Intercalated Architecture of the Ca2A2Z5 Monolayer with High Electron Mobilities and High Power Conversion Efficiencies

The exploration of novel two-dimensional (2D) materials with a direct band gap and high mobility has attracted huge attention due to their potential application in electronic and optoelectronic devices. Here, we propose a feasible way to construct multiatomic monolayer Ca2A2Z5 (A = Al and Ga and Z = S, Se, and Te) by first-principles calculations. Our results indicated that the energies of α1-phase Ca2A2Z5 are slightly lower than those of experimentally synthesized α3-phase-like Ca2A2Z5 monolayers with excellent structural stability. Moreover, the α1- and α3-phase Ca2A2Z5 monolayers possess not only direct band gaps but also high electron mobilities (up to ∼103 cm2 V–1 s–1), demonstrating an intriguing range of visible light absorption. Importantly, α1- and α3-phase Ca2Ga2Se5 monolayers are good donor materials, and the corresponding Ca2Ga2Se5/ZrSe2 type-II heterostructures exhibit desirable power conversion efficiencies of 22.4% and 22.9%, respectively. Our findings provide a feasible way to explore new 2D materials and offer several Ca2A2Z5 candidate monolayers for the application of high-performance solar cells.