Ternary metal-oxy-chalcogenides are emerging as next-generation layered semiconductors beyond binary metal-chalcogenides (i.e., MoS 2 ). Among ternary metal-oxy-chalcogenides, especially Bi 2 O 2 Se has been demonstrated in field-effect transistors and photodetectors, exhibiting ultrahigh performance with robust air stability. The growth method for Bi 2 O 2 Se that has been reported so far is a powder sublimation based chemical vapor deposition. The first step for pursuing the practical application of Bi 2 O 2 Se as a semiconductor material is developing a gas-phase growth process. Here, we report a cracking metal−organic chemical vapor deposition (c-MOCVD) for the gas-phase growth of Bi 2 O 2 Se. The resulting Bi 2 O 2 Se films at very low growth temperature (∼300 °C) show single-crystalline quality. By taking advantage of the gas-phase growth, the precise phase control was demonstrated by modulating the partial pressure of each precursor. In addition, c-MOCVD-grown Bi 2 O 2 Se exhibits outstanding electrical and optoelectronic performance at room temperature without passivation, including maximum electron mobility of 127 cm 2 /(V•s) and photoresponsivity of 45134 A/W.

Layered materials that do not form a covalent bond in a vertical direction can be prepared in a few atoms to one atom thickness without dangling bonds. This distinctive characteristic of limiting thickness around the sub-nanometer level allowed scientists to explore various physical phenomena in the quantum realm. In addition to the contribution to fundamental science, various applications were proposed. Representatively, they were suggested as a promising material for future electronics. This is because (i) the dangling-bond-free nature inhibits surface scattering, thus carrier mobility can be maintained at sub-nanometer range; (ii) the ultrathin nature allows the short-channel effect to be overcome. In order to establish fundamental discoveries and utilize them in practical applications, appropriate preparation methods are required. On the other hand, adjusting properties to fit the desired application properly is another critical issue. Hence, in this review, we first describe the preparation method of layered materials. Proper growth techniques for target applications and the growth of emerging materials at the beginning stage will be extensively discussed. In addition, we suggest interlayer engineering via intercalation as a method for the development of artificial crystal. Since infinite combinations of the host–intercalant combination are possible, it is expected to expand the material system from the current compound system. Finally, inevitable factors that layered materials must face to be used as electronic applications will be introduced with possible solutions. Emerging electronic devices realized by layered materials are also discussed.

Advances in large‐area and high‐quality 2D transition metal dichalcogenides (TMDCs) growth are essential for semiconductor applications. Here, the gas‐phase alkali metal‐assisted metal‐organic chemical vapor deposition (GAA‐MOCVD) of 2D TMDCs is reported. It is determined that sodium propionate (SP) is an ideal gas‐phase alkali‐metal additive for nucleation control in the MOCVD of 2D TMDCs. The grain size of MoS2 in the GAA‐MOCVD process is larger than that in the conventional MOCVD process. This method can be applied to the growth of various TMDCs (MoS2, MoSe2, WSe2, and WSe2) and the generation of large‐scale continuous films. Furthermore, the growth behaviors of MoS2 under different SP and oxygen injection time conditions are systematically investigated to determine the effects of SP and oxygen on nucleation control in the GAA‐MOCVD process. It is found that the combination of SP and oxygen increases the grain size and nucleation suppression of MoS2. Thus, the GAA‐MOCVD with a precise and controllable supply of a gas‐phase alkali metal and oxygen allows achievement of optimum growth conditions that maximizes the grain size of MoS2. It is expected that GAA‐MOCVD can provide a way for batch fabrication of large‐scale atomically thin electronic devices based on 2D semiconductors.

Van der Waals (vdW) heterostructures have drawn much interest over the last decade owing to their absence of dangling bonds and their intriguing low‐dimensional properties. The emergence of 2D materials has enabled the achievement of significant progress in both the discovery of physical phenomena and the realization of superior devices. In this work, the group IV metal chalcogenide 2D‐layered Ge4Se9 is introduced as a new selection of insulating vdW material. 2D‐layered Ge4Se9 is synthesized with a rectangular shape using the metalcorganic chemical vapor deposition system using a liquid germanium precursor at 240 °C. By stacking the Ge4Se9 and MoS2, vdW heterostructure devices are fabricated with a giant memory window of 129 V by sweeping back gate range of ±80 V. The gate‐independent decay time reveals that the large hysteresis is induced by the interfacial charge transfer, which originates from the low band offset. Moreover, repeatable conductance changes are observed over the 2250 pulses with low non‐linearity values of 0.26 and 0.95 for potentiation and depression curves, respectively. The energy consumption of the MoS2/Ge4Se9 device is about 15 fJ for operating energy and the learning accuracy of image classification reaches 88.3%, which further proves the great potential of artificial synapses.

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