emerged to tackle global health concerns, the demand for well-attested wearable healthcare devices with high user comfort also arises. Skin-wearables for health monitoring require mechanical flexibility and stretchability for not only high compatibility with the skin's dynamic nature but also a robust collection of fine health signals from within. Stretchable electrical interconnects, which determine the device's overall integrity, are one of the fundamental units being understated in wearable bioelectronics. In this review, a broad class of materials and engineering methodologies recently researched and developed are presented, and their respective attributes, limitations, and opportunities in designing stretchable interconnects for wearable bioelectronics are offered. Specifically, the electrical and mechanical characteristics of various materials (metals, polymers, carbons, and their composites) are highlighted, along with their compatibility with diverse geometric configurations. Detailed insights into fabrication techniques that are compatible with soft substrates are also provided. Importantly, successful examples of establishing reliable interfacial connections between soft and rigid elements using novel interconnects are reviewed. Lastly, some perspectives and prospects of remaining research challenges and potential pathways for practical utilization of interconnects in wearables are laid out.

Scale-Bridging Mechanics Transfer Enables Ultrabright Mechanoluminescent Fiber Electronics.

Mechanoluminescent (ML) fibers and textiles enable stress visualization without auxiliary power, showing great potential in wearable electronics, machine vision, and human-computer interaction. However, traditional ML devices suffer from inefficient stress transfer in soft-rigid material systems, leading to low luminescence brightness and short cycle life. Here, we propose a tendon-inspired scale-bridging mechanics transfer mechanism for ML composites, which employs molecular-scale copolymerized cross-linking and nanoscale inorganic nanoparticles as hierarchical stress transfer sites. This strategy effectively reduces the dissipation of stress in molecular chain segments and alleviates local stress concentration, increases luminescence by 9 times, and extends cycle life to more than 10,000 times. Furthermore, a scalable (kilometer-scale) anti-Plateau-Rayleigh instability manufacturing technology is developed for thermoset ML fibers, compatible with various existing textile techniques. We also demonstrate its system-level applications in motion capture, underwater interaction, etc., providing a feasible strategy for the next generation of smart visual textiles.

Kinetic monitoring of molecular interactions during surfactant-driven self-propelled droplet motion by high spatial resolution waveguide sensing.

HYPOTHESIS: Self-driven actions, like motion, are fundamental characteristics of life. Today, intense research focuses on the kinetics of droplet motion. Quantifying macroscopic motion and exploring the underlying mechanisms are crucial in self-structuring and self-healing materials, advancements in soft robotics, innovations in self-cleaning environmental processes, and progress within the pharmaceutical industry. Usually, the driving forces inducing macroscopic motion act at the molecular scale, making their real-time and high-resolution investigation challenging. Label-free surface sensitive measurements with high lateral resolution could in situ measure both molecular-scale interactions and microscopic motion. EXPERIMENTS: We employ surface-sensitive label-free sensors to investigate the kinetic changes in a self-assembled monolayer of the trimethyl(octadecyl)azanium chloride surfactant on a substrate surface during the self-propelled motion of nitrobenzene droplets. The adsorption-desorption of the surfactant at various concentrations, its removal due to the moving organic droplet, and rebuilding mechanisms at droplet-visited areas are all investigated with excellent time, spatial, and surface mass density resolution. FINDINGS: We discovered concentration dependent velocity fluctuations, estimated the adsorbed amount of surfactant molecules, and revealed multilayer coverage at high concentrations. The desorption rate of surfactant (18.4 s-1) during the microscopic motion of oil droplets was determined by in situ differentiating between droplet visited and non-visited areas.

Blade-Coated Porous 3D Carbon Composite Electrodes Coupled with Multiscale Interfaces for Highly Sensitive All-Paper Pressure Sensors.

Flexible and wearable pressure sensors hold immense promise for health monitoring, covering disease detection and postoperative rehabilitation. Developing pressure sensors with high sensitivity, wide detection range, and cost-effectiveness is paramount. By leveraging paper for its sustainability, biocompatibility, and inherent porous structure, herein, a solution-processed all-paper resistive pressure sensor is designed with outstanding performance. A ternary composite paste, comprising a compressible 3D carbon skeleton, conductive polymer poly(3,4-ethylenedioxythiophene):poly(styrenesulfonate), and cohesive carbon nanotubes, is blade-coated on paper and naturally dried to form the porous composite electrode with hierachical micro- and nano-structured surface. Combined with screen-printed Cu electrodes in submillimeter finger widths on rough paper, this creates a multiscale hierarchical contact interface between electrodes, significantly enhancing sensitivity (1014 kPa-1) and expanding the detection range (up to 300 kPa) of as-resulted all-paper pressure sensor with low detection limit and power consumption. Its versatility ranges from subtle wrist pulses, robust finger taps, to large-area spatial force detection, highlighting its intricate submillimeter-micrometer-nanometer hierarchical interface and nanometer porosity in the composite electrode. Ultimately, this all-paper resistive pressure sensor, with its superior sensing capabilities, large-scale fabrication potential, and cost-effectiveness, paves the way for next-generation wearable electronics, ushering in an era of advanced, sustainable technological solutions.

Electrolyte-Electrocatalyst Interfacial Effects of Polymeric Materials for Tandem CO2 Capture and Conversion Elucidated Using In Situ Electrochemical AFM.

Integrating CO2 capture and electrochemical conversion has been proposed as a strategy to reduce the net energy required for CO2 regeneration in traditional CO2 capture and conversion schemes and can be coupled with carbon-free renewable electricity. Polyethylenimine (PEI)-based materials have been previously studied as CO2 capture materials and can be integrated in these reactive capture processes. PEI-based electrolytes have been found to significantly increase the CO2 loading, and impact selectivity and rate of product formation when compared to the conventional aqueous electrolytes. However, the influence of these materials at the catalyst-electrode interface is currently not well understood. In this study, PEI-based electrolytes were prepared and their impact on the morphology of a silver electrode performing electrochemical CO2 reduction (CO2R) was studied using in situ electrochemical atomic force microscopy (EC-AFM). The presence of PEI on the electrode surface could be distinguished based on nanomechanical properties (DMT modulus), and changes were observed as negative polarization was applied, revealing a reorganization of the PEI chains due to electrostatic interactions. These changes were impacted by the electrolyte composition, including the addition of supporting electrolyte KHCO3 salt, as well as CO2 captured by the PEI-based electrolyte, which minimized the change in surface mechanical properties and degree of PEI alignment on the electrode surface. The changes in surface mechanical properties were also dependent on the PEI polymer length, with higher molecular weight PEI showing different reconfiguration than the shorter polymer brushes. The study highlights that the choice of polymer material, the electrolyte composition, and CO2 captured impact the near-electrode environment, which has implications for CO2R, and presents EC-AFM as a new tool that can be used to probe the dynamic behavior of these interfaces during electrocatalysis.

Charge Transfer Mechanisms of Adaptive Multicomponent Solutions at Solid-Liquid Interfaces for Real-Time Coolant State Monitoring.

Charge-transfer mechanisms in adaptive multicomponent solutions at liquid-solid interfaces with triboelectric probes are crucial for understanding chemistry dynamics. However, liquid-solid charge transfer becomes unpredictable, due to the components or interactions in solutions, restricting its potential application for precise monitoring of liquid environments. This study utilizes triboelectric probes to investigate the charge transfer of chemicals, applying this approach to real-time coolant state monitoring. Analysis of electrical signal dynamics induced by ethylene glycol and its oxidation byproduct, oxalic acid, in ethylene glycol solutions reveals that hydrogen bond and ion adsorption diminishes the efficiency of electron transfer at the liquid-solid interface. These findings promote the engineering of the triboelectric probe that enhances coolant quality with remarkable sensitivity (detection limit: 0.0001%) and a broad freezing point operational range (0 to -49 °C). This work advances the precise control of the charge dynamics and demonstrates the potential of triboelectric probes for interdisciplinary applications.

On-the-Fly Machine Learning Force Field Study of Liquid-Al/Solid-TiB2 Interfaces.

Using the on-the-fly machine learning force field, simulations were performed to study the atomic structure evolution of the liquid-Al/solid-TiB2 interface with two different terminations, aiming to deepen the understanding of the mechanism of TiB2 as nucleating particles in an aluminum alloy. We conducted simulations using MLFF for up to 100 ps, enabling us to observe the interfacial properties from a deeper and more comprehensive perspective. The nucleation potential of TiB2 particles is determined by the formation of various ordered structures at the interface, which is significantly influenced by the termination of the TiB2 (0001) surface. The evolution of the interface during heterogeneous nucleation processes with different terminations is described using structural information and dynamic characteristics. The Ti-terminated surface is more prone to forming quasi-solid regions compared to the B-termination. Analysis of mean square displacement and vibrational density of states indicates that the liquid layer at the Ti-terminated interface is closer in characteristics to a solid compared to the B-terminated interface. We also found that on the TiB2 (0001) surface different terminations give rise to distinct ordered structures at the interfaces, which is ascribed to their different diffusion abilities.