Semiconductors are the basis of many vital technologies such as electronics, computing, communications, optoelectronics, and sensing. Modern semiconductor technology can trace its origins to the invention of the point contact transistor in 1947. This demonstration paved the way for the development of discrete and integrated semiconductor devices and circuits that has helped to build a modern society where semiconductors are ubiquitous components of everyday life. A key property that determines the semiconductor electrical and optical properties is the bandgap. Beyond graphene, recently discovered two-dimensional (2D) materials possess semiconducting bandgaps ranging from the terahertz and mid-infrared in bilayer graphene and black phosphorus, visible in transition metal dichalcogenides, to the ultraviolet in hexagonal boron nitride. In particular, these 2D materials were demonstrated to exhibit highly tunable bandgaps, achieved via the control of layers number, heterostructuring, strain engineering, chemical doping, alloying, intercalation, substrate engineering, as well as an external electric field. We provide a review of the basic physical principles of these various techniques on the engineering of quasi-particle and optical bandgaps, their bandgap tunability, potentials and limitations in practical realization in future 2D device technologies.

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Bandgap engineering of two-dimensional semiconductor materials

Two-dimensional (2D) materials have attracted tremendous research interest since the breakthrough of graphene. Their unique optical, electronic, and mechanical properties hold great potential for harnessing them as key components in novel applications for electronics and optoelectronics. Their atomic thickness and exposed huge surface even make them highly designable and manipulable, leading to the extensive application potentials. What's more, after acquiring the qualification for being the candidate for next-generation devices, the assembly of 2D materials monomers into mass or ordered structure is also of great importance, which will determine their ultimate industrialization. By designing the monomers and regulating their assembling behavior, the exploration of 2D materials toward the next-generation circuits can be spectacularly achieved. In this review, we will first overview the emerging 2D materials and then offer a clear guideline of varied physical and chemical strategies for tuning their properties. Furthermore, assembly strategies of 2D materials will also be included. Finally, challenges and outlooks in this promising field are featured on the basis of its current progress.

Exploring Two-Dimensional Materials toward the Next-Generation Circuits: From Monomer Design to Assembly Control

Emerging in-plane anisotropic two-dimensional materials

Recent Advances in the Functional 2D Photonic and Optoelectronic Devices

Few-Layer Tin Sulfide: A Promising Black-Phosphorus-Analogue 2D Material with Exceptionally Large Nonlinear Optical Response, High Stability, and Applications in All-Optical Switching and Wavelength Conversion

We study the anisotropic electronic properties of two-dimensional (2D) SnS, an analogue of phosphorene, grown by physical vapor transport. With transmission electron microscopy and polarized Raman spectroscopy, we identify the zigzag and armchair directions of the as-grown 2D crystals. The 2D SnS field-effect transistors with a cross-Hall-bar structure are fabricated. They show heavily hole-doped (∼1019 cm–3) conductivity with strong in-plane anisotropy. At room temperature, the mobility along the zigzag direction exceeds 20 cm2 V–1 s–1, which can be up to 1.7 times that in the armchair direction. This strong anisotropy is then explained by the effective mass ratio along the two directions and agrees well with previous theoretical predictions. Temperature-dependent carrier density determined the acceptor energy level to be ∼45 meV above the valence band maximum. This value matches a calculated defect level of 42 meV for Sn vacancies, indicating that Sn deficiency is the main cause of the p-type conductivity.

Two-Dimensional SnS: A Phosphorene Analogue with Strong In-Plane Electronic Anisotropy.

We report the transport properties of mechanically exfoliated few-layer SnSe2 flakes, whose mobility is found to be ∼85 cm2 V−1 s−1 at 300 K, higher than those of the majority of few-layer transitional metal dichalcogenides. The mobility increases strongly with decreased temperature, indicating a phonon limited transport. The conductivity of the semiconducting SnSe2 shows a metallic behavior, which is explained by two competing factors involving the different temperature dependence of mobility and carrier density. The Fermi level is found to be 87 meV below the conduction band minima (CBM) at 300 K and 12 meV below the CBM at 78 K, resulting from a heavy n-type doping. Previous studies have found SnSe2 field-effect transistors to be very difficult to turn off. We find the limiting factor to be the flake thickness compared with the maximum depletion width. With fully depleted devices, we are able to achieve a current on-off ratio of ∼105. These results demonstrate the great potential of SnSe2 as a two dime...

Field-effect transistors of high-mobility few-layer SnSe2

Stacking order has a strong influence on the coupling between the two layers of twisted bilayer graphene (BLG), which in turn determines its physical properties. Here, we report the investigation of the interlayer coupling of the epitaxially grown single-crystal 30°-twisted BLG on Cu(111) at the atomic scale. The stacking order and morphology of BLG is controlled by a rationally designed two-step growth process, that is, the thermodynamically controlled nucleation and kinetically controlled growth. The crystal structure of the 30°-twisted bilayer graphene (30°-tBLG) is determined to have quasicrystal-like symmetry. The electronic properties and interlayer coupling of the 30°-tBLG are investigated using scanning tunneling microscopy and spectroscopy. The energy-dependent local density of states with in situ electrostatic doping shows that the electronic states in two graphene layers are decoupled near the Dirac point. A linear dispersion originated from the constituent graphene monolayers is discovered with doubled degeneracy. This study contributes to controlled growth of twist-angle-defined BLG and provides insights on the electronic properties and interlayer coupling in this intriguing system.

Interlayer Decoupling in 30° Twisted Bilayer Graphene Quasicrystal.

Two-dimensional (2D) materials with narrow band gaps (∼0.3 eV) are of great importance for realizing ambipolar transistors and mid-infrared (MIR) detections. However, most of the 2D materials studied to date have band gaps that are too large. A few of the materials with suitable band gaps are not stable under ambient conditions. In this study, the layered Nb2SiTe4 is shown to be a stable 2D material with a band gap of 0.39 eV. Field-effect transistors based on few-layer Nb2SiTe4 show ambipolar transport with a similar magnitude of electron and hole current and a high charge-carrier mobility of ∼100 cm2 V-1 s-1 at room temperature. Optoelectronic measurements of the devices show clear response to an MIR wavelength of 3.1 μm with a high responsivity of ∼0.66 AW-1. These results establish Nb2SiTe4 as a good candidate for ambipolar devices and MIR detection.

Nb2SiTe4: A Stable Narrow-Gap Two-Dimensional Material with Ambipolar Transport and Mid-Infrared Response.

Different two-dimensional (2D) materials, when combined together to form heterostructures, can exhibit exciting properties that do not exist in individual components. Therefore, intensive research efforts have been devoted to their fabrication and characterization. Previously, vertical and in-plane 2D heterostructures have been formed by mechanical stacking and chemical vapor deposition. Here, we report a new material system that can form in-plane p–n junctions by thermal conversion of n-type SnSe2 to p-type SnSe. Through scanning tunneling microscopy and density functional theory studies, we find that these two distinctively different lattices can form atomically sharp interfaces and have a type II to nearly type III band alignment. We also demonstrate that this method can be used to create micron-sized in-plane p–n junctions at predefined locations. These findings pave the way for further exploration of the intriguing properties of the SnSe2–SnSe heterostructure.

Zhen Tian

Papers

Two-Dimensional SnS: A Phosphorene Analogue with Strong In-Plane Electronic Anisotropy.

Field-effect transistors of high-mobility few-layer SnSe2

Interlayer Decoupling in 30° Twisted Bilayer Graphene Quasicrystal.

Nb2SiTe4: A Stable Narrow-Gap Two-Dimensional Material with Ambipolar Transport and Mid-Infrared Response.

Lateral Heterostructures Formed by Thermally Converting n-Type SnSe2 to p-Type SnSe