Upconversion Photovoltaic Effect of WS2/2D Perovskite Heterostructures by Two-Photon Absorption

Photovoltaic devices work by converting sunlight energy into electric energy. The efficiency of current photovoltaic devices, however, is significantly limited by the transmission loss of photons with energies below the bandgap of channel semiconductors, which can be circumvented by photon energy upconversion. Energy upconversion has been widely employed to improve the efficiency of traditional solar cells. However, the employment of energy upconversion in two-dimensional (2D) heterostructure photovoltaic devices has not been investigated yet. Here, we report the upconversion photovoltaic effect of WS₂ monolayer/(C₆H₅C₂H₄NH₃)₂PbI₄ (PEPI) 2D perovskite heterostructures by below-bandgap two-photon absorption via a virtual intermediate state. An open circuit voltage of 0.37 V and short circuit current of 7.4 pA are obtained with a photoresponsivity of 771 pA/W and current on/off ratio of 130:1. This work demonstrates that upconversion by two-photon absorption may potentially be a strategy for boosting the efficiency of 2D material-based photovoltaic devices by virtue of the absorption of photons below the bandgap energy of channel semiconductors.