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1.
Commun Mater ; 5(1): 202, 2024.
Article in English | MEDLINE | ID: mdl-39351280

ABSTRACT

Surfaces - by breaking bulk symmetries, introducing roughness, or hosting defects - can significantly influence magnetic order in magnetic materials. Determining their effect on the complex nanometer-scale phases present in certain non-centrosymmetric magnets is an outstanding problem requiring high-resolution magnetic microscopy. Here, we use scanning SQUID microscopy to image the surface of bulk Cu2OSeO3 at low temperature and in a magnetic field applied along 100 . Real-space maps measured as a function of applied field reveal the microscopic structure of the magnetic phases and their transitions. In low applied field, we observe a magnetic texture consistent with an in-plane stripe phase, pointing to the existence of a distinct surface state. In the low-temperature skyrmion phase, the surface is populated by clusters of disordered skyrmions, which emerge from rupturing domains of the tilted spiral phase. Furthermore, we displace individual skyrmions from their pinning sites by applying an electric potential to the scanning probe, thereby demonstrating local skyrmion control at the surface of a magnetoelectric insulator.

2.
ACS Nano ; 2024 Oct 02.
Article in English | MEDLINE | ID: mdl-39357008

ABSTRACT

Unwanted processes in metal anode batteries, e.g., non-uniform metal electrodeposition, electrolyte decomposition, and/or short-circuiting, are not fully captured by the electrolyte bulk solvation structure but rather defined by the electrode-electrolyte interface and its changes induced by cycling conditions. Specifically, for aluminum-ion batteries (AIBs), the role of the solid-electrolyte interphase (SEI) on the Al0 electrodeposition mechanism and associated changes during resting or cycling remain unclear. Here, we investigated the current-dependent changes at the electrified aluminum anode/ionic liquid electrolyte interface to reveal the conditions of the SEI formation leading to irreversible cycling in the AIBs. We identified that the mechanism of anode failure depends on the nature of the counter electrode, where the areal capacity and cycling current for Al0 electrodeposition dictates the number of successful cycles. Notwithstanding the differences behind unstable aluminum anode cycling in symmetrical cells and AIBs, the uniform removal of electrochemically inactive SEI components, e.g., oxide-rich or solvent-derived organic-rich interphases, leads to more efficient cycling behavior. These understandings raise the importance of using specific conditioning protocols for efficient cycling of the aluminum anode in conjugation with different cathode materials.

3.
ACS Appl Mater Interfaces ; 16(39): 53153-53162, 2024 Oct 02.
Article in English | MEDLINE | ID: mdl-39358896

ABSTRACT

Understanding and predicting interface diffusion phenomena in materials is crucial for various industrial applications, including semiconductor manufacturing, battery technology, and catalysis. In this study, we propose a novel approach utilizing Graph Neural Networks (GNNs) to investigate and model material interface diffusion. We begin by collecting experimental and simulated data on diffusion coefficients, concentration gradients, and other relevant parameters from diverse material systems. The data are preprocessed, and key features influencing interface diffusion are extracted. Subsequently, we construct a GNN model tailored to the diffusion problem, with a graph representation capturing the atomic structure of materials. The model architecture includes multiple graph convolutional layers for feature aggregation and update, as well as optional graph attention layers to capture complex relationships between atoms. We train and validate the GNN model using the preprocessed data, achieving accurate predictions of diffusion coefficients, diffusion rates, concentration profiles, and potential diffusion pathways. Our approach offers insights into the underlying mechanisms of interface diffusion and provides a valuable tool for optimizing material design and engineering. Additionally, our method offers possible strategies to solve the longstanding problems related to materials interface diffusion.

4.
Adv Mater ; : e2411244, 2024 Oct 02.
Article in English | MEDLINE | ID: mdl-39358939

ABSTRACT

Artificially stacking 2D materials (2DMs) into vdW heterostructures creates materials with properties not present in nature that offer great potential for various applications such as flexible electronics. Properties of such stacked structures are controlled largely by the interfacial interactions and the structural integrity of the 2DMs. In spite of their crucial roles, interfacial stress transfer and the failure mechanisms of the vdW heterostructures, particularly during deformation, have not been well addressed so far. In this work, the interfacial stress transfer and failure mechanisms of a MoS2/graphene vdW heterostructure are studied, through the strain distributions both laterally in individual 2DMs and vertically across different 2DMs revealed in-situ. The fracture of the MoS2 and the associated states of stress and strain are monitored experimentally. This enables various interfacial properties, such as the interfacial shear strength and interfacial fracture energy, to be estimated. Based only on the measured strength and interfacial properties of a single vdW heterostructure, a failure criterion is proposed to predict the failure mechanisms of similar vdW heterostructures with any lateral dimensions. This work provides an insight to the deformation micromechanics of vdW heterostructures that are of great value for their miniaturization and applications, especially in flexible electronics.

5.
Proc Natl Acad Sci U S A ; 121(38): e2407877121, 2024 Sep 17.
Article in English | MEDLINE | ID: mdl-39259594

ABSTRACT

Understanding the structure in the nanoscopic region of water that is in direct contact with solid surfaces, so-called contact layer, is key to quantifying macroscopic properties that are of interest to e.g. catalysis, ice nucleation, nanofluidics, gas adsorption, and sensing. We explore the structure of the water contact layer on various technologically relevant solid surfaces, namely graphene, MoS[Formula: see text], Au(111), Au(100), Pt(111), and Pt(100), which have been previously hampered by time and length scale limitations of ab initio approaches or force field inaccuracies, by means of molecular dynamics simulations based on ab initio machine learning potentials built using an active learning scheme. Our results reveal that the in-plane intermolecular correlations of the water contact layer vary greatly among different systems: Whereas the contact layer on graphene and on Au(111) is predominantly homogeneous and isotropic, it is inhomogeneous and anisotropic on MoS[Formula: see text], on Au(100), and on the Pt surfaces, where it additionally forms two distinct sublayers. We apply hydrodynamics and the theory of the hydrophobic effect, to relate the energy corrugation and the characteristic length-scales of the contact layer with wetting, slippage, the hydration of small hydrophobic solutes and diffusio-osmotic transport. Thus, this work provides a microscopic picture of the water contact layer and links it to macroscopic properties of liquid/solid interfaces that are measured experimentally and that are relevant to wetting, hydrophobic solvation, nanofluidics, and osmotic transport.

6.
ACS Nano ; 18(39): 26522-26531, 2024 Oct 01.
Article in English | MEDLINE | ID: mdl-39283814

ABSTRACT

Interfaces can actively control the nucleation kinetics, orientations, and polymorphs of calcium carbonate (CaCO3). Prior studies have revealed that CaCO3 formation can be affected by the interplay between chemical functional moieties on solid-liquid or air-liquid interfaces as well as CaCO3's precursors and facets. Yet little is known about the roles of a liquid-liquid interface, specifically an oil-liquid interface, in directing CaCO3 mineralization which are common in natural and engineered systems. Here, by using in situ X-ray scattering techniques to locate a meniscus formed between water and a representative oil, isooctane, we successfully monitored CaCO3 formation at the pliable isooctane-water interface and systematically investigated the pivotal roles of the interface in the formation of CaCO3 (i.e., particle size, its spatial distribution with respect to the interface, and its mineral phase). Different from bulk solution, ∼5 nm CaCO3 nanoparticles form at the isooctane-water interface. They stably exist for a long time (36 h), which can result from interface-stabilized dehydrated prenucleation clusters of CaCO3. There is a clear tendency for enhanced amounts and faster crystallization of CaCO3 at locations closer to isooctane, which is attributed to a higher pH and an easier dehydration environment created by the interface and oil. Our study provides insights into CaCO3 nucleation at an oil-water interface, which can deepen our understanding of pliable interfaces interacting with CaCO3 and benefit mineral scaling control during energy-related subsurface operation.

7.
ACS Nano ; 18(39): 26435-26476, 2024 Oct 01.
Article in English | MEDLINE | ID: mdl-39288275

ABSTRACT

The burgeoning demands for health care and human-machine interfaces call for the next generation of multifunctional integrated sensor systems with facile fabrication processes and reliable performances. Laser-induced graphene (LIG) with highly tunable physical and chemical characteristics plays vital roles in developing versatile skin-like flexible or stretchable sensor systems. This Progress Report presents an in-depth overview of the latest advances in LIG-based techniques in the applications of flexible sensors. First, the merits of the LIG technique are highlighted especially as the building blocks for flexible sensors, followed by the description of various fabrication methods of LIG and its variants. Then, the focus is moved to diverse LIG-based flexible sensors, including physical sensors, chemical sensors, and electrophysiological sensors. Mechanisms and advantages of LIG in these scenarios are described in detail. Furthermore, various representative paradigms of integrated LIG-based sensor systems are presented to show the capabilities of LIG technique for multipurpose applications. The signal cross-talk issues are discussed with possible strategies. The LIG technology with versatile functionalities coupled with other fabrication strategies will enable high-performance integrated sensor systems for next-generation skin electronics.

8.
Adv Healthc Mater ; : e2402576, 2024 Sep 27.
Article in English | MEDLINE | ID: mdl-39328088

ABSTRACT

Transparent microelectrode arrays have proven useful in neural sensing, offering a clear interface for monitoring brain activity without compromising high spatial and temporal resolution. The current landscape of transparent electrode technology faces challenges in developing durable, highly transparent electrodes while maintaining low interface impedance and prioritizing scalable processing and fabrication methods. To address these limitations, we introduce artifact-resistant transparent MXene microelectrode arrays optimized for high spatiotemporal resolution recording of neural activity. With 60% transmittance at 550 nm, these arrays enable simultaneous imaging and electrophysiology for multimodal neural mapping. Electrochemical characterization shows low impedance of 563 ± 99 kΩ at 1 kHz and a charge storage capacity of 58 mC cm⁻² without chemical doping. In vivo experiments in rodent models demonstrate the transparent arrays' functionality and performance. In a rodent model of chemically-induced epileptiform activity, we tracked ictal wavefronts via calcium imaging while simultaneously recording seizure onset. In the rat barrel cortex, we recorded multi-unit activity across cortical depths, showing the feasibility of recording high-frequency electrophysiological activity. The transparency and optical absorption properties of Ti3C2Tx MXene microelectrodes enable high-quality recordings and simultaneous light-based stimulation and imaging without contamination from light-induced artifacts.

9.
Int Environ Agreem ; 24(2-3): 325-348, 2024.
Article in English | MEDLINE | ID: mdl-39347380

ABSTRACT

A new legally binding agreement for the conservation and sustainable use of marine biodiversity beyond national jurisdiction (BBNJ) was adopted by consensus on 19th June, 2023. Setting new regulations and filling regulatory gaps of the United Nations Convention on the Law of the Sea are expected to be informed by "best available science". It is critical to understand how science entered the negotiations, which defined the global scientific knowledge base of decision-makers. This paper presents various pathways over which scientific input entered the BBNJ negotiations, using empirical data, collected through collaborative event ethnography, including participant observation and semi-structured interviews at the BBNJ negotiation site. Results show that scientific input in the BBNJ negotiations was not systematic and transparent but dependent on (a) available national scientific capacity, (b) financial resources, (c) established contacts and (d) active involvement of actors. Results of the study call for formalised science-policy interfaces, initiated by the UN Secretariat to guarantee a global knowledge base for decision-making. Keywords: international negotiations; United Nations; marine biodiversity; BBNJ; ocean protection; science-policy interfaces. Supplementary Information: The online version contains supplementary material available at 10.1007/s10784-024-09642-0.

10.
Nano Lett ; 24(39): 12095-12101, 2024 Oct 02.
Article in English | MEDLINE | ID: mdl-39291849

ABSTRACT

Aqueous calcium ion batteries, promising for energy storage, are still challenged by very limited anode choices. Although a Zn metal anode is popular in aqueous batteries, interface instability due to incessant corrosion and severe Zn dendrites hinders its development. Here, an interphase layer with densely packed nanocrystals of Ca3(CO3)2(OH)2·1.5H2O and ZnF2, and amorphous organic species, is demonstrated for a Zn metal anode with 1 M calcium trifluoromethyl sulfonate aqueous electrolyte. The hybrid interface fully avoids direct Zn-H2O contact, maintains fast ion conductivity, and effectively prevents corrosion and dendrite growth. Therefore, the symmetric cell stably lasts for 1600 h at 0.5 mA cm-2 and 2.5 mAh cm-2, far superior to 150 h for the control cell. Furthermore, the device maintains 80% capacity retention after 700 cycles at 1 A g-1, outperforming 13% retention after 200 cycles for the control device. This work indicates that interface and interphase engineering is also crucial for aqueous batteries.

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