Ab initio Nonadiabatic Dynamics of Semiconductor Nanomaterials via Surface Hopping Method

Photoinduced carrier dynamic processes are without doubt the main driving force responsible for the efficient performance of semiconductor nano-materials in applications like photoconversion and photonics. Nevertheless, establishing theoretical insights into these processes is computationally challenging owing to the multiple factors involved in the processes, namely reaction rate, material surface area, material composition etc. Modelling of photoinduced carrier dynamic processes can be performed via nonadiabatic molecular dynamics (NA-MD) methods, which are methods specifically designed to solve the time-dependent Schrodinger equation with the inclusion of nonadiabatic couplings. Among NA-MD methods, surface hopping methods have been proven to be a mighty tool to mimic the competitive nonadiabatic processes in semiconductor nanomaterials, a worth noticing feature is its exceptional balance between accuracy and computational cost. Consequently, surface hopping is the method of choice for modelling ultrafast dynamics and more complex phenomena like charge separation in Janus transition metal dichalcogenides-based van der Waals heterojunction materials. Covering latest state-of-the-art numerical simulations along with experimental results in the field, this review aims to provide a basic understanding of the tight relation between semiconductor nanomaterials and the proper simulation of their properties via surface hopping methods. Special stress is put on emerging state-ot-the-art techniques. By highlighting the challenge imposed by new materials, we depict emerging creative approaches, including high-level electronic structure methods and NA-MD methods to model nonadiabatic systems with high complexity.