Perovskite superlattices with efficient carrier dynamics

Compared with their three-dimensional (3D) counterparts, low-dimensional metal halide perovskites (2D and quasi-2D; B₂A_n-1M_nX_3n+1, such as B = R-NH₃⁺, A = HC(NH₂)₂⁺, Cs⁺; M = Pb²⁺, Sn²⁺; X = Cl^-, Br^-, I^-) with periodic inorganic-organic structures have shown promising stability and hysteresis-free electrical performance^1-6. However, their unique multiple-quantum-well structure limits the device efficiencies because of the grain boundaries and randomly oriented quantum wells in polycrystals⁷. In single crystals, the carrier transport through the thickness direction is hindered by the layered insulating organic spacers⁸. Furthermore, the strong quantum confinement from the organic spacers limits the generation and transport of free carriers^9,10. Also, lead-free metal halide perovskites have been developed but their device performance is limited by their low crystallinity and structural instability¹¹. Here we report a low-dimensional metal halide perovskite BA₂MA_n-1Sn_nI_3n+1 (BA, butylammonium; MA, methylammonium; n = 1, 3, 5) superlattice by chemical epitaxy. The inorganic slabs are aligned vertical to the substrate and interconnected in a criss-cross 2D network parallel to the substrate, leading to efficient carrier transport in three dimensions. A lattice-mismatched substrate compresses the organic spacers, which weakens the quantum confinement. The performance of a superlattice solar cell has been certified under the quasi-steady state, showing a stable 12.36% photoelectric conversion efficiency. Moreover, an intraband exciton relaxation process may have yielded an unusually high open-circuit voltage (V_OC).