Imprinting vision as memory is a core attribute of human cognitive learning. Fundamental to artificial intelligence systems are bioinspired neuromorphic vision components for the visible and invisible segments of the electromagnetic spectrum. Realization of a single imaging unit with a combination of in‐built memory and signal processing capability is imperative to deploy efficient brain‐like vision systems. However, the lack of a platform that can be fully controlled by light without the need to apply alternating polarity electric signals has hampered this technological advance. Here, a neuromorphic imaging element based on a fully light‐modulated 2D semiconductor in a simple reconfigurable phototransistor structure is presented. This standalone device exhibits inherent characteristics that enable neuromorphic image pre‐processing and recognition. Fundamentally, the unique photoresponse induced by oxidation‐related defects in 2D black phosphorus (BP) is exploited to achieve visual memory, wavelength‐selective multibit programming, and erasing functions, which allow in‐pixel image pre‐processing. Furthermore, all‐optically driven neuromorphic computation is demonstrated by machine learning to classify numbers and recognize images with an accuracy of over 90%. The devices provide a promising approach toward neurorobotics, human–machine interaction technologies, and scalable bionic systems with visual data storage/buffering and processing.

Atomically thin materials face an ongoing challenge of scalability, hampering practical deployment despite their fascinating properties. Tin monosulfide (SnS), a low‐cost, naturally abundant layered material with a tunable bandgap, displays properties of superior carrier mobility and large absorption coefficient at atomic thicknesses, making it attractive for electronics and optoelectronics. However, the lack of successful synthesis techniques to prepare large‐area and stoichiometric atomically thin SnS layers (mainly due to the strong interlayer interactions) has prevented exploration of these properties for versatile applications. Here, SnS layers are printed with thicknesses varying from a single unit cell (0.8 nm) to multiple stacked unit cells (≈1.8 nm) synthesized from metallic liquid tin, with lateral dimensions on the millimeter scale. It is reveal that these large‐area SnS layers exhibit a broadband spectral response ranging from deep‐ultraviolet (UV) to near‐infrared (NIR) wavelengths (i.e., 280–850 nm) with fast photodetection capabilities. For single‐unit‐cell‐thick layered SnS, the photodetectors show upto three orders of magnitude higher responsivity (927 A W−1) than commercial photodetectors at a room‐temperature operating wavelength of 660 nm. This study opens a new pathway to synthesize reproduceable nanosheets of large lateral sizes for broadband, high‐performance photodetectors. It also provides important technological implications for scalable applications in integrated optoelectronic circuits, sensing, and biomedical imaging.

Narrow spectral sensitivity in materials is one of the crucial challenges to develop high-performance broadband photodetectors. Here, we design a heterostructure of two-dimensional molybdenum disulfide (MoS2) and epitaxial gallium nitride (GaN) films to create an enhanced spectral absorption profile. This combination utilizes complementary optical absorption of MoS2 (visible) and GaN (UV) driven by type II band alignment at their interface to showcase highly sensitive photodetectors spanning across the UV–NIR regime. Concurrently, the heterostructure exhibits significantly enhanced responsivity (order of 104 A/W) and external quantum efficiency that are 500% higher than the bare GaN photodetectors. Given the available scalable synthesis approaches that have now been designed by the research community for both constituent materials, the demonstration of this heterostructure as a broadband photodetector with high figures-of-merit opens opportunities in designing efficient optoelectronic junctions and imaging applications.

High dielectric constant (high-k) ultrathin films are required as insulating gate materials. The well-known high-k dielectrics, including HfO2, ZrO2, and SrTiO3, feature three-dimensional lattice structures and are thus not easily obtained in the form of distinct ultrathin sheets. Therefore, their deposition as ultrathin layers still imposes challenges for electronic industries. Consequently, new high-k nanomaterials with k in the range of 40 to 100 and a band gap exceeding 4 eV are highly sought after. Antimony oxide nanosheets appear as a potential candidate that could fulfill these characteristics. Here, we report on the stoichiometric cubic polymorph of 2D antimony oxide (Sb2O3) as an ideal high-k dielectric sheet that can be synthesized via a low-temperature, substrate-independent, and silicon-industry-compatible liquid metal synthesis technique. A bismuth–antimony alloy was produced during the growth process. Preferential oxidation caused the surface of the melt to be dominated by α-Sb2O3. This ultrathin α-Sb2O3 was then deposited onto desired surfaces via a liquid metal print transfer. A tunable sheet thickness between ∼1.5 and ∼3 nm was achieved, while the lateral dimensions were within the millimeter range. The obtained α-Sb2O3 exhibited high crystallinity and a wide band gap of ∼4.4 eV. The relative permittivity assessment revealed a maximum k of 84, while a breakdown electric field of ∼10 MV/cm was observed. The isolated 2D α-Sb2O3 nanosheets were utilized in top-gated field-effect transistors that featured low leakage currents, highlighting that the obtained material is a promising gate oxide for conventional and van der Waals heterostructure-based electronics.

Wide bandgap semiconducting oxides are emerging as potential 2D materials for transparent electronics and optoelectronics. This fuels the quest for discovering new 2D metal oxides with ultrahigh transparency and high mobility. While the former can be achieved by reducing the thickness of oxide films to only a few nanometers, the latter is more commonly realized by intentional doping. This article reports a one‐step synthesis of few‐unit‐cell‐thick and laterally large antimony‐doped indium oxide (IAO). The doping process occurs spontaneously when the oxide is grown on the surface of a molten Sb–In alloy and 2D IAO nanosheets can be easily printed onto desired substrates. With thicknesses at the atomic scale, these materials exhibit excellent transparency exceeding 98% across the visible and near‐infrared range. Field‐effect transistors based on low‐doped IAO nanosheets reveal a high electron mobility of ≈40 cm2 V−1 s−1. Additionally, a notable photoresponse is observed in 2D IAO‐based photodetectors under ultraviolet (UV) radiation. Photoresponsivities of low‐doped and highly doped IAO at a wavelength of 285 nm are found to be 1.2 × 103 and 0.7 × 103 A W−1, respectively, identifying these materials as promising candidates for the fabrication of high‐performance optoelectronics in the UV region.