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Two-dimensional heterostructures (2D HSs) have emerged as a new class of materials where dissimilar 2D materials are combined to synergise their advantages and alleviate shortcomings. Such a combination of dissimilar components into 2D HSs offers fascinating properties and intriguing functionalities attributed to the newly formed heterointerface of constituent components. Understanding the nature of the surface and the complex heterointerface of HSs at the atomic level is crucial for realising the desired properties, designing innovative 2D HSs, and ultimately unlocking their full potential for practical applications. Therefore, this review provides the recent progress in the field of 2D HSs with a focus on the discussion of the fundamentals and the chemistry of heterointerfaces based on van der Waals (vdW) and covalent interactions. It also explains the challenges associated with the scalable synthesis and introduces possible methodologies to produce large quantities with good control over the heterointerface. Subsequently, it highlights the specialised characterisation techniques to reveal the heterointerface formation, chemistry and nature. Afterwards, we give an overview of the role of 2D HSs in various emerging applications, particularly in high-power batteries, bifunctional catalysts, electronics, and sensors. In the end, we present conclusions with the possible solutions to the associated challenges with the heterointerfaces and potential opportunities that can be adopted for innovative applications.

Liquid metals (LMs) are emerging as unique fluids for a variety of applications, but their nanoscale solvation properties remain largely understudied. In this work, a combination of atomic force microscopy (AFM) and molecular dynamics (MD) simulations are used to investigate the structure of the interface between the bulk room temperature liquid metal (RTLM) and the LM oxide in nanodroplet systems of gallium, EGaIn (75.5% gallium, 24.5% indium), and Galinstan (68.5% gallium, 21.5% indium, 10% tin). Field's metal (51% indium, 32.5% bismuth, 16.5% tin) is also investigated, which melts at ≈62 °C, as a contrast to the other systems. AFM measurements reveal distinct sub‐oxide nanostructured layering in all three RTLM systems, and Field's metal above the melting point, to differing degrees. EGaIn and Galinstan show multiple penetration events between 20 and 30 nm, with smaller, less complex events in Ga. MD simulations suggest that this layering is a result of the near‐surface ordering of LM atoms beneath the oxide layer. Importantly, the atoms in this region do not behave as solids but are more ordered than in a pure disordered liquid system. The surface nanostructure elucidated here significantly expands the understanding of LM systems and their behavior at interfaces. [ABSTRACT FROM AUTHOR]

Liquid metal nanodroplets are an emerging class of underexplored materials with significant potential in many applications, including catalysis, bio‐therapeutics, and phase‐change materials. These nanostructures are generally synthesized by mechanical agitation via ultrasonication of low‐melting metals like Ga. Once these materials are successfully synthesized, they can be suspended in a vast array of different solvents. However, one major issue arises specifically with liquid metal alloys which are found to de‐alloy in the sonication process. Here, it is demonstrated that this challenge can be overcome by undertaking sonication at high temperatures, suspending nanodroplets within molten sodium acetate (NaOAc). After cooling, the nanostructures become planet‐like nanodroplets which are covered by an interfacial oxide crust, feature a liquid metal mantle, and a solid core. The molten salt solvent can effectively be removed rendering this approach to be ideal, especially for catalysts. The proof‐of‐concept application is demonstrated by carrying out electrocatalytic ethanol oxidation, using the Cu–Ga system. The superior performance of the Cu–Ga nanodroplets highlights potential in catalyzing a vast array of reactions. Aside from the Cu–Ga system, this facile process can be applied to multiple other systems, including Ag–Ga, Zn–Ga, Bi–Ga, In–Cu, and Sn–Cu. [ABSTRACT FROM AUTHOR]

Crystallization of alloys from a molten state is a fundamental process underpinning metallurgy. Here the direct imaging of an intermetallic precipitation reaction at equilibrium in a liquid‐metal environment is demonstrated. It is shown that the outer layers of a solidified intermetallic are surprisingly unstable to the depths of several nanometers, fluctuating between a crystalline and a liquid state. This effect, referred to herein as crystal interface liquefaction, is observed at remarkably low temperatures and results in highly unstable crystal interfaces at temperatures exceeding 200 K below the bulk melting point of the solid. In general, any liquefaction process would occur at or close to the formal melting point of a solid, thus differentiating the observed liquefaction phenomenon from other processes such as surface pre‐melting or conventional bulk melting. Crystal interface liquefaction is observed in a variety of binary alloy systems and as such, the findings may impact the understanding of crystallization and solidification processes in metallic systems and alloys more generally. [ABSTRACT FROM AUTHOR]

Simple solution-based processes to generate pinhole-free bismuth iodide (BiI3) thin films with large, interconnected crystal grains have remained elusive. Here, a survey of the solvent systems for BiI3 is conducted. Using a novel binary solvent doping approach to carefully regulate the crystallization kinetics, we generate high-quality BiI3 thin films. Our method circumvents the current requirement for unreliable postprocessing techniques such as solvent vapor annealing or antisolvent dripping. Investigations reveal that 2-methoxyethanol doped with small amounts of N-methyl-2-pyrrolidone (NMP) is the ideal combination of parent and dopant solvent providing high vapor pressure and the intermediate coordination strength necessary to successfully achieve large grain formation in a single step. To evaluate optoelectronic performance, we integrated our optimized thin films into lithographically patterned lateral photodetectors (PDs). Our PD devices show fast millisecond response times, record responsivities of ∼1.61 A/W at moderate device bias (5 V), and excellent sensitivity, with detectivity reaching 1.9 × 1012 cm Hz1/2 W–1 (Jones). The high-quality BiI3 semiconductor thin films outlined here, coupled with their ease of fabrication, enhance the development of BiI3 optoelectronic devices and also serve as excellent template films for the fabrication of related bismuth perovskite materials. [ABSTRACT FROM AUTHOR]

Miniaturization and energy consumption by computational systems remain major challenges to address. Optoelectronics based synaptic and light sensing provide an exciting platform for neuromorphic processing and vision applications offering several advantages. It is highly desirable to achieve single‐element image sensors that allow reception of information and execution of in‐memory computing processes while maintaining memory for much longer durations without the need for frequent electrical or optical rehearsals. In this work, ultra‐thin (<3 nm) doped indium oxide (In2O3) layers are engineered to demonstrate a monolithic two‐terminal ultraviolet (UV) sensing and processing system with long optical state retention operating at 50 mV. This endows features of several conductance states within the persistent photocurrent window that are harnessed to show learning capabilities and significantly reduce the number of rehearsals. The atomically thin sheets are implemented as a focal plane array (FPA) for UV spectrum based proof‐of‐concept vision system capable of pattern recognition and memorization required for imaging and detection applications. This integrated light sensing and memory system is deployed to illustrate capabilities for real‐time, in‐sensor memorization, and recognition tasks. This study provides an important template to engineer miniaturized and low operating voltage neuromorphic platforms across the light spectrum based on application demand. [ABSTRACT FROM AUTHOR]

The structural characteristics of biological specimens, such as wet proteins and fixed living cells, can be conveniently probed in their host aqueous media using soft X‐rays in the water window region (200–600 eV). Conventional X‐ray detectors in this area exhibit low spatial resolution, have limited sensitivity, and require complex fabrication procedures. Here, many of these limitations are overcome by introducing a direct soft X‐ray detector based on ultrathin tin mono‐sulfide (SnS) nanosheets. The distinguishing characteristic of SnS is its high photon absorption efficiency in the soft X‐ray region. This factor enables the fabricated soft X‐ray detectors to exhibit excellent sensitivity values on the order of 104 μCGyVac−1 cm−2 at peak energies of ≈600 eV. The peak signal is found to be sensitive to the number of stacked SnS layers, with thicker SnS nanosheet assemblies yielding a peak response at higher energies and with peak sensitives of over 2.5 × 104 μCGyVac−1 cm−2 at 1 V. Detailed current–voltage and temporal characteristics of these detectors are also presented. These results showcase the excellent performance of SnS nanosheet‐based soft X‐ray detectors compared to existing direct soft X‐ray detectors, including that of the emerging organic–inorganic perovskite class of materials. [ABSTRACT FROM AUTHOR]