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.

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.

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.

Electrified Operando-Freezing of Electrocatalytic CO2 Reduction Cells for Cryogenic Electron Microscopy.

The ability to freeze and stabilize reaction intermediates in their metastable states and obtain their structural and chemical information with high spatial resolution is critical to advance materials technologies such as catalysis and batteries. Here, we develop an electrified operando-freezing methodology to preserve these metastable states under electrochemical reaction conditions for cryogenic electron microscopy (cryo-EM) imaging and spectroscopy. Using Cu catalysts for CO2 reduction as a model system, we observe restructuring of the Cu catalyst in a CO2 atmosphere while the same catalyst remains intact in air at the nanometer scale. Furthermore, we discover the existence of a single valence Cu (1+) state and C-O bonding at the electrified liquid-solid interface of the operando-frozen samples, which are key reaction intermediates that traditional ex situ measurements fail to detect. This work highlights our novel technique to study the local structure and chemistry of electrified liquid-solid interfaces, with broad impact beyond catalysis.

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.

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.

Stabilizing Bicontinuous Emulsions with Sub-Micrometer Domains Solely by Nanoparticles.

Nanoparticle-stabilized, bicontinuous interfacially jammed emulsion gels (bijels) find potential applications as battery, separation membrane, and chemical reactor materials. Decreasing the liquid domain sizes of bijels to sub-micrometer dimensions requires surfactants, complicating bijel synthesis and postprocessing into functional nanomaterials. This work introduces surfactant-free bijels with sub-micrometer domains, solely stabilized by nanoparticles. To this end, the covalent surface functionalization of silica nanoparticles is characterized by thermogravimetric analysis, mass spectrometry, Fourier-transform infrared spectroscopy, and contact angle measurements. Bijels are generated with the functionalized nanoparticles via solvent transfer induced phase separation (STrIPS), enabling the optimization of nanoparticle functionalization and surface ionization. Nanoparticles of intermediate functionalization and controlled negative surface charge stabilize bijels with sub-micrometer liquid domains. This remarkable control over bijel synthesis provides urgently needed progress to facilitate the widespread implementation of bijels as nanomaterials in research and applications.

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.

Superhydrophobic Array Devices for the Enhanced Formation of 3D Cancer Models.

During the metastatic cascade, cancer cells travel through the bloodstream as circulating tumor cells (CTCs) to a secondary site. Clustered CTCs have greater shear stress and treatment resistance, yet their biology remains poorly understood. We therefore engineered a tunable superhydrophobic array device (SHArD). The SHArD-C was applied to culture a clinically relevant model of CTC clusters. Using our device, we cultured a model of cancer cell aggregates of various sizes with immortalized cancer cell lines. These exhibited higher E-cadherin expression and are significantly more capable of surviving high fluid shear stress-related forces compared to single cells and model clusters grown using the control method, helping to explain why clustering may provide a metastatic advantage. Additionally, the SHArD-S, when compared with the AggreWell 800 method, provides a more consistent spheroid-forming device culturing reproducible sizes of spheroids for multiple cancer cell lines. Overall, we designed, fabricated, and validated an easily tunable engineered device which grows physiologically relevant three-dimensional (3D) cancer models containing tens to thousands of cells.

Design, Fabrication, and Implantation of Invasive Microelectrode Arrays as in vivo Brain Machine Interfaces: A Comprehensive Review.

Invasive Microelectrode Arrays (MEAs) have been a significant and useful tool for us to gain a fundamental understanding of how the brain works through high spatiotemporal resolution neuron-level recordings and/or stimulations. Through decades of research, various types of microwire, silicon, and flexible substrate-based MEAs have been developed using the evolving new materials, novel design concepts, and cutting-edge advanced manufacturing capabilities. Surgical implantation of the latest minimal damaging flexible MEAs through the hard-to-penetrate brain membranes introduces new challenges and thus the development of implantation strategies and instruments for the latest MEAs. In this paper, studies on the design considerations and enabling manufacturing processes of various invasive MEAs as in vivo brain-machine interfaces have been reviewed to facilitate the development as well as the state-of-art of such brain-machine interfaces from an engineering perspective. The challenges and solution strategies developed for surgically implanting such interfaces into the brain have also been evaluated and summarized. Finally, the research gaps have been identified in the design, manufacturing, and implantation perspectives, and future research prospects in invasive MEA development have been proposed.

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.

Tuning Ceramic Surface to Minimize the Ionic Resistance at the Interface between PEO- and LATP-Based Ceramic Electrolyte.

New battery technologies are currently under development, and among them, all-solid-state batteries should deliver better electrochemical performance and enhanced safety. Composite solid electrolytes, combining a solid polymer electrolyte (SPE) and a ceramic electrolyte (CE), should then provide high ionic conductivity coupled to high mechanical stability. To date, this synergy has not yet been reached due to the complexity of the Li-ion transport within the hybrid solid electrolyte, especially at the SPE/CE interface currently considered the limiting step. Yet, there is no proper kinetic model to elucidate the parameters influencing this interfacial barrier. The limited understanding of the SPE/CE interface can be partly explained by scattered SPE/CE interface resistances reported in the literature as well as the lack of systematic studies. Herein, we propose a systematic study of the effect on the SPE/CE interfacial resistance of chemical and thermal treatments of a model LATP-based ceramic based on a methodology relying on electrochemical impedance spectroscopy (EIS) and X-ray photoemission spectroscopy (XPS). The results provide different levers for the optimization of this interface and valuable insights into experimental precautions needed to obtain more reproducible results.

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.

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.

Interfacial Engineering for Controlled Crystal Mosaicity in Single-Crystalline Perovskite Films.

Organic-inorganic hybrid perovskites have attracted significant attention for optoelectronic applications due to their efficient photoconversion properties. However, grain boundaries and irregular crystal orientations in polycrystalline films remain issues. This study presents a method for producing crystalline-orientation-controlled perovskite single-crystal films using retarded solvent evaporation. It is shown that single-crystal films, grown via inverse temperature crystallization within a confined space, exhibit enhanced optoelectronic property. Using interfacial polymer layer, this method produces high-quality perovskite single-crystalline films with varying crystal orientations. Density functional theory calculations confirm favorable adsorption energies for (110) surfaces with methylammonium iodide and PbI2 terminations on poly(3-hexylthiophene), and stronger adsorption for (224) surfaces with I and methylammonium terminations on polystyrene, influenced by repulsive forces between the thiophene group and the perovskite surface. The correlation between charge transport characteristics and perovskite single-crystalline properties highlights potential advancements in perovskite optoelectronics, improving device performance and reliability.

Programmable 2D materials through shape-controlled capillary forces.

In recent years, self-assembly has emerged as a powerful tool for fabricating functional materials. Since self-assembly is fundamentally determined by the particle interactions in the system, if we can gain full control over these interactions, it would open the door for creating functional materials by design. In this paper, we exploit capillary interactions between colloidal particles at liquid interfaces to create two-dimensional (2D) materials where particle interactions and self-assembly can be fully programmed using particle shape alone. Specifically, we consider colloidal particles which are polygonal plates with homogeneous surface chemistry and undulating edges as this particle geometry gives us precise and independent control over both short-range hard-core repulsions and longer-range capillary interactions. To illustrate the immense potential provided by our system for programming self-assembly, we use minimum energy calculations and Monte Carlo simulations to show that polygonal plates with different in-plane shapes (hexagons, truncated triangles, triangles, squares) and edge undulations of different multipolar order (hexapolar, octopolar, dodecapolar) can be used to create a rich variety of 2D structures, including hexagonal close-packed, honeycomb, Kagome, and quasicrystal lattices. Since the required particle shapes can be readily fabricated experimentally, we can use our colloidal system to control the entire process chain for materials design, from initial design and fabrication of the building blocks, to final assembly of the emergent 2D material.

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.

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.