A novel
two-dimensional (2D) Ga2O3 monolayer
was constructed and systematically investigated by first-principles
calculations. The 2D Ga2O3 has an asymmetric
configuration with a quintuple-layer atomic structure, the same as
the well-studied α-In2Se3, and is expected
to be experimentally synthesized. The dynamic and thermodynamic calculations
show excellent stability properties of this monolayer material. The
relaxed Ga2O3 monolayer has an indirect band
gap of 3.16 eV, smaller than that of β-Ga2O3 bulk, and shows tunable electronic and optoelectronic properties
with biaxial strain engineering. An attractive feature is that the
asymmetric configuration spontaneously introduces an intrinsic dipole
and thus the electrostatic potential difference between the top and
bottom surfaces of the Ga2O3 monolayer, which
helps to separate photon-generated electrons and holes within the
quintuple-layer structure. By applying compressive strain, the Ga2O3 monolayer can be converted to a direct band
gap semiconductor with a wider gap reaching 3.5 eV. Also, enhancement
of hybridization between orbitals leads to an increase of electron
mobility, from the initial 5000 to 7000 cm2 V–1 s–1. Excellent optical absorption ability is confirmed,
which can be effectively tuned by strain engineering. With superior
stability, as well as strain-tunable electronic properties, carrier
mobility, and optical absorption, the studied novel Ga2O3 monolayer sheds light on low-dimensional electronic
and optoelectronic device applications.