2D ferroelectric material has emerged as an attractive building block for highdensity data storage nanodevices. Although monolayer van der Waals ferroelectrics have been theoretically predicted, a key experimental breakthrough for such calculations is still not realized. Here, hexagonally stacking α-In 2 Se 3 nanoflake, a rarely studied van der Waals polymorph, is reported to exhibit out-of-plane (OOP) and in-plane (IP) ferroelectricity at room temperature. Ferroelectric multidomain states in a hexagonal α-In 2 Se 3 nanoflake with uniform thickness can survive to 6 nm. Most strikingly, the electric-field-induced polarization switching and hysteresis loop are, respectively, observed down to the bilayer and monolayer (≈1.2 nm) thicknesses, which designates it as the thinnest layered ferroelectric and verifies the corresponding theoretical calculation. In addition, two types of ferroelectric nanodevices employing the OOP and IP polarizations in 2H α-In 2 Se 3 are developed, which are applicable for nonvolatile memories and heterostructure-based nanoelectronics/ optoelectronics.

Defect engineering represents a significant approach for atomically thick 2D semiconductor material development to explore the unique material properties and functions. Doping‐induced conversion of conductive polarity is particularly beneficial for optimizing the integration of layered electronics. Here, controllable doping behavior in palladium diselenide (PdSe2) transistor is demonstrated by manipulating its adatom‐vacancy groups. The underlying mechanisms, which originate from reversible adsorption/desorption of oxygen clusters near selenide vacancy defects, are investigated systematically via their dynamic charge transfer characteristics and scanning tunneling microscope analysis. The modulated doping effect allows the PdSe2 transistor to emulate the essential characteristics of photo nociceptor on a device level, including firing signal threshold and sensitization. Interestingly, electrostatic gating, acting as a neuromodulator, can regulate the adaptive modes in nociceptor to improve its adaptability and perceptibility to handle different danger levels. An integrated artificial nociceptor array is also designed to execute unique image processing functions, which suggests a new perspective for extension of the promise of defect engineered 2D electronics in simplified sensory systems toward use in advanced humanoid robots and artificial visual sensors.

The human brain is often likened to an incredibly complex and intricate computer, rather than electrical devices, consisting of billions of neuronal cells connected by synapses. Different brain circuits are responsible for coordinating and performing specific functions. The reward pathway of the synaptic plasticity in the brain is strongly related to the features of both drug addiction and relief. In the current study, a synaptic device based on layered hafnium disulfide (HfS2) is developed for the first time, to emulate the behavioral mechanisms of drug dosage modulation for neuroplasticity. A strong gate‐dependent persistent photocurrent is observed, arising from the modulation of substrate‐trapping events. By controlling the polarity of gate voltage, the basic functions of biological synapses are realized under a range of light spiking conditions. Furthermore, under the control of detrapping/trapping events at the HfS2/SiO2 interface, positive/negative correlations of the An/A1 index, which significantly reflected the weight change of synaptic plasticity, are realized under the same stimulation conditions for the emulation of the drug‐related addition/relief behaviors in the brain. The findings provide a new advance for mimicking human brain plasticity.

The oxygen (O 2 )-dependent resistance change of multilayered molybdenum ditelluride (MoTe 2 ) channels was characterized. A variation of the channel resistance could reproducibly determine relative O 2 content (denoted as the O 2 index). We found that Joule heating in a layered MoTe 2 field-effect transistor caused the O 2 index to decrease drastically from 100 to 12.1% in back gate modulation. Furthermore, Joule heating caused effective O 2 desorption from the MoTe 2 surface and repeatable O 2 detection by multilayered MoTe 2 channels was realized. This work not only explored the influence of O 2 on the electrical properties of multilayered MoTe 2 channels but also revealed that MoTe 2 channels are promising for sensing O 2 in an environmental condition.