A strategy for boosting photovoltaic performance based on a two-dimensional ZrSSe/HfSSe van der Waals heterostructure

Identifying high-efficiency solar photovoltaic systems with two-dimensional (2D) materials is still an urgent challenge to meet modern energy requirements. Very recently, a 2D heterostructure with type-II band alignment has been confirmed to be more favorable for application in photoelectric conversion. However, the staggered band offset of 2D type-II heterostructures cannot always be guaranteed, nor the intrinsic hindrance mechanism of carrier recombination being clear. In this study, taking the emerging ZrSSe/HfSSe van der Waals heterostructure (vdWH) as a generic example, a boosting strategy for improving the photoelectric performances of 2D vdWHs is proposed. Through a series of in-depth systematic research studies based on first-principles, we demonstrate that via applying a vertical strain, an anticipated band alignment transition from type-I to favorable type-II of this ZrSSe/HfSSe vdWH can be induced due to the interfacial charge redistribution, during which a corresponding enlarged photocurrent can be detected from the latter based device compared to the former. Essentially, such enhanced photocurrent at the incident photon energy (E_ph) around the band gap is attributed to the suppressed recombination rate of photoexcited carriers. Moreover, when E_ph is increased into the visible light region, the photoelectric conversion performances can be further controlled by vertical strain. These generalized findings not only provide an effective manipulation strategy for enhancing the performances of 2D solar photovoltaic systems, but the intrinsic physical mechanism can also be extended to the next practical design and regulation of other 2D photovoltaic devices.