DielectricBreakdown of 2D Hybrid Organic–InorganicPerovskites

Our knowledge about dielectric breakdown of 2D hybrid organic–inorganic perovskites (HOIPs) is limited, although the breakdown is widely observed and harnessed for new device applications. Here, we investigate the out-of-plane breakdown of a benchmark 2D HOIP family, (BA)₂MA_<i>n</i>–1Pb_<i>n</i>I_3<i>n</i>+1 (BA = butylammonium, MA = methylammonium, and <i>n</i> = 1–5), by conductive atomic force microscopy. Unlike conventional 2D materials, 2D HOIPs manifest milder breakdown morphologies, no clear trend of layer-by-layer damages, and stochastic characteristics of defect percolation, likely due to their low in-plane vs out-of-plane anisotropy. The influence of thickness, ramping rate, and <i>n</i> on the breakdown strength (<i>E</i>_BD) is evaluated, which is on the order of 10⁸ V/m, showing the intrinsic resilience of 2D HOIPs to breakdown and their potential as dielectric materials for 2D electronics. These results delineate the dielectric breakdown process in 2D HOIPs and provide indispensable insights into the electrical failure of 2D HOIPs in devices.