Giant bulk photovoltaic effect driven by the wall-to-wall charge shift in WS2 nanotubes

Abstract

The intrinsic light-matter characteristics of transition-metal dichalcogenides have not only been of great scientific interest but have also provided novel opportunities for the development of advanced optoelectronic devices. Among the family of transition-metal dichalcogenide structures, the one-dimensional nanotube is particularly attractive because it produces a spontaneous photocurrent that is prohibited in its higher-dimensional counterparts. Here, we show that WS2 nanotubes exhibit a giant shift current near the infrared region, amounting to four times the previously reported values in the higher frequency range. The wall-to-wall charge shift constitutes a key advantage of the one-dimensional nanotube geometry, and we consider a Janus-type heteroatomic configuration that can maximize this interwall effect. To assess the nonlinear effect of a strong field and the nonadiabatic effect of atomic motion, we carried out direct real-time integration of the photoinduced current using time-dependent density functional theory. Our findings provide a solid basis for a complete quantum mechanical understanding of the unique light-matter interaction hidden in the geometric characteristics of the reduced dimension. We demonstrate that double-wall or multi-wall WS2 nanotubes can exhibit unexpectedly efficient bulk photovoltaic effect owing to its unique inter-wall charge-shifting excitations.