Enhanced photocurrent in heterostructures formed between CH₃NH₃PbI₃ perovskite films and graphdiyne

Extending photoabsorption to the near-infrared region (NIR) of the spectrum remains a major challenge for the enhancement of the photoelectric performance of perovskites. In this work, we propose a model of van der Waals heterostructures formed by CH3NH3PbI3 perovskite films and graphdiyne (GDY) to improve the photocurrent in the NIR. To obtain better insights into the properties of GDY/perovskite heterostructures, we first determine its electronic properties using the first principles calculations. The charge transfer between GDY and perovskites leads to a built-in electrical field that facilitates the separation and the transport of the photogenerated carriers. Then, the non-equilibrium Green's function (NEGF) is used to calculate the photocurrents of perovskite slabs with and without GDY. The photocurrents of GDY/perovskite heterostructures are nearly an order of magnitude larger than that of pristine perovskites in NIR due to the synergistic effect between GDY and perovskites. Furthermore, a polarization-sensitive photocurrent is obtained for a GDY/PbI2 heterostructure.