As silicon-based transistors have approached their physical limits, it is urgent to explore alternative materials with a suitable bandgap and high mobility for next generation electronic logic devices. Two‐dimensional (2D) materials have attracted significant attention in the last few years due to their potential exotic transport physics and technological applications in various fields, such as a significant device downscaling for high intensity integration. Recently, a variety of 2D materials have been explored, including graphene [1] and transition metal dichalcogenides (TMDs), e.g., MoS2 [2,3], WS2 [4], and PtSe2 [5-7]. Although most research has focused on TMDs, recently 2D layered metal monochalcogenides, e.g., GaSe, have attracted increasing interest as a result of their unique electronic properties, making this class of materials different from TMDs.GaSe crystal structure comprises vertically stacked Ga-Se-Se-Ga layers with relatively weak van der Waals interactions. There are two main GaSe polytypes which differ in the stacking sequence of the basis layer units. Side- and top-view schematics of β‐GaSe and ε‐GaSe are shown in Fig. 1a. In this study, the electronic structure of both GaSe layered material polytypes is investigated using density functional theory (DFT) as implemented in QuantumATK [8]. Brillouin-zone integrations were performed according to the Monkhorst-Pack scheme [9] with a density of approximately 10 k-points per angstrom. Geometry optimizations were performed with the convergence criterion of 0.02 eV/Å [10]. Van der Waals (vdW) interactions improve the structural and electronic properties description obtained by DFT calculations and is included in our calculations through D3 version of Grimme’s dispersion corrections [11].To provide an improved determination of the bandgap energies, the GW (G: Green's function and W: screened Coulomb interaction) method in conjunction with a many body perturbation theory (MBPT) correction could be used. However, GW technique is computationally very expensive and could be implemented for systems with very limited number of atoms [12,13]. Hence, for this study, methods such as Heyd-Scuseria-Ernzerhof (HSE) hybrid functional [14,15] and GGA-1/2 [16] methods were included in our model to achieve more accurate bandgap compared to the experimental values. The β‐GaSe exhibits a DFT-obtained direct bandgap of ~1 eV while the corrected value is 2 eV. ε‐GaSe, however, shows slight indirect bandgap of 0.8 eV (DFT) and 1.7 eV (corrected), with just 25 meV difference between the indirect gap and indirect gap.A double-gate Schottky barrier field-effect transistor (FET) consisting of Ti source and drain contacts and ultrathin GaSe channel is also investigated. Schematic of the FET is shown in Fig. 1b. The device performance analysis such as current-voltage characteristics, subthreshold slope, and on/off ratio are carried out by means of non-equilibrium Green’s function together with DFT Hamiltonian [17]. The output characteristic of the proposed device exhibits an ON/OFF current ratio of more than 7 orders of magnitude.The presence of point defects in ultrathin 2D films is largely inevitable [18], even under optimized synthesis conditions, which can be either engineered and considered as a useful feature, or undesirable. In either case, understanding the impacts of point defects on the electronic structure of 2D materials are required to allow application-based optimization. In this talk, to provide insight into the defect-induced modifications to the GaSe electronic properties, in particular the properties of the states associated with the defects, we will compare the band-structure of the pristine GaSe with the band-structure of the GaSe with Ge and Se vacancies, for both GaSe polytypes.We have also fabricated back-gated devices by mechanically exfoliating ultrathin GaSe flakes from bulk crystal onto oxide-on-Si substrate. Fig. 1c shows an SEM image of the device. Our experimental results demonstrate the basic transport characteristics of thin-film transistor, which may offer more opportunities for potential applications such as photodetectors, gas sensors, and optoelectronic devices, in addition to nanoelectronics FETs, due to GaSe large bandgap.