“…Group III nitride semiconductors have drawn considerable attention in the past few decades because of their outstanding properties that lead to a variety of applications in electronics and optoelectronics. − Among these semiconductor materials, gallium nitride (GaN) is the most studied target since it possesses many advantages of properties including high room-temperature electron mobility (∼10 3 cm 2 V –1 s –1 ), wide band gap (∼3.4 eV), and large short-wavelength absorption coefficient, which makes it an important semiconductor for device applications in light emitting diodes, field effect transistors, solar cells, lasers, photodetectors, and high-speed optoelectronic devices. − With the development trend of device minimization and integration, low-dimensional GaN nanomaterials such as nanowires, nanotubes, and nanosheets have attracted more and more interest due to the advantages of their structures and potential properties with respect to their bulk counterpart. − In particular, two-dimensional (2D) GaN materials are expected to be realized for optoelectronic applications due to the success of atomically thin graphene and transition metal dichalcogenides (TMDs). − Hence, great efforts are devoted to the synthesis of 2D GaN materials, and they have been synthesized experimentally with thicknesses from dozens of nanometers to several atomic layers. ,− However, the structure of 2D GaN is still under debate. It is widely acceptable that the ultrathin GaN nanosheets with the wurtzite (WZ) phase are unstable and tend to transform into a graphitic (GP) phase. , Recent theoretical studies have found that few-layer GaN nanosheets can reconstruct into a haeckelite (HK) phase with alternating octagonal and square rings. , Therefore, the understanding of size effect on fundamental structural and electronic properties of GaN nanosheets is essential for their device applications.…”