First-principles calculation of ballistic current from electron-hole interaction
Zhenbang Dai, Andrew M. Rappe
Abstract
The bulk photovoltaic effect (BPVE) has attracted increasing interest due to its potential to overcome the efficiency limit of traditional photovoltaics, and much effort has been devoted to understanding its underlying physics. However, previous work has shown that theoretical models of the shift current and the phonon-assisted ballistic current in real materials do not fully account for the experimental BPVE photocurrent, so other mechanisms should be investigated in order to obtain a complete picture of BPVE. In this paper, we demonstrate two approaches that enable the ab initio calculation of the ballistic current originating from the electron-hole interaction in semiconductors. Using ${\mathrm{BaTiO}}_{3}$ and monolayer ${\mathrm{MoS}}_{2}$ as two examples, we show clearly that for them the asymmetric scattering from an electron-hole interaction is less appreciable than that from an electron-phonon interaction, indicating more scattering processes need to be included to further improve the BPVE theory. Moreover, we provide a first-principles approach for material prediction and design in order to search for materials with a larger ballistic current due to electron-hole interactions.